WorldWideScience

Sample records for negatively charged excitons

  1. Size Effect of a Negatively Charged Exciton in a Two-Dimensional Quantum Dot

    Institute of Scientific and Technical Information of China (English)

    LIU Chao; XIE Wen-Fang

    2009-01-01

    In this paper we study a negatively charged exciton (NCE), which is trapped by a two-dimensional (2D) parabolic potential.By using matrix diagonalization techniques, the correlation energies of the low-lying states with L = O, 1, and 2 are calculated as a function of confinement strength.We find that the size effects of different states are different.This phenomenon can be explained as a hidden symmetry, which is originated purely from symmetry.Based on symmetry, the features of the low-lying states are discussed in the influence of the 2D parabolic potential well.It is found that the confinement may cause accidental degeneracies between levels with different low-excited states.It is shown that the effect of quantum confinement on the binding energy of the heavy hole is stronger than that of a light hole.

  2. Charged-Exciton Complexes in Quantum Dots

    Institute of Scientific and Technical Information of China (English)

    XIE Wen-Fang

    2001-01-01

    It is known experimentally that stable charged-exciton complexes can exist in low-dimensional semiconductor nanostructures. Much less is known about the properties of such charged-exciton complexes since three-body problems are very difficult to be solved, even numerically. Here we introduce the correlated hyperspherical harmonics as basis functions to solve the hyperangular equation for negatively and positively charged excitons (trions) in a harmonic quantum dot. By using this method, we have calculated the energy spectra of the low-lying states of a charged exciton as a function of the radius of quantum dot. Based on symmetry analysis, the level crossover as the dot radius increases can be fully explained as the results of symmetry constraint.``

  3. Crossing behavior of the singlet and triplet State of the negatively charged magneto-exciton in a GaAs/AlGaAs quantum well

    Energy Technology Data Exchange (ETDEWEB)

    MUNTEANU,F.M.; KIM,YONGMIN; PERRY,C.H.; RICKEL,D.G.; SIMMONS,JERRY A.; RENO,JOHN L.

    2000-01-27

    Polarized magneto-photoluminescence (MPL) measurements on a high mobility {delta}-doped GaAs/AlGaAs single quantum well from 0--60 T at temperatures between 0.37--2.1 K are reported. In addition to the neutral heavy hole magneto-exciton (X{sup 0}), the singlet (X {sub s}{sup {minus}}) and triplet (X {sub t}{sup {minus}}) states of the negatively charged magneto-exciton are observed in both polarizations. The energy dispersive and time-resolved MPL data suggest that their development is fundamentally related to the formation of the neutral magneto-exciton. At a magnetic field of 40 T the singlet and the triplet states cross as a result of the role played by the higher Landau levels and higher energy subbands in their energetic evolution, confirming theoretical predictions. The authors also observed the formation of two higher energy peaks. One of them is completely right circularly polarized and its appearance can be considered a result of the electron-hole exchange interaction enhancement with an associated electron g-factor of 3.7 times the bulk value. The other peak completely dominates the MPL spectrum at fields around 30 T. Its behavior with magnetic field and temperature indicates that it may be related to previous anomalies observed in the integer and fractional quantum Hall regimes.

  4. Crossing behavior of the singlet and triplet State of the negatively charged magneto-exciton in a GaAs/AlGaAs quantum well

    Energy Technology Data Exchange (ETDEWEB)

    MUNTEANU,F.M.; KIM,YONGMIN; PERRY,C.H.; RICKEL,D.G.; SIMMONS,JERRY A.; RENO,JOHN L.

    2000-01-27

    Polarized magneto-photoluminescence (MPL) measurements on a high mobility {delta}-doped GaAs/AlGaAs single quantum well from 0--60 T at temperatures between 0.37--2.1 K are reported. In addition to the neutral heavy hole magneto-exciton (X{sup 0}), the singlet (X {sub s}{sup {minus}}) and triplet (X {sub t}{sup {minus}}) states of the negatively charged magneto-exciton are observed in both polarizations. The energy dispersive and time-resolved MPL data suggest that their development is fundamentally related to the formation of the neutral magneto-exciton. At a magnetic field of 40 T the singlet and the triplet states cross as a result of the role played by the higher Landau levels and higher energy subbands in their energetic evolution, confirming theoretical predictions. The authors also observed the formation of two higher energy peaks. One of them is completely right circularly polarized and its appearance can be considered a result of the electron-hole exchange interaction enhancement with an associated electron g-factor of 3.7 times the bulk value. The other peak completely dominates the MPL spectrum at fields around 30 T. Its behavior with magnetic field and temperature indicates that it may be related to previous anomalies observed in the integer and fractional quantum Hall regimes.

  5. Neutral and positively charged excitons in narrow quantum ring

    Energy Technology Data Exchange (ETDEWEB)

    Porras Monroy, L. C.; Rodríguez-Prada, F. A.; Mikhailov, I. D. [Escuela de Física, Universidad Industrial de Santander, A. A. 678, Bucaramanga (Colombia)

    2014-05-15

    We study theoretically quantized states of a neutral and a positively charged exciton (trion X{sup +}) confined in a heterostructure with the ring-like geometry. In order to assess the experimentally relevant domain of parameters, we adopt a simple model of a narrow ring when 3D wave equations for the neutral and positively charged excitons can be separated. By using the Fourier series method, we have calculated the energy spectra of excitons complexes in a quantum ring as a function of the electron-to-hole mass ratio, the ring radius, and the magnetic field strength. The quantum-size effect and the size-dependent magnetic oscillations of energy levels of excitons' complexes spectra have been revealed.

  6. Exciton transport, charge extraction, and loss mechanisms in organic photovoltaics

    Science.gov (United States)

    Scully, Shawn Ryan

    the primary losses that puts stringent requirements on the charge carrier mobilities in these cells is the recombination losses due to space charge build up at the heterojunction. Because electrons are confined to the acceptor and holes to the donor, net charge density always exists even when mobilities are matched, in contrast to bulk heterojunctions wherein matched mobilities lead to zero net charge. This net charge creates an electric field which opposes the built-in field and limits the current that can be carried away from this heterojunction. Using simulations we show that for relevant current densities charge carrier mobilities must be higher than 10-4 cm2/V.s to avoid significant losses due to space charge formation. In the last part of this work, we will focus on the second class of architectures in which exciton harvesting is efficient. We will present a systematic analysis of one of the leading polymer:fullerene bulk heterojunction cells to show that losses in this architecture are due to charge recombination. Using optical measurements and simulations, exciton harvesting measurements, and device characteristics we will show that the dominant loss is likely due to field-dependent geminate recombination of the electron and hole pair created immediately following exciton dissociation. No losses in this system are seen due to bimolecular recombination or space charge which provides information on charge-carrier mobility targets necessary for the future design of high efficiency organic photovoltaics.

  7. Primitive Virtual Negative Charge

    CERN Document Server

    Kim, Kiyoung

    2008-01-01

    Physical fields, such as gravity and electromagnetic field, are interpreted as results from rearrangement of vacuum particles to get the equilibrium of net charge density and net mass density in 4-dimensional complex space. Then, both fields should interact to each other in that physical interaction is considered as a field-to-field interaction. Hence, Mass-Charge interaction is introduced with primitive-virtual negative charge defined for the mass. With the concept of Mass-Charge interaction electric equilibrium of the earth is discussed, especially about the electric field and magnetic field of the earth. For unsettled phenomena related with the earth's gravity, such as antigravity phenomenon, gravity anomalies during the solar eclipses, the connection between geomagnetic storms and earthquakes, etc., possible explanations are discussed.

  8. Optical absorption of charged excitons in semiconducting carbon nanotubes

    DEFF Research Database (Denmark)

    Rønnow, Troels Frimodt; Pedersen, Thomas Garm; Cornean, Horia

    2012-01-01

    In this article we examine the absorption coefficient of charged excitons in carbon nanotubes. We investigate the temperature and damping dependence of the absorption spectra. We show that the trion peak in the spectrum is asymmetric for temperatures greater than approximately 1 K whereas the abs...

  9. From the artificial atom to the Kondo-Anderson model: Orientation-dependent magnetophotoluminescence of charged excitons in InAs quantum dots

    OpenAIRE

    Van Hattem, B.; Corfdir, P.; Brereton, P.; Pearce, P; Graham, A. M.; Stanley, M.J.; Hugues, M.; Hopkinson, M.; Phillips, R. T.

    2013-01-01

    We present a magnetophotoluminescence study on neutral and charged excitons confined to InAs/GaAs quantum dots. Our investigation relies on a confocal microscope that allows arbitrary tuning of the angle between the applied magnetic field and the sample growth axis. First, from experiments on neutral excitons and trions, we extract the in-plane and on-axis components of the Land? tensor for electrons and holes in the s shell. Then, based on the doubly negatively charged exciton magnetophotolu...

  10. Charge transfer excitons in C60-dimers and polymers

    CERN Document Server

    Harigaya, K

    1996-01-01

    Charge-transfer (CT) exciton effects are investigated for the optical absorption spectra of crosslinked C60 systems by using the intermediate exciton theory. We consider the C60-dimers, and the two (and three) molecule systems of the C60-polymers. We use a tight-binding model with long-range Coulomb interactions among electrons, and the model is treated by the Hartree-Fock approximation followed by the single-excitation configuration interaction method. We discuss the variations in the optical spectra by changing the conjugation parameter between molecules. We find that the total CT-component increases in smaller conjugations, and saturates at the intermediate conjugations. It decreases in the large conjugations. We also find that the CT-components of the doped systems are smaller than those of the neutral systems, indicating that the electron-hole distance becomes shorter in the doped C60-polymers.

  11. Symposium GC: Nanoscale Charge Transport in Excitonic Solar Cells

    Energy Technology Data Exchange (ETDEWEB)

    Bommisetty, Venkat [Univ. of South Dakota, Vermillion, SD (United States)

    2011-06-23

    This paper provides a summary only and table of contents of the sessions. Excitonic solar cells, including all-organic, hybrid organic-inorganic and dye-sensitized solar cells (DSSCs), offer strong potential for inexpensive and large-area solar energy conversion. Unlike traditional inorganic semiconductor solar cells, where all the charge generation and collection processes are well understood, these excitonic solar cells contain extremely disordered structures with complex interfaces which results in large variations in nanoscale electronic properties and has a strong influence on carrier generation, transport, dissociation and collection. Detailed understanding of these processes is important for fabrication of highly efficient solar cells. Efforts to improve efficiency are underway at a large number of research groups throughout the world focused on inorganic and organic semiconductors, photonics, photophysics, charge transport, nanoscience, ultrafast spectroscopy, photonics, semiconductor processing, device physics, device structures, interface structure etc. Rapid progress in this multidisciplinary area requires strong synergetic efforts among researchers from diverse backgrounds. Such effort can lead to novel methods for development of new materials with improved photon harvesting and interfacial treatments for improved carrier transport, process optimization to yield ordered nanoscale morphologies with well defined electronic structures.

  12. Optical studies of charged excitons in II-VI semiconductor quantum wells

    CERN Document Server

    Kossacki, P

    2003-01-01

    A brief review is given of optical studies of doped II-VI quantum wells. The properties of exciton states, neutral as well as positively and negatively charged, are discussed. A wide range of optical measurements is presented: CW as well as picosecond and femtosecond time-resolved absorption, photoluminescence (PL) and PL excitation. The experiments were performed at various carrier concentrations (> 10 sup 1 sup 1 cm sup - sup 2) and temperatures (up to a few tens of kelvins). This review is limited to zero or low magnetic fields, used only to polarize spins of carriers. We discuss the obtained values of various fundamental parameters of the excitonic states: energies, optical transition probabilities and characteristic times of their formation, thermalization and decay. (topical review)

  13. A benchmark of excitonic couplings derived from atomic transition charges.

    Science.gov (United States)

    Kistler, Kurt A; Spano, Francis C; Matsika, Spiridoula

    2013-02-21

    In this report we benchmark Coulombic excitonic couplings between various pairs of chromophores calculated using transition charges localized on the atoms of each monomer chromophore, as derived from a Mulliken population analysis of the monomeric transition densities. The systems studied are dimers of 1-methylthymine, 1-methylcytosine, 2-amino-9-methylpurine, all-trans-1,3,5-hexatriene, all-trans-1,3,5,7-octatetraene, trans-stilbene, naphthalene, perylenediimide, and dithia-anthracenophane. Transition densities are taken from different single-reference electronic structure excited state methods: time-dependent density functional theory (TDDFT), configuration-interaction singles (CIS), and semiempirical methods based on intermediate neglect of differential overlap. Comparisons of these results with full ab initio calculations of the electronic couplings using a supersystem are made, as are comparisons with experimental data. Results show that the transition charges do a good job of reproducing the supersystem couplings for dimers with moderate to long-range interchromophore separation. It is also found that CIS supermolecular couplings tend to overestimate the couplings, and often the transition charges approach may be better, due to fortuitous cancellation of errors.

  14. Negative activation energy and dielectric signatures of excitons and excitonic Mott transitions in quantum confined laser structures

    Science.gov (United States)

    Bhunia, Amit; Bansal, Kanika; Henini, Mohamed; Alshammari, Marzook S.; Datta, Shouvik

    2016-10-01

    Mostly, optical spectroscopies are used to investigate the physics of excitons, whereas their electrical evidences are hardly explored. Here, we examined a forward bias activated differential capacitance response of GaInP/AlGaInP based multi-quantum well laser diodes to trace the presence of excitons using electrical measurements. Occurrence of "negative activation energy" after light emission is understood as thermodynamical signature of steady state excitonic population under intermediate range of carrier injections. Similar corroborative results are also observed in an InGaAs/GaAs quantum dot laser structure grown by molecular beam epitaxy. With increasing biases, the measured differential capacitance response slowly vanishes. This represents gradual Mott transition of an excitonic phase into an electron-hole plasma in a GaInP/AlGaInP laser diode. This is further substantiated by more and more exponentially looking shapes of high energy tails in electroluminescence spectra with increasing forward bias, which originates from a growing non-degenerate population of free electrons and holes. Such an experimental correlation between electrical and optical properties of excitons can be used to advance the next generation excitonic devices.

  15. Excitons versus free charges in organo-lead tri-halide perovskites

    Science.gov (United States)

    D'Innocenzo, Valerio; Grancini, Giulia; Alcocer, Marcelo J. P.; Kandada, Ajay Ram Srimath; Stranks, Samuel D.; Lee, Michael M.; Lanzani, Guglielmo; Snaith, Henry J.; Petrozza, Annamaria

    2014-04-01

    Excitonic solar cells, within which bound electron-hole pairs have a central role in energy harvesting, have represented a hot field of research over the last two decades due to the compelling prospect of low-cost solar energy. However, in such cells, exciton dissociation and charge collection occur with significant losses in energy, essentially due to poor charge screening. Organic-inorganic perovskites show promise for overcoming such limitations. Here, we use optical spectroscopy to estimate the exciton binding energy in the mixed-halide crystal to be in the range of 50 meV. We show that such a value is consistent with almost full ionization of the exciton population under photovoltaic cell operating conditions. However, increasing the total photoexcitation density, excitonic species become dominant, widening the perspective of this material for a host of optoelectronic applications.

  16. Influence of Exciton Lifetime on Charge Carrier Dynamics in an Organic Heterostructure

    Energy Technology Data Exchange (ETDEWEB)

    Agrawal, Kanika L.; Sykes, Matthew E; An, Kwang Hyup; Friedberg, Bradley; Green, Peter F.; Shtein, Max

    2013-03-18

    Interactions between charge carriers and excitons, as well as between excitons and optical cavity modes in organic optoelectronic devices are fundamental to their operational limits and chief in preventing the realization of certain phenomena, such as electrically pumped organic lasing. We uncovered a previously unreported phenomenon, wherein optical cavity-modulated exciton decay rate leads to a concomitant modulation in the electrical current of an archetypal NPD/Alq₃ organic light emitting device operated in forward bias. The magnitude of this variation is sensitive to the local dielectric environment of the device and is found to be as large as 15%.

  17. Effects of Charge-Transfer Excitons on the Photophysics of Organic Semiconductors

    Science.gov (United States)

    Hestand, Nicholas J.

    -aggregate characteristics including a positive band curvature, a red shifted main absorption peak, and an increase in the ratio of the first two vibronic peaks relative to the monomer. On the other hand, when the charge-transfer integrals are out of phase and the energy of the charge-transfer state is higher than the Frenkel state, the system exhibits H-aggregate characteristics including a negative band curvature, a blue shifted main absorption peak, and a decrease in the ratio of the first two vibronic peaks relative to the monomer. Notably, these signatures are consistent with those exhibited by Coulombically coupled J- and H-aggregates. Additional signatures of charge-transfer J- and H-aggregation are also discovered, the most notable of which is the appearance of a second absorption band when the charge-transfer integrals are in phase and the charge-transfer and Frenkel excitons are near resonance. In such instances, the peak-to-peak spacing is found to be proportional to the sum of the electron and hole transfer integrals. Further analysis of the charge-transfer interactions within the context of an effective Frenkel exciton coupling reveals that the charge-transfer interactions interfere directly with the intermolecular Coulombic coupling. The interference can be either constructive or destructive resulting in either enhanced or suppressed J- or H- aggregate behavior relative to what is expected based on Coulombic coupling alone. Such interferences result in four new aggregate types, namely HH-, HJ-, JH-, and JJ-aggregates, where the first letter indicates the nature of the Coulombic coupling and the second indicates the nature of the charge-transfer coupling. Vibronic signatures of such aggregates are developed and provide a means by which to rapidly screen materials for certain electronic characteristics. Notably, a large total (Coulombic plus charge-transfer) exciton coupling is associated with an absorption spectrum in which the ratio of the first two vibronic peaks deviates

  18. Charge Transfer Fluorescence and 34 nm Exciton Diffusion Length in Polymers with Electron Acceptor End Traps.

    Science.gov (United States)

    Zaikowski, Lori; Mauro, Gina; Bird, Matthew; Karten, Brianne; Asaoka, Sadayuki; Wu, Qin; Cook, Andrew R; Miller, John R

    2015-06-18

    Photoexcitation of conjugated poly-2,7-(9,9-dihexylfluorene) polyfluorenes with naphthylimide (NI) and anthraquinone (AQ) electron-acceptor end traps produces excitons that form charge transfer states at the end traps. Intramolecular singlet exciton transport to end traps was examined by steady state fluorescence for polyfluorenes of 17-127 repeat units in chloroform, dimethylformamide (DMF), tetrahydrofuran (THF), and p-xylene. End traps capture excitons and form charge transfer (CT) states at all polymer lengths and in all solvents. The CT nature of the end-trapped states is confirmed by their fluorescence spectra, solvent and trap group dependence, and DFT descriptions. Quantum yields of CT fluorescence are as large as 46%. This strong CT emission is understood in terms of intensity borrowing. Energies of the CT states from onsets of the fluorescence spectra give the depths of the traps which vary with solvent polarity. For NI end traps, the trap depths are 0.06 (p-xylene), 0.13 (THF), and 0.19 eV (CHCl3). For AQ, CT fluorescence could be observed only in p-xylene where the trap depth is 0.27 eV. Quantum yields, emission energies, charge transfer energies, solvent reorganization, and vibrational energies were calculated. Fluorescence measurements on chains >100 repeat units indicate that end traps capture ∼50% of the excitons, and that the exciton diffusion length is LD = 34 nm, which is much larger than diffusion lengths reported in polymer films or than previously known for diffusion along isolated chains. The efficiency of exciton capture depends on chain length but not on trap depth, solvent polarity, or which trap group is present.

  19. Excitonic and vibrational coherence in artificial photosynthetic systems studied by negative-time ultrafast laser spectroscopy.

    Science.gov (United States)

    Han, Dongjia; Xue, Bing; Du, Juan; Kobayashi, Takayoshi; Miyatake, Tomohiro; Tamiaki, Hitoshi; Xing, Xin; Yuan, Wei; Li, Yanyan; Leng, Yuxin

    2016-09-21

    Quantum coherences between excitonic states are believed to have a substantial impact on excitation energy transfer in photosynthetic systems. Here, the excitonic and vibrational coherence relaxation dynamics of artificially synthetic chlorosomes are studied by a sub 7 fs negative-time-delay laser spectroscopy at room temperature. The results provide direct evidence for the quantum coherence of the excitonic dephasing time of 23 ± 1 fs at physiologically relevant temperatures, which is significant in the initial step of energy transfer in chlorosome or chlorosome-like photosynthetic systems. Meanwhile, coherent molecular vibrations in the excited state are also detected without the effect of wave-packet motion in the ground state, which shows that the excited state wave-packet motion contributes greatly to the vibrational modes of ∼150 and ∼1340 cm(-1) in artificial chlorosome systems.

  20. Exciton Diffusion Length and Charge Extraction Yield in Organic Bilayer Solar Cells.

    Science.gov (United States)

    Siegmund, Bernhard; Sajjad, Muhammad T; Widmer, Johannes; Ray, Debdutta; Koerner, Christian; Riede, Moritz; Leo, Karl; Samuel, Ifor D W; Vandewal, Koen

    2017-03-01

    A method for resolving the diffusion length of excitons and the extraction yield of charge carriers is presented based on the performance of organic bilayer solar cells and careful modeling. The technique uses a simultaneous variation of the absorber thickness and the excitation wavelength. Rigorously differing solar cell structures as well as independent photoluminescence quenching measurements give consistent results. © 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  1. Binding Energies of a Positively Charged Exciton in a Quantum Disc

    Institute of Scientific and Technical Information of China (English)

    2005-01-01

    The binding energies of the lowest singlet and triplet states of positively charged excitons confined to a quantum disc are studied using exact diagonalization techniques. We investigate the dependence of the binding energies on the confinement strength and on the effective electron-to-hole mass ratio. The results we have obtained show that the binding energies are closely correlated to the strength of the confinement potential and the effective electron-to-hole mass ratio.

  2. Effects of energy correlations and superexchange on charge transport and exciton formation in amorphous molecular semiconductors: An ab initio study

    Science.gov (United States)

    Massé, Andrea; Friederich, Pascal; Symalla, Franz; Liu, Feilong; Meded, Velimir; Coehoorn, Reinder; Wenzel, Wolfgang; Bobbert, Peter A.

    2017-03-01

    In this study, we investigate on the basis of ab initio calculations how the morphology, molecular on-site energies, reorganization energies, and charge transfer integral distribution affect the hopping charge transport and the exciton formation process in disordered organic semiconductors. We focus on three materials applied frequently in organic light-emitting diodes: α -NPD , TCTA, and Spiro-DPVBi. Spatially correlated disorder and, more importantly, superexchange contributions to the transfer integrals, are found to give rise to a significant increase of the electric field dependence of the electron and hole mobility. Furthermore, a material-specific correlation is found between the HOMO and LUMO energy on each specific molecular site. For α -NPD and TCTA, we find a positive correlation between the HOMO and LUMO energies, dominated by a Coulombic contribution to the energies. In contrast, Spiro-DPVBi shows a negative correlation, dominated by a conformational contribution. The size and sign of this correlation have a strong influence on the exciton formation rate.

  3. Ultrafast exciton dissociation followed by nongeminate charge recombination in PCDTBT:PCBM photovoltaic blends.

    Science.gov (United States)

    Etzold, Fabian; Howard, Ian A; Mauer, Ralf; Meister, Michael; Kim, Tae-Dong; Lee, Kwang-Sup; Baek, Nam Seob; Laquai, Frédéric

    2011-06-22

    The precise mechanism and dynamics of charge generation and recombination in bulk heterojunction polymer:fullerene blend films typically used in organic photovoltaic devices have been intensively studied by many research groups, but nonetheless remain debated. In particular the role of interfacial charge-transfer (CT) states in the generation of free charge carriers, an important step for the understanding of device function, is still under active discussion. In this article we present direct optical probes of the exciton dynamics in pristine films of a prototypic polycarbazole-based photovoltaic donor polymer, namely poly[N-11''-henicosanyl-2,7-carbazole-alt-5,5-(4',7'-di-2-thienyl-2',1',3'-benzothiadiazole)] (PCDTBT), as well as the charge generation and recombination dynamics in as-cast and annealed photovoltaic blend films using methanofullerene (PC(61)BM) as electron acceptor. In contrast to earlier studies we use broadband (500-1100 nm) transient absorption spectroscopy including the previously unobserved but very important time range between 2 ns and 1 ms, which allows us not only to observe the entire charge carrier recombination dynamics but also to quantify the existing decay channels. We determine that ultrafast exciton dissociation occurs in blends and leads to two separate pools of products, namely Coulombically bound charge-transfer (CT) states and unbound (free) charge carriers. The recombination dynamics are analyzed within the framework of a previously reported model for poly(3-hexylthiophene):PCBM (Howard, I. A. J. Am. Chem. Soc. 2010, 132, 14866) based on concomitant geminate recombination of CT states and nongeminate recombination of free charge carriers. The results reveal that only ~11% of the initial photoexcitations generate interfacial CT states that recombine exclusively by fast nanosecond geminate recombination and thus do not contribute to the photocurrent, whereas ~89% of excitons create free charge carriers on an ultrafast time scale

  4. Slow Auger Recombination of Charged Excitons in Nonblinking Perovskite Nanocrystals without Spectral Diffusion

    CERN Document Server

    Hu, Fengrui; Zhang, Huichao; Sun, Chun; Yu, William W; Zhang, Chunfeng; Wang, Xiaoyong; Zhang, Yu; Xiao, Min

    2016-01-01

    Over the last two decades, intensive research efforts have been devoted to the suppressions of photoluminescence (PL) blinking and Auger recombination in metal-chalcogenide nanocrystals (NCs), with significant progresses being made only very recently in several specific heterostructures. Here we show that nonblinking PL is readily available in the newly-synthesized perovskite CsPbI3 (cesium lead iodide) NCs, and their Auger recombination of charged excitons is greatly slowed down, as signified by a PL lifetime about twice shorter than that of neutral excitons. Moreover, spectral diffusion is completely absent in single CsPbI3 NCs at the cryogenic temperature, leading to a resolution-limited PL linewidth of ~200 {\\mu}eV.

  5. Recombination Kinetics in Organic-Inorganic Perovskites: Excitons, Free Charge, and Subgap States

    Science.gov (United States)

    Stranks, Samuel D.; Burlakov, Victor M.; Leijtens, Tomas; Ball, James M.; Goriely, Alain; Snaith, Henry J.

    2014-09-01

    Organic-inorganic perovskites are attracting increasing attention for their use in high-performance solar cells. Nevertheless, a detailed understanding of charge generation, interplay of excitons and free charge carriers, and recombination pathways, crucial for further device improvement, remains incomplete. Here, we present an analytical model describing both equilibrium properties of free charge carriers and excitons in the presence of electronic subgap trap states and their time evolution after photoexcitation in CH3NH3PbI3-xClx. At low fluences the charge-trapping pathways limit the photoluminescence quantum efficiency, whereas at high fluences the traps are predominantly filled and recombination of the photogenerated species is dominated by efficient radiative processes. We show experimentally that the photoluminescence quantum efficiency approaches 100% at low temperatures and at high fluences, as predicted by our model. Our approach provides a theoretical framework to understand the fundamental physics of perovskite semiconductors and to help in designing and enhancing the material for improved optoelectronic device operation.

  6. Short-lived charge-transfer excitons in organic photovoltaic cells studied by high-field magneto-photocurrent.

    Science.gov (United States)

    Devir-Wolfman, Ayeleth H; Khachatryan, Bagrat; Gautam, Bhoj R; Tzabary, Lior; Keren, Amit; Tessler, Nir; Vardeny, Z Valy; Ehrenfreund, Eitan

    2014-07-29

    The main route of charge photogeneration in efficient organic photovoltaic cells based on bulk hetero-junction donor-acceptor blends involves short-lived charge-transfer excitons at the donor-acceptor interfaces. The cell efficiency is critically affected by the charge-transfer exciton recombination and dissociation processes. By measuring the magneto-photocurrent under ambient conditions at room temperature, we show here that magnetic field-induced spin-mixing among the charge-transfer exciton spin sublevels occurs in fields up to at least 8.5 Tesla. The resulting magneto-photocurrent increases at high fields showing non-saturating behaviour up to the highest applied field. We attribute the observed high-field spin-mixing mechanism to the difference in the donor-acceptor g-factors. The non-saturating magneto-photocurrent response at high field indicates that there exist charge-transfer excitons with lifetime in the sub-nanosecond time domain. The non-Lorentzian high-field magneto-photocurrent response indicates a dispersive decay mechanism that originates due to a broad distribution of charge-transfer exciton lifetimes.

  7. Charge transport through exciton shelves in cadmium chalcogenide quantum dot-DNA nano-bioelectronic thin films

    Energy Technology Data Exchange (ETDEWEB)

    Goodman, Samuel M.; Singh, Vivek [Department of Chemical and Biological Engineering, University of Colorado Boulder, 3415 Colorado Avenue, Boulder, Colorado 80303 (United States); Noh, Hyunwoo [Department of Chemical and Biological Engineering, University of Colorado Boulder, 3415 Colorado Avenue, Boulder, Colorado 80303 (United States); Materials Science and Engineering Program and Department of Nanoengineering, University of California, 9500 Gilman Drive, La Jolla, San Diego, California 92093 (United States); Cha, Jennifer N. [Department of Chemical and Biological Engineering, University of Colorado Boulder, 3415 Colorado Avenue, Boulder, Colorado 80303 (United States); Materials Science and Engineering Program and Department of Nanoengineering, University of California, 9500 Gilman Drive, La Jolla, San Diego, California 92093 (United States); Materials Science and Engineering, University of Colorado Boulder, 3415 Colorado Avenue, Boulder, Colorado 80303 (United States); Nagpal, Prashant, E-mail: pnagpal@colorado.edu [Department of Chemical and Biological Engineering, University of Colorado Boulder, 3415 Colorado Avenue, Boulder, Colorado 80303 (United States); Materials Science and Engineering, University of Colorado Boulder, 3415 Colorado Avenue, Boulder, Colorado 80303 (United States); BioFrontiers Institute, University of Colorado Boulder, 3415 Colorado Avenue, Boulder, Colorado 80303 (United States); Renewable and Sustainable Energy Institute, University of Colorado Boulder, 2445 Kittredge Loop, Boulder, Colorado 80309 (United States)

    2015-02-23

    Quantum dot (QD), or semiconductor nanocrystal, thin films are being explored for making solution-processable devices due to their size- and shape-tunable bandgap and discrete higher energy electronic states. While DNA has been extensively used for the self-assembly of nanocrystals, it has not been investigated for the simultaneous conduction of multiple energy charges or excitons via exciton shelves (ES) formed in QD-DNA nano-bioelectronic thin films. Here, we present studies on charge conduction through exciton shelves, which are formed via chemically coupled QDs and DNA, between electronic states of the QDs and the HOMO-LUMO levels in the complementary DNA nucleobases. While several challenges need to be addressed in optimizing the formation of devices using QD-DNA thin films, a higher charge collection efficiency for hot-carriers and our detailed investigations of charge transport mechanism in these thin films highlight their potential for applications in nano-bioelectronic devices and biological transducers.

  8. Tuning the role of charge-transfer states in intramolecular singlet exciton fission through side-group engineering

    Science.gov (United States)

    Lukman, Steven; Chen, Kai; Hodgkiss, Justin M.; Turban, David H. P.; Hine, Nicholas D. M.; Dong, Shaoqiang; Wu, Jishan; Greenham, Neil C.; Musser, Andrew J.

    2016-12-01

    Understanding the mechanism of singlet exciton fission, in which a singlet exciton separates into a pair of triplet excitons, is crucial to the development of new chromophores for efficient fission-sensitized solar cells. The challenge of controlling molecular packing and energy levels in the solid state precludes clear determination of the singlet fission pathway. Here, we circumvent this difficulty by utilizing covalent dimers of pentacene with two types of side groups. We report rapid and efficient intramolecular singlet fission in both molecules, in one case via a virtual charge-transfer state and in the other via a distinct charge-transfer intermediate. The singlet fission pathway is governed by the energy gap between singlet and charge-transfer states, which change dynamically with molecular geometry but are primarily set by the side group. These results clearly establish the role of charge-transfer states in singlet fission and highlight the importance of solubilizing groups to optimize excited-state photophysics.

  9. Theoretical Studies of the Interaction of Excitons with Charged Impurities in Single-Walled Carbon Nanotubes

    Science.gov (United States)

    Tayo, Benjamin O.

    A fundamental theory of the electronic and optical properties of semiconductors shows the importance of impurities, which are often unavoidable and can alter intrinsic properties of semiconductor materials substantially. While the subject of impurity doping is well understood in bulk semiconductors, the role and impact of doping in low dimensional materials like carbon nanotubes is still under investigation and there exists significant debate on the exact nature of electronic impurity levels in single-walled carbon nanotubes associated with adatoms. In this work, we address the role of impurities in single-walled carbon nanotubes. A simple model is developed for studying the interaction of bright (singlet) excitons in semiconducting single-wall nanotubes with charged impurities. The model reveals a red shift in the energy of excitonic states in the presence of an impurity, thus indicating binding of excitons in the impurity potential well. Signatures of several bound states were found in the absorption spectrum below the onset of excitonic optical transitions in the bare nanotube. The dependence of the binding energy on the model parameters, such as impurity charge and position, was determined and analytical fits were derived for a number of tubes of different diameter. The nanotube family splitting is seen in the diameter dependence, gradually decreasing with the diameter. By calculating the partial absorption coefficient for a small segment of nanotube the local nature of the wave function of the bound states was derived. Our studies provide useful insights into the role of the physical environment (here, a charged impurity atom) in the manipulation of the excited states of carbon nanotubes. We performed very detailed calculations of the electronic and optical properties of carbon nanotubes in the presence of an immobile impurity atom, thus going beyond previous many-body perturbation theory (MBPT) studies in which the carbon nanotubes were considered in vacuum

  10. Pressure-Dependent Light Emission of Charged and Neutral Excitons in Monolayer MoSe 2

    Energy Technology Data Exchange (ETDEWEB)

    Fu, Xinpeng [State; Li, Fangfei [State; Lin, Jung-Fu [Department; Gong, Yuanbo [State; Huang, Xiaoli [State; Huang, Yanping [State; Han, Bo [State; Zhou, Qiang [State; Cui, Tian [State

    2017-07-19

    Tailoring the excitonic properties in two-dimensional monolayer transition metal dichalcogenides (TMDs) through strain engineering is an effective means to explore their potential applications in optoelectronics and nanoelectronics. Here we report pressure-tuned photon emission of trions and excitons in monolayer MoSe2 via a diamond anvil cell (DAC) through photoluminescence measurements and theoretical calculations. Under quasi-hydrostatic compressive strain, our results show neutral (X0) and charged (X–) exciton emission of monolayer MoSe2 can be effectively tuned by alcohol mixture vs inert argon pressure transmitting media (PTM). During this process, X– emission undergoes a continuous blue shift until reaching saturation, while X0 emission turns up splitting. The pressure-dependent charging effect observed in alcohol mixture PTM results in the increase of the X– exciton component and facilitates the pressure-tuned emission of X– excitons. This substantial tunability of X– and X0 excitons in MoSe2 can be extended to other 2D TMDs, which holds potential for developing strained and optical sensing devices.

  11. Electronic Enhancement of the Exciton Coherence Time in Charged Quantum Dots

    Science.gov (United States)

    Moody, G.; McDonald, C.; Feldman, A.; Harvey, T.; Mirin, R. P.; Silverman, K. L.

    2016-01-01

    Minimizing decoherence due to coupling of a quantum system to its fluctuating environment is at the forefront of quantum information and photonics research. Nature sets the ultimate limit, however, given by the strength of the system’s coupling to the electromagnetic field. Here, we establish the ability to electronically control this coupling and enhance the optical coherence time of the charged exciton transition in quantum dots embedded in a photonic waveguide. By manipulating the electronic wavefunctions through an applied lateral electric field, we increase the coherence time from ~ 1.4 ns to ~ 2.7 ns. Numerical calculations reveal that longer coherence arises from the separation of charge carriers by up to ~ 6 nm, which leads to a 30% weaker transition dipole moment. The ability to electronically control the coherence time opens new avenues for quantum communication and novel coupling schemes between distant qubits. PMID:26849614

  12. A Model of Charge Transfer Excitons: Diffusion, Spin Dynamics, and Magnetic Field Effects

    CERN Document Server

    Lee, Chee Kong; Willard, Adam P

    2016-01-01

    In this letter we explore how the microscopic dynamics of charge transfer (CT) excitons are influenced by the presence of an external magnetic field in disordered molecular semiconductors. This influence is driven by the dynamic interplay between the spin and spatial degrees of freedom of the electron-hole pair. To account for this interplay we have developed a numerical framework that combines a traditional model of quantum spin dynamics with a coarse-grained model of stochastic charge transport. This combination provides a general and efficient methodology for simulating the effects of magnetic field on CT state dynamics, therefore providing a basis for revealing the microscopic origin of experimentally observed magnetic field effects. We demonstrate that simulations carried out on our model are capable of reproducing experimental results as well as generating theoretical predictions related to the efficiency of organic electronic materials.

  13. Nonuniform Excitonic Charge Distribution Enhances Exciton-Phonon Coupling in ZnSe/CdSe Alloyed Quantum Dots.

    Science.gov (United States)

    Gong, Ke; Kelley, David F; Kelley, Anne Myers

    2017-02-02

    Zinc to cadmium cation exchange of ZnSe quantum dots has been used to produce a series of alloyed Zn1-xCdxSe quantum dots. As x increases and the lowest-energy exciton shifts to the red, the peak initially broadens and then sharpens as x approaches 1. Resonance Raman spectra obtained with excitation near the lowest excitonic absorption peak show a gradual shift of the longitudinal optical phonon peak from 251 cm(-1) in pure ZnSe to 210 cm(-1) in nearly pure CdSe with strong broadening at intermediate compositions. The LO overtone to fundamental intensity ratio, a rough gauge of exciton-phonon coupling strength, increases considerably for intermediate compositions compared with those of either pure ZnSe or pure CdSe. The results indicate that partial localization of the hole in locally Cd-rich regions of the alloyed particles increases the strengths of local internal electric fields, increasing the coupling between the exciton and polar optical phonons.

  14. Production of negatively charged radioactive ion beams

    Science.gov (United States)

    Liu, Y.; Stracener, D. W.; Stora, T.

    2017-08-01

    Beams of short-lived radioactive nuclei are needed for frontier experimental research in nuclear structure, reactions, and astrophysics. Negatively charged radioactive ion beams have unique advantages and allow for the use of a tandem accelerator for post-acceleration, which can provide the highest beam quality and continuously variable energies. Negative ion beams can be obtained with high intensity and some unique beam purification techniques based on differences in electronegativity and chemical reactivity can be used to provide beams with high purity. This article describes the production of negative radioactive ion beams at the former holifield radioactive ion beam facility at Oak Ridge National Laboratory and at the CERN ISOLDE facility with emphasis on the development of the negative ion sources employed at these two facilities. ).

  15. Mapping the Competition between Exciton Dissociation and Charge Transport in Organic Solar Cells.

    Science.gov (United States)

    Oh, Soong Ju; Kim, Jong Bok; Mativetsky, Jeffrey M; Loo, Yueh-Lin; Kagan, Cherie R

    2016-10-03

    The competition between exciton dissociation and charge transport in organic solar cells comprising poly(3-hexylthiophene) [P3HT] and phenyl-C61-butyric acid methyl ester [PCBM] is investigated by correlated scanning confocal photoluminescence and photocurrent microscopies. Contrary to the general expectation that higher photoluminescence quenching is indicative of higher photocurrent, microscale mapping of bulk-heterojunction solar-cell devices shows that photoluminescence quenching and photocurrent can be inversely proportional to one another. To understand this phenomenon, we construct a model system by selectively laminating a PCBM layer onto a P3HT film to form a PCBM/P3HT planar junction on half of the device and a P3HT single junction on the other half. Upon thermal annealing to allow for interdiffusion of PCBM into P3HT, an inverse relationship between photoluminescence quenching and photocurrent is observed at the boundary between the PCBM/P3HT junction and P3HT layer. Incorporation of PCBM in P3HT works to increase photoluminescence quenching, consistent with efficient charge separation, but conductive atomic force microscopy measurements reveal that PCBM acts to decrease P3HT hole mobility, limiting the efficiency of charge transport. This suggests that photoluminescence-quenching measurements should be used with caution in evaluating new organic materials for organic solar cells.

  16. Understanding the charge-transfer state and singlet exciton emission from solution-processed small-molecule organic solar cells.

    Science.gov (United States)

    Ran, Niva A; Kuik, Martijn; Love, John A; Proctor, Christopher M; Nagao, Ikuhiro; Bazan, Guillermo C; Nguyen, Thuc-Quyen

    2014-11-19

    Electroluminescence (EL) from the charge-transfer state and singlet excitons is observed at low applied voltages from high-performing small-molecule bulk-heterojunction solar cells. Singlet emission from the blends emerges upon altering the processing conditions, such as thermal annealing and processing with a solvent additive, and correlates with improved photovoltaic performance. Low-temperature EL measurements are utilized to access the physics behind the singlet emission.

  17. Spectroscopy and dynamics of charge transfer excitons in type-II band aligned quantum confined heterostructures

    Science.gov (United States)

    Kushavah, Dushyant; Mohapatra, P. K.; Rustagi, K. C.; Bahadur, D.; Vasa, P.; Singh, B. P.

    2015-05-01

    We illustrate effect of charge transfer (CT) in type-II quantum confined heterostructure by comparing CdSe quantum dots (QDs), CdSe/CdTe heterostructure quantum dots (HQDs) and CdSe/CdTe/CdSe quantum well-quantum dots (QWQDs) heterostructures. CdSe core QDs were synthesized using a kinetic growth method where QD size depends on reaction time. For shell coating we used modified version of successive ionic layer adsorption and reaction (SILAR). Size of different QDs ˜5 to 7 nm were measured by transmission electron microscopy (TEM). Strong red shift from ˜597 to ˜746 nm in photoluminescence (PL) spectra from QDs to QWQDs shows high tunability which is not possible with single constituent semiconductor QDs. PL spectra have been recorded at different temperatures (10K-300K). Room temperature time correlated single photon counting (TCSPC) measurements for QDs to QWQDs show three exponential radiative decay. The slowest component decay constant in QWQDs comes around eight fold to ˜51 ns as compared to ˜6.5 ns in HQD suggesting new opportunities to tailor the radiative carrier recombination rate of CT excitons.

  18. Spectroscopy and dynamics of charge transfer excitons in type-II band aligned quantum confined heterostructures

    Energy Technology Data Exchange (ETDEWEB)

    Kushavah, Dushyant [Centre for Research in Nanotechnology and Science, IIT Bombay-400076, Mumbai (India); Mohapatra, P. K.; Vasa, P.; Singh, B. P., E-mail: bhanups@iitb.ac.in [Department of physics, IIT Bombay, Mumbai-400076 (India); Rustagi, K. C. [Indian Institute of Science Education and Research Bhopal-462066, Bhopal (India); Bahadur, D. [Department of Metallurgical Engineering and Materials Science, IIT Bombay, Mumbai-400076 (India)

    2015-05-15

    We illustrate effect of charge transfer (CT) in type-II quantum confined heterostructure by comparing CdSe quantum dots (QDs), CdSe/CdTe heterostructure quantum dots (HQDs) and CdSe/CdTe/CdSe quantum well-quantum dots (QWQDs) heterostructures. CdSe core QDs were synthesized using a kinetic growth method where QD size depends on reaction time. For shell coating we used modified version of successive ionic layer adsorption and reaction (SILAR). Size of different QDs ∼5 to 7 nm were measured by transmission electron microscopy (TEM). Strong red shift from ∼597 to ∼746 nm in photoluminescence (PL) spectra from QDs to QWQDs shows high tunability which is not possible with single constituent semiconductor QDs. PL spectra have been recorded at different temperatures (10K-300K). Room temperature time correlated single photon counting (TCSPC) measurements for QDs to QWQDs show three exponential radiative decay. The slowest component decay constant in QWQDs comes around eight fold to ∼51 ns as compared to ∼6.5 ns in HQD suggesting new opportunities to tailor the radiative carrier recombination rate of CT excitons.

  19. Origin and impact of recombination via charge transfer excitons in polymer/fullerene solar cells

    Science.gov (United States)

    Hallermann, Markus; da Como, Enrico; Feldmann, Jochen

    2010-03-01

    To further advance the performances of organic photovoltaic cells a thorough understanding of loss mechanisms in polymer/fullerene blends is mandatory. Recombination via charge transfer excitons (CTEs) appears to be a fundamental loss, potentially impacting the open circuit voltage (VOC) and the short circuit current (ISC) of cells. We unravel the origin of CTEs forming in polymer/fullerene blends and discuss their importance in recombination processes considering binding energy [1], polymer conformation [2], and energetic position. CTE photoluminescence (PL) is observed in material combinations such as P3HT and PPV blended with fullerene acceptors. By combining electron microscopy and PL spectroscopy, we show that CTE recombination is only slightly influenced by the mesoscopic morphology, whereas strongly by the polymer chain conformation [2]. By shifting the orbital energies of the fullerene, we tune the CTE PL characteristics. High energy CTE emission results in cells with a beneficial increase in VOC. On the other hand, high energy CTE emission leads to a more efficient recombination impacting directly the ISC. The results highlight a fundamental limit in the efficiency of organic solar cells with CTE recombination. [1] Hallermann et al. APL 2008 [2] Hallermann et al. AFM 2009

  20. Charge carriers and excitons transport in an organic solar cell-theory and simulation

    Science.gov (United States)

    Shahini, Ali.; Abbasian, Karim.

    2012-08-01

    An organic solar cell model is developed that consists of both excitonic and classical bipolar aspects of solar cells. In order to achieve this goal, the photon recycling term is imported into the equations to connect the Shockley-Queisser theory and the classical diode theory. This model for excitonic and classical bipolar solar cells can describe the combined transport and interaction of electrons, holes and excitons. For high mobilities this model reproduces the Shockley Queisser efficiency limit. We show how varying the respective mobilities of the different species changes the operation mode of the solar cell path between excitonic and bipolar. Then, the effect of conduction band offset on transport will be described in this paper. Finally, validity of reciprocity theorem between quantum efficiency and electroluminescence in this model will be discussed.

  1. Arabinogalactan Proteins Are Incorporated in Negatively Charged Coffee Brew Melanoidins

    NARCIS (Netherlands)

    Bekedam, E.K.; Laat, de M.P.F.C.; Schols, H.A.; Boekel, van M.A.J.S.; Smit, G.

    2007-01-01

    The charge properties of melanoidins in high molecular weight (HMw) coffee brew fractions, isolated by diafiltration and membrane dialysis, were studied. Ion exchange chromatography experiments with the HMw fractions showed that coffee brew melanoidins were negatively charged whereas these molecules

  2. Arabinogalactan Proteins Are Incorporated in Negatively Charged Coffee Brew Melanoidins

    NARCIS (Netherlands)

    Bekedam, E.K.; Laat, de M.P.F.C.; Schols, H.A.; Boekel, van M.A.J.S.; Smit, G.

    2007-01-01

    The charge properties of melanoidins in high molecular weight (HMw) coffee brew fractions, isolated by diafiltration and membrane dialysis, were studied. Ion exchange chromatography experiments with the HMw fractions showed that coffee brew melanoidins were negatively charged whereas these molecules

  3. Multiply-negatively charged aluminium clusters and fullerenes

    Energy Technology Data Exchange (ETDEWEB)

    Walsh, Noelle

    2008-07-15

    Multiply negatively charged aluminium clusters and fullerenes were generated in a Penning trap using the 'electron-bath' technique. Aluminium monoanions were generated using a laser vaporisation source. After this, two-, three- and four-times negatively charged aluminium clusters were generated for the first time. This research marks the first observation of tetra-anionic metal clusters in the gas phase. Additionally, doubly-negatively charged fullerenes were generated. The smallest fullerene dianion observed contained 70 atoms. (orig.)

  4. Stark effect of intrinsic and extrinsic charge-transfer excitons in a linear donor-acceptor stack: anthracene-pyromellitic dianhydride.

    Science.gov (United States)

    Weiser, Gerhard; Elschner, Andreas

    2009-06-25

    Anthracene-PMDA single crystals display at 2K about 70 meV below a well-known intrinsic charge-transfer exciton three narrow absorption lines, which are attributed to CT excitons bound to defects of a few 10(-5) concentration. All excitons respond very sensitively to electric fields along the molecular stack because of the large dipole moment, about 2 eA, of an ionized donor-acceptor pair, but only intrinsic excitons observe an optical selection rule. Although the triclinic unit cell contains only one pair of molecules, excitons appear in field-modulated spectra as near-degenerate doublets of different parity with very small splitting. The line shape of the EA spectra and selection rules with respect to the polarization of light and orientation of the field are consistent with the inversion symmetry of the lattice and the molecules. The simple crystal structure enables identification of the defects that are responsible for extrinsic excitons. Symmetry consideration based on translation invariance lead to a new interpretation of intrinsic excitons as true crystal states with charge transfer from the donor to the acceptor sublattice.

  5. Excitonic complexes in GaN/(Al,Ga)N quantum dots

    Science.gov (United States)

    Elmaghraoui, D.; Triki, M.; Jaziri, S.; Muñoz-Matutano, G.; Leroux, M.; Martinez-Pastor, J.

    2017-03-01

    Here we report a theoretical investigation of excitonic complexes in polar GaN/(Al,Ga)N quantum dots (QDs). A sum rule between the binding energies of charged excitons is used to calculate the biexciton binding energy. The binding energies of excitonic complexes in GaN/AlN are shown to be strongly correlated to the QD size. Due to the large hole localization, the positively charged exciton energy is found to be always blueshifted compared to the exciton one. The negatively charged exciton and the biexciton energy can be blueshifted or redshifted according to the QD size. Increasing the size of GaN/AlN QDs makes the identification of charged excitons difficult, and the use of an Al0.5Ga0.5N barrier can be advantageous for clear identification. Our theoretical results for the binding energy of exciton complexes are also confronted with values deduced experimentally for InAs/GaAs QDs, confirming our theoretical prediction for charged excitonic complexes in GaN/(Al,Ga)N QDs. Finally, we realize that the trends of excitonic complexes in QDs are significantly related to competition between the local charge separation (whatever its origin) and the correlation effect. Following our findings, entangled photons pairs can be produced in QDs with careful control of their size in order to obtain zero exciton–biexciton energy separation.

  6. Determining the spatial coherence of excitons from the photoluminescence spectrum in charge-transfer J-aggregates

    Science.gov (United States)

    Hestand, Nicholas J.; Spano, Frank C.

    2016-12-01

    The importance of spatial coherence in energy and charge transfer processes in biological systems and photovoltaic devices has been hotly debated over the past several years. While larger spatial coherences are thought to benefit transport, a clear correlation has yet to be established, partly because a simple and accurate measure of the coherence length has remained elusive. Previously, it was shown that the number of coherently connected chromophores, NCoh , can be determined directly from the ratio (SR) of the 0-0 and 0-1 vibronic line strengths in the photoluminescence (PL) spectrum. The relation NCoh = λ02SR, where λ02 is the associated monomeric Huang-Rhys parameter, was derived in the Frenkel exciton limit. Here, it is shown that SR remains a highly accurate measure of coherence for systems characterized by significant charge transfer interactions (e.g. conjugated π-stacked systems). The only requirement is that the exciton band curvature must be positive, as in a J-aggregate.

  7. A comparative theoretical study of exciton-dissociation and charge-recombination processes in oligothiophene/fullerene and oligothiophene/perylenediimide complexes for organic solar cells

    KAUST Repository

    Yi, Yuanping

    2011-01-01

    The exciton-dissociation and charge-recombination processes in donor-acceptor complexes found in α-sexithienyl/C60 and α-sexithienyl/perylenetetracarboxydiimide (PDI) solar cells are investigated by means of quantum-chemical methods. The electronic couplings and exciton-dissociation and charge-recombination rates have been evaluated for various configurations of the complexes. The results suggest that the decay of the lowest charge-transfer state to the ground state in the PDI-based devices: (i) is faster than that in the fullerene-based devices and (ii) in most cases, can compete with the dissociation of the charge-transfer state into mobile charge carriers. This faster charge-recombination process is consistent with the lower performance observed experimentally for the devices using PDI derivatives as the acceptor. © 2011 The Royal Society of Chemistry.

  8. Negative Trions Trapped by a Spherical Parabolic Quantum Dot

    Institute of Scientific and Technical Information of China (English)

    2006-01-01

    In this paper, a negatively charged exciton trapped by a spherical parabolic quantum dot has been investigated. The energy spectra of low-lying states are calculated by means of matrix diagonalization. The important feature of the low-lying states of the negatively charged excitons in a spherical quantum dot is obtained via an analysis of the energy spectra.

  9. Charged excitonic complexes in GaAs/Al0.35Ga0.65As p-i-n double quantum wells

    DEFF Research Database (Denmark)

    Timofeev, V. B.; Larionov, A. V.; Alessi, M. Grassi

    1999-01-01

    Photoluminescence (PL) and PL excitation measurements (PLE) have been performed in GaAs/AlxGa1-xAs double quantum well (QW) structures under different applied electric fields. An emission due to charged excitons (trions) has been identified in the PL spectra similar to 3 meV below the heavy...

  10. Electrostatic Power Generation from Negatively Charged, Simulated Lunar Regolith

    Science.gov (United States)

    Choi, Sang H.; King, Glen C.; Kim, Hyun-Jung; Park, Yeonjoon

    2010-01-01

    Research was conducted to develop an electrostatic power generator for future lunar missions that facilitate the utilization of lunar resources. The lunar surface is known to be negatively charged from the constant bombardment of electrons and protons from the solar wind. The resulting negative electrostatic charge on the dust particles, in the lunar vacuum, causes them to repel each other minimizing the potential. The result is a layer of suspended dust about one meter above the lunar surface. This phenomenon was observed by both Clementine and Surveyor spacecrafts. During the Apollo 17 lunar landing, the charged dust was a major hindrance, as it was attracted to the astronauts' spacesuits, equipment, and the lunar buggies. The dust accumulated on the spacesuits caused reduced visibility for the astronauts, and was unavoidably transported inside the spacecraft where it caused breathing irritation [1]. In the lunar vacuum, the maximum charge on the particles can be extremely high. An article in the journal "Nature", titled "Moon too static for astronauts?" (Feb 2, 2007) estimates that the lunar surface is charged with up to several thousand volts [2]. The electrostatic power generator was devised to alleviate the hazardous effects of negatively charged lunar soil by neutralizing the charged particles through capacitive coupling and thereby simultaneously harnessing power through electric charging [3]. The amount of power generated or collected is dependent on the areal coverage of the device and hovering speed over the lunar soil surface. A thin-film array of capacitors can be continuously charged and sequentially discharged using a time-differentiated trigger discharge process to produce a pulse train of discharge for DC mode output. By controlling the pulse interval, the DC mode power can be modulated for powering devices and equipment. In conjunction with a power storage system, the electrostatic power generator can be a power source for a lunar rover or other

  11. Single photon emission up to liquid nitrogen temperature from charged excitons confined in GaAs-based epitaxial nanostructures

    Energy Technology Data Exchange (ETDEWEB)

    Dusanowski, Ł., E-mail: lukasz.dusanowski@pwr.edu.pl; Syperek, M.; Maryński, A.; Misiewicz, J.; Sęk, G. [Laboratory for Optical Spectroscopy of Nanostructures, Department of Experimental Physics, Wrocław University of Technology, Wybrzeże Wyspiańskiego 27, 50-370 Wrocław (Poland); Li, L. H. [Ecole Polytechnique Fédérale de Lausanne, Institute of Quantum Electronics and Photonics, Station 3, CH-1015 Lausanne (Switzerland); Höfling, S. [Technische Physik and Wilhelm-Conrad-Röntgen-Research Center for Complex Material Systems, University of Würzburg, Am Hubland, D-97074 Würzburg (Germany); SUPA, School of Physics and Astronomy, University of St. Andrews, North Haugh, KY16 9SS St. Andrews (United Kingdom); Kamp, M. [Technische Physik and Wilhelm-Conrad-Röntgen-Research Center for Complex Material Systems, University of Würzburg, Am Hubland, D-97074 Würzburg (Germany); Fiore, A. [Ecole Polytechnique Fédérale de Lausanne, Institute of Quantum Electronics and Photonics, Station 3, CH-1015 Lausanne (Switzerland); COBRA Research Institute, Eindhoven University of Technology, PO Box 513, 5600 MB Eindhoven (Netherlands)

    2015-06-08

    We demonstrate a non-classical photon emitter at near infrared wavelength based on a single (In,Ga)As/GaAs epitaxially grown columnar quantum dot. Charged exciton complexes have been identified in magneto-photoluminescence. Photon auto-correlation histograms from the recombination of a trion confined in a columnar dot exhibit sub-Poissonian statistics with an antibunching dip yielding g{sup (2)}(0) values of 0.28 and 0.46 at temperature of 10 and 80 K, respectively. Our experimental findings allow considering the GaAs-based columnar quantum dot structure as an efficient single photon source operating at above liquid nitrogen temperatures, which in some characteristics can outperform the existing solutions of any material system.

  12. Exciton center-of-mass localization and dielectric environment effect in monolayer WS2

    Science.gov (United States)

    Hichri, Aïda; Ben Amara, Imen; Ayari, Sabrine; Jaziri, Sihem

    2017-06-01

    The ultrathin transition metal dichalcogenides (TMDs) have emerged as promising materials for various applications using two dimensional semiconductors. They have attracted increasing attention due to their unique optical properties originate from neutral and charged excitons. In this paper, we study the strong localization of exciton center-of-mass motion within random potential fluctuations caused by the monolayer defects. Here, we report negatively charged exciton formation in monolayer TMDs, notably tungsten disulfide WS2. Our theory is based on an effective mass model of neutral and charged excitons, parameterized by ab-initio calculations. Taking into the account the strong correlation between the monolayer WS2 and the surrounding dielectric environment, our theoretical results are in good agreement with one-photon photoluminescence (PL) and reflectivity measurements. We also show that the exciton state with p-symmetry, experimentally observed by two-photon PL emission, is energetically below the 2s-state. We use the equilibrium mass action law, to quantify the relative weight of exciton and trion PL. We show that exciton and trion emission can be tuned and controlled by external parameters like temperature, pumping, and injection electrons. Finally, in comparison with experimental measurements, we show that exciton emission in monolayer tungsten dichalcogenides is substantially reduced. This feature suggests that free exciton can be trapped in disordered potential wells to form a localized exciton and therefore offers a route toward novel optical properties.

  13. Magnetic field control of the neutral and charged exciton fine structure in single quantum dashes emitting at 1.55 μm

    Energy Technology Data Exchange (ETDEWEB)

    Mrowiński, P.; Musiał, A.; Maryński, A.; Syperek, M.; Misiewicz, J.; Sęk, G. [Laboratory for Optical Spectroscopy of Nanostructures, Department of Experimental Physics, Wrocław University of Technology, Wybrzeże Wyspiańskiego 27, Wrocław (Poland); Somers, A. [Technische Physik, University of Würzburg and Wilhelm-Conrad-Röntgen-Research Center for Complex Material Systems, Am Hubland, D-97074 Würzburg (Germany); Reithmaier, J. P. [Technische Physik, University of Würzburg and Wilhelm-Conrad-Röntgen-Research Center for Complex Material Systems, Am Hubland, D-97074 Würzburg (Germany); Institute of Nanostructure Technologies and Analytics (INA), CINSaT, University of Kassel, Heinrich-Plett-Str. 40, 34132 Kassel (Germany); Höfling, S. [Technische Physik, University of Würzburg and Wilhelm-Conrad-Röntgen-Research Center for Complex Material Systems, Am Hubland, D-97074 Würzburg (Germany); SUPA, School of Physics and Astronomy, University of St. Andrews, North Haugh, KY16 9SS St. Andrews (United Kingdom)

    2015-02-02

    We investigated the neutral and charged exciton fine structure in single InAs/InGaAlAs/InP quantum dashes emitting at 1.55 μm using polarization-resolved microphotoluminescence in a magnetic field. Inverted spin configuration of horizontally [1–10] and vertically [110] polarized transitions has been observed. An in-plane magnetic field of up to 5 Tesla has been applied to tailor the fine structure, and eventually to reduce the splitting of the bright exciton states down to zero. This inverted structure has been observed for all the investigated excitons, making it a characteristic feature for this class of nanostructures with the largest splitting reduction of 170 μeV.

  14. Arabinogalactan proteins are incorporated in negatively charged coffee brew melanoidins.

    Science.gov (United States)

    Bekedam, E Koen; De Laat, Marieke P F C; Schols, Henk A; Van Boekel, Martinus A J S; Smit, Gerrit

    2007-02-07

    The charge properties of melanoidins in high molecular weight (HMw) coffee brew fractions, isolated by diafiltration and membrane dialysis, were studied. Ion exchange chromatography experiments with the HMw fractions showed that coffee brew melanoidins were negatively charged whereas these molecules did not expose any positive charge at the pH of coffee brew. Fractions with different ionic charges were isolated and subsequently characterized by means of the specific extinction coefficient (K(mix 405nm)), sugar composition, phenolic group content, nitrogen content, and the arabinogalactan protein (AGP) specific Yariv gel-diffusion assay. The isolated fractions were different in composition and AGP was found to be present in one of the HMw fractions. The AGP accounted for 6% of the coffee brew dry matter and had a moderate negative charge, probably caused by the presence of uronic acids. As the fraction that precipitated with Yariv was brown (K(mix 405nm) = 1.2), compared to a white color in the green bean, it was concluded that these AGPs had undergone Maillard reaction resulting in an AGP-melanoidin complex. The presence of mannose (presumably from galactomannan) indicates the incorporation of galactomannans in the AGP-melanoidin complex. As the uronic acid content in the more negatively charged melanoidin-rich, AGP-poor HMw fractions decreased, it was hypothesized that acidic groups are formed or incorporated during melanoidin formation.

  15. Positive, Neutral, and Negative Mass-Charges in General Relativity

    Directory of Open Access Journals (Sweden)

    Borissova L.

    2006-07-01

    Full Text Available As shown, any four-dimensional proper vector has two observable projections onto time line, attributed to our world and the mirror world (for a mass-bearing particle, the projections posses are attributed to positive and negative mass-charges. As predicted, there should be a class of neutrally mass-charged particles that inhabit neither our world nor the mirror world. Inside the space-time area (membrane the space rotates at the light speed, and all particles move at as well the light speed. So, the predicted particles of the neutrally mass-charged class should seem as light-like vortices.

  16. Positive, Neutral and Negative Mass-Charges in General Relativity

    Directory of Open Access Journals (Sweden)

    Smarandache F.

    2006-07-01

    Full Text Available As shown, any four-dimensional proper vector has two observable projections onto time line, attributed to our world and the mirror world (for a mass-bearing particle, the projections posses are attributed to positive and negative mass-charges. As predicted, there should be a class of neutrally mass-charged particles that inhabit neither our world nor the mirror world. Inside the space-time area (membrane the space rotates at the light speed, and all particles move at as well the light speed. So, the predicted particles of the neutrally mass-charged class should seem as light-like vortices.

  17. Exciton-Dissociation and Charge-Recombination Processes in Pentacene/C 60 Solar Cells: Theoretical Insight into the Impact of Interface Geometry

    KAUST Repository

    Yi, Yuanping

    2009-11-04

    The exciton-dissociation and charge-recombination processes in organic solar cells based on pentacene/C60 heterojunctions are investigated by means of quantum-mechanical calculations. The electronic couplings and the rates of exciton dissociation and charge recombination have been evaluated for several geometrical configurations of the pentacene/C60 complex, which are relevant to bilayer and bulk heterojunctions. The results suggest that, irrespective of the actual pentacene-fullerene orientation, both pentacene-based and C60-based excitons are able to dissociate efficiently. Also, in the case of parallel configurations of the molecules at the pentacene/C60 interface, the decay of the lowest charge-transfer state to the ground state is calculated to be very fast; as a result, it can compete with the dissociation process into mobile charge carriers. Since parallel configurations are expected to be found more frequently in bulk heterojunctions than in bilayer heterojunctions, the performance of pentacene/C60 bulk-heterojunction solar cells is likely to be more affected by charge recombination than that of bilayer devices. © 2009 American Chemical Society.

  18. The interplay between neutral exciton and charge transfer states in single-strand polyadenine: a quantum dynamical investigation.

    Science.gov (United States)

    Santoro, Fabrizio; Improta, Roberto; Avila, Francisco; Segado, Mireia; Lami, Alessandro

    2013-08-01

    We investigate the quantum dynamics of the internal conversion of excitons into charge transfer (CT) states in single-strand oligomers of adenine (An) of different length (n up to 10 units) excited by a short-time laser pulse. Calculations are based on a model vibronic Hamiltonian whose parameters are fitted to accurate time-dependent density functional theory (TD-DFT) calculations, which was shown to reproduce the experimental absorption spectrum with the increase of n. As a first step, we analyze the impact of the vibrational motion on the population transfer in the dimer, highlighting that it causes loss of coherence and slows down the dynamics. For longer oligomers we resort to a simplified approach considering only electronic states and solving the equation of motion for the density matrix driven by inter-state couplings. In this way we are able also to include phenomenologically dephasing terms that mainly simulate intra-molecular effects, and lifetimes of local excitations mimicking monomer-like decay processes. Relaxation effects, whose role is to drive the system towards the thermal equilibrium allowing population exchange among states, are deliberately not considered here, since the focus is on very short-time dynamics. We consider both the cases of an instantaneous and of a finite-time (full width at half maximum 50 fs) laser pulse. According to our calculations, the photoexcited oligomers exhibit a complex dynamics and CT population rises on a 20-30 fs timescale and it persists even on the picosecond timescale. CT population increases with the length of the oligomer and it is only weakly dependent on the relative stability of CT and exciton states (within a range of 1500 cm(-1)). The chain length already modifies the photoexcited dynamics for A2 and A4 systems, but this effect saturates for small n so that the A10 oligomer is also representative of longer chains.

  19. Charge density wave and excitonic magnetic polarons in CeTe sub 2

    CERN Document Server

    Kasuya, T; Takabatake, T

    2000-01-01

    Mechanisms of anomalous magnetic and transport properties in CeTe sub 2 observed recently on single-crystal samples are studied by comparing with the nonmagnetic reference material LaTe sub 2 , as well as other typical low carrier-density systems such as Ce monopnictides, doped Eu chalcogenides and Yb sub 4 As sub 3. The present system is unique on the point of low-carrier semimetal due to CDW of near perfect nesting, which is shown to be nearly independent of the spin-orbit splitting. The large residual resistivity indicates the giant molecular scattering due to excitonic states forming the distorted Wigner crystal, similar to Yb sub 4 As sub 3. At low temperatures, induced magnetic polarons cause unusual novel transport properties with a sharp peak of resistivity without any anomaly on other physical properties. This is attributed to a sharp glassy transition from an antiferromagnetic short-range ordering to the ferromagnetic ordering of the magnetic polarons within each CeTe double layer sandwiching the mo...

  20. Direct quantification of negatively charged functional groups on membrane surfaces

    KAUST Repository

    Tiraferri, Alberto

    2012-02-01

    Surface charge plays an important role in membrane-based separations of particulates, macromolecules, and dissolved ionic species. In this study, we present two experimental methods to determine the concentration of negatively charged functional groups at the surface of dense polymeric membranes. Both techniques consist of associating the membrane surface moieties with chemical probes, followed by quantification of the bound probes. Uranyl acetate and toluidine blue O dye, which interact with the membrane functional groups via complexation and electrostatic interaction, respectively, were used as probes. The amount of associated probes was quantified using liquid scintillation counting for uranium atoms and visible light spectroscopy for the toluidine blue dye. The techniques were validated using self-assembled monolayers of alkanethiols with known amounts of charged moieties. The surface density of negatively charged functional groups of hand-cast thin-film composite polyamide membranes, as well as commercial cellulose triacetate and polyamide membranes, was quantified under various conditions. Using both techniques, we measured a negatively charged functional group density of 20-30nm -2 for the hand-cast thin-film composite membranes. The ionization behavior of the membrane functional groups, determined from measurements with toluidine blue at varying pH, was consistent with published data for thin-film composite polyamide membranes. Similarly, the measured charge densities on commercial membranes were in general agreement with previous investigations. The relative simplicity of the two methods makes them a useful tool for quantifying the surface charge concentration of a variety of surfaces, including separation membranes. © 2011 Elsevier B.V.

  1. Efficient charge-carrier extraction from Ag2S quantum dots prepared by the SILAR method for utilization of multiple exciton generation

    Science.gov (United States)

    Zhang, Xiaoliang; Liu, Jianhua; Johansson, Erik M. J.

    2015-01-01

    The utilization of electron-hole pairs (EHPs) generated from multiple excitons in quantum dots (QDs) is of great interest toward efficient photovoltaic devices and other optoelectronic devices; however, extraction of charge carriers remains difficult. Herein, we extract photocharges from Ag2S QDs and investigate the dependence of the electric field on the extraction of charges from multiple exciton generation (MEG). Low toxic Ag2S QDs are directly grown on TiO2 mesoporous substrates by employing the successive ionic layer adsorption and reaction (SILAR) method. The contact between QDs is important for the initial charge separation after MEG and for the carrier transport, and the space between neighbor QDs decreases with more SILAR cycles, resulting in better charge extraction. At the optimal electric field for extraction of photocharges, the results suggest that the threshold energy (hνth) for MEG is 2.41Eg. The results reveal that Ag2S QD is a promising material for efficient extraction of charges from MEG and that QDs prepared by SILAR have an advantageous electrical contact facilitating charge separation and extraction.The utilization of electron-hole pairs (EHPs) generated from multiple excitons in quantum dots (QDs) is of great interest toward efficient photovoltaic devices and other optoelectronic devices; however, extraction of charge carriers remains difficult. Herein, we extract photocharges from Ag2S QDs and investigate the dependence of the electric field on the extraction of charges from multiple exciton generation (MEG). Low toxic Ag2S QDs are directly grown on TiO2 mesoporous substrates by employing the successive ionic layer adsorption and reaction (SILAR) method. The contact between QDs is important for the initial charge separation after MEG and for the carrier transport, and the space between neighbor QDs decreases with more SILAR cycles, resulting in better charge extraction. At the optimal electric field for extraction of photocharges, the

  2. Membrane Permeabilization Induced by Sphingosine: Effect of Negatively Charged Lipids

    Science.gov (United States)

    Jiménez-Rojo, Noemi; Sot, Jesús; Viguera, Ana R.; Collado, M. Isabel; Torrecillas, Alejandro; Gómez-Fernández, J.C.; Goñi, Félix M.; Alonso, Alicia

    2014-01-01

    Sphingosine [(2S, 3R, 4E)-2-amino-4-octadecen-1, 3-diol] is the most common sphingoid long chain base in sphingolipids. It is the precursor of important cell signaling molecules, such as ceramides. In the last decade it has been shown to act itself as a potent metabolic signaling molecule, by activating a number of protein kinases. Moreover, sphingosine has been found to permeabilize phospholipid bilayers, giving rise to vesicle leakage. The present contribution intends to analyze the mechanism by which this bioactive lipid induces vesicle contents release, and the effect of negatively charged bilayers in the release process. Fluorescence lifetime measurements and confocal fluorescence microscopy have been applied to observe the mechanism of sphingosine efflux from large and giant unilamellar vesicles; a graded-release efflux has been detected. Additionally, stopped-flow measurements have shown that the rate of vesicle permeabilization increases with sphingosine concentration. Because at the physiological pH sphingosine has a net positive charge, its interaction with negatively charged phospholipids (e.g., bilayers containing phosphatidic acid together with sphingomyelins, phosphatidylethanolamine, and cholesterol) gives rise to a release of vesicular contents, faster than with electrically neutral bilayers. Furthermore, phosphorous 31-NMR and x-ray data show the capacity of sphingosine to facilitate the formation of nonbilayer (cubic phase) intermediates in negatively charged membranes. The data might explain the pathogenesis of Niemann-Pick type C1 disease. PMID:24940775

  3. Internal Electric Field In The Space Charge Layer Of A Solar Cell Based On Silicon In The Presence Of Excitons

    Directory of Open Access Journals (Sweden)

    Modou Faye

    2015-08-01

    Full Text Available Abstract The author faced with the impossibility of assessing the relative importance of the different contributions of physical quantities appearing in the equations of transport he appealed to the dimensional analysis. Thus by grouping the physical parameters the dependent and independent variables it generates dimensionless numbers. The latter having a physical significance make it possible to characterize the various contributions. To solve the dimensionless equations obtained strongly coupled reduced scale the author opts for a numerical method. The spatial discretization variable pitch and tight at the interfaces of different zones of the field because of the strong gradients in these regions is adopted. The equations are then integrated in the numerical domain using the finite volume method and the coefficients are approached by the schema of the power Patankar law. The resulting system of algebraic equations is solved by the method of double course combined with an iterative relaxation line by line type Gauss-Seidel. Furthermore with a volumetric coefficient of coupling which depends on the dissociation of the excitons and the average temperature field the author has studied the influence of some physical parameters on the total density of photocurrent such that the heating factor the conversion velocity and the volume coupling coefficient of charge carriers.

  4. Distinct exciton dissociation behavior of organolead trihalide perovskite and excitonic semiconductors studied in the same system.

    Science.gov (United States)

    Hu, Miao; Bi, Cheng; Yuan, Yongbo; Xiao, Zhengguo; Dong, Qingfeng; Shao, Yuchuan; Huang, Jinsong

    2015-05-13

    The nonexcitonic character for organometal trihalide perovskites is demonstrated by examining the field-dependent exciton dissociation behavior. It is found that photogenerated excitons can be effectively dissociated into free charges inside perovskite without the assistance of charge extraction layer or external field, which is a stark contrast to the charge-separation behavior in excitonic materials in the same photovoltaic operation system.

  5. Study on space charge compensation in negative hydrogen ion beam

    Energy Technology Data Exchange (ETDEWEB)

    Zhang, A. L.; Chen, J. E. [University of Chinese Academy of Sciences, Beijing 100049 (China); State Key Laboratory of Nuclear Physics and Technology, Institute of Heavy Ion Physics, School of Physics, Peking University, Beijing 100871 (China); Peng, S. X., E-mail: sxpeng@pku.edu.cn; Ren, H. T.; Zhang, T.; Zhang, J. F.; Xu, Y.; Guo, Z. Y. [State Key Laboratory of Nuclear Physics and Technology, Institute of Heavy Ion Physics, School of Physics, Peking University, Beijing 100871 (China)

    2016-02-15

    Negative hydrogen ion beam can be compensated by the trapping of ions into the beam potential. When the beam propagates through a neutral gas, these ions arise due to gas ionization by the beam ions. However, the high neutral gas pressure may cause serious negative hydrogen ion beam loss, while low neutral gas pressure may lead to ion-ion instability and decompensation. To better understand the space charge compensation processes within a negative hydrogen beam, experimental study and numerical simulation were carried out at Peking University (PKU). The simulation code for negative hydrogen ion beam is improved from a 2D particle-in-cell-Monte Carlo collision code which has been successfully applied to H{sup +} beam compensated with Ar gas. Impacts among ions, electrons, and neutral gases in negative hydrogen beam compensation processes are carefully treated. The results of the beam simulations were compared with current and emittance measurements of an H{sup −} beam from a 2.45 GHz microwave driven H{sup −} ion source in PKU. Compensation gas was injected directly into the beam transport region to modify the space charge compensation degree. The experimental results were in good agreement with the simulation results.

  6. Study on space charge compensation in negative hydrogen ion beam.

    Science.gov (United States)

    Zhang, A L; Peng, S X; Ren, H T; Zhang, T; Zhang, J F; Xu, Y; Guo, Z Y; Chen, J E

    2016-02-01

    Negative hydrogen ion beam can be compensated by the trapping of ions into the beam potential. When the beam propagates through a neutral gas, these ions arise due to gas ionization by the beam ions. However, the high neutral gas pressure may cause serious negative hydrogen ion beam loss, while low neutral gas pressure may lead to ion-ion instability and decompensation. To better understand the space charge compensation processes within a negative hydrogen beam, experimental study and numerical simulation were carried out at Peking University (PKU). The simulation code for negative hydrogen ion beam is improved from a 2D particle-in-cell-Monte Carlo collision code which has been successfully applied to H(+) beam compensated with Ar gas. Impacts among ions, electrons, and neutral gases in negative hydrogen beam compensation processes are carefully treated. The results of the beam simulations were compared with current and emittance measurements of an H(-) beam from a 2.45 GHz microwave driven H(-) ion source in PKU. Compensation gas was injected directly into the beam transport region to modify the space charge compensation degree. The experimental results were in good agreement with the simulation results.

  7. Efficient charge-carrier extraction from Ag₂S quantum dots prepared by the SILAR method for utilization of multiple exciton generation.

    Science.gov (United States)

    Zhang, Xiaoliang; Liu, Jianhua; Johansson, Erik M J

    2015-01-28

    The utilization of electron-hole pairs (EHPs) generated from multiple excitons in quantum dots (QDs) is of great interest toward efficient photovoltaic devices and other optoelectronic devices; however, extraction of charge carriers remains difficult. Herein, we extract photocharges from Ag2S QDs and investigate the dependence of the electric field on the extraction of charges from multiple exciton generation (MEG). Low toxic Ag2S QDs are directly grown on TiO2 mesoporous substrates by employing the successive ionic layer adsorption and reaction (SILAR) method. The contact between QDs is important for the initial charge separation after MEG and for the carrier transport, and the space between neighbor QDs decreases with more SILAR cycles, resulting in better charge extraction. At the optimal electric field for extraction of photocharges, the results suggest that the threshold energy (hνth) for MEG is 2.41Eg. The results reveal that Ag2S QD is a promising material for efficient extraction of charges from MEG and that QDs prepared by SILAR have an advantageous electrical contact facilitating charge separation and extraction.

  8. Coherent dynamics of mixed Frenkel and Charge Transfer Excitons in Dinaphtho[2,3-b:2'3'-f]thieno[3,2-b]-thiophene Thin Films: The Importance of Hole Delocalization

    CERN Document Server

    Fujita, Takatoshi; Sawaya, Nicolas P D; Aspuru-Guzik, Alan

    2016-01-01

    Charge transfer states in organic semiconductors play crucial roles in processes such as singlet fission and exciton dissociation at donor/acceptor interfaces. Recently, a time-resolved spectroscopy study of dinaphtho[2,3-b:2'3'-f]thieno[3,2-b]-thiophene (DNTT) thin films provided evidence for the formation of mixed Frenkel and charge-transfer excitons after the photoexcitation. Here we investigate optical properties and excitation dynamics of the DNTT thin films by combining ab initio calculations and a stochastic Schrodinger equation. Our theory predicts that the low-energy Frenkel exciton band consists of 8 to 47% CT character. The quantum dynamics simulations show coherent dynamics of Frenkel and CT states in 50 fs after the optical excitation. We demonstrate the role of charge delocalization and localization in the mixing of CT states with Frenkel excitons as well as the role of their decoherence.

  9. Effect of uniaxial compression on traps of excitons and charge carriers in poly(9-vinylcarbazole) films

    Science.gov (United States)

    Skryshevski, Yu. A.

    2014-03-01

    The effect of uniaxial pressure (1 × 108 Pa) on the photoluminescence spectra and thermally stimulated luminescence curves of poly(9-vinylcarbazole) has been investigated in the temperature range of 5-295 K. The thermally stimulated luminescence curve of crystalline carbazole has been measured for comparison. The high-temperature wings of the thermally stimulated luminescence curves are approximated by a Gaussian function, the half-width of which characterizes the disorder of energy states of deep structural traps. It is concluded that the pressure inhibits conformational changes of polymer chains of poly(9-vinylcarbazole), which leads to the formation of sandwich-like excimers as well as to an ordering of the spatial arrangement of the side carbazolyl groups. As a result, the concentration of "excimer-forming" centers increases, whereas the degree of disorder of energy states of deep structural traps of charge carriers is reduced by almost half and remains unchanged after the depressurization.

  10. Dimensional and correlation effects of charged excitons in low-dimensional semiconductors

    Energy Technology Data Exchange (ETDEWEB)

    Roennow, Troels F; Pedersen, Thomas G [Department of Physics and Nanotechnology, Aalborg University, Skjernvej 4A, 9220 Aalborg Oest (Denmark); Cornean, Horia D, E-mail: tfr@nanophysics.d [Department of Mathematical Sciences, Aalborg University, Frederik Bajers Vej 7G, 9220 Aalborg (Denmark)

    2010-11-26

    In this paper, we investigate the existence of bound trion states in fractional dimensional nanostructures, in terms of variational calculus. We start with trial states, then we refine the result with the help of the Hartree-Fock approximation and finally we use a partial basis expansion. We show that Hartree-Fock significantly underestimates the trion binding energy and that the correlation energy is comparable with the trion binding energy. Furthermore we calculate the binding energies of positive and negative trions restricted to a large subspace of functions, which we expect to span the low-lying eigenstates of the full Hamiltonian. We find that the difference between the positive and negative trion binding energies varies very little for the electron-hole mass fractions m{sub e}/m{sub h} = {sigma} in [0.8; 1.0] and that the difference between the positive and negative trion energies grows as the dimension decreases. Finally, we compare a cylindrical effective-mass model of a typical carbon nanotube, with a fractional dimensional model with D = 1.71. We find very good agreement between the trion binding energies predicted by the two models.

  11. Auger Recombination in Self-Assembled Quantum Dots: Quenching and Broadening of the Charged Exciton Transition.

    Science.gov (United States)

    Kurzmann, Annika; Ludwig, Arne; Wieck, Andreas D; Lorke, Axel; Geller, Martin

    2016-05-11

    In quantum dots (QDs), the Auger recombination is a nonradiative process in which the electron-hole recombination energy is transferred to an additional carrier. It has been studied mostly in colloidal QDs, where the Auger recombination time is in the picosecond range and efficiently quenches the light emission. In self-assembled QDs, on the other hand, the influence of Auger recombination on the optical properties is in general neglected, assuming that it is masked by other processes such as spin and charge fluctuations. Here, we use time-resolved resonance fluorescence to analyze the Auger recombination and its influence on the optical properties of a single self-assembled QD. From excitation-power-dependent measurements, we find a long Auger recombination time of about 500 ns and a quenching of the trion transition by about 80%. Furthermore, we observe a broadening of the trion transition line width by up to a factor of 2. With a model based on rate equations, we are able to identify the interplay between tunneling and Auger rate as the underlying mechanism for the reduced intensity and the broadening of the line width. This demonstrates that self-assembled QDs can serve as an ideal model system to study how the charge recapture process, given by the band-structure surrounding the confined carriers, influences the Auger process. Our findings are not only relevant for improving the emission properties of colloidal QD-based emitters and dyes, which have recently entered the consumer market, but also of interest for more visionary applications, such as quantum information technologies, based on self-assembled quantum dots.

  12. Tuning the g-factor of neutral and charged excitons confined to self-assembled (Al,Ga)As shell quantum dots

    Energy Technology Data Exchange (ETDEWEB)

    Corfdir, P., E-mail: corfdir@pdi-berlin.de; Van Hattem, B.; Phillips, R. T. [Cavendish Laboratory, University of Cambridge, J. J. Thomson Avenue, Cambridge CB3 0HE (United Kingdom); Fontana, Y.; Russo-Averchi, E.; Heiss, M.; Fontcuberta i Morral, A. [Laboratoire des Matériaux Semiconducteurs, Institut des Matériaux, École Polytechnique Fédérale de Lausanne, 1015 Lausanne (Switzerland)

    2014-12-01

    We study the neutral exciton (X) and charged exciton (CX) transitions from (Al,Ga)As shell quantum dots located in core-shell nanowires, in the presence of a magnetic field. The g-factors and the diamagnetic coefficients of both the X and the CX depend on the orientation of the field with respect to the nanowire axis. The aspect ratio of the X wavefunction is quantified based on the anisotropy of the diamagnetic coefficient. For specific orientations of the magnetic field, it is possible to cancel the g-factor of the bright states of the X and the CX by means of an inversion of the sign of the hole's g-factor, which is promising for quantum information processing applications.

  13. Negative thermal expansion induced by intermetallic charge transfer.

    Science.gov (United States)

    Azuma, Masaki; Oka, Kengo; Nabetani, Koichiro

    2015-06-01

    Suppression of thermal expansion is of great importance for industry. Negative thermal expansion (NTE) materials which shrink on heating and expand on cooling are therefore attracting keen attention. Here we provide a brief overview of NTE induced by intermetallic charge transfer in A-site ordered double perovskites SaCu3Fe4O12 and LaCu3Fe4-x Mn x O12, as well as in Bi or Ni substituted BiNiO3. The last compound shows a colossal dilatometric linear thermal expansion coefficient exceeding -70 × 10(-6) K(-1) near room temperature, in the temperature range which can be controlled by substitution.

  14. Negative plates for dry-charged lead storage batteries. [higher charging capacity when impregnated with tannin solution

    Energy Technology Data Exchange (ETDEWEB)

    Fiedler, V.; Malikova, V.; Weber, H.

    1970-09-15

    Impregnation of negative plates with acid solutions of sulfomethylated tannins was found to improve the charging properties at low temperatures. Methods for synthesizing tannins are described. Charging capacity at 0/sup 0/ was 7.3A. (RWR)

  15. Charge carrier resolved relaxation of the first excitonic state in CdSe quantum dots probed with near-infrared transient absorption spectroscopy.

    Science.gov (United States)

    McArthur, Eric A; Morris-Cohen, Adam J; Knowles, Kathryn E; Weiss, Emily A

    2010-11-18

    This manuscript describes a global regression analysis of near-infrared (NIR, 900-1300 nm) transient absorptions (TA) of colloidal CdSe quantum dots (QDs) photoexcited to their first (1S(e)1S(3/2)) excitonic state. Near-IR TA spectroscopy facilitates charge carrier-resolved analysis of excitonic decay of QDs because signals in the NIR are due exclusively to absorptions of photoexcited electrons and holes, as probe energies in this region are not high enough to induce absorptions across the optical bandgap that crowd the visible TA spectra. The response of each observed component of the excitonic decay to the presence of a hole-trapping ligand (1-octanethiol) and an electron-accepting ligand (1,4-benzoquinone), and comparison of time constants to those for recovery of the ground state bleaching feature in the visible TA spectrum, allow for the assignment of the components to (i) a 1.6 ps hole trapping process, (ii) 19 ps and 274 ps surface-mediated electron trapping processes, and (iii) a ∼5 ns recombination of untrapped electrons.

  16. Negatively charged crown ethers for binding paraquat in water

    Institute of Scientific and Technical Information of China (English)

    2010-01-01

    A water soluble negatively charged fluorescent 1,4-benzo-1,5-naphtho-36-crown-10-based host has been devised and synthesized.As shown by proton NMR,ESI mass spectrometry and UV-vis spectroscopy,it binds paraquat with a 1:1 stoichiometry and an association constant of 4.50(±0.02) ×103 M-1 in water.Its complexation with paraquat in water was further investigated by fluorescence emission spectroscopy.The results revealed that when paraquat was added to the water solution of the host,the fluorescence emission of the host was quenched by the charge transfer between the crown ether host and paraquat guest.A similar bis-p-phenylene-34-crown-10-based host was synthesized as a contrasting host.Lacking the naphthalene unit,the second host binds paraquat with a 1:1 stoichiometry and a lower association constant,1.04(±0.04) ×103 M-1,in water.This demonstrated that the naphthalene unit could not only act as a strong fluorescence group but also improve the π-πstacking interactions between the host and guest.

  17. Conformation-related exciton localization and charge-pair formation in polythiophenes: ensemble and single-molecule study.

    Science.gov (United States)

    Sugimoto, Toshikazu; Habuchi, Satoshi; Ogino, Kenji; Vacha, Martin

    2009-09-10

    We study conformation-dependent photophysical properties of polythiophene (PT) by molecular dynamics simulations and by ensemble and single-molecule optical experiments. We use a graft copolymer consisting of a polythiophene backbone and long polystyrene branches and compare its properties with those obtained on the same polythiophene derivative without the side chains. Coarse-grain molecular dynamics simulations show that in a poor solvent, the PT without the side chains (PT-R) forms a globulelike conformation in which distances between any two conjugated segments on the chain are within the Forster radius for efficient energy transfer. In the PT with the polystyrene branches (PT-PS), the polymer main PT chain retains an extended coillike conformation, even in a poor solvent, and the calculated distances between conjugated segments favor energy transfer only between a few neighboring chromophores. The theoretical predictions are confirmed by measurements of fluorescence anisotropy and fluorescence blinking of the polymers' single chains. High anisotropy ratios and two-state blinking in PT-R are due to localization of the exciton on a single conjugated segment. These signatures of exciton localization are absent in single chains of PT-PS. Electric-field-induced quenching measured as a function of concentration of PT dispersed in an inert matrix showed that in well-isolated chains of PT-PS, the exciton dissociation is an intrachain process and that aggregation of the PT-R chains causes an increase in quenching due to the onset of interchain interactions. Measurements of the field-induced quenching on single chains indicate that in PT-R, the exciton dissociation is a slower process that takes place only after the exciton is localized on one conjugated segment.

  18. Controllable transition from positive space charge to negative space charge in an inverted cylindrical magnetron

    Energy Technology Data Exchange (ETDEWEB)

    Rane, R., E-mail: ramu@ipr.res.in; Ranjan, M.; Mukherjee, S. [FCIPT, Institute for Plasma Research, Gandhinagar-382044 (India); Bandyopadhyay, M. [ITER-India, Institute for Plasma Research, Gandhinagar-382044 (India)

    2016-01-15

    The combined effect of magnetic field (B), gas pressure (P), and the corresponding discharge voltage on the discharge properties of argon in inverted cylindrical magnetron has been investigated. In the experiment, anode is biased with continuous 10 ms sinusoidal half wave. It is observed that at a comparatively higher magnetic field (i.e., >200 gauss) and lower operating pressure (i.e., <1 × 10{sup −3} mbar), the discharge extinguishes and demands a high voltage to reignite. Discharge current increases with increase in magnetic field and starts reducing at sufficiently higher magnetic field for a particular discharge voltage due to restricted electron diffusion towards the anode. It is observed that B/P ratio plays an important role in sustaining the discharge and is constant for a discharge voltage. The discharge is transformed to negative space charge regime from positive space charge regime at certain B/P ratio and this ratio varies linearly with the discharge voltage. The space charge reversal is indicated by the radial profile of the floating potential and plasma potential in between two electrodes for different magnetic fields. At a particular higher magnetic field (beyond 100 gauss), the floating potential increases gradually with the radial distance from cathode, whereas it remains almost constant at lower magnetic field.

  19. Exciton generation/dissociation/charge-transfer enhancement in inorganic/organic hybrid solar cells by robust single nanocrystalline LnPxOy (Ln = Eu, Y) doping.

    Science.gov (United States)

    Jin, Xiao; Sun, Weifu; Chen, Zihan; Wei, Taihuei; Chen, Chuyang; He, Xingdao; Yuan, Yongbiao; Li, Yue; Li, Qinghua

    2014-06-11

    Low-temperature solution-processed photovoltaics suffer from low efficiencies because of poor exciton or electron-hole transfer. Inorganic/organic hybrid solar cell, although still in its infancy, has attracted great interest thus far. One of the promising ways to enhance exciton dissociation or electron-hole transport is the doping of lanthanide phosphate ions. However, the underlying photophysical mechanism remains poorly understood. Herein, by applying femtosecond transient absorption spectroscopy, we successfully distinguished hot electron, less energetic electron, hole transport from electron-hole recombination. Concrete evidence has been provided that lanthanide phosphate doping improves the efficiency of both hot electron and "less energetic" electron transfers from donor to acceptor, but the hole transport almost remains unchanged. In particular, the hot electron transfer lifetime was shortened from 30.2 to 12.7 ps, that is, more than 60% faster than pure TiO2 acceptor. Such improvement was ascribed to the facts that the conduction band (CB) edge energy level of TiO2 has been elevated by 0.2 eV, while the valence band level almost remains unchanged, thus not only narrowing the energy offset between CB levels of TiO2 and P3HT, but also meanwhile enlarging the band gap of TiO2 itself that permits one to inhibit electron-hole recombination within TiO2. Consequently, lanthanide phosphate doped TiO2/P3HT bulk-heterojunction solar cell has been demonstrated to be a promising hybrid solar cell, and a notable power conversion efficiency of 2.91% is therefore attained. This work indicates that lanthanide compound ions can efficiently facilitate exciton generation, dissociation, and charge transport, thus enhancing photovoltaic performance.

  20. Negative differential mobility for negative carriers as revealed by space charge measurements on crosslinked polyethylene insulated model cables

    Science.gov (United States)

    Teyssedre, G.; Vu, T. T. N.; Laurent, C.

    2015-12-01

    Among features observed in polyethylene materials under relatively high field, space charge packets, consisting in a pulse of net charge that remains in the form of a pulse as it crosses the insulation, are repeatedly observed but without complete theory explaining their formation and propagation. Positive charge packets are more often reported, and the models based on negative differential mobility(NDM) for the transport of holes could account for some charge packets phenomenology. Conversely, NDM for electrons transport has never been reported so far. The present contribution reports space charge measurements by pulsed electroacoustic method on miniature cables that are model of HVDC cables. The measurements were realized at room temperature or with a temperature gradient of 10 °C through the insulation under DC fields on the order 30-60 kV/mm. Space charge results reveal systematic occurrence of a negative front of charges generated at the inner electrode that moves toward the outer electrode at the beginning of the polarization step. It is observed that the transit time of the front of negative charge increases, and therefore the mobility decreases, with the applied voltage. Further, the estimated mobility, in the range 10-14-10-13 m2 V-1 s-1 for the present results, increases when the temperature increases for the same condition of applied voltage. The features substantiate the hypothesis of negative differential mobility used for modelling space charge packets.

  1. From Recombination Dynamics to Device Performance: Quantifying the Efficiency of Exciton Dissociation, Charge Separation, and Extraction in Bulk Heterojunction Solar Cells with Fluorine-Substituted Polymer Donors

    KAUST Repository

    Gorenflot, Julien

    2017-09-28

    An original set of experimental and modeling tools is used to quantify the yield of each of the physical processes leading to photocurrent generation in organic bulk heterojunction solar cells, enabling evaluation of materials and processing condition beyond the trivial comparison of device performances. Transient absorption spectroscopy, “the” technique to monitor all intermediate states over the entire relevant timescale, is combined with time-delayed collection field experiments, transfer matrix simulations, spectral deconvolution, and parametrization of the charge carrier recombination by a two-pool model, allowing quantification of densities of excitons and charges and extrapolation of their kinetics to device-relevant conditions. Photon absorption, charge transfer, charge separation, and charge extraction are all quantified for two recently developed wide-bandgap donor polymers: poly(4,8-bis((2-ethylhexyl)oxy)benzo[1,2-b:4,5-b′]dithiophene-3,4-difluorothiophene) (PBDT[2F]T) and its nonfluorinated counterpart poly(4,8-bis((2-ethylhexyl)oxy)benzo[1,2-b:4,5-b′]dithiophene-3,4-thiophene) (PBDT[2H]T) combined with PC71BM in bulk heterojunctions. The product of these yields is shown to agree well with the devices\\' external quantum efficiency. This methodology elucidates in the specific case studied here the origin of improved photocurrents obtained when using PBDT[2F]T instead of PBDT[2H]T as well as upon using solvent additives. Furthermore, a higher charge transfer (CT)-state energy is shown to lead to significantly lower energy losses (resulting in higher VOC) during charge generation compared to P3HT:PCBM.

  2. Exciton Transport in Organic Semiconductors

    Science.gov (United States)

    Menke, Stephen Matthew

    Photovoltaic cells based on organic semiconductors are attractive for their use as a renewable energy source owing to their abundant feedstock and compatibility with low-cost coating techniques on flexible substrates. In contrast to photovoltaic cells based traditional inorganic semiconductors, photon absorption in an organic semiconductor results in the formation of a coulombically bound electron-hole pair, or exciton. The transport of excitons, consequently, is of critical importance as excitons mediate the interaction between charge and light in organic photovoltaic cells (OPVs). In this dissertation, a strong connection between the fundamental photophysical parameters that control nanoscopic exciton energy transfer and the mesoscopic exciton transport is established. With this connection in place, strategies for enhancing the typically short length scale for exciton diffusion (L D) can be developed. Dilution of the organic semiconductor boron subphthalocyanine chloride (SubPc) is found to increase the LD for SubPc by 50%. In turn, OPVs based on dilute layers of SubPc exhibit a 30% enhancement in power conversion efficiency. The enhancement in power conversion efficiency is realized via enhancements in LD, optimized optical spacing, and directed exciton transport at an exciton permeable interface. The role of spin, energetic disorder, and thermal activation on L D are also addressed. Organic semiconductors that exhibit thermally activated delayed fluorescence and efficient intersystem and reverse intersystem crossing highlight the balance between singlet and triplet exciton energy transfer and diffusion. Temperature dependent measurements for LD provide insight into the inhomogeneously broadened exciton density of states and the thermal nature of exciton energy transfer. Additional topics include energy-cascade OPV architectures and broadband, spectrally tunable photodetectors based on organic semiconductors.

  3. Formation of Negatively Charged AgI Colloid Nanoparticles by Condensation

    OpenAIRE

    Kalniņa, D; Gross, K; Medvids, A.; Onufrijevs, P.

    2015-01-01

    The stability of silver halide colloids is reported to be important for the toxicological outcome. This study shows a well-suited and cheap condensation reaction to obtain negatively charged silver iodide (AgI) nanoparticles without additional stabilization agents. Charged AgI colloids were synthesized from silver nitrate and potassium iodide solutions. An excess of potassium iodide not only imparted a negative charge, but provided a narrow particle size distribution (50 ± 10 n...

  4. Negative differential mobility for negative carriers as revealed by space charge measurements on crosslinked polyethylene insulated model cables

    Energy Technology Data Exchange (ETDEWEB)

    Teyssedre, G., E-mail: gilbert.teyssedre@laplace.univ-tlse.fr; Laurent, C. [Université de Toulouse, UPS, INPT, LAPLACE (Laboratoire Plasma et Conversion d' Energie), 118 route de Narbonne, F-31062 Toulouse cedex 9 (France); CNRS, LAPLACE, F-31062 Toulouse (France); Vu, T. T. N. [Université de Toulouse, UPS, INPT, LAPLACE (Laboratoire Plasma et Conversion d' Energie), 118 route de Narbonne, F-31062 Toulouse cedex 9 (France); Electric Power University, 235 Hoang Quoc Viet, 10000 Hanoi (Viet Nam)

    2015-12-21

    Among features observed in polyethylene materials under relatively high field, space charge packets, consisting in a pulse of net charge that remains in the form of a pulse as it crosses the insulation, are repeatedly observed but without complete theory explaining their formation and propagation. Positive charge packets are more often reported, and the models based on negative differential mobility(NDM) for the transport of holes could account for some charge packets phenomenology. Conversely, NDM for electrons transport has never been reported so far. The present contribution reports space charge measurements by pulsed electroacoustic method on miniature cables that are model of HVDC cables. The measurements were realized at room temperature or with a temperature gradient of 10 °C through the insulation under DC fields on the order 30–60 kV/mm. Space charge results reveal systematic occurrence of a negative front of charges generated at the inner electrode that moves toward the outer electrode at the beginning of the polarization step. It is observed that the transit time of the front of negative charge increases, and therefore the mobility decreases, with the applied voltage. Further, the estimated mobility, in the range 10{sup −14}–10{sup −13} m{sup 2} V{sup −1} s{sup −1} for the present results, increases when the temperature increases for the same condition of applied voltage. The features substantiate the hypothesis of negative differential mobility used for modelling space charge packets.

  5. Energy dependence of negatively charged pion production in proton-proton interactions at the CERN SPS

    CERN Document Server

    AUTHOR|(SzGeCERN)663936; Dominik, Wojciech; Gaździck, Marek

    2016-01-01

    This thesis presents inclusive spectra of the negatively charged pions produced in inelastic proton-proton interactions measured at five beam momenta: 20, 31, 40, 80 and 158 GeV/c. The measurements were conducted in the NA61/SHINE experiment at CERN using a system of five Time Projection Chambers. The negatively charged pion spectra were calculated based on the negatively charged hadron spectra. Contribution of hadrons other than the primary pions was removed using EPOS simulations. The results were corrected for effects related to detection, acceptance, reconstruction efficiency and the analysis technique. Two-dimensional spectra were derived as a function of rapidity and transverse momentum or transverse mass. The spectra were parametrised by widths of the rapidity distributions, inverse slope parameters of the transverse mass distributions, mean transverse masses and the total pion multiplicities. The negatively charged pion spectra in proton-proton interactions belong to a broad NA61/SHINE programme of se...

  6. Aberration of a negative ion beam caused by space charge effect

    Energy Technology Data Exchange (ETDEWEB)

    Miyamoto, K. [Naruto University of Education, 748 Nakashima, Takashima, Naruto-cho, Naruto-shi, Tokushima 772-8502 (Japan); Wada, S.; Hatayama, A. [Faculty of Science and Technology, Keio University, 3-14-1 Hiyoshi, Kohoku-ku, Yokohama 223-8522 (Japan)

    2010-02-15

    Aberrations are inevitable when the charged particle beams are extracted, accelerated, transmitted, and focused with electrostatic and magnetic fields. In this study, we investigate the aberration of a negative ion accelerator for a neutral beam injector theoretically, especially the spherical aberration caused by the negative ion beam expansion due to the space charge effect. The negative ion current density profiles with the spherical aberration are compared with those without the spherical aberration. It is found that the negative ion current density profiles in a log scale are tailed due to the spherical aberration.

  7. Positively charged biomaterials exert antimicrobial effects on gram-negative bacilli in rats

    NARCIS (Netherlands)

    Gottenbos, B; van der Mei, HC; Klatter, F; Grijpma, DW; Feijen, J; Nieuwenhuis, P; Busscher, HJ

    Biomaterial-centered infection is a much-dreaded complication associated with the use of biomedical implants. Although positively charged biomaterial surfaces stimulate bacterial adhesion, it has been suggested that surface growth of adhering Gram-negative bacilli is inhibited on positively charged

  8. Positively charged biomaterials exert antimicrobial effects on gram-negative bacilli in rats

    NARCIS (Netherlands)

    Gottenbos, B; van der Mei, HC; Klatter, F; Grijpma, DW; Feijen, J; Nieuwenhuis, P; Busscher, HJ

    2003-01-01

    Biomaterial-centered infection is a much-dreaded complication associated with the use of biomedical implants. Although positively charged biomaterial surfaces stimulate bacterial adhesion, it has been suggested that surface growth of adhering Gram-negative bacilli is inhibited on positively charged

  9. Antimicrobial effects of positively charged surfaces on adhering Gram-positive and Gram-negative bacteria

    NARCIS (Netherlands)

    Gottenbos, B; Grijpma, DW; van der Mei, HC; Feijen, J; Busscher, HJ

    The infection of biomaterials is determined by an interplay of adhesion and surface growth of the infecting organisms. In this study, the antimicrobial effects on adhering bacteria of a positively charged poly(methacrylate) surface ( potential +12 mV) were compared with those of negatively charged

  10. Binding Energies of Negatively Charged Donors in a Gaussian Potential Quantum Dot

    Institute of Scientific and Technical Information of China (English)

    XIE Wen-Fang

    2005-01-01

    @@ We investigate a negatively charged donor centre (D-) trapped by a quantum dot, which is subjected to a Gaussian potential confinement. Calculations are carried out by using the method of numerical diagonalization of Hamiltonian within the effective-mass approximation. The dependence of the ground state of the negatively charged donor on the dot size and the potential depth is studied. The same calculations performed with the parabolic approximation of the Gaussian potential lead to the results that are qualitatively and quantitatively different.

  11. The influence of charge clustering on the anti-HIV-1 activity and in vivo distribution of negatively charged albumins

    NARCIS (Netherlands)

    Beljaars, Leonie; Floris, René; Berkhout, Ben; Smit, Catharina; Meijer, Dirk K F; Molema, Grietje

    2002-01-01

    The substitution of human serum albumin with negatively charged molecules, such as succinic acid (Suc-HSA) or aconitic acid (Aco-HSA), resulted in proteins with potent anti-HIV activities, by binding to viral gp120 (V3 loop). The aim of the present study was to investigate whether the distribution o

  12. Wigner molecules and charged excitons in near-field magnetophotoluminescence spectra of self-organized InP/GaInP quantum dots

    Science.gov (United States)

    Mintairov, A. M.; Kapaldo, J.; Merz, J. L.; Vlasov, A. S.; Blundell, S. A.

    2017-03-01

    We used high-spatial-resolution, low-temperature near-field scanning optical microscopy (NSOM) operating at magnetic fields B =0 -10 T to study the effects of Wigner localization (WL) on emission spectra of single self-organized InP/GaInP quantum dots (QDs) and investigate the stability of singly (trion) and doubly (tetron) charged exciton complexes in the weak quantum confinement regime. Using NSOM measurements together with configuration interaction calculations, we identify the dots having different electron population N (N =1 -12 ) , quantum confinement (ℏ ω0=0.6 -8 meV ) and size D (D =70 -170 nm ) . For N =2 , we observed a magnetic-field-induced molecular-droplet transition, accompanied by the decomposition of the tetron into a Wigner molecule complex (WMC), and the activation of rotovibronic structure. For N =1 , unusually strong vibronic structure resulting from a trion-type WMC was observed. We have shown that magnetic-field-induced shifts of this structure allow measurement of single particle Fock-Darwin levels and angular momentum transitions of the WMC. In addition, we demonstrated the use of NSOM imaging to probe the charge density distribution and observed anomalous dependence of the image size on the quantum confinement, implying a pairing of electrons or formation of whispering gallery modes in the QD. We demonstrated that InP/GaInP QDs, provide a Wigner-Seitz radius (rs) up to 13, and that the measurements of NSOM magneto-optical spectroscopy using these dots makes it possible to study effects arising from strong Coulomb interaction of a few confined electrons (holes).

  13. Unstable, metastable, or stable halogen bonding interaction involving negatively charged donors? A statistical and computational chemistry study.

    Science.gov (United States)

    Yang, Zhuo; Xu, Zhijian; Liu, Yingtao; Wang, Jinan; Shi, Jiye; Chen, Kaixian; Zhu, Weiliang

    2014-12-11

    The noncovalent halogen bonding could be attributed to the attraction between the positively charged σ-hole and a nucleophile. Quantum mechanics (QM) calculation indicated that the negatively charged organohalogens have no positively charged σ-hole on their molecular surface, leading to a postulation of repulsion between negatively charged organohalogens and nucleophiles in vacuum. However, PDB survey revealed that 24% of the ligands with halogen bonding geometry could be negatively charged. Moreover, 36% of ionizable drugs in CMC (Comprehensive Medicinal Chemistry) are possibly negatively charged at pH 7.0. QM energy scan showed that the negatively charged halogen bonding is probably metastable in vacuum. However, the QM calculated bonding energy turned negative in various solvents, suggesting that halogen bonding with negatively charged donors should be stable in reality. Indeed, QM/MM calculation on three crystal structures with negatively charged ligands revealed that the negatively charged halogen bonding was stable. Hence, we concluded that halogen bonding with negatively charged donors is unstable or metastable in vacuum but stable in protein environment, and possesses similar geometric and energetic characteristics as conventional halogen bonding. Therefore, negatively charged organohalogens are still effective halogen bonding donors for medicinal chemistry and other applications.

  14. Effect of Negatively Charged Ions on the Formation of Microarc Oxidation Coating on 2024 Aluminium Alloy

    Institute of Scientific and Technical Information of China (English)

    Wei Yang; Bailing Jiang; Aiying Wang; Huiying Shi

    2012-01-01

    The present study deals with the effect of negatively charged ions on the ceramic coating formation on 2024 aluminium alloy during microarc oxidation (MAO) process. On the basis of the experimental results, two steps (the formation of an incipient film without arc presence and the growth of a ceramic coating with arc discharge) of MAO process have been observed. For comparison, four different negatively charged ions studied. It is proved that negatively charged ions strongly participated in the formation of an incipient film with high impedance value at the first step. The growth of ceramic coating depends on the combination between AI of the substrate and O from the electrolyte, and the negatively charged ions are little consumed. As an anodic oxide coating is prepared on the sample surface instead of the incipient film, the first step occurs easily and the growth of ceramic coating is accelerated. Furthermore, the mechanism of negatively charged ions in the formation of the MAO coating has been proposed.

  15. Charge transport and exciton dissociation in organic solar cells consisting of dipolar donors mixed with C70

    Science.gov (United States)

    Griffith, Olga L.; Liu, Xiao; Amonoo, Jojo A.; Djurovich, Peter I.; Thompson, Mark E.; Green, Peter F.; Forrest, Stephen R.

    2015-08-01

    We investigate dipolar donor materials mixed with a C70 acceptor in an organic photovoltaic (OPV) cell. Dipolar donors that have donor-acceptor-acceptor (d-a-a') structure result in high conductivity pathways due to close coupling between neighboring molecules in the mixed films. We analyze the charge transfer properties of the dipolar donor:C70 mixtures and corresponding neat donors using a combination of time-resolved electroluminescence from intermolecular polaron pair states and conductive tip atomic force microscopy, from which we infer that dimers of the d-a-a' donors tend to form a continuous network of nanocrystalline clusters within the blends. Additional insights are provided by quantum-mechanical calculations of hole transfer coupling and hopping rates between donor molecules using nearest-neighbor donor packing motifs taken from crystal structural data. The approximation using only nearest-neighbor interactions leads to good agreement between donor hole hopping rates and the conductive properties of the donor:C70 blends. This represents a significant simplification from requiring details of the nano- and mesoscale morphologies of thin films to estimate their electronic characteristics. Using these dipolar donors, we obtain a maximum power conversion efficiency of 9.6 ±0.5 % under 1 sun, AM1.5G simulated illumination for an OPV comprised of an active layer containing a dipolar donor mixed with C70.

  16. Ballistic spin transport in exciton gases

    Science.gov (United States)

    Kavokin, A. V.; Vladimirova, M.; Jouault, B.; Liew, T. C. H.; Leonard, J. R.; Butov, L. V.

    2013-11-01

    Traditional spintronics relies on spin transport by charge carriers, such as electrons in semiconductor crystals. The challenges for the realization of long-range electron spin transport include rapid spin relaxation due to electron scattering. Scattering and, in turn, spin relaxation can be effectively suppressed in excitonic devices where the spin currents are carried by electrically neutral bosonic quasiparticles: excitons or exciton-polaritons. They can form coherent quantum liquids that carry spins over macroscopic distances. The price to pay is a finite lifetime of the bosonic spin carriers. We present the theory of exciton ballistic spin transport which may be applied to a range of systems supporting bosonic spin transport, in particular to indirect excitons in coupled quantum wells. We describe the effect of spin-orbit interaction for the electron and the hole on the exciton spin, account for the Zeeman effect induced by external magnetic fields and long-range and short-range exchange splittings of the exciton resonances. We also consider exciton transport in the nonlinear regime and discuss the definitions of the exciton spin current, polarization current, and spin conductivity.

  17. Influence of negative charge on the optical properties of a silver sol

    Directory of Open Access Journals (Sweden)

    JOVAN M. NEDELJKOVIC

    2000-03-01

    Full Text Available The effects of negative charge on the optical properties of a silver sol prepared using sodium borohydride as a reductant were studied. The oscillations in the position of the maximum and the intensity of the surface plasmon absorption band were obesrved. The observed effects were explained as a consequence of the fluctuation of the density of free electrons due to the alternate charging and discharging of the silver particles. The charging process involves electron injection from borohydride ions and intermediate species formed during the course of the metal-catalyzed hydrolysis of borohydride ions (BH3OH-, BH2(OH2 and BH(OH3- into the silver particles, while discharge of the silver sol, by reduction of water to hydrogen, limits the attainable negative charge on the particles.

  18. Space Charge Compensation in the Linac4 Low Energy Beam Transport Line with Negative Hydrogen Ions

    CERN Document Server

    Valerio-Lizarraga, C; Leon-Monzon, I; Lettry, J; Midttun, O; Scrivens, R

    2014-01-01

    The space charge effect of low energy, unbunched ion beams can be compensated by the trapping of ions or electrons into the beam potential. This has been studied for the 45 keV negative hydrogen ion beam in the CERN Linac4 Low Energy Beam Tranport (LEBT) using the package IBSimu1, which allows the space charge calculation of the particle trajectories. The results of the beam simulations will be compared to emittance measurements of an H- beam at the CERN Linac4 3 MeV test stand, where the injection of hydrogen gas directly into the beam transport region has been used to modify the space charge compensation degree.

  19. Determination of the negatively charged pion-proton scattering length from pionic hydrogen

    CERN Document Server

    Ericson, Torleif Eric Oskar; Wycech, S

    2003-01-01

    We derive a closed, model independent, expression for the electromagnetic correction factor to the hadronic scattering length extracted from a hydrogenic atom with an extended charge and in the limit of a short ranged hadronic interaction to terms of order ((alpha)**2)(log(alpha)) in the limit of a non-relativistic approach. A hadronic negatively charged pion-proton scattering length of 0.0870(5), in units of inverse charged pion-mass, is deduced, leading to a pion-nucleon coupling constant from the GMO relation equals to 14.00(19).

  20. Bionic design for surface optimization combining hydrophilic and negative charged biological macromolecules.

    Science.gov (United States)

    Ran, Fen; Song, Haiming; Niu, Xiaoqin; Yang, Aimei; Nie, Shengqiang; Wang, Lingren; Li, Jie; Sun, Shudong; Zhao, Changsheng

    2014-06-01

    While polyethersulfone (PES) membrane represents a promising option for blood purification, the blood compatibility must be dramatically enhanced to meet today's ever-increasing demands for many emerging application. In this study, we report a bionic design for optimization and development of a modified PES membrane combining hydrophilic and negative charged biological macromolecules on its surface. The hydrophilic and ionic charged biological macromolecules sulfonated poly(styrene)-b-poly(methyl methacrylate)-b-poly-(styrene) (PSSMSS) and poly(vinyl pyrrolidone)-b-poly(methyl methacrylate)-b-poly-(vinyl pyrrolidone) were synthesized via reversible addition-fragmentation chain transfer polymerization and used together to modify PES membranes by blending method. A hydrophilic membrane surface with negative charged surface coating was obtained, imitating the hydrophilic and negatively charged structure feature of heparin. The modified PES membranes showed suppressed platelet adhesion, and a prolonged blood clotting time, and thereby improved blood compatibility. In addition, the blood clotting time of the modified membranes increased with the blended PSSMSS amounts increment, indicating that both the hydrophilic and negative charged groups play important roles in improving the blood compatibility of PES membranes.

  1. Charging behavior of Al2O3 and AlN under positive and negative charge injection using a kV electron beam

    Science.gov (United States)

    Belhaj, M.; Paulmier, T.; Hanna, R.; Arnaout, M.; Balcon, N.; Payan, D.; Puech, J.

    2014-02-01

    Under electron irradiation, insulating materials may charge either negatively or positively depending on their electron emission properties and characteristics of the incident electrons. The electrical behavior of these materials is linked to the sign of the injected charge. The aim here is to describe an electron beam based method that can be used to study the electrical behaviors of insulators under either positive or negative charge injection. The method was tested on ceramics samples, Al2O3 and AlN. It was shown that the electrical behaviors of both materials under e-irradiation are very different according the sign of the injected charge. Negative charging results to stable space charge for Al2O3 and on the contrary it leads to a fast charge-decay for AlN. Remarkably, reversed trends are observed for positive charge injection. The practical consequences of these results are then discussed.

  2. Charging behavior of Al{sub 2}O{sub 3} and AlN under positive and negative charge injection using a kV electron beam

    Energy Technology Data Exchange (ETDEWEB)

    Belhaj, M., E-mail: Mohamed.Belhaj@onera.fr [ONERA, The French Aerospace Lab, 31055 Toulouse (France); Paulmier, T.; Hanna, R.; Arnaout, M. [ONERA, The French Aerospace Lab, 31055 Toulouse (France); Balcon, N.; Payan, D.; Puech, J. [CNES, Av Edourad Belin, Toulouse (France)

    2014-02-01

    Under electron irradiation, insulating materials may charge either negatively or positively depending on their electron emission properties and characteristics of the incident electrons. The electrical behavior of these materials is linked to the sign of the injected charge. The aim here is to describe an electron beam based method that can be used to study the electrical behaviors of insulators under either positive or negative charge injection. The method was tested on ceramics samples, Al{sub 2}O{sub 3} and AlN. It was shown that the electrical behaviors of both materials under e-irradiation are very different according the sign of the injected charge. Negative charging results to stable space charge for Al{sub 2}O{sub 3} and on the contrary it leads to a fast charge-decay for AlN. Remarkably, reversed trends are observed for positive charge injection. The practical consequences of these results are then discussed.

  3. The description of charge transfer in fast negative ions scattering on water covered Si(100) surfaces

    Science.gov (United States)

    Chen, Lin; Qiu, Shunli; Liu, Pinyang; Xiong, Feifei; Lu, Jianjie; Liu, Yuefeng; Li, Guopeng; Liu, Yiran; Ren, Fei; Xiao, Yunqing; Gao, Lei; Zhao, Qiushuang; Ding, Bin; Li, Yuan; Guo, Yanling; Chen, Ximeng

    2016-11-01

    Doping has significantly affected the characteristics and performance of semiconductor electronic devices. In this work, we study the charge transfer processes for 8.5-22.5 keV C- and F- ions scattering on H2O-terminated p-type Si(100) surfaces with two different doping concentrations. We find that doping has no influence on negative-ion formation for fast collisions in this relatively high energy range. Moreover, we build a model to calculate negative ion fractions including the contribution from positive ions. The calculations support the nonadiabatic feature of charge transfer.

  4. Bactericidal action mechanism of negatively charged food grade clove oil nanoemulsions.

    Science.gov (United States)

    Majeed, Hamid; Liu, Fei; Hategekimana, Joseph; Sharif, Hafiz Rizwan; Qi, Jing; Ali, Barkat; Bian, Yuan-Yuan; Ma, Jianguo; Yokoyama, Wallace; Zhong, Fang

    2016-04-15

    Clove oil (CO) anionic nanoemulsions were prepared with varying ratios of CO to canola oil (CA), emulsified and stabilized with purity gum ultra (PGU), a newly developed succinylated waxy maize starch. Interfacial tension measurements showed that CO acted as a co-surfactant and there was a gradual decrease in interfacial tension which favored the formation of small droplet sizes on homogenization until a critical limit (5:5% v/v CO:CA) was reached. Antimicrobial activity of the negatively charged CO nanoemulsion was determined against Gram positive GPB (Listeria monocytogenes and Staphylococcus aureus) and Gram negative GNB (Escherichia coli) bacterial strains using minimum inhibitory concentration (MIC) and a time kill dynamic method. Negatively charged PGU emulsified CO nanoemulsion showed prolonged antibacterial activities against Gram positive bacterial strains. We concluded that negatively charged CO nanoemulsion droplets self-assemble with GPB cell membrane, and facilitated interaction with cellular components of bacteria. Moreover, no electrostatic interaction existed between negatively charged droplets and the GPB membrane.

  5. Negative Ion CID Fragmentation of O-linked Oligosaccharide Aldoses—Charge Induced and Charge Remote Fragmentation

    Science.gov (United States)

    Doohan, Roisin A.; Hayes, Catherine A.; Harhen, Brendan; Karlsson, Niclas Göran

    2011-06-01

    Collision induced dissociation (CID) fragmentation was compared between reducing and reduced sulfated, sialylated, and neutral O-linked oligosaccharides. It was found that fragmentation of the [M - H]- ions of aldoses with acidic residues gave unique Z-fragmentation of the reducing end GalNAc containing the acidic C-6 branch, where the entire C-3 branch was lost. This fragmentation pathway, which is not seen in the alditols, showed that the process involved charge remote fragmentation catalyzed by a reducing end acidic anomeric proton. With structures containing sialic acid on both the C-3 and C-6 branch, the [M - H]- ions were dominated by the loss of sialic acid. This fragmentation pathway was also pronounced in the [M - 2H]2- ions revealing both the C-6 Z-fragment plus its complementary C-3 C-fragment in addition to glycosidic and cross ring fragmentation. This generation of the Z/C-fragment pairs from GalNAc showed that the charges were not participating in their generation. Fragmentation of neutral aldoses showed pronounced Z-fragmentation believed to be generated by proton migration from the C-6 branch to the negatively charged GalNAc residue followed by charge remote fragmentation similar to the acidic oligosaccharides. In addition, A-type fragments generated by charge induced fragmentation of neutral oligosaccharides were observed when the charge migrated from C-1 of the GalNAc to the GlcNAc residue followed by rearrangement to accommodate the 0,2A-fragmentation. LC-MS also showed that O-linked aldoses existed as interchangeable α/β pyranose anomers, in addition to a third isomer (25% of the total free aldose) believed to be the furanose form.

  6. Negative charge and charging dynamics in Al2O3 films on Si characterized by second-harmonic generation

    Science.gov (United States)

    Gielis, J. J. H.; Hoex, B.; van de Sanden, M. C. M.; Kessels, W. M. M.

    2008-10-01

    Thin films of Al2O3 synthesized by atomic layer deposition provide an excellent level of interface passivation of crystalline silicon (c-Si) after a postdeposition anneal. The Al2O3 passivation mechanism has been elucidated by contactless characterization of c-Si/Al2O3 interfaces by optical second-harmonic generation (SHG). SHG has revealed a negative fixed charge density in as-deposited Al2O3 on the order of 1011 cm-2 that increased to 1012-1013 cm-2 upon anneal, causing effective field-effect passivation. In addition, multiple photon induced charge trapping dynamics suggest a reduction in recombination channels after anneal and indicate a c-Si/Al2O3 conduction band offset of 2.02±0.04 eV.

  7. The magnetized dusty plasma discharge negative and positive space charge modes

    CERN Document Server

    Cramer, N F; Cramer, Neil F.; Vladimirov, Sergey

    2004-01-01

    The structure of a discharge across a magnetic field in a dusty plasma is analysed. The dust macroparticles are negatively charged, but are unmagnetized because of their high mass. The electrons are highly magnetized, and the ions have intermediate magnetization. This results in different transport rates of the different species across the magnetic field. Depending on the size of the magnetic field, and the relative charge on the different species, the dust grains can be the dominant current carrier. The space charge clouds near the electrodes will then be determined by the relative mobility of the different species. The discharge can operate in one of two modes, a positive space charge (PSC) mode, characterized by a strong cathode fall, and a negative space charge (NSC) mode, characterized by a broad anode fall. Features unique to the dust particles can also play a role in the structure of the discharge, such as the variable equilibrium charge on the grains, dependent on the local potential and species tempe...

  8. Ion-exchange molecularly imprinted polymer for the extraction of negatively charged acesulfame from wastewater samples.

    Science.gov (United States)

    Zarejousheghani, Mashaalah; Schrader, Steffi; Möder, Monika; Lorenz, Pierre; Borsdorf, Helko

    2015-09-11

    Acesulfame is a known indicator that is used to identify the introduction of domestic wastewater into water systems. It is negatively charged and highly water-soluble at environmental pH values. In this study, a molecularly imprinted polymer (MIP) was synthesized for negatively charged acesulfame and successfully applied for the selective solid phase extraction (SPE) of acesulfame from influent and effluent wastewater samples. (Vinylbenzyl)trimethylammonium chloride (VBTA) was used as a novel phase transfer reagent, which enhanced the solubility of negatively charged acesulfame in the organic solvent (porogen) and served as a functional monomer in MIP synthesis. Different molecularly imprinted polymers were synthesized to optimize the extraction capability of acesulfame. The different materials were evaluated using equilibrium rebinding experiments, selectivity experiments and scanning electron microscopy (SEM). The most efficient MIP was used in a molecularly imprinted-solid phase extraction (MISPE) protocol to extract acesulfame from wastewater samples. Using high-performance liquid chromatography-tandem mass spectrometry (HPLC-MS-MS) analysis, detection and quantification limits were achieved at 0.12μgL(-1) and 0.35μgL(-1), respectively. Certain cross selectivity for the chemical compounds containing negatively charged sulfonamide functional group was observed during selectivity experiments.

  9. Pharmacokinetics and anti-HIV-1 efficacy of negatively charged human serum albumins in mice

    NARCIS (Netherlands)

    Kuipers, M E; Swart, P J; Schutten, M; Smit, C; Proost, J H; Osterhaus, A D; Meijer, D K

    1997-01-01

    Negatively charged albumins (NCAs, with the prototypes succinylated human serum albumin (Suc-HSA) and aconitylated human serum albumin (Aco-HSA)), modified proteins with a potent anti-human immunodeficiency virus type 1 (anti-HIV-1) activity in vitro, were studied for their pharmacokinetic behaviour

  10. Translocation of positively and negatively charged polystyrene nanoparticles in an in vitro placental model

    NARCIS (Netherlands)

    Kloet, S.K.; Walczak, A.P.; Louisse, J.; Berg, H.H.J. van den; Bouwmeester, H.; Tromp, P.; Fokkink, R.G.; Rietjens, I.M.C.M.

    2015-01-01

    To obtain insight in translocation of nanoparticles across the placental barrier, translocation was studied for one positively and two negatively charged polystyrene nanoparticles (PS-NPs) of similar size in an in vitro model. The model consisted of BeWo b30 cells, derived from a human choriocarcino

  11. Bound state properties and photodetachment of the negatively charged hydrogen ions

    Science.gov (United States)

    Frolov, Alexei M.

    2015-05-01

    Absorption of infrared and visible radiation from stellar emission spectra by the negatively charged hydrogen ions H- is considered. The explicit formula for the photodetachment cross-section of the negatively charged hydrogen ion(s) is derived. Photodetachemnt cross-sections of the {∞}H-, {3}H- (or T-), {2}H- (or D-) and {1}H- ions are determined to high accuracy and for a large number of photo-electron momenta/energies. We introduce criteria which can be used to evaluate the overall quality of highly accurate wave functions of the hydrogen ion(s). One of these criteria is based on highly accurate calculations of the lowest order QED corrections in the negatively charged hydrogen ions, including {1}H- (protium), {2}H- (deuterium), {3}H- (tritium) and model ion with the infinitely heavy nucleus {∞}H-. An effective approach has been developed to calculate three-body integrals with the Bessel functions of different orders. Some preliminary evaluations of the phototdetachment cross-sections of the negatively charged hydrogen ions are performed. Inverse bremsstrahlung in the field of the neutral hydrogen atom is briefly discussed.

  12. Charged excitons in parabolic quantum-well wires under magnetic filed%外加磁场下抛物型量子线中的带电激子

    Institute of Scientific and Technical Information of China (English)

    张红; 张春元; 张慧亮; 刘建军

    2011-01-01

    The binding energies of the charged excitons(negative X- and positive X + excitons) are calculated using the finite- difference method within the quasi-one-dimensional effective potential model. The effects due to the magnetic filed and quantum confinements on the binding energy are analyzed, and the following results are obtained : ( 1 ) relative electron and hole harmonic oscillator confinement each have a strong effect on the stablity of charged excitons, the binding energy of X + is not always larger than that of X- , e. g. , due to the increase of the hole harmonic oscillator length, leading to the crossing of X + and X- lines as recently observed experimentally ; (2) the magnetic field leads to an increase of the binding energy, and the magnetic field dependence of the binding energy is related to the harmonic oscillator length.%在一维等效模型下采用有效差分法对抛物型量子阱线中带电激子的束缚能进行了计算,分析了约束势以及磁场对带电激子束缚能的影响,并对带正电激子(x^+)和带负电激子(X^-)的情况进行了比较.结果表明:电子和空穴的振子强度对带电激子的稳定性有重要影响,X^-的束缚能不总是比X^-的大,随着空穴振子强度的增加束缚能的函数曲线将会出现交叉,这同实验得到的结果符合;磁场的存在会增加粒子间的束缚,并且磁场对束缚能的影响同振子强度大小有关.

  13. Dust charging processes with a Cairns-Tsallis distribution function with negative ions

    Energy Technology Data Exchange (ETDEWEB)

    Abid, A. A., E-mail: abidaliabid1@hotmail.com [Applied Physics Department, Federal Urdu University of Arts, Science and Technology, Islamabad Campus, Islamabad 45320 (Pakistan); Khan, M. Z., E-mail: mzk-qau@yahoo.com [Applied Physics Department, Federal Urdu University of Arts, Science and Technology, Islamabad Campus, Islamabad 45320 (Pakistan); Plasma Technology Research Center, Department of Physics, Faculty of Science, University of Malaya, Kuala Lumpur 50603 (Malaysia); Yap, S. L. [Plasma Technology Research Center, Department of Physics, Faculty of Science, University of Malaya, Kuala Lumpur 50603 (Malaysia); Terças, H., E-mail: hugo.tercas@tecnico.ul.pt [Physics of Information Group, Instituto de Telecomunicações, Av. Rovisco Pais, Lisbon 1049-001 (Portugal); Mahmood, S. [Science Place, University of Saskatchewan, Saskatoon, Saskatchewan S7N5A2 (Canada)

    2016-01-15

    Dust grain charging processes are presented in a non-Maxwellian dusty plasma following the Cairns-Tsallis (q, α)–distribution, whose constituents are the electrons, as well as the positive/negative ions and negatively charged dust grains. For this purpose, we have solved the current balance equation for a negatively charged dust grain to achieve an equilibrium state value (viz., q{sub d} = constant) in the presence of Cairns-Tsallis (q, α)–distribution. In fact, the current balance equation becomes modified due to the Boltzmannian/streaming distributed negative ions. It is numerically found that the relevant plasma parameters, such as the spectral indexes q and α, the positive ion-to-electron temperature ratio, and the negative ion streaming speed (U{sub 0}) significantly affect the dust grain surface potential. It is also shown that in the limit q → 1 the Cairns-Tsallis reduces to the Cairns distribution; for α = 0 the Cairns-Tsallis distribution reduces to pure Tsallis distribution and the latter reduces to Maxwellian distribution for q → 1 and α = 0.

  14. Photodissociation and charge transfer dynamics of negative ions studied with femtosecond photoelectron spectroscopy

    Energy Technology Data Exchange (ETDEWEB)

    Zanni, Martin Thomas [Univ. of California, Berkeley, CA (United States)

    1999-12-01

    This dissertation presents studies aimed at understanding the potential energy surfaces and dynamics of isolated negative ions, and the effects of solvent on each. Although negative ions play important roles in atmospheric and solution phase chemistry, to a large extent the ground and excited state potential energy surfaces of gas phase negative ions are poorly characterized, and solvent effects even less well understood. In an effort to fill this gap, the author's coworkers and the author have developed a new technique, anion femtosecond photoelectron spectroscopy, and applied it to gas phase photodissociation and charge transfer processes. Studies are presented that (1) characterize the ground and excited states of isolated and clustered anions, (2) monitor the photodissociation dynamics of isolated and clustered anions, and (3) explore the charge-transfer-to-solvent states of atomic iodide clustered with polar and non-polar solvents.

  15. Photodissociation and charge transfer dynamics of negative ions studied with femtosecond photoelectron spectroscopy

    Energy Technology Data Exchange (ETDEWEB)

    Zanni, Martin T.

    1999-12-17

    This dissertation presents studies aimed at understanding the potential energy surfaces and dynamics of isolated negative ions, and the effects of solvent on each. Although negative ions play important roles in atmospheric and solution phase chemistry, to a large extent the ground and excited state potential energy surfaces of gas phase negative ions are poorly characterized, and solvent effects even less well understood. In an effort to fill this gap, the author's coworkers and the author have developed a new technique, anion femtosecond photoelectron spectroscopy, and applied it to gas phase photodissociation and charge transfer processes. Studies are presented that (1) characterize the ground and excited states of isolated and clustered anions, (2) monitor the photodissociation dynamics of isolated and clustered anions, and (3) explore the charge-transfer-to-solvent states of atomic iodide clustered with polar and non-polar solvents.

  16. Excitons in the Fractional Quantum Hall Effect

    Science.gov (United States)

    Laughlin, R. B.

    1984-09-01

    Quasiparticles of charge 1/m in the Fractional Quantum Hall Effect form excitons, which are collective excitations physically similar to the transverse magnetoplasma oscillations of a Wigner crystal. A variational exciton wavefunction which shows explicitly that the magnetic length is effectively longer for quasiparticles than for electrons is proposed. This wavefunction is used to estimate the dispersion relation of these excitons and the matrix elements to generate them optically out of the ground state. These quantities are then used to describe a type of nonlinear conductivity which may occur in these systems when they are relatively clean.

  17. Glutamic acid 181 is negatively charged in the bathorhodopsin photointermediate of visual rhodopsin.

    Science.gov (United States)

    Sandberg, Megan N; Amora, Tabitha L; Ramos, Lavoisier S; Chen, Min-Hsuan; Knox, Barry E; Birge, Robert R

    2011-03-09

    Assignment of the protonation state of the residue Glu-181 is important to our understanding of the primary event, activation processes and wavelength selection in rhodopsin. Despite extensive study, there is no general agreement on the protonation state of this residue in the literature. Electronic assignment is complicated by the location of Glu-181 near the nodal point in the electrostatic charge shift that accompanies excitation of the chromophore into the low-lying, strongly allowed ππ* state. Thus, the charge on this residue is effectively hidden from electronic spectroscopy. This situation is resolved in bathorhodopsin, because photoisomerization of the chromophore places Glu-181 well within the region of negative charge shift following excitation. We demonstrate that Glu-181 is negatively charged in bathorhodopsin on the basis of the shift in the batho absorption maxima at 10 K [λ(max) band (native) = 544 ± 2 nm, λ(max) band (E181Q) = 556 ± 3 nm] and the decrease in the λ(max) band oscillator strength (0.069 ± 0.004) of E181Q relative to that of the native protein. Because the primary event in rhodopsin does not include a proton translocation or disruption of the hydrogen-bonding network within the binding pocket, we may conclude that the Glu-181 residue in rhodopsin is also charged.

  18. Negative Resistance Effect and Charge Transfer Mechanisms in the lon Beam Deposited Diamond Like Carbon Superlattices

    Directory of Open Access Journals (Sweden)

    Andrius VASILIAUSKAS

    2011-03-01

    Full Text Available In the present study DLC:SiOx/DLC/DLC:SiOx/nSi and DLC:SiOx/DLC/DLC:SiOx/pSi structures were fabricated by ion beam deposition using a closed drift ion source. Current-voltage (I-V characteristics of the multilayer samples were measured at room temperature. The main charge transfer mechanisms were considered. Unstable negative resistance effect was observed for some DLC:SiOx/DLC/DLC:SiOx/nSi and DLC:SiOx/DLC/DLC:SiOx/pSi structures. In the case of the diamond like carbon superlattices fabricated on nSi it was observed only during the first measurement. In the case of the some DLC:SiOx/DLC/DLC:SiOx/pSi negative resistance "withstood" several measurements. Changes of the charge carrier mechanisms were observed along with the dissapear of the negative resistance peaks. It seems, that in such a case influence of the bulk related charge transfer mechanisms such as Poole-Frenkel emission increased, while the influence of the contact limited charge transfer mechanisms such as Schottky emission decreased. Observed results were be explained by current flow through the local microconducting channels and subsequent destruction of the localized current pathways as a result of the heating by flowing electric current.http://dx.doi.org/10.5755/j01.ms.17.1.240

  19. Exciton in type-II quantum dot

    Energy Technology Data Exchange (ETDEWEB)

    Sierra-Ortega, J; Escorcia, R A [Universidad del Magdalena, A. A. 731, Santa Marta (Colombia); Mikhailov, I D, E-mail: jsierraortega@gmail.co [Universidad Industrial de Santander, A. A. 678, Bucaramanga (Colombia)

    2009-05-01

    We study the quantum-size effect and the influence of the external magnetic field on the exciton ground state energy in the type-II InP quantum disk, lens and pyramid deposited on a wetting layer and embedded in a GaInP matrix. We show that the charge distribution over and below quantum dot and wetting layer induced by trapped exciton strongly depends on the quantum dot morphology and the strength of the magnetic field.

  20. Space charge compensation in the Linac4 low energy beam transport line with negative hydrogen ions

    Energy Technology Data Exchange (ETDEWEB)

    Valerio-Lizarraga, Cristhian A., E-mail: cristhian.alfonso.valerio.lizarraga@cern.ch [CERN, Geneva (Switzerland); Departamento de Investigación en Física, Universidad de Sonora, Hermosillo (Mexico); Lallement, Jean-Baptiste; Lettry, Jacques; Scrivens, Richard [CERN, Geneva (Switzerland); Leon-Monzon, Ildefonso [Facultad de Ciencias Fisico-Matematicas, Universidad Autónoma de Sinaloa, Culiacan (Mexico); Midttun, Øystein [CERN, Geneva (Switzerland); University of Oslo, Oslo (Norway)

    2014-02-15

    The space charge effect of low energy, unbunched ion beams can be compensated by the trapping of ions or electrons into the beam potential. This has been studied for the 45 keV negative hydrogen ion beam in the CERN Linac4 Low Energy Beam Transport using the package IBSimu [T. Kalvas et al., Rev. Sci. Instrum. 81, 02B703 (2010)], which allows the space charge calculation of the particle trajectories. The results of the beam simulations will be compared to emittance measurements of an H{sup −} beam at the CERN Linac4 3 MeV test stand, where the injection of hydrogen gas directly into the beam transport region has been used to modify the space charge compensation degree.

  1. Space charge compensation in the Linac4 low energy beam transport line with negative hydrogen ions.

    Science.gov (United States)

    Valerio-Lizarraga, Cristhian A; Lallement, Jean-Baptiste; Leon-Monzon, Ildefonso; Lettry, Jacques; Midttun, Øystein; Scrivens, Richard

    2014-02-01

    The space charge effect of low energy, unbunched ion beams can be compensated by the trapping of ions or electrons into the beam potential. This has been studied for the 45 keV negative hydrogen ion beam in the CERN Linac4 Low Energy Beam Transport using the package IBSimu [T. Kalvas et al., Rev. Sci. Instrum. 81, 02B703 (2010)], which allows the space charge calculation of the particle trajectories. The results of the beam simulations will be compared to emittance measurements of an H(-) beam at the CERN Linac4 3 MeV test stand, where the injection of hydrogen gas directly into the beam transport region has been used to modify the space charge compensation degree.

  2. Space charge compensation in the Linac4 low energy beam transport line with negative hydrogen ions

    Science.gov (United States)

    Valerio-Lizarraga, Cristhian A.; Lallement, Jean-Baptiste; Leon-Monzon, Ildefonso; Lettry, Jacques; Midttun, Øystein; Scrivens, Richard

    2014-02-01

    The space charge effect of low energy, unbunched ion beams can be compensated by the trapping of ions or electrons into the beam potential. This has been studied for the 45 keV negative hydrogen ion beam in the CERN Linac4 Low Energy Beam Transport using the package IBSimu [T. Kalvas et al., Rev. Sci. Instrum. 81, 02B703 (2010)], which allows the space charge calculation of the particle trajectories. The results of the beam simulations will be compared to emittance measurements of an H- beam at the CERN Linac4 3 MeV test stand, where the injection of hydrogen gas directly into the beam transport region has been used to modify the space charge compensation degree.

  3. Positively and Negatively Charged Cesium and (C60) m Cs n Cluster Ions.

    Science.gov (United States)

    Renzler, Michael; Kranabetter, Lorenz; Goulart, Marcelo; Scheier, Paul; Echt, Olof

    2017-05-25

    We report on the formation and ionization of cesium and C60Cs clusters in superfluid helium nanodroplets. Size distributions of positively and negatively charged (C60) m Cs n(±) ions have been measured for m ≤ 7, n ≤ 12. Reproducible intensity anomalies are observed in high-resolution mass spectra. For both charge states, (C60) m Cs3(±) and (C60) m Cs5(±) are particularly abundant, with little dependence on the value of m. Distributions of bare cesium cluster ions also indicate enhanced stability of Cs3(±) and Cs5(±), in agreement with theoretical predictions. These findings contrast with earlier reports on highly Cs-doped cationic fullerene aggregates which showed enhanced stability of C60Cs6 building blocks attributed to charge transfer. The dependence of the (C60) m Cs3(-) anion yield on electron energy shows a resonance that, surprisingly, oscillates in strength as m increases from 1 to 6.

  4. Deuterium isotope effects on 13C chemical shifts of negatively charged NH.N systems

    DEFF Research Database (Denmark)

    Hansen, Poul Erik; Pietrzak, Mariusz; Grech, Eugeniusz

    2013-01-01

    Deuterium isotope effects on 13C chemical shifts are investigated in anions of 1,8-bis(4-toluenesulphonamido)naphthalenes together with N,N-(naphthalene-1,8-diyl)bis(2,2,2-trifluoracetamide) all with bis(1,8-dimethylamino)napthaleneH+ as counter ion. These compounds represent both “static......” and equilibrium cases. NMR assignments of the former have been revised. The NH proton is deuteriated. The isotope effects on 13C chemical shifts are rather unusual in these strongly hydrogen bonded systems between a NH and a negatively charged nitrogen atom. The formal four-bond effects are found to be negative...

  5. Quantum mechanical investigations on the role of neutral and negatively charged enamine intermediates in organocatalyzed reactions

    Energy Technology Data Exchange (ETDEWEB)

    Hubin, Pierre O., E-mail: pierre.hubin@unamur.be [Laboratoire de Physico-Chimie Informatique (PCI), Unité de Chimie Physique Théorique et Structurale, University of Namur, 61 rue de Bruxelles, 5000 Namur (Belgium); Jacquemin, Denis [Laboratoire CEISAM – UMR CNRS 6230, Université de Nantes, 2 rue de la Houssinière, BP92208, 44322 Nantes Cedex 3 (France); Institut Universitaire de France 103, Boulevard St Michel, 75005 Paris Cedex 5 (France); Leherte, Laurence; Vercauteren, Daniel P. [Laboratoire de Physico-Chimie Informatique (PCI), Unité de Chimie Physique Théorique et Structurale, University of Namur, 61 rue de Bruxelles, 5000 Namur (Belgium)

    2014-04-15

    Highlights: • M06-2X functional is suitable to model key steps of proline-catalyzed reactions. • Investigation of the proline-catalyzed aldol reaction mechanism. • Influence of water molecules on the C–C bond formation step. • Mechanism for the reaction of proline-derived enamines with benzhydrylium cations. - Abstract: The proline-catalyzed aldol reaction is the seminal example of asymmetric organocatalysis. Previous theoretical and experimental studies aimed at identifying its mechanism in order to rationalize the outcome of this reaction. Here, we focus on key steps with modern first principle methods, i.e. the M06-2X hybrid exchange–correlation functional combined to the solvation density model to account for environmental effects. In particular, different pathways leading to the formation of neutral and negatively charged enamine intermediates are investigated, and their reactivity towards two electrophiles, i.e. an aldehyde and a benzhydrylium cation, are compared. Regarding the self-aldol reaction, our calculations confirm that the neutral enamine intermediate is more reactive than the negatively charged one. For the reaction with benzhydrylium cations however, the negatively charged enamine intermediate is more reactive.

  6. High flux and antifouling properties of negatively charged membrane for dyeing wastewater treatment by membrane distillation.

    Science.gov (United States)

    An, Alicia Kyoungjin; Guo, Jiaxin; Jeong, Sanghyun; Lee, Eui-Jong; Tabatabai, S Assiyeh Alizadeh; Leiknes, TorOve

    2016-10-15

    This study investigated the applicability of membrane distillation (MD) to treat dyeing wastewater discharged by the textile industry. Four different dyes containing methylene blue (MB), crystal violet (CV), acid red 18 (AR18), and acid yellow 36 (AY36) were tested. Two types of hydrophobic membranes made of polytetrafluoroethylene (PTFE) and polyvinylidene fluoride (PVDF) were used. The membranes were characterized by testing against each dye (foulant-foulant) and the membrane-dye (membrane-foulant) interfacial interactions and their mechanisms were identified. The MD membranes possessed negative charges, which facilitated the treatment of acid and azo dyes of the same charge and showed higher fluxes. In addition, PTFE membrane reduced the wettability with higher hydrophobicity of the membrane surface. The PTFE membrane evidenced especially its resistant to dye absorption, as its strong negative charge and chemical structure caused a flake-like (loose) dye-dye structure to form on the membrane surface rather than in the membrane pores. This also enabled the recovery of flux and membrane properties by water flushing (WF), thereby direct-contact MD with PTFE membrane treating 100 mg/L of dye mixtures showed stable flux and superior color removal during five days operation. Thus, MD shows a potential for stable long-term operation in conjunction with a simple membrane cleaning process, and its suitability in dyeing wastewater treatment. Copyright © 2016 Elsevier Ltd. All rights reserved.

  7. High flux and antifouling properties of negatively charged membrane for dyeing wastewater treatment by membrane distillation

    KAUST Repository

    An, Alicia Kyoungjin

    2016-07-25

    This study investigated the applicability of membrane distillation (MD) to treat dyeing wastewater discharged by the textile industry. Four different dyes containing methylene blue (MB), crystal violet (CV), acid red 18 (AR), and acid yellow 36 (AY) were tested. Two types of hydrophobic membranes made of polytetrafluoroethylene (PTFE) and polyvinylidene fluoride (PVDF) were used. The membranes were characterized by testing against each dye (foulant-foulant) and the membrane–dye (membrane-foulant) interfacial interactions and their mechanisms were identified. The MD membranes possessed negative charges, which facilitated the treatment of acid and azo dyes of the same charge and showed higher fluxes. In addition, PTFE membrane reduced the wettability with higher hydrophobicity of the membrane surface. The PTFE membrane evidenced especially its resistant to dye absorption, as its strong negative charge and chemical structure caused a flake-like (loose) dye–dye structure to form on the membrane surface rather than in the membrane pores. This also enabled the recovery of flux and membrane properties by water flushing (WF), thereby direct-contact MD with PTFE membrane treating 100 mg/L of dye mixtures showed stable flux and superior color removal during five days operation. Thus, MD shows a potential for stable long-term operation in conjunction with a simple membrane cleaning process, and its suitability in dyeing wastewater treatment.

  8. Theoretical study of excitonic complexes in semiconductors quantum wells; Estudo teorico de complexos excitonicos em pocos quanticos de semicondutores

    Energy Technology Data Exchange (ETDEWEB)

    Dacal, Luis Carlos Ogando

    2001-08-01

    A physical system where indistinguishable particles interact with each other creates the possibility of studying correlation and exchange effect. The simplest system is that one with only two indistinguishable particles. In condensed matter physics, these complexes are represented by charged excitons, donors and acceptors. In quantum wells, the valence band is not parabolic, therefore, the negatively charged excitons and donors are theoretically described in a simpler way. Despite the fact that the stability of charged excitons (trions) is known since the late 50s, the first experimental observation occurred only at the early 90s in quantum well samples, where their binding energies are one order of magnitude larger due to the one dimensional carriers confinement. After this, these complexes became the subject of an intense research because the intrinsic screening of electrical interactions in semiconductor materials allows that magnetic fields that are usual in laboratories have strong effects on the trion binding energy. Another rich possibility is the study of trions as an intermediate state between the neutral exciton and the Fermi edge singularity when the excess of doping carriers is increased. In this thesis, we present a theoretical study of charged excitons and negatively charged donors in GaAs/Al{sub 0.3}Ga{sub 0.7}As quantum wells considering the effects of external electric and magnetic fields. We use a simple, accurate and physically clear method to describe these systems in contrast with the few and complex treatments s available in the literature. Our results show that the QW interface defects have an important role in the trion dynamics. This is in agreement with some experimental works, but it disagrees with other ones. (author)

  9. Negatively Charged Strangelet Search using the E864 Spectrometer at the AGS

    CERN Document Server

    Van Buren, G

    1999-01-01

    We provide a status report on the progress of searching for negatively charged strangelets using the E864 spectrometer at the AGS. About 200 million recorded events representing approximately 14 billion 10% central interactions of Au + Pt at 11.5 GeV/c taken during the 1996-1997 run of the experiment are used in the analysis. No strangelet candidates are seen for charges Z=-1 and Z=-2, corresponding to a 90% confidence level for upper limits of strangelet production of ~1 x 10^{-8} and ~4 x 10^{-9} per central collision respectively. The limits are nearly uniform over a wide range of masses and are valid only for strangelets which are stable or have lifetimes greater than ~50 ns.

  10. Colossal negative thermal expansion in BiNiO3 induced by intermetallic charge transfer

    Science.gov (United States)

    Azuma, Masaki; Chen, Wei-tin; Seki, Hayato; Czapski, Michal; Olga, Smirnova; Oka, Kengo; Mizumaki, Masaichiro; Watanuki, Tetsu; Ishimatsu, Naoki; Kawamura, Naomi; Ishiwata, Shintaro; Tucker, Matthew G.; Shimakawa, Yuichi; Attfield, J. Paul

    2011-01-01

    The unusual property of negative thermal expansion is of fundamental interest and may be used to fabricate composites with zero or other controlled thermal expansion values. Here we report that colossal negative thermal expansion (defined as linear expansion <−10−4 K−1 over a temperature range ~100 K) is accessible in perovskite oxides showing charge-transfer transitions. BiNiO3 shows a 2.6% volume reduction under pressure due to a Bi/Ni charge transfer that is shifted to ambient pressure through lanthanum substitution for Bi. Changing proportions of coexisting low- and high-temperature phases leads to smooth volume shrinkage on heating. The crystallographic linear expansion coefficient for Bi0.95La0.05NiO3 is −137×10−6 K−1 and a value of −82×10−6 K−1 is observed between 320 and 380 K from a dilatometric measurement on a ceramic pellet. Colossal negative thermal expansion materials operating at ambient conditions may also be accessible through metal-insulator transitions driven by other phenomena such as ferroelectric orders. PMID:21673668

  11. The nature of singlet excitons in oligoacene molecular crystals

    KAUST Repository

    Yamagata, H.

    2011-01-01

    A theory for polarized absorption in crystalline oligoacenes is presented, which includes Frenkel exciton coupling, the coupling between Frenkel and charge-transfer (CT) excitons, and the coupling of all neutral and ionic excited states to the dominant ring-breathing vibrational mode. For tetracene, spectra calculated using all Frenkel couplings among the five lowest energy molecular singlet states predict a Davydov splitting (DS) of the lowest energy (0-0) vibronic band of only -32cm-1, far smaller than the measured value of 631cm-1 and of the wrong sign-a negative sign indicating that the polarizations of the lower and upper Davydov components are reversed from experiment. Inclusion of Frenkel-CT coupling dramatically improves the agreement with experiment, yielding a 0-0 DS of 601cm-1 and a nearly quantitative reproduction of the relative spectral intensities of the 0-n vibronic components. Our analysis also shows that CT mixing increases with the size of the oligoacenes. We discuss the implications of these results on exciton dissociation and transport. © 2011 American Institute of Physics.

  12. Multiply Charged Negative Ions of Hydrogen Induced by Superintense Laser Fields

    Energy Technology Data Exchange (ETDEWEB)

    van Duijn, E.; Gavrila, M.; Muller, H.G. [FOM--Institute for Atomic and Molecular Physics, Kruislaan 407, 1098 SJ Amsterdam (The Netherlands)

    1996-10-01

    Using the high-frequency Floquet theory of laser-atom interactions we predict that in superintense fields a proton can bind more than two electrons. For linear polarization, a self-consistent solution of the structure equation shows that H{sup 2{minus}} becomes bound for {alpha}{sub 0}=155 a.u. The fields and frequencies needed for binding H{sup 2{minus}} are within reach of lasers under construction. By choosing appropriately polarized bichromatic radiation, the production of more highly charged negative ions also lies within experimental reach. The ions are (adiabatically) stabilized against ionization, from their very appearance. {copyright} {ital 1996 The American Physical Society.}

  13. Importance of separated efficiencies between positively and negatively charged particles for cumulant calculations

    CERN Document Server

    Nonaka, Toshihiro; Esumi, ShinIchi; Masui, Hiroshi; Luo, Xiaofeng

    2016-01-01

    We show the importance of separated efficiency corrections between positively and negatively charged particles for cumulant calculations by Monte Carlo toy models and analytical calculations. Our results indicate that S{\\sigma} in published net-proton results from the STAR experiment will be suppressed about 5 to 10% in central collisions, and 10 to 20% in peripheral collisions at the beam energy of \\sqrt s_{NN} = 62.4 and 200 GeV if the separated efficiencies are used to efficiency correction.

  14. Positive and negative contribution to birefringence in a family of carbonates: A Born effective charges analysis

    Science.gov (United States)

    Jing, Qun; Yang, Guang; Hou, Juan; Sun, Maozhu; Cao, Haibin

    2016-12-01

    It is an important topic to investigate the birefringence and reveal the contribution from ions to birefringence because it plays an important role in nonlinear optical materials. In this paper, the birefringence of carbonates with coplanar CO3 groups were investigated using the first-principles method. The results show that the lead carbonates exhibit relative large birefringence. After detailed investigate the electronic structures, and Born effective charges, the authors find out that anisotropic electron distribution in the CO3 groups and Pb atoms give positive contribution, while the negative contribution was found from fluorine atoms, meanwhile the Ca, Mg, and Cd atoms give very small contribution to birefringence.

  15. Tuning the affinity of anion binding sites in porin channels with negatively charged residues: molecular details for OprP.

    Science.gov (United States)

    Modi, Niraj; Bárcena-Uribarri, Iván; Bains, Manjeet; Benz, Roland; Hancock, Robert E W; Kleinekathöfer, Ulrich

    2015-02-20

    The cell envelope of the Gram negative opportunistic pathogen Pseudomonas aeruginosa is poorly permeable to many classes of hydrophilic molecules including antibiotics due to the presence of the narrow and selective porins. Here we focused on one of the narrow-channel porins, that is, OprP, which is responsible for the high-affinity uptake of phosphate ions. Its two central binding sites for phosphate contain a number of positively charged amino acids together with a single negatively charged residue (D94). The presence of this negatively charged residue in a binding site for negatively charged phosphate ions is highly surprising due to the potentially reduced binding affinity. The goal of this study was to better understand the role of D94 in phosphate binding, selectivity, and transport using a combination of mutagenesis, electrophysiology, and free-energy calculations. The presence of a negatively charged residue in the binding site is critical for this specific porin OprP as emphasized by the evolutionary conservation of such negatively charged residue in the binding site of several anion-selective porins. Mutations of D94 in OprP to any positively charged or neutral residue increased the binding affinity of phosphate for OprP. Detailed analysis indicated that this anionic residue in the phosphate binding site of OprP, despite its negative charge, maintained energetically favorable phosphate binding sites in the central region of the channel and at the same time decreased residence time thus preventing excessively strong binding of phosphate that would oppose phosphate flux through the channel. Intriguingly mutations of D94 to positively charged residues, lysine and arginine, resulted in very different binding affinities and free energy profiles, indicating the importance of side chain conformations of these positively charged residues in phosphate binding to OprP.

  16. Translocation of positively and negatively charged polystyrene nanoparticles in an in vitro placental model.

    Science.gov (United States)

    Kloet, Samantha K; Walczak, Agata P; Louisse, Jochem; van den Berg, Hans H J; Bouwmeester, Hans; Tromp, Peter; Fokkink, Remco G; Rietjens, Ivonne M C M

    2015-10-01

    To obtain insight in translocation of nanoparticles across the placental barrier, translocation was studied for one positively and two negatively charged polystyrene nanoparticles (PS-NPs) of similar size in an in vitro model. The model consisted of BeWo b30 cells, derived from a human choriocarcinoma grown on a transwell insert forming a cell layer that separates an apical from a basolateral compartment. PS-NPs were characterized with respect to size, surface charge, morphology and protein corona. Translocation of PS-NPs was not related to PS-NP charge. Two PS-NPs were translocated across the BeWo transwell model to a lower extent than amoxicillin, a model compound known to be translocated over the placental barrier to only a limited extent, whereas one PS-NP showed a slightly higher translocation. Studies on the effect of transporter inhibitors on the translocation of the PS-NPs indicated that their translocation was not mediated by known transporters and mainly dependent on passive diffusion. It is concluded that the BeWo b30 model can be used as an efficient method to get an initial qualitative impression about the capacity of NPs to translocate across the placental barrier and set priorities in further in vivo studies on translocation of NPs to the fetus.

  17. Diamagnetic excitons and exciton magnetopolaritons in semiconductors

    Science.gov (United States)

    Seisyan, R. P.

    2012-05-01

    Interband magneto-absorption in semiconductors is reviewed in the light of the diamagnetic exciton (DE) concept. Beginning with a proof of the exciton nature of oscillating-magnetoabsorption (the DE discovery), development of the DE concept is discussed, including definition of observation conditions, quasi-cubic approximation for hexagonal crystals, quantum-well effects in artificial structures, and comprehension of an important role of the DE polariton. The successful use of the concept application to a broad range of substances is reviewed, namely quasi-Landau magnetic spectroscopy of the ‘Rydberg’ exciton states in cubic semiconductors such as InP and GaAs and in hexagonal ones such as CdSe, the proof of exciton participation in the formation of optical spectra in narrow-gap semiconductors such as InSb, InAs, and, especially, PbTe, observation of DE spectra in semiconductor solid solutions like InGaAs. The most fundamental findings of the DE spectroscopy for various quantum systems are brought together, including the ‘Coulomb-well’ effect, fine structure of discrete oscillatory states in the InGaAs/GaAs multiple quantum wells, the magneto-optical observation of above-barrier exciton. Prospects of the DE physics in ultrahigh magnetic field are discussed, including technological creation of controllable low-dimensional objects with extreme oscillator strengths, formation of magneto-quantum exciton polymer, and even modelling of the hydrogen behaviour in the atmosphere of a neutron star.

  18. The negatively charged regions of lactoferrin binding protein B, an adaptation against anti-microbial peptides.

    Directory of Open Access Journals (Sweden)

    Ari Morgenthau

    Full Text Available Lactoferrin binding protein B (LbpB is a bi-lobed membrane bound lipoprotein that is part of the lactoferrin receptor complex in a variety of Gram-negative pathogens. Despite high sequence diversity among LbpBs from various strains and species, a cluster of negatively charged amino acids is invariably present in the protein's C-terminal lobe in all species except Moraxella bovis. The function of LbpB in iron acquisition has yet to be experimentally demonstrated, whereas in vitro studies have shown that LbpB confers protection against lactoferricin, a short cationic antimicrobial peptide released from the N- terminus of lactoferrin. In this study we demonstrate that the negatively charged regions can be removed from the Neisseria meningitidis LbpB without compromising stability, and this results in the inability of LbpB to protect against the bactericidal effects of lactoferricin. The release of LbpB from the cell surface by the autotransporter NalP reduces the protection against lactoferricin in the in vitro killing assay, attributed to removal of LbpB during washing steps, but is unlikely to have a similar impact in vivo. The protective effect of the negatively charged polysaccharide capsule in the killing assay was less than the protection conferred by LbpB, suggesting that LbpB plays a major role in protection against cationic antimicrobial peptides in vivo. The selective release of LbpB by NalP has been proposed to be a mechanism for evading the adaptive immune response, by reducing the antibody binding to the cell surface, but may also provide insights into the primary function of LbpB in vivo. Although TbpB and LbpB have been shown to be major targets of the human immune response, the selective release of LbpB suggests that unlike TbpB, LbpB may not be essential for iron acquisition, but important for protection against cationic antimicrobial peptides.

  19. The negatively charged regions of lactoferrin binding protein B, an adaptation against anti-microbial peptides.

    Science.gov (United States)

    Morgenthau, Ari; Beddek, Amanda; Schryvers, Anthony B

    2014-01-01

    Lactoferrin binding protein B (LbpB) is a bi-lobed membrane bound lipoprotein that is part of the lactoferrin receptor complex in a variety of Gram-negative pathogens. Despite high sequence diversity among LbpBs from various strains and species, a cluster of negatively charged amino acids is invariably present in the protein's C-terminal lobe in all species except Moraxella bovis. The function of LbpB in iron acquisition has yet to be experimentally demonstrated, whereas in vitro studies have shown that LbpB confers protection against lactoferricin, a short cationic antimicrobial peptide released from the N- terminus of lactoferrin. In this study we demonstrate that the negatively charged regions can be removed from the Neisseria meningitidis LbpB without compromising stability, and this results in the inability of LbpB to protect against the bactericidal effects of lactoferricin. The release of LbpB from the cell surface by the autotransporter NalP reduces the protection against lactoferricin in the in vitro killing assay, attributed to removal of LbpB during washing steps, but is unlikely to have a similar impact in vivo. The protective effect of the negatively charged polysaccharide capsule in the killing assay was less than the protection conferred by LbpB, suggesting that LbpB plays a major role in protection against cationic antimicrobial peptides in vivo. The selective release of LbpB by NalP has been proposed to be a mechanism for evading the adaptive immune response, by reducing the antibody binding to the cell surface, but may also provide insights into the primary function of LbpB in vivo. Although TbpB and LbpB have been shown to be major targets of the human immune response, the selective release of LbpB suggests that unlike TbpB, LbpB may not be essential for iron acquisition, but important for protection against cationic antimicrobial peptides.

  20. The Negatively Charged Regions of Lactoferrin Binding Protein B, an Adaptation against Anti-Microbial Peptides

    Science.gov (United States)

    Morgenthau, Ari; Beddek, Amanda; Schryvers, Anthony B.

    2014-01-01

    Lactoferrin binding protein B (LbpB) is a bi-lobed membrane bound lipoprotein that is part of the lactoferrin receptor complex in a variety of Gram-negative pathogens. Despite high sequence diversity among LbpBs from various strains and species, a cluster of negatively charged amino acids is invariably present in the protein’s C-terminal lobe in all species except Moraxella bovis. The function of LbpB in iron acquisition has yet to be experimentally demonstrated, whereas in vitro studies have shown that LbpB confers protection against lactoferricin, a short cationic antimicrobial peptide released from the N- terminus of lactoferrin. In this study we demonstrate that the negatively charged regions can be removed from the Neisseria meningitidis LbpB without compromising stability, and this results in the inability of LbpB to protect against the bactericidal effects of lactoferricin. The release of LbpB from the cell surface by the autotransporter NalP reduces the protection against lactoferricin in the in vitro killing assay, attributed to removal of LbpB during washing steps, but is unlikely to have a similar impact in vivo. The protective effect of the negatively charged polysaccharide capsule in the killing assay was less than the protection conferred by LbpB, suggesting that LbpB plays a major role in protection against cationic antimicrobial peptides in vivo. The selective release of LbpB by NalP has been proposed to be a mechanism for evading the adaptive immune response, by reducing the antibody binding to the cell surface, but may also provide insights into the primary function of LbpB in vivo. Although TbpB and LbpB have been shown to be major targets of the human immune response, the selective release of LbpB suggests that unlike TbpB, LbpB may not be essential for iron acquisition, but important for protection against cationic antimicrobial peptides. PMID:24465982

  1. How to Draw Energy Level Diagrams in Excitonic Solar Cells.

    Science.gov (United States)

    Zhu, X-Y

    2014-07-03

    Emerging photovoltaic devices based on molecular and nanomaterials are mostly excitonic in nature. The initial absorption of a photon in these materials creates an exciton that can subsequently dissociate in each material or at their interfaces to give charge carriers. Any attempt at mechanistic understanding of excitonic solar cells must start with drawing energy level diagrams. This seemingly elementary exercise, which is described in textbooks for inorganic solar cells, has turned out to be a difficult subject in the literature. The problem stems from conceptual confusion of single-particle energy with quasi-particle energy and the misleading practice of mixing the two on the same energy level diagram. Here, I discuss how to draw physically accurate energy diagrams in excitonic solar cells using only single-particle energies (ionization potentials and electron affinities) of both ground and optically excited states. I will briefly discuss current understanding on the electronic energy landscape responsible for efficient charge separation in excitonic solar cells.

  2. Negatively charged silver nanoparticles with potent antibacterial activity and reduced toxicity for pharmaceutical preparations.

    Science.gov (United States)

    Salvioni, Lucia; Galbiati, Elisabetta; Collico, Veronica; Alessio, Giulia; Avvakumova, Svetlana; Corsi, Fabio; Tortora, Paolo; Prosperi, Davide; Colombo, Miriam

    2017-01-01

    The discovery of new solutions with antibacterial activity as efficient and safe alternatives to common preservatives (such as parabens) and to combat emerging infections and drug-resistant bacterial pathogens is highly expected in cosmetics and pharmaceutics. Colloidal silver nanoparticles (NPs) are attracting interest as novel effective antimicrobial agents for the prevention of several infectious diseases. Water-soluble, negatively charged silver nanoparticles (AgNPs) were synthesized by reduction with citric and tannic acid and characterized by transmission electron microscopy, dynamic light scattering, zeta potential, differential centrifuge sedimentation, and ultraviolet-visible spectroscopy. AgNPs were tested with model Gram-negative and Gram-positive bacteria in comparison to two different kinds of commercially available AgNPs. In this work, AgNPs with higher antibacterial activity compared to the commercially available colloidal silver solutions were prepared and investigated. Bacteria were plated and the antibacterial activity was tested at the same concentration of silver ions in all samples. The AgNPs did not show any significant reduction in the antibacterial activity for an acceptable time period. In addition, AgNPs were transferred to organic phase and retained their antibacterial efficacy in both aqueous and nonaqueous media and exhibited no toxicity in eukaryotic cells. We developed AgNPs with a 20 nm diameter and negative zeta potential with powerful antibacterial activity and low toxicity compared to currently available colloidal silver, suitable for cosmetic preservatives and pharmaceutical preparations administrable to humans and/or animals as needed.

  3. Colossal negative thermal expansion in BiNiO3 induced by intermetallic charge transfer.

    Science.gov (United States)

    Azuma, Masaki; Chen, Wei-tin; Seki, Hayato; Czapski, Michal; Olga, Smirnova; Oka, Kengo; Mizumaki, Masaichiro; Watanuki, Tetsu; Ishimatsu, Naoki; Kawamura, Naomi; Ishiwata, Shintaro; Tucker, Matthew G; Shimakawa, Yuichi; Attfield, J Paul

    2011-06-14

    The unusual property of negative thermal expansion is of fundamental interest and may be used to fabricate composites with zero or other controlled thermal expansion values. Here we report that colossal negative thermal expansion (defined as linear expansion transfer transitions. BiNiO(3) shows a 2.6% volume reduction under pressure due to a Bi/Ni charge transfer that is shifted to ambient pressure through lanthanum substitution for Bi. Changing proportions of coexisting low- and high-temperature phases leads to smooth volume shrinkage on heating. The crystallographic linear expansion coefficient for Bi(0.95)La(0.05)NiO(3) is -137×10(-6) K(-1) and a value of -82×10(-6) K(-1) is observed between 320 and 380 K from a dilatometric measurement on a ceramic pellet. Colossal negative thermal expansion materials operating at ambient conditions may also be accessible through metal-insulator transitions driven by other phenomena such as ferroelectric orders.

  4. One dimensional models of excitons in carbon nanotubes

    DEFF Research Database (Denmark)

    Cornean, Horia Decebal; Duclos, P.; Pedersen, Thomas Garm

    Excitons in carbon nanotubes may be modeled by two oppositely charged particles living on the surface of a cylinder. We derive three one dimensional effective Hamiltonians which become exact as the radius of the cylinder vanishes. Two of them are solvable.......Excitons in carbon nanotubes may be modeled by two oppositely charged particles living on the surface of a cylinder. We derive three one dimensional effective Hamiltonians which become exact as the radius of the cylinder vanishes. Two of them are solvable....

  5. Effective models for excitons in carbon nanotubes

    DEFF Research Database (Denmark)

    Cornean, Horia; Duclos, Pierre; Ricaud, Benjamin

    2007-01-01

    We analyse the low lying spectrum of a model of excitons in carbon nanotubes. Consider two particles with opposite charges and a Coulomb self-interaction, placed on an infinitely long cylinder. If the cylinder radius becomes small, the low lying spectrum of their relative motion is well described...

  6. Impact of electric field on Hofmeister effects in aggregation of negatively charged colloidal minerals

    Indian Academy of Sciences (India)

    Ying Tang; Hang Li; Hualing Zhu; Rui Tian; Xiaodan Gao

    2016-01-01

    In this study, the aggregation kinetics of negatively charged colloidal minerals in Na+, K+, NH+4 , Mg2+, Ca2+ and Cu2+ solutions were measured and Hofmeister effects therein were estimated through total average aggregation (TAA) rates and critical coagulation concentration (CCC). Hofmeister effects of TAA rates increased exponentially with the increase in electric field strength, which cannot be explained by the classical theories (i.e., ionic size, hydration and dispersion forces), indicating strong electric field at colloidal surface was an indispensable factor in studying Hofmeister effects. Meanwhile, Hofmeister series of CCC values Na+ > K+ > NH+4 > Mg2+ > Ca2+ > Cu2+ show fine correlation with the polarization of various cations, implying that onic polarization in strong electric field would be responsible for Hofmeister effects in aggregation of colloidal minerals, and the deduction was confirmed by the calculated results of electrostatic interactions between colloidal minerals.

  7. Self-organization and oscillation of negatively charged dust particles in a 2-dimensional dusty plasma

    Energy Technology Data Exchange (ETDEWEB)

    Song, Y.L. [College of Science, China Agricultural University, Beijing 100083 (China); Huang, F., E-mail: huangfeng@cau.edu.cn [College of Science, China Agricultural University, Beijing 100083 (China); Chen, Z.Y., E-mail: chenzy@mail.buct.edu.cn [Department of Physics, Beijing University of Chemical Technology, Beijing 100029 (China); State Key Laboratory of Laser Propulsion & Application, Beijing 101416 (China); Liu, Y.H. [School of Physics and Optoelectronic Engineering, Ludong University, Yantai 264025 (China); Yu, M.Y. [Institute for Fusion Theory and Simulation, Zhejiang University, Hangzhou 310027 (China); Institute for Theoretical Physics I, Ruhr University, D-44801 Bochum (Germany)

    2016-02-22

    Negatively charged dust particles immersed in 2-dimensional dusty plasma system are investigated by molecular dynamics simulations. The effects of the confinement potential and attraction interaction potential on dust particle self-organization are studied in detail and two typical dust particle distributions are obtained when the system reaches equilibrium. The average radial velocity (ARV), average radial force (ARF) and radial mean square displacement are employed to analyze the dust particles' dynamics. Both ARVs and ARFs exhibit oscillation behaviors when the simulation system reaches equilibrium state. The relationships between the oscillation and confinement potential and attraction potential are studied in this paper. The simulation results are qualitatively similar to experimental results. - Highlights: • Self-organization and oscillation of a 2-dimensional dusty plasma is investigated. • Effect of the confinement potential on dust self-organization and oscillation is given. • Effect of the attraction potential on dust self-organization and oscillation is studied.

  8. Stroke multiplicity and horizontal scale of negative charge regions in thunderclouds

    Science.gov (United States)

    Williams, Earle R.; Mattos, Enrique V.; Machado, Luiz A. T.

    2016-05-01

    An X-band polarimetric radar and multiple lightning detection systems are used to document the initial cloud-to-ground lightning flash in a large number (46 cases) of incipient thunderstorms, as part of the CHUVA-Vale field campaign during the 2011/2012 spring-summer in southeast Brazil. The results show an exceptionally low stroke multiplicity (87% of flashes with single stroke) in the initial ground flashes, a finding consistent with the limited space available for the positive leader extension into new regions of negative space charge in compact cells. The results here are contrasted with the behavior of ground flashes in mesoscale thunderstorms in previous studies. Additionally, we found evidence for a minimum scale (radar echo >20 dBZ) for lightning initiation (>3 km in radius) and that the peak currents of initial cloud-to-ground flashes in these compact thunderstorms are only half as large as return stroke peak currents in general.

  9. Negatively Charged Hyperbranched Polyglycerol Grafted Membranes for Osmotic Power Generation from Municipal Wastewater

    KAUST Repository

    Li, Xue

    2015-11-18

    Osmotic power holds great promise as a clean, sustainable and largely unexploited energy resource. Recent membrane development for pressure-retarded osmosis (PRO) is making the osmotic power generation more and more realistic. However, severe performance declines have been observed because the porous layer of PRO membranes is fouled by the feed stream. To overcome it, a negatively charged antifouling PRO hollow fiber membrane has been designed and studied in this work. An antifouling polymer, derived from hyperbranched polyglycerol and functionalized by α-lipoic acid and succinic anhydride, was synthesized and grafted onto the polydopamine (PDA) modified poly(ether sulfone) (PES) hollow fiber membranes. In comparison to unmodified membranes, the charged hyperbranched polyglycerol (CHPG) grafted membrane is much less affected by organic deposition, such as bovine serum albumin (BSA) adsorption, and highly resistant to microbial growths, demonstrated by E. coli adhesion and S. aureus attachment. CHPG-g-TFC was also examined in PRO tests using a concentrated wastewater as the feed. Comparing to the plain PES-TFC and non-charged HPG-g-TFC, the newly developed membrane exhibits not only the smallest decline in water flux but also the highest recovery rate. When using 0.81 M NaCl and wastewater as the feed pair in PRO tests at 15 bar, the average power density remains at 5.6 W/m2 in comparison to an average value of 3.6 W/m2 for unmodified membranes after four PRO runs. In summary, osmotic power generation may be sustained by properly designing and anchoring the functional polymers to PRO membranes.

  10. Gap state charge induced spin-dependent negative differential resistance in tunnel junctions

    Science.gov (United States)

    Jiang, Jun; Zhang, X.-G.; Han, X. F.

    2016-04-01

    We propose and demonstrate through first-principles calculation a new spin-dependent negative differential resistance (NDR) mechanism in magnetic tunnel junctions (MTJ) with cubic cation disordered crystals (CCDC) AlO x or Mg1-x Al x O as barrier materials. The CCDC is a class of insulators whose band gap can be changed by cation doping. The gap becomes arched in an ultrathin layer due to the space charge formed from metal-induced gap states. With an appropriate combination of an arched gap and a bias voltage, NDR can be produced in either spin channel. This mechanism is applicable to 2D and 3D ultrathin junctions with a sufficiently small band gap that forms a large space charge. It provides a new way of controlling the spin-dependent transport in spintronic devices by an electric field. A generalized Simmons formula for tunneling current through junction with an arched gap is derived to show the general conditions under which ultrathin junctions may exhibit NDR.

  11. Charge Kondo effect in negative-U quantum dots with superconducting electrodes

    Science.gov (United States)

    Fang, Tie-Feng; Guo, Ai-Min; Lu, Han-Tao; Luo, Hong-Gang; Sun, Qing-Feng

    2017-08-01

    Recent experimental realization of superconducting quantum dot devices with intradot attraction U [Nature (London) 521, 196 (2015), 10.1038/nature14398; Phys. Rev. X 6, 041042 (2016), 10.1103/PhysRevX.6.041042] offers unique opportunities to study the charge Kondo effect in a superconducting environment. In such devices pseudospin flips are caused by two tunneling processes. One is the cotunneling of normal electrons which generates near-gap Kondo resonances in the single-electron spectral density. This negative-U charge Kondo effect is more robust than the conventional spin Kondo effect against the suppression by the superconductivity. The other tunneling is the mean-field Cooper-pair tunneling which produces a zero-energy bound state in the pair spectral density. Interesting crossover physics from the strongly-correlated Kondo screening to the mean-field polarization of local pseudospin is demonstrated. Due to the interplay of these two tunnelings, the supercurrent is suppressed for intermediate couplings, but it can increase to the unitary limits both in the strong and weak coupling regimes. We obtain the magnetic field-dependent supercurrent which is consistent with the key experimental findings.

  12. Synthesis of positively and negatively charged silver nanoparticles and their deposition on the surface of titanium

    Science.gov (United States)

    Sharonova, A.; Loza, K.; Surmeneva, M.; Surmenev, R.; Prymak, O.; Epple, M.

    2016-02-01

    Bacterial infections related to dental implants are currently a significant complication. A good way to overcome this challenge is functionalization of implant surface with Ag nanoparticles (NPs) as antibacterial agent. This article aims at review the synthesis routes, size and electrical properties of AgNPs. Polyvinyl pyrrolidone (PVP) and polyethyleneimine (PEI) were used as stabilizers. Dynamic Light Scattering, Nanoparticle Tracking Analysis, X-ray diffraction (XRD), scanning electron microscopy (SEM), and energy dispersive spectroscopy (EDX) have been used to characterize the prepared AgNPs. Two types of NPs were synthesized in aqueous solutions: PVP-stabilized NPs with a diameter of the metallic core of 70 ± 20 nm, and negative charge of -20 mV, PEI-stabilized NPs with the size of the metallic core of 50 ± 20 nm and positive charge of +55 mV. According to SEM results, all the NPs have a spherical shape. Functionalization of the titanium substrate surface with PVP and PEI-stabilized AgNPs was carried out by dropping method. XRD patterns revealed that the AgNPs are crystalline with the crystallite size of 14 nm.

  13. HBV maintains electrostatic homeostasis by modulating negative charges from phosphoserine and encapsidated nucleic acids

    Science.gov (United States)

    Su, Pei-Yi; Yang, Ching-Jen; Chu, Tien-Hua; Chang, Chih-Hsu; Chiang, Chiayn; Tang, Fan-Mei; Lee, Chih-Yin; Shih, Chiaho

    2016-01-01

    Capsid assembly and stability of hepatitis B virus (HBV) core protein (HBc) particles depend on balanced electrostatic interactions between encapsidated nucleic acids and an arginine-rich domain (ARD) of HBc in the capsid interior. Arginine-deficient ARD mutants preferentially encapsidated spliced viral RNA and shorter DNA, which can be fully or partially rescued by reducing the negative charges from acidic residues or serine phosphorylation of HBc, dose-dependently. Similarly, empty capsids without RNA encapsidation can be generated by ARD hyper-phosphorylation in insect, bacteria, and human hepatocytes. De-phosphorylation of empty capsids by phosphatase induced capsid disassembly. Empty capsids can convert into RNA-containing capsids by increasing HBc serine de-phosphorylation. In an HBV replicon system, we observed a reciprocal relationship between viral and non-viral RNA encapsidation, suggesting both non-viral RNA and serine-phosphorylation could serve as a charge balance buffer in maintaining electrostatic homeostasis. In addition, by comparing the biochemistry assay results between a replicon and a non-replicon system, we observed a correlation between HBc de-phosphorylation and viral replication. Balanced electrostatic interactions may be important to other icosahedral particles in nature. PMID:27958343

  14. Negative-charge-functionalized carbon nanodot: a low-cost smart cold emitter.

    Science.gov (United States)

    Santra, Saswati; Das, Nirmalya Sankar; Senapati, Subrata; Sen, Dipayan; Chattopadhyay, Kalyan Kumar; Nanda, Karuna Kar

    2017-09-27

    Cold emission properties of carbon nanodots (CNDs) evaluated using ANSYS Maxwell software are predicted to be size-dependent and then verified experimentally. In order to correlate the electron emission properties with the size of CNDs, the work function values were determined using ultraviolet photoelectron spectroscopy. This is the first report on theoretical calculations based on density functional theory and experimental results that confirm the work function dependency on the charge state of the functional group attached on the particle surface. The smallest CND (2.5 nm) has the highest percentage of negatively charged groups as well as the lowest work function (5.18 eV). The smallest dimension with the lowest work function assures that this sample is the best suited for field emission. It shows excellent field emission properties with a high current density of ∼1.45 mA cm(-2) at 2 V μm(-1) electric field, turn-on field as low as 0.04 V μm(-1), very high field enhancement factor of 2.7 × 10(5) and high stability. Overall, the zero-dimensional CNDs showed superior field emission activity as compared to the higher dimensional carbon nanomaterials.

  15. The Production of Negative Lithium Beams by Charge Exchange in Cesium Vapours

    CERN Document Server

    Re, Maurizio; Chines, Francesco; Cuttone, Giacomo; Menna, Mariano; Messina, Esteban; Stracener, Dan

    2005-01-01

    These measurements were carried out at the Holifield Radioactive Ion Beam Facility of the Oak Ridge National Laboratory (ORNL-HRIBF) by researchers from the Istituto Nazionale di Fisica Nucleare - Laboratori Nazionali del Sud (INFN-LNS), Catania, Italy and local staff. The Charge Exchange Cell (CEC) consisted of a vacuum chamber containing cesium vapours at a variable temperature, T, in which positive ions accelerated from an ion source were transformed into negative ones by collisions with the Cs atoms. The main goal of this test was to measure the production efficiency for 7Li- ions at different operating conditions, such as 7Li+ beam energy (5 to 55 keV) and Cs temperature (190 to 300 °C). Moreover, the efficiency measurements performed with a 6Li+ projectile beam gave clear indications about the isotopic shift effect. These results are useful to estimate the charge exchange efficiency for 8, 9Li, which will be the first radioactive beams to be produced at the EXCYT facility (EXotics with CYclotro...

  16. Both intra- and interstrand charge-transfer excited states in aqueous B-DNA are present at energies comparable to, or just above, the (1)pipi* excitonic bright states.

    Science.gov (United States)

    Lange, Adrian W; Herbert, John M

    2009-03-25

    Vertical electronic excitations in model systems representing single- and double-stranded B-DNA are characterized using electronic structure theory, including both time-dependent density functional theory (TD-DFT) and correlated wave function techniques. Previous TD-DFT predictions of charge-transfer (CT) states well below the optically bright (1)pipi* states are shown to be artifacts of the improper long-range behavior of standard density-functional exchange approximations, which we rectify here using a long-range correction (LRC) procedure. For nucleobase dimers (hydrogen-bonded or pi-stacked), TD-LRC-DFT affords vertical excitation energies in reasonable agreement with the wave function methods, not only for the (1)npi* and (1)pipi* states but also for the CT states, and qualitatively reproduces well-known base-stacking effects on the absorption spectrum of DNA. The emergence of (1)pipi* Frenkel exciton states, localized on a single strand, is clearly evident, and these states (rather than low-energy CT states) are primarily responsible for the fact that DNA's absorption spectrum exhibits a red tail that is absent in monomer absorption spectra. For B-DNA in aqueous solution, the low-energy tail of the CT band (representing both intra- and interstrand CT states) appears at energies comparable to those of the optically bright (1)pipi* exciton states. In systems with more than one base pair, we also observe the emergence of delocalized, interstrand CT excitations, whose excitation energies may be significantly lower than the lowest CT excitation in a single base pair. Together, these observations suggest that a single Watson-Crick base pair is an inadequate model of the photophysics of B-DNA.

  17. Exciton laser rate equations

    Directory of Open Access Journals (Sweden)

    Garkavenko A. S.

    2011-08-01

    Full Text Available The rate equations of the exciton laser in the system of interacting excitons have been obtained and the inverted population conditions and generation have been derived. The possibility of creating radically new gamma-ray laser has been shown.

  18. Kinetic theory of exciton-exciton annihilation.

    Science.gov (United States)

    May, Volkhard

    2014-02-07

    Weakly excited states of dye aggregates and supramolecular complexes can be characterized by single or two exciton states. Stronger excitation results in the presence of multiple excited molecules, and complex processes of internal energy transfer dynamics take place. The direct consideration of all excited states is limited to systems with a few molecules only. Therefore, an approach is used based on transition operators among the molecular states of interest and resulting in a dynamic theory for excitation energy transfer in strongly excited molecular systems. As a first application of this theory a detailed description of exciton-exciton annihilation is given. The obtained novel nonlinear theory is related to the standard description. Possible further approximation schemes in the offered theoretical framework are discussed.

  19. Interaction of cationic hydrophobic surfactants at negatively charged surfaces investigated by atomic force microscopy.

    Science.gov (United States)

    McNamee, Cathy E; Butt, Hans-Jürgen; Higashitani, Ko; Vakarelski, Ivan U; Kappl, Michael

    2009-10-06

    Atomic force microscopy was used to study the adsorption of the surfactant octadecyl trimethyl ammonium chloride (C18TAC) at a low concentration (0.03 mM) to negatively charged surfaces in water. Atomic force microscopy tips were functionalized with dimethyloctadecyl(3-tripropyl)ammonium chloride (C18TAC-si) or N-trimethoxysilylpropyl-N,N,N-trimethylammomium chloride (hydrophilpos-si) to facilitate imaging of the adsorbed surfactant without artifacts. Tapping mode images and force measurements revealed C18TAC patches, identified as partial surfactant bilayers or hemimicelles. The forces controlling the adsorption process of the C18TAC to a negatively charged surface were investigated by measuring the forces between a C18TAC-si or a hydrophilpos-si tip and a silica surface in the presence of varying concentrations of either NaCl or NaNO3. Screening of forces with an increasing NaCl concentration was observed for the C18TAC-si and hydrophilpos-si tips, proving an electrostatic contribution. Screening was also observed for the hydrophilpos-si tip in NaNO3, whereas a long-range attraction was observed for the C18TAC-si tip for all NaNO3 concentrations. These results indicate that screening of the forces for the C18TAC-si tip depended on the type and/or size of the anion, possibly due to a different probability of the anions to enter the silane layers. The interaction of C18TAC patches with C18TAC-si tips in the presence of NaCl and the interaction of the patches with hydrophilpos-si tips in either NaCl or NaNO3 were repulsive and independent of the number of force curves measured, indicating a stable, positively charged C18TAC patch. However, the forces measured between the patches and a C18TAC-si tip in NaNO3 depended on the number of force curves measured, indicating a change in patch structure induced by the first interaction.

  20. Ex vivo complement protein adsorption on positively and negatively charged cellulose dialyser membranes.

    Science.gov (United States)

    Mahiout, A; Matata, B M; Vienken, J; Courtney, J M

    1997-05-01

    An ex vivo test system was used to measure complement protein C3 and factor B adsorption onto small dialyser modules made from regenerated and modified cellulosic hollow fibre membranes in which positive diethylaminoethyl (DEAE) or negative carboxymethyl (CM) groups were introduced into the cellulose matrix. The extracorporeal system, which included test-dialysers and the dialysis environment, allowed the use of labelled proteins without contaminating the blood donors which were connected in an open-loop fashion to the extracorporeal test system. The modules were removed at selected time points from the extracorporeal system for radioactivity counting. The results were used to evaluate the mechanisms involved in complement reactions to foreign surfaces. The system therefore allowed the analysis of complement protein adsorption occurring in the dialyser modules and its relationship to the complement generation rate in the extracorporeal system to be evaluated. It was possible to demonstrate that significant complement C3 and factor B adsorption occurred in the test modules made of cellulosic membranes. Complement adsorption as a function of the pH and the release reaction of the adsorbed C3 and factor B after membrane blood perfusion were therefore found to be variable according to the cellulosic membrane type and the presence of positive or negative charged groups within the cellulose matrix. The data obtained from the ex vivo model therefore provided additional evidence on the discussion of the mechanisms involved in the increased complement activation by regenerated cellulose and in its attenuation by DEAE- or CM-modified cellulose.

  1. Positive Charge Region in Lower Part of Thunderstorm and Preliminary Breakdown Process of Negative Cloud-to-Ground Lightning

    Institute of Scientific and Technical Information of China (English)

    ZHANG Yijun; MENG Qing; LU Weitao; MA Ming; ZHENG Dong; Pau R. Krehbiel

    2009-01-01

    A new lightning locating technology, called Lightning Mapping Array (LMA), has been developed. The system takes advantage of GPS technology to measure the times of arrival (TOA) of lightning impulsive very high frequency (VHF) radiation events at each remote location. The spatiotemporal development processes of lightning are described in three-dimension by measurement of the system with high time resolution (50 ns) and space precision (50-100 m). The charge structures in thunderstorm and their relationship with lightning discharge processes are revealed. The temporal and spatial characteristics of preliminary breakdown process involved in negative cloud-to-ground (CG) lightning discharges are analyzed based on the data of lightning VHF radiation events. The effect of positive charge region in lower part of thunderstorm on the occurrence of negative CG lightning discharge is discussed. The results indicate that the preliminary breakdown process with longer duration in negative CG lightning discharges is an intracloud discharge process. It occurs between negative and positive charge regions located in middle and lower parts of thunderstorm respectively.It initiates from the negative charge region and propagates downward. After propagating into the positive charge region, the lightning channel develops horizontally. The characteristics of the preliminary breakdown process are consistent with that of intracloud lightning discharges. The stepped leaders are initiated by the K type breakdown which occurs in the last stage of the preliminary breakdown process and develops downward through the positive charge region. The existence of positive charge region in lower part of thunderstorm results in the occurrence of preliminary breakdown process with longer duration before the return stroke of negative CG lightning discharges.

  2. Positively versus negatively charged moral emotion expectancies in adolescence: the role of situational context and the developing moral self.

    Science.gov (United States)

    Krettenauer, Tobias; Johnston, Megan

    2011-09-01

    The study analyses adolescents' positively charged versus negatively charged moral emotion expectancies. Two hundred and five students (M= 14.83 years, SD= 2.21) participated in an interview depicting various situations in which a moral norm was either regarded or transgressed. Emotion expectancies were assessed for specific emotions (pride, guilt) as well as for overall strength and valence. In addition, self-importance of moral values was measured by a questionnaire. Results revealed that positively charged emotion expectancies were more pronounced in contexts of prosocial action than in the context of moral transgressions, whereas the opposite was true for negatively charged emotions. At the same time, expectations of guilt and pride were substantially related to the self-importance of moral values.

  3. Highly efficient bioinspired molecular Ru water oxidation catalysts with negatively charged backbone ligands.

    Science.gov (United States)

    Duan, Lele; Wang, Lei; Li, Fusheng; Li, Fei; Sun, Licheng

    2015-07-21

    The oxygen evolving complex (OEC) of the natural photosynthesis system II (PSII) oxidizes water to produce oxygen and reducing equivalents (protons and electrons). The oxygen released from PSII provides the oxygen source of our atmosphere; the reducing equivalents are used to reduce carbon dioxide to organic products, which support almost all organisms on the Earth planet. The first photosynthetic organisms able to split water were proposed to be cyanobacteria-like ones appearing ca. 2.5 billion years ago. Since then, nature has chosen a sustainable way by using solar energy to develop itself. Inspired by nature, human beings started to mimic the functions of the natural photosynthesis system and proposed the concept of artificial photosynthesis (AP) with the view to creating energy-sustainable societies and reducing the impact on the Earth environments. Water oxidation is a highly energy demanding reaction and essential to produce reducing equivalents for fuel production, and thereby effective water oxidation catalysts (WOCs) are required to catalyze water oxidation and reduce the energy loss. X-ray crystallographic studies on PSII have revealed that the OEC consists of a Mn4CaO5 cluster surrounded by oxygen rich ligands, such as oxyl, oxo, and carboxylate ligands. These negatively charged, oxygen rich ligands strongly stabilize the high valent states of the Mn cluster and play vital roles in effective water oxidation catalysis with low overpotential. This Account describes our endeavors to design effective Ru WOCs with low overpotential, large turnover number, and high turnover frequency by introducing negatively charged ligands, such as carboxylate. Negatively charged ligands stabilized the high valent states of Ru catalysts, as evidenced by the low oxidation potentials. Meanwhile, the oxygen production rates of our Ru catalysts were improved dramatically as well. Thanks to the strong electron donation ability of carboxylate containing ligands, a seven

  4. Activated singlet exciton fission in a semiconducting polymer.

    Science.gov (United States)

    Musser, Andrew J; Al-Hashimi, Mohammed; Maiuri, Margherita; Brida, Daniele; Heeney, Martin; Cerullo, Giulio; Friend, Richard H; Clark, Jenny

    2013-08-28

    Singlet exciton fission is a spin-allowed process to generate two triplet excitons from a single absorbed photon. This phenomenon offers great potential in organic photovoltaics, but the mechanism remains poorly understood. Most reports to date have addressed intermolecular fission within small-molecular crystals. However, through appropriate chemical design chromophores capable of intramolecular fission can also be produced. Here we directly observe sub-100 fs activated singlet fission in a semiconducting poly(thienylenevinylene). We demonstrate that fission proceeds directly from the initial 1Bu exciton, contrary to current models that involve the lower-lying 2Ag exciton. In solution, the generated triplet pairs rapidly recombine and decay through the 2Ag state. In films, exciton diffusion breaks this symmetry and we observe long-lived triplets which form charge-transfer states in photovoltaic blends.

  5. Charge effects controlling the current hysteresis and negative differential resistance in periodical nanosize Si/CaF sub 2 structures

    CERN Document Server

    Berashevich, Y A; Kholod, A N; Borisenko, V E

    2002-01-01

    A kinetic model of charge carrier transport in nanosize periodical Si/CaF sub 2 structures via localized states in dielectric is proposed. Computer simulation of the current-voltage characteristics of such structures has shown that the built-in field arises in a dielectric due to polarization of the trapped charge by localized centers. This results in current hysteresis and negative differential resistance region at the current-voltage characteristics when the bias polarity is changed. At temperature below 250 K, the portion of negative differential resistance vanishes

  6. Fabrication of Negative Charged Poly (Ethylene glycol)-diacrylate Hydrogel as a Bone Tissue Engineering scaffold

    Institute of Scientific and Technical Information of China (English)

    WANG Ya-qi; LIU Jie; TAN Fei; XIE Wei

    2016-01-01

    Objective To improve the cell attachment of PEGDA hydrogel, the SMAS small molecule was used to modify the PEGDA hydrogel. The charged hydrogel would show improved cell attachment and enhanced protein adsorption caused by enhancement of electrostatic adsorption.Method In this study, a series of charged hydrogels were produced by adding different concentrations of charged small molecule monomer into the PEGDA solution. Then, we investigate the physicochemical and biological characteristics of charged hydrogels, including FTIR, swelling ratio, contact angle, cell attachment.Result The results indicate that the charged monomer had been successfully incorporated into PEGDA hydrogel. Meanwhile, the protein adsorption of the hydrogel increased with increasing concentration of charge modification. Moreover, compared to PEGDA hydrogel, the cell attachment significantly improved on the charged hydrogel.Conclusion The charged hydrogel would be a promising scaffold candidate for bone tissue engineering.

  7. Energy losses of positive and negative charged particles in electron gas

    Science.gov (United States)

    Diachenko, M. M.; Kholodov, R. I.

    2017-02-01

    A heavy charged particle propagation through electron gas has been studied using combination of non-relativistic quantum mechanics and the Green’s functions method. The energy loss of a charged particle has been found in the case of large transferred momentum taking into account the interference term in the expression for the rate. The dependence of the energy loss of a charged particles in electron gas with nonzero temperature on the sign of the charge has been obtained.

  8. In vitro and in vivo performance of biocompatible negatively-charged salbutamol-loaded nanoparticles.

    Science.gov (United States)

    Rytting, Erik; Bur, Michael; Cartier, Regis; Bouyssou, Thierry; Wang, Xiaoying; Krüger, Michael; Lehr, Claus-Michael; Kissel, Thomas

    2010-01-04

    The development and performance of a novel nanoparticle-based formulation for pulmonary delivery has been characterized chronologically through the particle preparation process, in vitro testing of drug release, biocompatibility, degradation, drug transport in cell culture, and in vivo bronchoprotection studies in anaesthetised guinea pigs. This study demonstrates excellent agreement of the in vitro and in vivo experiments undertaken to prove the feasibility of the design, thereby serving as an example highlighting the importance of in vitro test methods that predict in vivo performance. Nanoparticles were prepared from the newly designed negatively-charged polymer poly(vinyl sulfonate-co-vinyl alcohol)-g-poly(d,l-lactic-co-glycolic acid) loaded with salbutamol free base. Average particle sizes of blank and drug-loaded nanoparticles prepared at the various stages of the investigations were between 91 and 204nm; average zeta potential values were between -50.1 and -25.6mV. Blank nanoparticles showed no significant toxicity, and no inflammatory activity was detected in Calu-3 cells. Sustained release of salbutamol from the nanoparticles was observed for 2.5h in vitro, and a prolonged effect was observed for 120min in vivo. These results demonstrate good agreement between in vitro and in vivo tests and also present a promising foundation for future advancement in nanomedicine strategies for pulmonary drug delivery.

  9. Solute Transport of Negatively Charged Contrast Agents Across Articular Surface of Injured Cartilage.

    Science.gov (United States)

    Kokkonen, H T; Chin, H C; Töyräs, J; Jurvelin, J S; Quinn, T M

    2017-04-01

    Solute transport through the extracellular matrix (ECM) is crucial to chondrocyte metabolism. Cartilage injury affects solute transport in cartilage due to alterations in ECM structure and solute-matrix interactions. Therefore, cartilage injury may be detected by using contrast agent-based clinical imaging. In the present study, effects of mechanical injury on transport of negatively charged contrast agents in cartilage were characterized. Using cartilage plugs injured by mechanical compression protocol, effective partition coefficients and diffusion fluxes of iodine- and gadolinium-based contrast agents were measured using high resolution microCT imaging. For all contrast agents studied, effective diffusion fluxes increased significantly, particularly at early times during the diffusion process (38 and 33% increase after 4 min, P integrity in cartilage superficial zone. This study suggests that alterations in contrast agent diffusion flux, a non-equilibrium transport parameter, provides a more sensitive indicator for assessment of cartilage matrix integrity than partition coefficient and the equilibrium distribution of solute. These findings may help in developing clinical methods of contrast agent-based imaging to detect cartilage injury.

  10. Charged rotating black holes in Einstein--Maxwell--Chern-Simons theory with negative cosmological constant

    CERN Document Server

    Blázquez-Salcedo, Jose Luis; Navarro-Lérida, Francisco; Radu, Eugen

    2016-01-01

    We consider rotating black hole solutions in five-dimensional Einstein-Maxwell-Chern-Simons theory with a negative cosmological constant and a generic value of the Chern-Simons coupling constant $\\lambda$. Using both analytical and numerical techniques, we focus on cohomogeneity-1 configurations, with two equal-magnitude angular momenta, which approach at infinity a globally AdS background. We find that the generic solutions share a number of basic properties with the known Cvetic, L\\"u and Pope black holes which have $\\lambda=1$. New features occur as well, for example, when the Chern-Simons coupling constant exceeds a critical value, the solutions are no longer uniquely determined by their global charges. Moreover, the black holes possess radial excitations which can be labelled by the node number of the magnetic gauge potential function. Solutions with small values of $\\lambda$ possess other distinct features. For instance, the extremal black holes there form two disconnected branches, while not all near-h...

  11. Wave packet study of the secondary emission of negatively charged, monoatomic ions from sputtered metals

    Energy Technology Data Exchange (ETDEWEB)

    Sindona, A. [Dipartimento di Fisica, Universita della Calabria, Via P. Bucci 31C, 87036 Rende (Italy) and Istituto Nazionale di Fisica Nucleare (INFN), Gruppo collegato di Cosenza, Via P. Bucci 31C, 87036 Rende (Italy)]. E-mail: sindona@fis.unical.it; Riccardi, P. [Dipartimento di Fisica, Universita della Calabria, Via P. Bucci 31C, 87036 Rende (Italy); Istituto Nazionale di Fisica Nucleare (INFN), Gruppo collegato di Cosenza, Via P. Bucci 31C, 87036 Rende (Italy); Maletta, S. [Dipartimento di Fisica, Universita della Calabria, Via P. Bucci 31C, 87036 Rende (Italy); Rudi, S.A. [Dipartimento di Fisica, Universita della Calabria, Via P. Bucci 31C, 87036 Rende (Italy); Istituto Nazionale di Fisica Nucleare (INFN), Gruppo collegato di Cosenza, Via P. Bucci 31C, 87036 Rende (Italy); Falcone, G. [Dipartimento di Fisica, Universita della Calabria, Via P. Bucci 31C, 87036 Rende (Italy); Istituto Nazionale di Fisica Nucleare (INFN), Gruppo collegato di Cosenza, Via P. Bucci 31C, 87036 Rende (Italy)

    2007-05-15

    Secondary emission of Ag{sup -} and Au{sup -} particles, following the sputtering of clean Ag(1 0 0) and Au(1 0 0) targets, respectively, is studied with a Crank-Nicholson wave-packet propagation method. A one-electron pseudo-potential is used to describe the plane metal surface, with a projected band gap, the ejected ion, whose charge state is investigated, and its nearest-neighbor substrate ion, put in motion by the collision cascade generated by the primary ion beam. Time-dependent Schroedinger equation is solved backwards in time to determine the evolution of the affinity orbital of the negative particles from an instant when they are unperturbed, at distances of the order of {approx}10{sup 2} a.u. from the surface, to the instant of ejection. The probability that a band electron will be eventually detected in affinity state of the ejected particle is, thus, calculated and compared with the result of another method based on the spectral decomposition of the one-electron Hamiltonian.

  12. Negatively charged silver nanoparticles with potent antibacterial activity and reduced toxicity for pharmaceutical preparations

    Directory of Open Access Journals (Sweden)

    Salvioni L

    2017-03-01

    Full Text Available Lucia Salvioni,1 Elisabetta Galbiati,1 Veronica Collico,1 Giulia Alessio,1 Svetlana Avvakumova,1 Fabio Corsi,2,3 Paolo Tortora,1 Davide Prosperi,1 Miriam Colombo1 1Nanobiolab, Department of Biotechnology and Bioscience, University of Milano-Bicocca, 2Biological and Clinical Science Department, University of Milan, Milano, 3Surgery Department, Breast Unit, IRCCS S Maugeri Foundation, Pavia, Italy Background: The discovery of new solutions with antibacterial activity as efficient and safe alternatives to common preservatives (such as parabens and to combat emerging infections and drug-resistant bacterial pathogens is highly expected in cosmetics and pharmaceutics. Colloidal silver nanoparticles (NPs are attracting interest as novel effective antimicrobial agents for the prevention of several infectious diseases.Methods: Water-soluble, negatively charged silver nanoparticles (AgNPs were synthesized by reduction with citric and tannic acid and characterized by transmission electron microscopy, dynamic light scattering, zeta potential, differential centrifuge sedimentation, and ultraviolet–visible spectroscopy. AgNPs were tested with model Gram-negative and Gram-positive bacteria in comparison to two different kinds of commercially available AgNPs.Results: In this work, AgNPs with higher antibacterial activity compared to the commercially available colloidal silver solutions were prepared and investigated. Bacteria were plated and the antibacterial activity was tested at the same concentration of silver ions in all samples. The AgNPs did not show any significant reduction in the antibacterial activity for an acceptable time period. In addition, AgNPs were transferred to organic phase and retained their antibacterial efficacy in both aqueous and nonaqueous media and exhibited no toxicity in eukaryotic cells.Conclusion: We developed AgNPs with a 20 nm diameter and negative zeta potential with powerful antibacterial activity and low toxicity compared

  13. Charged Frenkel biexcitons in organic molecular crystals

    CERN Document Server

    Agranovich, V M; Kamchatnov, A M

    2001-01-01

    It is known that the energy of the lowest electronic transition in neutral molecules of anthracene, tetracene and other polyacenes is blue shifted in comparison with the corresponding transition energy in mono-valent molecular ions. This effect in molecular crystal may be responsible for the attraction between molecular (Frenkel) exciton and charge carrier. Due to this attraction the bound state of Frenkel exciton and free charge (charged Frenkel exciton) may be formed. The same mechanism can be responsible for formation of charged biexcitons (bound state of two Frenkel excitons and a charge carrier). Calculations are performed for molecular crystals like tetracene by means of one-dimensional lattice model

  14. CHARGE-EXCHANGE SCATTERING OF NEGATIVE PIONS BY HYDROGEN AT 230,260, 290, 317 AND 371 MeV

    Energy Technology Data Exchange (ETDEWEB)

    Caris, John C

    1960-03-18

    The differential cross section for charge-exchange scattering of negative pions by hydrogen has been observed at 230, 260, 290, 317, and 371 Mev. The reaction was observed by detecting one gamma ray from the {pi}{sup 0} decay with a scintillation-counter telescope.

  15. The in vitro anti-HIV efficacy of negatively charged human serum albumin is antagonized by heparin

    NARCIS (Netherlands)

    Swart, P J; Sun, C S; Kuipers, M E; Asuncion, C; Josephs, S; Smit, C; Meijer, D K

    1997-01-01

    Succinylated human serum albumin (Suc-HSA) was synthesized by treating human serum albumin with succinic anhydride, Among similar proteins and neo(glyco)proteins tested, Suc-HSA exhibits a pronounced net negative charge, a feature that largely contributes to its efficacy against replication of human

  16. Interwell excitons in GaAs superlattices

    DEFF Research Database (Denmark)

    Birkedal, Dan; Sayed, Karim El; Sanders, G.;

    1996-01-01

    The formation of spatially indirect excitons in superlattices with narrow minibands is theoretically and experimentally investigated. We identify the experimental conditions for the observation of interwell excitons and find a distinct excitonic state energetically located between the Is exciton ...

  17. Design, synthesis and biological evaluation of negatively charged ¹¹¹In-DTPA-octreotide derivatives.

    Science.gov (United States)

    Oshima, Nobuhiro; Akizawa, Hiromichi; Zhao, Songji; Zhao, Yan; Nishijima, Ken-ichi; Kitamura, Yoji; Arano, Yasushi; Kuge, Yuji; Ohkura, Kazue

    2014-02-15

    Our previous studies indicated that (111)In-diethylenetriaminepentaacetic acid ((111)In-DTPA)-octreotide derivatives with an additional negative charge by replacing N-terminal d-phenylalanine (d-Phe) with an acidic amino acid such as l-aspartic acid (Asp) or its derivative exhibited low renal radioactivity levels when compared with (111)In-DTPA-D-Phe(1)-octreotide. On the basis of the findings, we designed, synthesized and evaluated two Asp-modified (111)In-DTPA-conjugated octreotide derivatives, (111)In-DTPA-Asp(1)-octreotide and (111)In-DTPA-Asp(0)-D-Phe(1)-octreotide. While (111)In-DTPA-Asp(1)-octreotide showed negligible AR42J cell uptake, (111)In-DTPA-Asp(0)-D-Phe(1)-octreotide exhibited AR42J cell uptake similar to that of (111)In-DTPA-D-Phe(1)-octreotide. When administered to AR42J tumor-bearing mice, (111)In-DTPA-Asp(0)-D-Phe(1)-octreotide exhibited renal radioactivity levels significantly lower than did (111)In-DTPA-D-Phe(1)-octreotide at 1 and 3 h post-injection. No significant differences were observed in tumor accumulation between (111)In-DTPA-Asp(0)-D-Phe(1)-octreotide and (111)In-DTPA-D-Phe(1)-octreotide after 1 and 3h injection. The findings in this study suggested that an interposition of an Asp at an appropriate position in (111)In-DTPA-D-Phe(1)-octreotide would constitute a useful strategy to develop (111)In-DTPA-D-Phe(1)-octreotide derivatives of low renal radioactivity levels while preserving tumor accumulation. Copyright © 2014 Elsevier Ltd. All rights reserved.

  18. Machine Learning Exciton Dynamics

    CERN Document Server

    Häse, Florian; Pyzer-Knapp, Edward; Aspuru-Guzik, Alán

    2015-01-01

    Obtaining the exciton dynamics of large photosynthetic complexes by using mixed quantum mechanics/molecular mechanics (QM/MM) is computationally demanding. We propose a machine learning technique, multi-layer perceptrons, as a tool to reduce the time required to compute excited state energies. With this approach we predict time-dependent density functional theory (TDDFT) excited state energies of bacteriochlorophylls in the Fenna-Matthews-Olson (FMO) complex. Additionally we compute spectral densities and exciton populations from the predictions. Different methods to determine multi-layer perceptron training sets are introduced, leading to several initial data selections. In addition, we compute spectral densities and exciton populations. Once multi-layer perceptrons are trained, predicting excited state energies was found to be significantly faster than the corresponding QM/MM calculations. We showed that multi-layer perceptrons can successfully reproduce the energies of QM/MM calculations to a high degree o...

  19. Multiscale photosynthetic exciton transfer

    CERN Document Server

    Ringsmuth, A K; Stace, T M; 10.1038/nphys2332

    2012-01-01

    Photosynthetic light harvesting provides a natural blueprint for bioengineered and biomimetic solar energy and light detection technologies. Recent evidence suggests some individual light harvesting protein complexes (LHCs) and LHC subunits efficiently transfer excitons towards chemical reaction centers (RCs) via an interplay between excitonic quantum coherence, resonant protein vibrations, and thermal decoherence. The role of coherence in vivo is unclear however, where excitons are transferred through multi-LHC/RC aggregates over distances typically large compared with intra-LHC scales. Here we assess the possibility of long-range coherent transfer in a simple chromophore network with disordered site and transfer coupling energies. Through renormalization we find that, surprisingly, decoherence is diminished at larger scales, and long-range coherence is facilitated by chromophoric clustering. Conversely, static disorder in the site energies grows with length scale, forcing localization. Our results suggest s...

  20. Daylight-driven photocatalytic degradation of ionic dyes with negatively surface-charged In2S3 nanoflowers: dye charge-dependent roles of reactive species

    Science.gov (United States)

    Ge, Suxiang; Cai, Lejuan; Li, Dapeng; Fa, Wenjun; Zhang, Yange; Zheng, Zhi

    2015-12-01

    Even though dye degradation is a successful application of semiconductor photocatalysis, the roles of reactive species in dye degradation have not received adequate attention. In this study, we systematically investigated the degradation of two cationic dyes (rhodamine B and methylene blue) and two anionic dyes (methyl orange and orange G) over negatively surface-charged In2S3 nanoflowers synthesized at 80 °C under indoor daylight lamp irradiation. It is notable to find In2S3 nanoflowers were more stable in anionic dyes degradation compared to that in cationic dyes removal. The active species trapping experiments indicated photogenerated electrons were mainly responsible for cationic dyes degradation, but holes were more important in anionic dyes degradation. A surface-charge-dependent role of reactive species in ionic dye degradation was proposed for revealing such interesting phenomenon. This study would provide a new insight for preparing highly efficient daylight-driven photocatalyst for ionic dyes degradation.

  1. The UCCSD(T)/CBS Description of the C2h Symmetric, Negatively Charged Dimer of SF2

    Science.gov (United States)

    Czernek, Jiří

    2007-12-01

    A highly accurate potential energy curve of the C2h symmetric, negatively charged dimer of SF2 was obtained by estimating the complete basis set limits of the UCCSD(T) energies at the intermonomer separations ranging from 2.15 to 7.75 Å. The results serve as a benchmark for assessing the quality of methods describing the energetics of open-shell species. Thus, a remarkably good performance of the UMP2 method was observed.

  2. Quasienergy Spectroscopy of Excitons

    DEFF Research Database (Denmark)

    Johnsen, Kristinn; Jauho, Antti-Pekka

    1999-01-01

    We theoretically study nonlinear optics of excitons under intense THz irradiation. In particular, the linear near-infrared absorption and resonantly enhanced nonlinear sideband generation are described. We predict a rich structure in the spectra which an be interpreted in terms of the quasienergy...

  3. Energy and Information Transfer Via Coherent Exciton Wave Packets

    Science.gov (United States)

    Zang, Xiaoning

    Electronic excitons are bound electron-hole states that are generated when light interacts with matter. Such excitations typically entangle with phonons and rapidly decohere; the resulting electronic state dynamics become diffusive as a result. However, if the exciton-phonon coupling can be reduced, it may be possible to construct excitonic wave packets that offer a means of efficiently transmitting information and energy. This thesis is a combined theory/computation investigation to design condensed matter systems which support the requisite coherent transport. Under the idealizing assumption that exciton-phonon entanglement could be completely suppressed, the majority of this thesis focuses on the creation and manipulation of exciton wave packets in quasi-one-dimensional systems. While each site could be a silicon quantum dot, the actual implementation focused on organic molecular assemblies for the sake of computational simplicity, ease of experimental implementation, potential for coherent transport, and promise because of reduced structural uncertainty. A laser design was derived to create exciton wave packets with tunable shape and speed. Quantum interference was then exploited to manipulate these packets to block, pass, and even dissociate excitons based on their energies. These developments allow exciton packets to be considered within the arena of quantum information science. The concept of controllable excitonic wave packets was subsequently extended to consider molecular designs that allow photons with orbital angular momentum to be absorbed to create excitons with a quasi-angular momentum of their own. It was shown that a well-defined measure of topological charge is conserved in such light-matter interactions. Significantly, it was also discovered that such molecules allow photon angular momenta to be combined and later emitted. This amounts to a new way of up/down converting photonic angular momentum without relying on nonlinear optical materials. The

  4. One-dimensional models of excitons in carbon nanotubes

    DEFF Research Database (Denmark)

    Cornean, Horia Decebal; Duclos, Pierre; Pedersen, Thomas Garm

    2004-01-01

    Excitons in carbon nanotubes may be modeled by two oppositely charged particles living on the surface of a cylinder. We derive three one-dimensional effective Hamiltonians which become exact as the radius of the cylinder vanishes. Two of them are solvable.......Excitons in carbon nanotubes may be modeled by two oppositely charged particles living on the surface of a cylinder. We derive three one-dimensional effective Hamiltonians which become exact as the radius of the cylinder vanishes. Two of them are solvable....

  5. Control of excitons in multi-layer van der Waals heterostructures

    Energy Technology Data Exchange (ETDEWEB)

    Calman, E. V., E-mail: ecalman@gmail.com; Dorow, C. J.; Fogler, M. M.; Butov, L. V. [Department of Physics, University of California at San Diego, La Jolla, California 92093-0319 (United States); Hu, S.; Mishchenko, A.; Geim, A. K. [School of Physics and Astronomy, University of Manchester, Manchester M13 9PL (United Kingdom)

    2016-03-07

    We report an experimental study of excitons in a double quantum well van der Waals heterostructure made of atomically thin layers of MoS{sub 2} and hexagonal boron nitride. The emission of neutral and charged excitons is controlled by gate voltage, temperature, and both the helicity and the power of optical excitation.

  6. Formation and condensation of excitonic bound states in the generalized Falicov-Kimball model

    Science.gov (United States)

    Farkašovský, Pavol

    2017-01-01

    The density-matrix-renormalization-group method and the Hartree-Fock approximation with the charge-density-wave instability are used to study a formation and condensation of excitonic bound states in the generalized Falicov-Kimball model. In particular, we examine effects of various factors, such as the f -electron hopping, the local and nonlocal hybridizations, as well as the increasing dimension of the system on the excitonic momentum distribution N (q ) and especially on the number of zero-momentum excitons N0=N (q =0 ) in the condensate. It is found that the negative values of the f -electron hopping integrals tf support the formation of a zero-momentum condensate, whereas the positive values of tf have the fully opposite effect. The opposite effects on the formation of the condensate exhibit also the local and nonlocal hybridizations. The first one strongly supports the formation of the condensate, whereas the second one destroys it completely. Moreover, it was shown that the zero-momentum condensate remains robust with increasing dimension of the system.

  7. Negative charging effect of traps on the gate leakage current of an AlGaN/GaN HEMT

    Energy Technology Data Exchange (ETDEWEB)

    Kim, J. J.; Lim, J. H.; Yang, J. W. [Chonbuk National University, Jeonju (Korea, Republic of); Stanchina, W. [University of Pittsburgh, Pittsburgh, PA (United States)

    2014-08-15

    The negative charging effect of surface traps on the gate leakage current of AlGaN/GaN high electron mobility transistors (HEMTs) was investigated. The gate leakage current could be decreased by two orders of magnitude by using a photo-electrochemical process to treat of the source and the drain region, but current flowed into the gate even at a negative voltage in a limited region when the measurement was executed with a gate voltage sweep from negative to positive voltage. Also the electrical characteristics of the HEMT were degraded by pulsed operation of the gate. Traps newly generated on the surface were regarded as sources for the current that flowed against the applied voltage, and the number of traps was estimated. Also, a slow transient in the drain current was confirmed based on the results of delayed sweep measurements.

  8. Comparison of humic acid rejection and flux decline during filtration with negatively charged and uncharged ultrafiltration membranes.

    Science.gov (United States)

    Shao, Jiahui; Hou, Juan; Song, Hongchen

    2011-01-01

    Increasingly stringent regulations for drinking water quality have stimulated the ultrafiltration (UF) to become one of the best alternatives replacing conventional drinking water treatment technologies. However, UF is not very effectively to remove humic acid due to the comparatively larger pore size compared to the size of humic acid. Fouling issue is another factor that restricts its widespread application. In this study, rejection of humic acid and flux decline were compared with essentially neutral, negatively charged version of a regenerated cellulose membrane, in which electrostatic interaction was explored for a better humic acid removal and less fouling. Solution environment, including ionic strength, pH and calcium ion concentration, affecting humic acid removal and flux decline on negatively charged and neutral membranes was also compared. Results indicated that the appropriate charge modification on the neutral UF membrane could be an effective way for better removal of NOM and reduction of the membrane fouling due to the electrostatic interactions with the combination effect of membrane pore size. Electrostatic interactions are significant important to achieve high humic acid removal and less fouling, and to improve the water quality and protect people's health. Copyright © 2010 Elsevier Ltd. All rights reserved.

  9. Negative Compressibility and Charge Partitioning Between Graphene and MoS2 Two-Dimensional Electron Gases

    Science.gov (United States)

    Tolsma, John; Larentis, Stefano; Tutuc, Emanuel; MacDonald, Allan

    2014-03-01

    Electron-electron interactions often have opposite influences on thermodynamic properties of electrons in graphene compared to conventional two-dimensional electron gases (2DEGs), for example by lowering charge and spin-susceptibilities in the graphene case and enhancing them in the ordinary 2DEG case. In ordinary 2DEGs the charge susceptibility diverges at a finite carrier density, below which the compressibility becomes negative. We theoretically explore the influence of this qualitative difference on how charge is partitioned between a MoS2 and a graphene sheet 2DEG when they act as a compound capacitor electrode. Our theory is based on a random phase approximation for charge fluctuations in the 2DEGS and the coupling constant formulation for the ground state energy. We find that in the ideal case the MoS2 2DEG carrier density jumps immediately to a finite value when it is initially populated and discuss how this effect is moderated by disorder. Work supported by the Welch Foundation grant TBF1473 and the DOE Division of Materials Sciences Engineering grant DE-FG03-02ER45958.

  10. Triplet exciton dissociation in singlet exciton fission photovoltaics

    Energy Technology Data Exchange (ETDEWEB)

    Jadhav, Priya J.; Mohanty, Aseema; Bulovic, Vladimir; Baldo, Marc A. [Department of Electrical Engineering and Computer Science, Massachusetts Institute of Technology, Cambridge, MA (United States); Brown, Patrick R. [Department of Physics, Massachusetts Institute of Technology, Cambridge, MA (United States); Thompson, Nicholas [Department of Materials Science, Massachusetts Institute of Technology, Cambridge, MA (United States); Wunsch, Benjamin [School of Chemistry and Biochemistry, Georgia Institute of Technology, Atlanta, GA (United States); Yost, Shane R.; Hontz, Eric; Van Voorhis, Troy; Bawendi, Moungi G. [Department of Chemistry, Massachusetts Institute of Technology, Cambridge, MA (United States)

    2012-12-04

    Triplet exciton dissociation in singlet exciton fission devices with three classes of acceptors are characterized: fullerenes, perylene diimides, and PbS and PbSe colloidal nanocrystals. Using photocurrent spectroscopy and a magnetic field probe it is found that colloidal PbSe nanocrystals are the most promising acceptors, capable of efficient triplet exciton dissociation and long wavelength absorption. (Copyright copyright 2012 WILEY-VCH Verlag GmbH and Co. KGaA, Weinheim)

  11. Preparation and characteri-zation of some surface nega-tively charged residue mu-tants of cytochrome b5

    Institute of Scientific and Technical Information of China (English)

    2001-01-01

    Site-directed mutagenesis was used to obtain seven variants of tryptic fragment of bovine liver cytochrome b5 (cyt b5), in which the negatively charged residues around the heme exposed edge of cyt b5 were replaced by hydrophobic amino acid alanine. Double-site mutants, triple-site mutants and even quadruple-site mutants were obtained. DNA sequencing and molecular weight measurements of the mutant proteins both confirmed that these site-directed muta- genesises were successfully performed. Spectroelectrochemistry of these mutant proteins revealed that the apparent redox potentials of these mutant proteins caused a positive shift of 2-10 mV. The global structure of these mutant proteins did not show much difference from that of the wild type cyt b5, providing a solid base for the further study on the roles of the proteins' surface charges.

  12. Exciton polarizability in semiconductor nanocrystals.

    Science.gov (United States)

    Wang, Feng; Shan, Jie; Islam, Mohammad A; Herman, Irving P; Bonn, Mischa; Heinz, Tony F

    2006-11-01

    The response of charge to externally applied electric fields is an important basic property of any material system, as well as one critical for many applications. Here, we examine the behaviour and dynamics of charges fully confined on the nanometre length scale. This is accomplished using CdSe nanocrystals of controlled radius (1-2.5 nm) as prototype quantum systems. Individual electron-hole pairs are created at room temperature within these structures by photoexcitation and are probed by terahertz (THz) electromagnetic pulses. The electronic response is found to be instantaneous even for THz frequencies, in contrast to the behaviour reported in related measurements for larger nanocrystals and nanocrystal assemblies. The measured polarizability of an electron-hole pair (exciton) amounts to approximately 10(4) A(3) and scales approximately as the fourth power of the nanocrystal radius. This size dependence and the instantaneous response reflect the presence of well-separated electronic energy levels induced in the system by strong quantum-confinement effects.

  13. Novel exciton systems in 2D TMD monolayers and heterobilayers

    Science.gov (United States)

    Yu, Hongyi

    In this talk, two exciton systems in transition metal dichalcogenides (TMDs) monolayer and heterobilayer will be discussed. In TMD monolayers, the strong e-h Coulomb exchange interaction splits the exciton and trion dispersions into two branches with zero and finite gap, respectively. Each branch is a center-of-mass wave vector dependent coherent superposition of the two valleys, which leads to a valley-orbit coupling and possibly a trion valley Hall effect. The exchange interaction also eliminates the linear polarization of the negative trion PL emission. In TMD heterobilayers with a type-II band alignment, the low energy exciton has an interlayer configuration with the e and h localized in opposite layers. Because of the inevitable twist or/and lattice mismatch between the two layers, the bright interlayer excitons are located at finite center-of-mass velocities with a six-fold degeneracy. The corresponding photon emission is elliptically polarized, with the major axis locked to the direction of exciton velocity, and helicity determined by the valley indices of the e and h. Some experimental results on the interlayer excitons in the WSe2-MoSe2 heterobilayers will also be presented. The interlayer exciton exhibits a long lifetime as well as a long depolarization time, which facilitate the observation of a PL polarization ring pattern due to the valley dependent exciton-exciton interaction induced expansion. The works were supported by the Research Grant Council of Hong Kong (HKU17305914P, HKU705513P), the Croucher Foundation, and the HKU OYRA and ROP.

  14. Controlled Spin Transport in Planar Systems Through Topological Exciton

    CERN Document Server

    Abhinav, Kumar

    2015-01-01

    It is shown that a charge-neutral spin-1 exciton, possibly realizable only in planar systems like graphene and topological insulators, can be effectively used for controlled spin transport in such media. The effect of quantum and thermal fluctuations yield a parametric excitation threshold for its realization. This planar exciton differs from the conventional ones, as it owes its existence to the topological Chern-Simons (CS) term. The parity and time-reversal violating CS term can arise from quantum effects in systems with parity-breaking mass-gap. The spinning exciton naturally couples to magnetic field, leading to the possibility of controlled spin transport. Being neutral, it is immune to a host of effect, which afflicts spin transport through charged fermions.

  15. Steroidal Surfactants: Detection of Premicellar Aggregation, Secondary Aggregation Changes in Micelles, and Hosting of a Highly Charged Negative Substance.

    Science.gov (United States)

    Barnadas-Rodríguez, Ramon; Cladera, Josep

    2015-08-25

    CHAPSO and CHAPS are zwitterionic surfactants derived from bile salts which are usually employed in protein purification and for the preparation of liposomes and bicelles. Despite their spread use, there are significant discrepancies on the critical concentrations that determine their aggregation behavior. In this work, we study the interaction between these surfactants with the negative fluorescent dye pyranine (HPTS) by absorbance, fluorescence, and infrared spectrometry to establish their concentration-dependent aggregation. For the studied surfactants, we detect three critical concentrations showing their concentration-dependent presence as a monomeric form, premicellar aggregates, micelles, and a second type of micelle in aqueous medium. The nature of the interaction of HPTS with the surfactants was studied using analogues of their tails and the negative bile salt taurocholate (TC) as reference for the sterol ring. The results indicate that the chemical groups involved are the hydroxyl groups of the polar face of the sterol ring and the sulfonate groups of the dye. This interaction causes not only the incorporation of the negative dye in CHAPSO and CHAPS micelles but also its association with their premicellar aggregates. Surprisingly, this hosting behavior for a negative charged molecule was also detected for the negative bile salt TC, bypassing, in this way, the electrostatic repulsion between the guest and the host.

  16. Conserved N-terminal negative charges support optimally efficient N-type inactivation of Kv1 channels.

    Directory of Open Access Journals (Sweden)

    Alison Prince

    Full Text Available N-type inactivation is produced by the binding of a potassium channel's N-terminus within the open pore, blocking conductance. Previous studies have found that introduction of negative charges into N-terminal inactivation domains disrupts inactivation; however, the Aplysia AKv1 N-type inactivation domain contains two negatively charged residues, E2 and E9. Rather than being unusual, sequence analysis shows that this N-terminal motif is highly conserved among Kv1 sequences across many phyla. Conservation analysis shows some tolerance at position 9 for other charged residues, like D9 and K9, whereas position 2 is highly conserved as E2. To examine the functional importance of these residues, site directed mutagenesis was performed and effects on inactivation were recorded by two electrode voltage clamp in Xenopus oocytes. We find that inclusion of charged residues at positions 2 and 9 prevents interactions with non-polar sites along the inactivation pathway increasing the efficiency of pore block. In addition, E2 appears to have additional specific electrostatic interactions that stabilize the inactivated state likely explaining its high level of conservation. One possible explanation for E2's unique importance, consistent with our data, is that E2 interacts electrostatically with a positive charge on the N-terminal amino group to stabilize the inactivation domain at the block site deep within the pore. Simple electrostatic modeling suggests that due to the non-polar environment in the pore in the blocked state, even a 1 Å larger separation between these charges, produced by the E2D substitution, would be sufficient to explain the 65× reduced affinity of the E2D N-terminus for the pore. Finally, our studies support a multi-step, multi-site N-type inactivation model where the N-terminus interacts deep within the pore in an extended like structure placing the most N-terminal residues 35% of the way across the electric field in the pore blocked

  17. Exciton size and binding energy limitations in one-dimensional organic materials

    Energy Technology Data Exchange (ETDEWEB)

    Kraner, S., E-mail: stefan.kraner@iapp.de; Koerner, C.; Leo, K. [Institut für Angewandte Photophysik, Technische Universität Dresden, Dresden (Germany); Scholz, R. [Institut für Angewandte Photophysik, Technische Universität Dresden, Dresden (Germany); Dresden Center of Computational Materials Science, Technische Universität Dresden, D-01062 Dresden (Germany); Plasser, F. [Institute for Theoretical Chemistry, University of Vienna, A-1090 Vienna (Austria)

    2015-12-28

    In current organic photovoltaic devices, the loss in energy caused by the charge transfer step necessary for exciton dissociation leads to a low open circuit voltage, being one of the main reasons for rather low power conversion efficiencies. A possible approach to avoid these losses is to tune the exciton binding energy to a value of the order of thermal energy, which would lead to free charges upon absorption of a photon, and therefore increase the power conversion efficiency towards the Shockley-Queisser limit. We determine the size of the excitons for different organic molecules and polymers by time dependent density functional theory calculations. For optically relevant transitions, the exciton size saturates around 0.7 nm for one-dimensional molecules with a size longer than about 4 nm. For the ladder-type polymer poly(benzimidazobenzophenanthroline), we obtain an exciton binding energy of about 0.3 eV, serving as a lower limit of the exciton binding energy for the organic materials investigated. Furthermore, we show that charge transfer transitions increase the exciton size and thus identify possible routes towards a further decrease of the exciton binding energy.

  18. Implications of surface charge and curvature for the binding orientation of Thermomyces lanuginosus lipase on negatively charged or zwitterionic phospholipid vesicles as studied by ESR spectroscopy

    DEFF Research Database (Denmark)

    Hedin, E.M.K.; Høyrup, Lise Pernille Kristine; Patkar, S.A.;

    2005-01-01

    , Y., et al. (2000) Biochemistry 39, 413-423]. The productive-mode binding orientation of TLL at the lipid-water interface of small unilamellar vesicles (SUV) consisting of 1-palmitoyl-2-oleoyi-sn-glycero-3-phosphati-dylglycerol (POPG) was previously determined using electron spin resonance (ESR......) spectroscopy in combination with site-directed spin-labeling [Hedin, E. M. K., et al. (2002) Biochemistry 41, 1418514196]. In our investigation, we have studied the interfacial orientation of TLL when bound to large unilamellar vesicles (LUV) consisting of POPG, and bound to SUV consisting of 1-palmitoyl-2...... fluorescence quenching efficiency between each spin-label positioned on TLL, and the lipid membrane. ESR exposure and fluorescence quenching data show that TILL associates closer to the negatively charged PG surface than the zwitterionic PC surface, and binds to both POPG LUV and POPC SUV predominantly through...

  19. Insights into the mechanisms of electromediated gene delivery and application to the loading of giant vesicles with negatively charged macromolecules

    CERN Document Server

    Portet, Thomas; Teissié, Justin; Dean, David S; Rols, Marie-Pierre

    2011-01-01

    We present experimental results regarding the electrotransfer of plasmid DNA into phosphatidylcholine giant unilamellar vesicles (GUVs). Our observations indicate that a direct entry is the predominant mechanism of electrotransfer. A quantitative analysis of the DNA concentration increments inside the GUVs is also performed, and we find that our experimental data are very well described by a simple theoretical model in which DNA entry is mostly driven by electrophoresis. Our theoretical framework allows for the prediction of the amount of transfered DNA as a function of the electric field parameters, and thus paves the way towards a novel method for encapsulating with high efficiency not only DNA, but any negatively charged macromolecule into GUVs.

  20. The Effect of Charge at the Surface of Silver Nanoparticles on Antimicrobial Activity against Gram-Positive and Gram-Negative Bacteria: A Preliminary Study

    Directory of Open Access Journals (Sweden)

    Abbas Abbaszadegan

    2015-01-01

    Full Text Available The bactericidal efficiency of various positively and negatively charged silver nanoparticles has been extensively evaluated in literature, but there is no report on efficacy of neutrally charged silver nanoparticles. The goal of this study is to evaluate the role of electrical charge at the surface of silver nanoparticles on antibacterial activity against a panel of microorganisms. Three different silver nanoparticles were synthesized by different methods, providing three different electrical surface charges (positive, neutral, and negative. The antibacterial activity of these nanoparticles was tested against gram-positive (i.e., Staphylococcus aureus, Streptococcus mutans, and Streptococcus pyogenes and gram-negative (i.e., Escherichia coli and Proteus vulgaris bacteria. Well diffusion and micro-dilution tests were used to evaluate the bactericidal activity of the nanoparticles. According to the obtained results, the positively-charged silver nanoparticles showed the highest bactericidal activity against all microorganisms tested. The negatively charged silver nanoparticles had the least and the neutral nanoparticles had intermediate antibacterial activity. The most resistant bacteria were Proteus vulgaris. We found that the surface charge of the silver nanoparticles was a significant factor affecting bactericidal activity on these surfaces. Although the positively charged nanoparticles showed the highest level of effectiveness against the organisms tested, the neutrally charged particles were also potent against most bacterial species.

  1. Excitons in asymmetric quantum wells

    Science.gov (United States)

    Grigoryev, P. S.; Kurdyubov, A. S.; Kuznetsova, M. S.; Ignatiev, I. V.; Efimov, Yu. P.; Eliseev, S. A.; Petrov, V. V.; Lovtcius, V. A.; Shapochkin, P. Yu.

    2016-09-01

    Resonance dielectric response of excitons is studied for the high-quality InGaAs/GaAs heterostructures with wide asymmetric quantum wells (QWs). To highlight effects of the QW asymmetry, we have grown and studied several heterostructures with nominally square QWs as well as with triangle-like QWs. Several quantum confined exciton states are experimentally observed as narrow exciton resonances. A standard approach for the phenomenological analysis of the profiles is generalized by introducing different phase shifts for the light waves reflected from the QWs at different exciton resonances. Good agreement of the phenomenological fit to the experimentally observed exciton spectra for high-quality structures allowed us to reliably obtain parameters of the exciton resonances: the exciton transition energies, the radiative broadenings, and the phase shifts. A direct numerical solution of the Schrödinger equation for the heavy-hole excitons in asymmetric QWs is used for microscopic modeling of the exciton resonances. Remarkable agreement with the experiment is achieved when the effect of indium segregation is taken into account. The segregation results in a modification of the potential profile, in particular, in an asymmetry of the nominally square QWs.

  2. Enhanced antidepressant-like effects of the macromolecule trefoil factor 3 by loading into negatively charged liposomes

    Directory of Open Access Journals (Sweden)

    Qin J

    2014-11-01

    Full Text Available Jing Qin,1 Xu Yang,1–3 Jia Mi,4 Jianxin Wang,1 Jia Hou,1,2 Teng Shen,1 Yongji Li,2 Bin Wang,4 Xuri Li,4 Weili Zhu5 1Department of Pharmaceutics, School of Pharmacy, Fudan University, Key Laboratory of Smart Drug Delivery, Ministry of Education, Shanghai, 2Department of Pharmaceutics, School of Pharmacy, Heilongjiang University of Chinese Medicine, Harbin, 3Department of Pharmacy, The Fifth People’s Hospital of Shanghai, Fudan University, Shanghai, 4Binzhou Medical University, Yantai, 5National Institute on Drug Dependence, Peking University, Beijing, People’s Republic of China Abstract: Immunocytes, mainly neutrophils and monocytes, exhibit an intrinsic homing property, enabling them to migrate to sites of injury and inflammation. They can thus act as Trojan horses carrying concealed drug cargoes while migrating across impermeable barriers to sites of disease, especially the blood–brain barrier (BBB. In this study, to target circulating phagocytic cells, we formulated negatively charged nanosize liposomes and loaded trefoil factor 3 (TFF3 into liposomes by the pH-gradient method. According to the optimized formulation (5:1.5 of lipid to cholesterol, 10:1 of lipid to drug, 10 mg/mL of lipid concentration, and 10 mmol/L of phosphate-buffered saline, 44.47% entrapment efficiency was obtained for TFF3 liposomes with 129.6 nm particle size and –36.6 mV zeta potential. Compared with neutrally charged liposomes, the negatively charged liposomes showed a strong binding capacity with monocytes and were effectively carried by monocytes to cross the BBB in vitro. Furthermore, enhanced antidepressant-like effects were found in the tail-suspension and forced-swim tests in mice, as measured by decreased immobility time, as well as increased swimming time and reduced immobility in rats. These results suggested that negatively charged liposomes could improve the behavioral responses of TFF3, and our study opens up a new way for the development of

  3. Optimization of tetravalent manganese feroxyhyte's negative charge density: A high-performing mercury adsorbent from drinking water.

    Science.gov (United States)

    Kokkinos, E; Simeonidis, K; Pinakidou, F; Katsikini, M; Mitrakas, M

    2017-01-01

    This study demonstrates an optimization procedure for the development of an Hg-specified adsorbent able to comply with the regulation limit for drinking water of 1μg/L. On this purpose, the synthesis of Mn(IV)-feroxyhyte was modified to achieve high negative charge density by combining alkaline and extreme oxidizing conditions. In particular, precipitation of FeSO4 at pH9 and excess of KMnO4 follows a very fast nucleation step providing a product with very small nanocrystal size (1-2nm), high specific surface area (300m(2)/g) and maximum negative charge density (1.8mmol H(+)/g). The adsorbent was validated for Hg removal in batch experiments and column tests using natural-like water indicating an adsorption capacity as high as 2.5μg/mg at equilibrium concentration 1μg/L under reliable conditions of application. Importantly, the adsorption is an exothermic spontaneous process, resulting in the formation of inner sphere complexes by sharing both A-type and B-type oxygen atoms with the metal surface octahedral as revealed by the X-ray absorption fine structure results. Copyright © 2016 Elsevier B.V. All rights reserved.

  4. Comparison of chiral separation of basic drugs in capillary electrophoresis and liquid chromatography using neutral and negatively charged cyclodextrins.

    Science.gov (United States)

    Kwaterczak, Arkadiusz; Duszczyk, Kazimiera; Bielejewska, Anna

    2009-07-10

    Liquid chromatography (LC) and capillary electrophoresis (CE) are very widely used as chiral separation methods. In this publication we try to find if the results obtained in CE and LC with the chiral selector added to the electrolyte and the mobile phase, respectively, can be used as tools for studying weak stereoselective interactions, and how this information can be useful for optimizing chiral separation processes. The manuscript presents a systematic comparison of chiral discrimination of model compounds in HPLC and CE using neutral and negatively charged cyclodextrins. The enantiomeric separation of basic chiral pharmaceuticals such as pheniramine, brompheniramine, metoxyphenamine, cyclopentolate, doxylamine and ketamine was investigated in capillary electrophoresis (CE) and liquid chromatography (HPLC) using negatively charged sulfated-beta-cyclodextrin (S-beta-CD) and neutral cyclodextrins (CDs). The apparent stability constants between the model compounds and cyclodextrins were estimated in both techniques. We discuss the influence of the stability constant and K1/K2 ratio of the investigated complexes on chiral separation obtained in both techniques.

  5. NaV2O5 : An exotic exciton system

    NARCIS (Netherlands)

    Mostovoy, MV; Khomskii, DI; Knoester, J; Cho, K; Matsui, A

    2001-01-01

    We show that the phase transition which sodium vanadate undergoes at T-c = 34 K is driven by a charge ordering. The relevant effective Hamiltonian is of the Frenkel exciton type, with a very large bandwidth to molecular energy ratio. This causes strong non-Heitler-London effects and a temperature de

  6. NaV2O5 : An Exotic Exciton System

    NARCIS (Netherlands)

    Mostovoy, Maxim V.; Khomskii, Daniel I.; Knoester, Jasper

    2001-01-01

    We show that the phase transition which sodium vanadate undergoes at Tc = 34 K is driven by a charge ordering. The relevant effective Hamiltonian is of the Frenkel exciton type, with a very large bandwidth to molecular energy ratio. This causes strong non-Heitler-London effects and a temperature dep

  7. Negative Ion MALDI Mass Spectrometry of Polyoxometalates (POMs): Mechanism of Singly Charged Anion Formation and Chemical Properties Evaluation

    Science.gov (United States)

    Boulicault, Jean E.; Alves, Sandra; Cole, Richard B.

    2016-08-01

    MALDI-MS has been developed for the negative ion mode analysis of polyoxometalates (POMs). Matrix optimization was performed using a variety of matrix compounds. A first group of matrixes offers MALDI mass spectra containing abundant intact singly charged anionic adduct ions, as well as abundant in-source fragmentations at elevated laser powers. A relative ranking of the ability to induce POM fragmentation is found to be: DAN > CHCA > CNA > DIT> HABA > DCTB > IAA. Matrixes of a second group provide poorer quality MALDI mass spectra without observable fragments. Sample preparation, including the testing of salt additives, was performed to optimize signals for a model POM, POMc12, the core structure of which bears four negative charges. The matrix 9-cyanoanthracene (CNA) provided the best signals corresponding to singly charged intact POMc12 anions. Decompositions of these intact anionic species were examined in detail, and it was concluded that hydrogen radical-induced mechanisms were not prevalent, but rather that the observed prompt fragments originate from transferred energy derived from initial electronic excitation of the CNA matrix. Moreover, in obtained MALDI mass spectra, clear evidence of electron transfer to analyte POM species was found: a manifestation of the POMs ability to readily capture electrons. The affinity of polyanionic POMc12 toward a variety of cations was evaluated and the following affinity ranking was established: Fe3+ > Al3+ > Li+ > Ga3+ > Co2+ > Cr3+ > Cu2+ > [Mn2+, Mg2+] > [Na+, K+]. Thus, from the available cationic species, specific adducts are preferentially formed, and evidence is given that these higher affinity POM complexes are formed in the gas phase during the early stages of plume expansion.

  8. Binding of β-Amyloid (1–42) Peptide to Negatively Charged Phospholipid Membranes in the Liquid-Ordered State: Modeling and Experimental Studies

    OpenAIRE

    Ahyayauch, Hasna; Raab, Michal; Busto, Jon V.; Andraka, Nagore; Arrondo, José-Luis R.; Masserini, Massimo; Tvaroska, Igor; Goñi, Félix M.

    2012-01-01

    To explore the initial stages of amyloid β peptide (Aβ42) deposition on membranes, we have studied the interaction of Aβ42 in the monomeric form with lipid monolayers and with bilayers in either the liquid-disordered or the liquid-ordered (Lo) state, containing negatively charged phospholipids. Molecular dynamics (MD) simulations of the system have been performed, as well as experimental measurements. For bilayers in the Lo state, in the absence of the negatively charged lipids, interaction i...

  9. Charge recombination mechanism to explain the negative capacitance in dye-sensitized solar cells

    Science.gov (United States)

    Lie-Feng, Feng; Kun, Zhao; Hai-Tao, Dai; Shu-Guo, Wang; Xiao-Wei, Sun

    2016-03-01

    Negative capacitance (NC) in dye-sensitized solar cells (DSCs) has been confirmed experimentally. In this work, the recombination behavior of carriers in DSC with semiconductor interface as a carrier’s transport layer is explored theoretically in detail. Analytical results indicate that the recombination behavior of carriers could contribute to the NC of DSCs under small signal perturbation. Using this recombination capacitance we propose a novel equivalent circuit to completely explain the negative terminal capacitance. Further analysis based on the recombination complex impedance show that the NC is inversely proportional to frequency. In addition, analytical recombination resistance is composed by the alternating current (AC) recombination resistance (Rrac) and the direct current (DC) recombination resistance (Rrdc), which are caused by small-signal perturbation and the DC bias voltage, respectively. Both of two parts will decrease with increasing bias voltage. Project supported by the National Natural Science Foundation of China (Grant Nos. 11204209 and 60876035) and the Natural Science Foundation of Tianjin City, China (Grant No. 13JCZDJC32800).

  10. Cell surface hydrophobicity and charge of Staphylococcus aureus and coagulase-negative staphylococci from bovine mastitis.

    Science.gov (United States)

    Mamo, W; Rozgonyi, F; Brown, A; Hjertén, S; Wadström, T

    1987-03-01

    The effects of seven growth media on cell surface hydrophobicity of a collection of Staphylococcus aureus and coagulase-negative staphylococci isolated from bovine mastitis were compared in the salt-aggregation test. Thirty-three per cent of Staph. aureus strains showed extremely high cell surface hydrophobicity (auto-aggregated) and 28% were moderately hydrophobic while 26% were hydrophilic after growth on horse blood agar at 37 degrees C for 18 h. There were great variations in the proportion and degree of the hydrophobicity depending on the medium used. Cultivations on/in capsule-inducing media caused a shift from a high to a low degree of hydrophobicity, although a microscopically detectable capsule or slime layer was seen in only one strain. This strain and encapsulated reference strains had a hydrophilic cell surface and migrated faster in free zone electrophoresis than cells of unencapsulated strains. Cells of strains grown on staphylococcus medium 110 agar migrated faster than those grown on horse blood agar regardless of their capsule production. Coagulase-negative staphylococci showed uniformly hydrophilic cell surface after cultivation on horse blood agar, but not when grown in tryptic soy broth or proteose peptone broth. It was concluded that most of the Staph. aureus strains from bovine mastitis under a variety of growth conditions in stationary phase culture constantly expressed hydrophobic cell surface.

  11. Hot exciton dissociation in polymer solar cells.

    Science.gov (United States)

    Grancini, G; Maiuri, M; Fazzi, D; Petrozza, A; Egelhaaf, H-J; Brida, D; Cerullo, G; Lanzani, G

    2013-01-01

    The standard picture of photovoltaic conversion in all-organic bulk heterojunction solar cells predicts that the initial excitation dissociates at the donor/acceptor interface after thermalization. Accordingly, on above-gap excitation, the excess photon energy is quickly lost by internal dissipation. Here we directly target the interfacial physics of an efficient low-bandgap polymer/PC(60)BM system. Exciton splitting occurs within the first 50 fs, creating both interfacial charge transfer states (CTSs) and polaron species. On high-energy excitation, higher-lying singlet states convert into hot interfacial CTSs that effectively contribute to free-polaron generation. We rationalize these findings in terms of a higher degree of delocalization of the hot CTSs with respect to the relaxed ones, which enhances the probability of charge dissociation in the first 200 fs. Thus, the hot CTS dissociation produces an overall increase in the charge generation yield.

  12. PbSe Nanocrystal Excitonic Solar Cells

    KAUST Repository

    Choi, Joshua J.

    2009-11-11

    We report the design, fabrication, and characterization of colloidal PbSe nanocrystal (NC)-based photovoltaic test structures that exhibit an excitonic solar cell mechanism. Charge extraction from the NC active layer is driven by a photoinduced chemical potential energy gradient at the nanostructured heterojunction. By minimizing perturbation to PbSe NC energy levels and thereby gaining insight into the "intrinsic" photovoltaic properties and charge transfer mechanism of PbSe NC, we show a direct correlation between interfacial energy level offsets and photovoltaic device performance. Size dependent PbSe NC energy levels were determined by cyclic voltammetry and optical spectroscopy and correlated to photovoltaic measurements. Photovoltaic test structures were fabricated from PbSe NC films sandwiched between layers of ZnO nanoparticles and PEDOT:PSS as electron and hole transporting elements, respectively. The device current-voltage characteristics suggest a charge separation mechanism that Is distinct from previously reported Schottky devices and consistent with signatures of excitonic solar cells. Remarkably, despite the limitation of planar junction structure, and without film thickness optimization, the best performing device shows a 1-sun power conversion efficiency of 3.4%, ranking among the highest performing NC-based solar cells reported to date. © 2009 American Chemical Society.

  13. On the gas-phase dimerization of negatively charged closo-dodecaborates: a theoretical study.

    Science.gov (United States)

    Zeonjuk, Lei Liu; Vankova, Nina; Knapp, Carsten; Gabel, Detlef; Heine, Thomas

    2013-07-07

    We have studied the intriguing gas-phase dimerization of the B12In(-) (n = 9, 8) anions to B24I2n(2-) dianions by means of density functional theory calculations. The dimerization of B12I9(-) to B24I18(2-) has been detected experimentally in a previous study (Phys. Chem. Chem. Phys., 2011, 13, 5712) utilizing electrospray ionization ion trap mass spectrometry (ESI-IT-MS), whereas the formation of B24I16(2-) from B12I8(-) is modeled here prior to experiment. Calculations are carried out to determine the molecular and electronic structures, the bonding situation and the stability of the dimers relative to the respective monomers. The dimerization process is found to be thermodynamically favorable, and the stability of the lowest-energy structures is substantiated by molecular dynamics simulations. The calculations imply that the experimentally observed B24I18(2-) and the hypothetical B24I16(2-) species are formed through dimerization of the respective B12In(-) (n = 9, 8) monomers, rather than through loss of two I radicals from B24I2n+2(2-) dimers. Electronic properties such as natural charges, vertical detachment energies (VDEs), frontier molecular orbitals (FMOs), and HOMO-LUMO gaps are computed and analyzed in detail for all monomers and dimers. The analysis shows that the most stable B24I2n(2-) dimers are formed through two 2c-2e B-B and two 3c-2e B-I-B bridges between the parent B12In(-) (n = 9, 8) monomers. These new bridging bonds engage the deiodinated (bare) faces of the two B12 icosahedra, as well as one (per monomer) of the nearest boron neighbors and its iodine substituent.

  14. Exciton Formation in Disordered Semiconductors

    DEFF Research Database (Denmark)

    Klochikhin, A.; Reznitsky, A.; Permogorov, S.

    1999-01-01

    Stationary luminescence spectra of disordered solid solutions can be accounted by the model of localized excitons. Detailed analysis of the long time decay kinetics of luminescence shows that exciton formation in these systems is in great extent due to the bimolecular reaction of separated carrie...

  15. Exciton Formation in Disordered Semiconductors

    DEFF Research Database (Denmark)

    Klochikhin, A.; Reznitsky, A.; Permogorov, S.

    1999-01-01

    Stationary luminescence spectra of disordered solid solutions can be accounted by the model of localized excitons. Detailed analysis of the long time decay kinetics of luminescence shows that exciton formation in these systems is in great extent due to the bimolecular reaction of separated carrier...

  16. Dynamics of Photogenerated Polaron-Excitons in Organic Semiconductors

    Science.gov (United States)

    Junior, Luiz A. Ribeiro; Neto, Pedro H. Oliveira; da Cunha, Wiliam F.; Silva, Geraldo M. e.

    In this work we performed numerical simulations of one π-conjugated polymer chain subjected to photogeneration. Within the SSH model modified to include the Brazoviskii-Kirova symmetry breaking term, we investigate the dynamics of photoexcitations to address the generation mechanism of polaron-excitons using the unrestricted Hartree-Fock approximation. It was obtained that after the photoexcitation the system relaxes spontaneously into a polaron-exciton in a transient state in a range of 200 fs. Our results also show that charged polarons are generated directly after this transient state.

  17. Effect of secondary electron emission on nonlinear dust acoustic wave propagation in a complex plasma with negative equilibrium dust charge

    Science.gov (United States)

    Bhakta, Subrata; Ghosh, Uttam; Sarkar, Susmita

    2017-02-01

    In this paper, we have investigated the effect of secondary electron emission on nonlinear propagation of dust acoustic waves in a complex plasma where equilibrium dust charge is negative. The primary electrons, secondary electrons, and ions are Boltzmann distributed, and only dust grains are inertial. Electron-neutral and ion-neutral collisions have been neglected with the assumption that electron and ion mean free paths are very large compared to the plasma Debye length. Both adiabatic and nonadiabatic dust charge variations have been separately taken into account. In the case of adiabatic dust charge variation, nonlinear propagation of dust acoustic waves is governed by the KdV (Korteweg-de Vries) equation, whereas for nonadiabatic dust charge variation, it is governed by the KdV-Burger equation. The solution of the KdV equation gives a dust acoustic soliton, whose amplitude and width depend on the secondary electron yield. Similarly, the KdV-Burger equation provides a dust acoustic shock wave. This dust acoustic shock wave may be monotonic or oscillatory in nature depending on the fact that whether it is dissipation dominated or dispersion dominated. Our analysis shows that secondary electron emission increases nonadiabaticity induced dissipation and consequently increases the monotonicity of the dust acoustic shock wave. Such a dust acoustic shock wave may accelerate charge particles and cause bremsstrahlung radiation in space plasmas whose physical process may be affected by secondary electron emission from dust grains. The effect of the secondary electron emission on the stability of the equilibrium points of the KdV-Burger equation has also been investigated. This equation has two equilibrium points. The trivial equilibrium point with zero potential is a saddle and hence unstable in nature. The nontrivial equilibrium point with constant nonzero potential is a stable node up to a critical value of the wave velocity and a stable focus above it. This critical

  18. Systematic effects in the measurement of the negatively charged pion mass using laser spectroscopy of pionic helium atoms

    CERN Document Server

    Obreshkov, Boyan

    2016-01-01

    The collision-induced shift and broadening of selected dipole transition lines of pionic helium in gaseous helium at low temperatures up to $T=12$ K and pressure up to a few bar are calculated within variable phase function approach. We predict blue shift of the resonance frequencies of the $(n,l)=(16,15) \\rightarrow (16,14) $ and $(16,15) \\rightarrow (17,14)$ unfavored transitions and red shift for the favored transition $(17,16) \\rightarrow (16,15)$. The result may be helpful in reducing the systematic error in proposed future experiments for determination of the negatively charged pion mass from laser spectroscopy of metastable pionic helium atoms.

  19. Very low surface recombination velocities on p-type silicon wafers passivated with a dielectric with fixed negative charge

    Energy Technology Data Exchange (ETDEWEB)

    Agostinelli, G.; Delabie, A.; Dekkers, H.F.W.; De Wolf, S.; Beaucarne, G. [IMEC vzw, Kapeldreef 75, Leuven (Belgium); Vitanov, P.; Alexieva, Z. [CL SENES, Sofia (Bulgaria)

    2006-11-23

    Surface recombination velocities as low as 10cm/s have been obtained by treated atomic layer deposition (ALD) of Al{sub 2}O{sub 3} layers on p-type CZ silicon wafers. Low surface recombination is achieved by means of field induced surface passivation due to a high density of negative charges stored at the interface. In comparison to a diffused back surface field, an external field source allows for higher band bending, that is, a better performance. While this process yields state of the art results, it is not suited for large-scale production. Preliminary results on an industrially viable, alternative process based on a pseudo-binary system containing Al{sub 2}O{sub 3} are presented, too. With this process, surface recombination velocities of 500-1000cm/s have been attained on mc-Si wafers. (author)

  20. Cell Type-Specific Activation of AKT and ERK Signaling Pathways by Small Negatively-Charged Magnetic Nanoparticles

    Science.gov (United States)

    Rauch, Jens; Kolch, Walter; Mahmoudi, Morteza

    2012-11-01

    The interaction of nanoparticles (NPs) with living organisms has become a focus of public and scientific debate due to their potential wide applications in biomedicine, but also because of unwanted side effects. Here, we show that superparamagnetic iron oxide NPs (SPIONs) with different surface coatings can differentially affect signal transduction pathways. Using isogenic pairs of breast and colon derived cell lines we found that the stimulation of ERK and AKT signaling pathways by SPIONs is selectively dependent on the cell type and SPION type. In general, cells with Ras mutations respond better than their non-mutant counterparts. Small negatively charged SPIONs (snSPIONs) activated ERK to a similar extent as epidermal growth factor (EGF), and used the same upstream signaling components including activation of the EGF receptor. Importantly, snSPIONs stimulated the proliferation of Ras transformed breast epithelial cells as efficiently as EGF suggesting that NPs can mimic physiological growth factors.

  1. Activation energy of negative fixed charges in thermal ALD Al{sub 2}O{sub 3}

    Energy Technology Data Exchange (ETDEWEB)

    Kühnhold-Pospischil, S. [Fraunhofer Institute for Solar Energy Systems ISE, Heidenhofstr. 2, 79110 Freiburg (Germany); Institute of Physical Chemistry, Albert-Ludwigs-Universität Freiburg, Albertstr. 21, 79104 Freiburg (Germany); Freiburg Materials Research Center FMF, Albert-Ludwigs-Universität Freiburg, Stefan-Meier-Str. 21, 79104 Freiburg (Germany); Saint-Cast, P.; Richter, A.; Hofmann, M. [Fraunhofer Institute for Solar Energy Systems ISE, Heidenhofstr. 2, 79110 Freiburg (Germany)

    2016-08-08

    A study of the thermally activated negative fixed charges Q{sub tot} and the interface trap densities D{sub it} at the interface between Si and thermal atomic-layer-deposited amorphous Al{sub 2}O{sub 3} layers is presented. The thermal activation of Q{sub tot} and D{sub it} was conducted at annealing temperatures between 220 °C and 500 °C for durations between 3 s and 38 h. The temperature-induced differences in Q{sub tot} and D{sub it} were measured using the characterization method called corona oxide characterization of semiconductors. Their time dependency were fitted using stretched exponential functions, yielding activation energies of E{sub A} = (2.2 ± 0.2) eV and E{sub A} = (2.3 ± 0.7) eV for Q{sub tot} and D{sub it}, respectively. For annealing temperatures from 350 °C to 500 °C, the changes in Q{sub tot} and D{sub it} were similar for both p- and n-type doped Si samples. In contrast, at 220 °C the charging process was enhanced for p-type samples. Based on the observations described in this contribution, a charging model leading to Q{sub tot} based on an electron hopping process between the silicon and Al{sub 2}O{sub 3} through defects is proposed.

  2. Characterization of oil-free and oil-loaded liquid-crystalline particles stabilized by negatively charged stabilizer citrem.

    Science.gov (United States)

    Nilsson, Christa; Edwards, Katarina; Eriksson, Jonny; Larsen, Susan Weng; Østergaard, Jesper; Larsen, Claus; Urtti, Arto; Yaghmur, Anan

    2012-08-14

    The present study was designed to evaluate the effect of the negatively charged food-grade emulsifier citrem on the internal nanostructures of oil-free and oil-loaded aqueous dispersions of phytantriol (PHYT) and glyceryl monooleate (GMO). To our knowledge, this is the first report in the literature on the utilization of this charged stabilizing agent in the formation of aqueous dispersions consisting of well-ordered interiors (either inverted-type hexagonal (H(2)) phases or inverted-type microemulsion systems). Synchrotron small-angle X-ray scattering (SAXS) and cryogenic transmission electron microscopy (cryo-TEM) were used to characterize the dispersed and the corresponding nondispersed phases of inverted-type nonlamellar liquid-crystalline phases and microemulsions. The results suggest a transition between different internal nanostructures of the aqueous dispersions after the addition of the stabilizer. In addition to the main function of citrem as a stabilizer that adheres to the surface of the dispersed particles, it has a significant impact on the internal nanostructures, which is governed by the following factors: (1) its penetration between the hydrophobic tails of the lipid molecules and (2) its degree of incorporation into the lipid-water interfacial area. In the presence of citrem, the formation of aqueous dispersions with functionalized hydrophilic domains by the enlargement of the hydrophilic nanochannels of the internal H(2) phase in hexosomes and the hydrophilic core of the L(2) phase in emulsified microemulsions (EMEs) could be particularly attractive for solubilizing and controlling the release of positively charged drugs.

  3. Interaction of quinine with negatively charged lipid vesicles studied by fluorescence spectroscopy Influence of the pH

    Science.gov (United States)

    Pedrós, Jesús; Porcar, Iolanda; Gómez, Clara M.; Campos, Agustín; Abad, Concepción

    1997-03-01

    The interaction of quinine with dimyristoylphosphatidic acid (DMPA) and dimyristoylphosphatidyl glycerol (DMPG) small unilamellar vesicles in the gel phase was studied by steady-state fluorescence spectroscopy at pHs 7, 6, 5 and 4 and 20°C. In aqueous solution, with excitation at 335 nm, the emission fluorescence spectrum of quinine varied with pH reflecting the occurrence of different charged species of the drug. In all cases, the emission maximum centered at 383 or 443 nm shifted to lower wavelength in the presence of vesicles. This indicates that the membrane-bound state quinine is in an environment of low polarity. Drug monocationic species were deeply buried in DMPG relative to DMPA bilayers whereas no significant differences were observed for dicationic species, the fluorophore being located in this case in a more aqueous-like environment. Experimental association isotherms generated from fluorescence intensity changes were quantitatively analyzed in terms of the binding equilibrium model. Although the binding affinity of quinine to anionic membranes was always higher for DMPG over DMPA, dicationic species showed a reduced ability to bind the negatively charged membrane. In addition, the binding model has been related with the partition model leading to a good agreement between the theoretical (calculated from the binding model) and the experimental (from the initial slope of the experimental isotherms) partition coefficient derived in each case.

  4. Channel-forming activity of syringopeptin 25A in mercury-supported phospholipid monolayers and negatively charged bilayers.

    Science.gov (United States)

    Becucci, Lucia; Toppi, Arianna; Fiore, Alberto; Scaloni, Andrea; Guidelli, Rolando

    2016-10-01

    Interactions of the cationic lipodepsipeptide syringopeptin 25A (SP25A) with mercury-supported dioleoylphosphatidylcholine (DOPC), dioleoylphosphatidylserine (DOPS) and dioeleoylphosphatidic acid (DOPA) self-assembled monolayers (SAMs) were investigated by AC voltammetry in 0.1M KCl at pH3, 5.4 and 6.8. SP25A targets and penetrates the DOPS SAM much more effectively than the other SAMs not only at pH6.8, where the DOPS SAM is negatively charged, but also at pH3, where it is positively charged just as SP25A. Similar investigations at tethered bilayer lipid membranes (tBLMs) consisting of a thiolipid called DPTL anchored to mercury, with a DOPS, DOPA or DOPC distal monolayer on top of it, showed that, at physiological transmembrane potentials, SP25A forms ion channels spanning the tBLM only if DOPS is the distal monolayer. The distinguishing chemical feature of the DOPS SAM is the ionic interaction between the protonated amino group of a DOPS molecule and the carboxylate group of an adjacent phospholipid molecule. Under the reasonable assumption that SP25A preferentially interacts with this ion pair, the selective lipodepsipeptide antimicrobial activity against Gram-positive bacteria may be tentatively explained by its affinity for similar protonated amino-carboxylate pairs, which are expected to be present in the peptide moieties of peptidoglycan strands.

  5. Exposure to negatively charged-particle dominant air-conditions on human lymphocytes in vitro activates immunological responses.

    Science.gov (United States)

    Nishimura, Yasumitsu; Takahashi, Kazuaki; Mase, Akinori; Kotani, Muneo; Ami, Kazuhisa; Maeda, Megumi; Shirahama, Takashi; Lee, Suni; Matsuzaki, Hidenori; Kumagai-Takei, Naoko; Yoshitome, Kei; Otsuki, Takemi

    2015-12-01

    Indoor air-conditions may play an important role in human health. Investigation of house conditions that promote health revealed that negatively charged-particle dominant indoor air-conditions (NAC) induced immune stimulation. NAC was established using fine charcoal powder on walls and ceilings and utilizing forced negatively charged particles (approximate diameter: 20 nm) dominant in indoor air-conditions created by applying an electric voltage (72 V) between the backside of the walls and the ground. We reported previously that these conditions induced a slight and significant increase of interleukin-2 during 2.5 h stay, and an increase of natural killer (NK) cell cytotoxicity, when examining human subjects after a two-week night stay under these conditions. In the present study, we investigated whether exposure to NAC in vitro affects immune conditions. Although the concentrations of particles were different, an incubator for cell culture with NAC was set and cellular compositions and functions of various freshly isolated human lymphocytes derived from healthy donors were assayed in the NAC incubator and compared with those of cultures in a standard (STD) incubator. Results showed that NAC cultivation caused an increase of CD25 and PD-1 expressing cells in the CD4 positive fraction, enhancement of NK cell cytotoxicity, production of interferon-y (IFNγ), and slight enhancement of regulatory T cell function. In addition, the formula designated as the "immune-index" clearly differed between STD and NAC culture conditions. Thus, NAC conditions may promote human health through slight activation of the immune system against cancer cells and virus infection as shown by this in vitro study and our previously reported human studies.

  6. Integrating high electrical conductivity and photocatalytic activity in cotton fabric by cationizing for enriched coating of negatively charged graphene oxide.

    Science.gov (United States)

    Sahito, Iftikhar Ali; Sun, Kyung Chul; Arbab, Alvira Ayoub; Qadir, Muhammad Bilal; Jeong, Sung Hoon

    2015-10-01

    Electroconductive textiles have attended tremendous focus recently and researchers are making efforts to increase conductivity of e-textiles, in order to increase the use of such flexible and low cost textile materials. In this study, surface conductivity and photo catalytic activity of standard cotton fabric (SCF) was enhanced by modifying its surface charge, from negative to positive, using Bovine Serum Albumin (BSA) as a cationic agent, to convert it into cationised cotton fabric (CCF). Then, both types of fabrics were dip coated with a simple dip and dry technique for the adsorption of negatively charged graphene oxide (GO) sheets onto its surface. This resulted in 67.74% higher loading amount of GO on the CCF making self-assembly. Finally, this coating was chemically converted by vapor reduction using hydrazine hydrate to reduced graphene oxide (rGO) for restoration of a high electrical conductivity at the fabric surface. Our results revealed that with such high loading of GO, the surface resistance of CCF was only 40Ω/sq as compared to 510Ω/sq of the SCF and a 66% higher photo catalytic activity was also achieved through cationization for improved GO coating. Graphene coated SCF and CCF were characterized using FE-SEM, FTIR, Raman, UV-vis, WAXD, EDX and XPS spectroscopy to ascertain successful reduction of GO to rGO. The effect of BSA treatment on adsorption of cotton fabric was studied using drop shape analyzer to measure contact angle and for thermal and mechanical resistance, the fabric was tested for TGA and tensile strength, respectively. rGO coated fabric also showed slightly improved thermal stability yet a minor loss of strength was observed. The high flexibility, photocatalytic activity and excellent conductivity of this fabric suggests that it can be used as an electrode material for various applications.

  7. Monte Carlo simulations of the distributions of intra- and extra-vesicular ions and membrane associated charges in hybrid liposomes composed of negatively charged tetraether and zwitterionic diester phospholipids

    Directory of Open Access Journals (Sweden)

    István P. Sugár

    2017-04-01

    Full Text Available Here, we model a negatively charged lipid vesicle, composed of a mixture of bipolar tetraether and diester (or diether phospholipid molecules, by a spherical shell that has zero ion permeability. We take into consideration all the charge-charge interactions between intra-vesicular ions, extra-vesicular ions, and membrane lipid associated charges. Monte Carlo simulations result in homogeneous and double-exponential ion distribution, respectively, in the intra- and extra-vesicular space. The extra-vesicular ion concentration close to the membrane surface is proportional to the total amount of the membrane charges (Nm and is independent of the partitioning of the membrane charges between the outer (Nom and inner membrane (Nim surface. This result shows that one should not disregard the effect of the charges on the inner membrane surface when calculating the ion distributions around a charged vesicle. If the partitioning of the membrane charges is not restricted (i.e., lipid flip-flop is allowed, then at different Nm, the Nom/Nim ratio remains constant and the value of Nom/Nim, as a consequence of the interaction between every charges of the model, is close to, but significantly higher than, the ratio of the outer to the inner surface area of the membrane. These results indicate that the amount and the orientation of the negatively-charged tetraether lipids in the membrane are important determinants of membrane properties in tetraether/zwitterionic diester phospholipid liposomes. Finally we compared the results of our discrete charge model and continuous models based on the solutions of the Poisson-Boltzmann equation and pointed out qualitative similarities and sometimes major quantitative differences between these two types of models.

  8. Femtosecond study of the interplay between excitons, trions, and carriers in (Cd,Mn)Te quantum wells.

    Science.gov (United States)

    Płochocka, P; Kossacki, P; Maślana, W; Cibert, J; Tatarenko, S; Radzewicz, C; Gaj, J A

    2004-04-30

    We study the absorption by neutral excitons and positively charged excitons (trions) following a femtosecond, circularly polarized, resonant pump pulse. Three populations are involved: free holes, excitons, and trions, all exhibiting transient spin polarization. In particular, a polarization of the gas of free holes is created by the formation of trions. The evolution of these populations is described, including spin flip and trion formation. We evaluate the contributions of phase space filling and spin-dependent screening. We propose a new explanation of the oscillator strength stealing phenomena observed in doped quantum wells, based on the screening of neutral excitons by charge carriers. We have also found that binding holes into charged excitons excludes them from the interaction with the rest of the system, so that oscillator strength stealing is partially blocked.

  9. Editorial on indirect excitons: Physics and applications

    Science.gov (United States)

    2017-08-01

    This special issue contains 9 original review papers, research papers and discussion papers on indirect excitons. An exciton is a Coulomb-correlated electron-hole pair. Frenkel excitons dominate optical properties of organic semiconductors, while Wannier-Mott excitons are responsible for the hydrogen-like absorption spectra of inorganic semiconductors at low temperatures. The interest to the physics of excitons has strongly increased in the new century. This interest is motivated by unique bosonic properties of excitons that lead to the phenomena of exciton-polariton lasing and stimulated scattering, build-up of the spontaneous coherence and polarisation in cold exciton gases. In addition to the rich fundamental physics, excitons offer the perspective of applications in opto-electronic devices such as exciton transistors, switches, optical integrated circuits, etc.

  10. Control of homogeneous charge compression ignition combustion in a two-cylinder gasoline direct injection engine with negative valve overlap

    Institute of Scientific and Technical Information of China (English)

    WANG Zhi; WANG Jianxin; SHUAI Shijin; MA Qingjun; TIAN Guohong

    2007-01-01

    Homogeneous charge compression ignition(HCCI) has challenges in ignition timing control,combustion rate control,and operating range extension.In this paper,HCCI combustion was studied in a two-cylinder gasoline direct injection (GDI) engine with negative valve overlap (NVO).A two-stage gasoline direct injection strategy combined with negative valve overlap was used to control mixture formation and combustion.The gasoline engine could be operated in HCCI combustion mode at a speed range of 800-2 200 r/min and load,indicated mean effective pressure (IMEP) range of 0.1-0.53 MPa.The engine fuel consumption 4× 10-5 without soot emission.The effect of different injection strategies on HCCI combustion was studied.The experimental results indicated that the coefficient of variation of the engine cycle decreased by using NVO with two-stage direct injection;the ignition timing and combustion rate could be controlled;and the operational range of HCCI combustion could be extended.

  11. On the c-Si surface passivation mechanism by the negative-charge-dielectric Al2O3

    Science.gov (United States)

    Hoex, B.; Gielis, J. J. H.; van de Sanden, M. C. M.; Kessels, W. M. M.

    2008-12-01

    Al2O3 is a versatile high-κ dielectric that has excellent surface passivation properties on crystalline Si (c-Si), which are of vital importance for devices such as light emitting diodes and high-efficiency solar cells. We demonstrate both experimentally and by simulations that the surface passivation can be related to a satisfactory low interface defect density in combination with a strong field-effect passivation induced by a negative fixed charge density Qf of up to 1013 cm-2 present in the Al2O3 film at the interface with the underlying Si substrate. The negative polarity of Qf in Al2O3 is especially beneficial for the passivation of p-type c-Si as the bulk minority carriers are shielded from the c-Si surface. As the level of field-effect passivation is shown to scale with Qf2, the high Qf in Al2O3 tolerates a higher interface defect density on c-Si compared to alternative surface passivation schemes.

  12. Van der Waals Interactions and Exciton Condensation

    Science.gov (United States)

    Handel, P. H.; Kittel, C.

    1971-01-01

    It is shown that the van der Waals interaction can lead at low temperatures to a condensed state of excitons with properties in qualitative agreement with the observations of exciton droplets. Our calculation gives a binding energy of the correct sign and magnitude for the exciton condensate. In a diclectric medium, the strong enhancement of the exciton polarizability leads to a giant van der Waals interaction, and this interaction appears to make possible a condensed exciton phase. PMID:16591958

  13. Direct detection of photoinduced charge transfer complexes in polymer fullerene blends

    Science.gov (United States)

    Behrends, Jan; Sperlich, Andreas; Schnegg, Alexander; Biskup, Till; Teutloff, Christian; Lips, Klaus; Dyakonov, Vladimir; Bittl, Robert

    2012-03-01

    We report transient electron paramagnetic resonance (trEPR) measurements with submicrosecond time resolution performed on a polymer:fullerene blend consisting of poly(3-hexylthiophene) (P3HT) and [6,6]-phenyl C61-butyric acid methyl ester (PCBM) at low temperatures. The trEPR spectrum immediately following photoexcitation reveals signatures of spin-correlated polaron pairs. The pair partners (positive polarons in P3HT and negative polarons in PCBM) can be identified by their characteristic g values. The fact that the polaron pair states exhibit strong non-Boltzmann population unambiguously shows that the constituents of each pair are geminate, i.e., originate from one exciton. We demonstrate that coupled polaron pairs are present even several microseconds after charge transfer and suggest that they embody the intermediate charge transfer complexes that form at the donor/acceptor interface and mediate the conversion from excitons into free charge carriers.

  14. Hyperspherical theory of anisotropic exciton

    CERN Document Server

    Muljarov, E A; Tikhodeev, S G; Bulatov, A E; Birman, Joseph L; 10.1063/1.1286772

    2012-01-01

    A new approach to the theory of anisotropic exciton based on Fock transformation, i.e., on a stereographic projection of the momentum to the unit 4-dimensional (4D) sphere, is developed. Hyperspherical functions are used as a basis of the perturbation theory. The binding energies, wave functions and oscillator strengths of elongated as well as flattened excitons are obtained numerically. It is shown that with an increase of the anisotropy degree the oscillator strengths are markedly redistributed between optically active and formerly inactive states, making the latter optically active. An approximate analytical solution of the anisotropic exciton problem taking into account the angular momentum conserving terms is obtained. This solution gives the binding energies of moderately anisotropic exciton with a good accuracy and provides a useful qualitative description of the energy level evolution.

  15. Radiation effects from first principles : the role of excitons in electronic-excited processes.

    Energy Technology Data Exchange (ETDEWEB)

    Wong, Bryan Matthew

    2009-09-01

    Electron-hole pairs, or excitons, are created within materials upon optical excitation or irradiation with X-rays/charged particles. The ability to control and predict the role of excitons in these energetically-induced processes would have a tremendous impact on understanding the effects of radiation on materials. In this report, the excitonic effects in large cycloparaphenylene carbon structures are investigated using various first-principles methods. These structures are particularly interesting since they allow a study of size-scaling properties of excitons in a prototypical semi-conducting material. In order to understand these properties, electron-hole transition density matrices and exciton binding energies were analyzed as a function of size. The transition density matrices allow a global view of electronic coherence during an electronic excitation, and the exciton binding energies give a quantitative measure of electron-hole interaction energies in these structures. Based on overall trends in exciton binding energies and their spatial delocalization, we find that excitonic effects play a vital role in understanding the unique photoinduced dynamics in these systems.

  16. Targeted delivery of chemically modified anti-miR-221 to hepatocellular carcinoma with negatively charged liposomes

    Directory of Open Access Journals (Sweden)

    Zhang W

    2015-07-01

    Full Text Available Wendian Zhang,1 Fangqi Peng,1 Taotao Zhou,1 Yifei Huang,2 Li Zhang,3 Peng Ye,4 Miao Lu,1 Guang Yang,5 Yongkang Gai,1 Tan Yang,1 Xiang Ma,1 Guangya Xiang1 1School of Pharmacy, Tongji Medical College, 2Department of Pharmacy, 3Department of Ultrasound, Union Hospital, Tongji Medical College, Huazhong University of Science and Technology, 4Department of Pharmacy, Wuhan University, Renmin Hospital, 5School of Medicine, Jianghan University, Wuhan, People’s Republic of China Abstract: Hepatocellular carcinoma (HCC is one of the leading causes of cancer-related death. Gene therapy was established as a new strategy for treating HCC. To explore the potential delivery system to support the gene therapy of HCC, negatively charged liposomal delivery system was used to deliver miR-221 antisense oligonucleotide (anti-miR-221 to the transferrin (Tf receptor over expressed HepG2 cells. The liposome exhibited a mean particle size of 122.5 nm, zeta potential of -15.74 mV, anti-miR-221 encapsulation efficiency of 70%, and excellent colloidal stability at 4°C. Anti-miR-221-encapsulated Tf-targeted liposome demonstrated a 15-fold higher delivery efficiency compared to nontargeted liposome in HepG2 cells in vitro. Anti-miR-221 Tf-targeted liposome effectively delivered anti-miR-221 to HepG2 cells, upregulated miR-221 target genes PTEN, P27kip1, and TIMP3, and exhibited greater silencing efficiency over nontargeted anti-miR-221 liposome. After intravenous injection into HepG2 tumor-bearing xenografted mice with Cy3-labeled anti-miR-221 Tf-targeted liposome, Cy3-anti-miR-221 was successfully delivered to the tumor site and increased the expressions of PTEN, P27kip1, and TIMP3. Our results demonstrate that the Tf-targeted negatively charged liposome could be a potential therapeutic modality in the gene therapy of human HCC. Keywords: transferrin, gene, HCC, target delivery system, anionic liposome 

  17. Non-Markovian Quantum Jumps in Excitonic Energy Transfer

    CERN Document Server

    Rebentrost, Patrick; Aspuru-Guzik, Alan

    2009-01-01

    We utilize the novel non-Markovian quantum jump (NMQJ) approach to stochastically simulate exciton dynamics derived from a time-convolutionless master equation. For relevant parameters and time scales, the time-dependent, oscillatory decoherence rates can have negative regions, a signature of non-Markovian behavior and of the revival of coherences. This can lead to non-Markovian population beatings for a dimer system at room temperature. We show that strong exciton-phonon coupling to low frequency modes can considerably modify transport properties. We observe increased exciton transport, which can be seen as an extension of recent environment-assisted quantum transport (ENAQT) concepts to the non-Markovian regime. Within the NMQJ method, the Fenna-Matthew-Olson protein is investigated as a prototype for larger photosynthetic complexes.

  18. Scaling laws of Rydberg excitons

    Science.gov (United States)

    Heckötter, J.; Freitag, M.; Fröhlich, D.; Aßmann, M.; Bayer, M.; Semina, M. A.; Glazov, M. M.

    2017-09-01

    Rydberg atoms have attracted considerable interest due to their huge interaction among each other and with external fields. They demonstrate characteristic scaling laws in dependence on the principal quantum number n for features such as the magnetic field for level crossing or the electric field of dissociation. Recently, the observation of excitons in highly excited states has allowed studying Rydberg physics in cuprous oxide crystals. Fundamentally different insights may be expected for Rydberg excitons, as the crystal environment and associated symmetry reduction compared to vacuum give not only optical access to many more states within an exciton multiplet but also extend the Hamiltonian for describing the exciton beyond the hydrogen model. Here we study experimentally and theoretically the scaling of several parameters of Rydberg excitons with n , for some of which we indeed find laws different from those of atoms. For others we find identical scaling laws with n , even though their origin may be distinctly different from the atomic case. At zero field the energy splitting of a particular multiplet n scales as n-3 due to crystal-specific terms in the Hamiltonian, e.g., from the valence band structure. From absorption spectra in magnetic field we find for the first crossing of levels with adjacent principal quantum numbers a Br∝n-4 dependence of the resonance field strength, Br, due to the dominant paramagnetic term unlike for atoms for which the diamagnetic contribution is decisive, resulting in a Br∝n-6 dependence. By contrast, the resonance electric field strength shows a scaling as Er∝n-5 as for Rydberg atoms. Also similar to atoms with the exception of hydrogen we observe anticrossings between states belonging to multiplets with different principal quantum numbers at these resonances. The energy splittings at the avoided crossings scale roughly as n-4, again due to crystal specific features in the exciton Hamiltonian. The data also allow us to

  19. The association of defensin HNP-2 with negatively charged membranes: A combined fluorescence and linear dichroism study.

    Science.gov (United States)

    Pridmore, Catherine J; Rodger, Alison; Sanderson, John M

    2016-04-01

    The association of defensin HNP-2 with negatively charged membranes has been studied using a new approach that combines fluorescence and linear dichroism (LD) spectroscopies with simulated LD spectra in order to characterise the binding kinetics and bound configurations of the peptide. Binding to membranes composed of mixtures of diacylglycerophosphocholines (PC) with either diacylglycerophosphoglycerol (PG) or diacylglycerophosphoserine (PS) was conducted at lipid:peptide ratios that yielded binding, but not membrane fusion. HNP-2 association with membranes under these conditions was a 2 stage-process, with both stages exhibiting first order kinetics. The fast initial step, with a half-life of 3 min. Conversion between the states was estimated to have an enthalpy of activation of approximately 10 kJ mol(-1) and an entropy of activation of -0.2 kJ K mol(-1). LD spectra corresponding to each of the membrane bound states were generated by non-linear regression using a standard kinetic model. These spectra are interpreted in comparison with spectra calculated using the program Dichrocalc and reveal that the peptide associates with membranes in a small number of stable configurations. All of these configurations have a significant proportion of β-sheet structure residing in the plane of the membrane. Two configurations support structures previously proposed for defensins in membranes. Copyright © 2016 The Authors. Published by Elsevier B.V. All rights reserved.

  20. Manufacturing and characterization of bent silicon crystals for studies of coherent interactions with negatively charged particles beams

    Energy Technology Data Exchange (ETDEWEB)

    Germogli, G.; Mazzolari, A.; Bandiera, L.; Bagli, E.; Guidi, V.

    2015-07-15

    Efficient steering of GeV-energy negatively charged particle beams was demonstrated to be possible with a new generation of thin bent silicon crystals. Suitable crystals were produced at the Sensor Semiconductor Laboratory of Ferrara starting from Silicon On Insulator wafers, adopting proper revisitation of silicon micromachining techniques such as Low Pressure Chemical Vapor Deposition, photolithography and anisotropic chemical etching. Mechanical holders, which allow to properly bend the crystal and to reduce unwanted torsions, were employed. Crystallographic directions and crystal holder design were optimized in order to excite quasi-mosaic effect along (1 1 1) planes. Prior to exposing the crystal to particle beams, a full set of characterizations were performed. Infrared interferometry was used to measure crystal thickness with high accuracy. White-light interferometry was employed to characterize surface deformational state and its torsion. High-resolution X-rays diffraction was used to precisely measure crystal bending angle along the beam. Manufactured crystals were installed and tested at the MAMI MAinz MIcrotron to steer sub-GeV electrons, and at SLAC to deflect an electron beam in the 1 to 10 GeV energy range.

  1. Energy Migration in Organic Thin Films--From Excitons to Polarons

    Science.gov (United States)

    Mullenbach, Tyler K.

    The rise of organic photovoltaic devices (OPVs) and organic light-emitting devices has generated interest in the physics governing exciton and polaron dynamics in thin films. Energy transfer has been well studied in dilute solutions, but there are emergent properties in thin films and greater complications due to complex morphologies which must be better understood. Despite the intense interest in energy transport in thin films, experimental limitations have slowed discoveries. Here, a new perspective of OPV operation is presented where photovoltage, instead of photocurrent, plays the fundamental role. By exploiting this new vantage point the first method of measuring the diffusion length (LD) of dark (non-luminescent) excitons is developed, a novel photodetector is invented, and the ability to watch exciton arrival, in real-time, at the donor-acceptor heterojunction is presented. Using an enhanced understanding of exciton migration in thin films, paradigms for enhancing LD by molecular modifications are discovered, and the first exciton gate is experimentally and theoretically demonstrated. Generation of polarons from exciton dissociation represents a second phase of energy migration in OPVs that remains understudied. Current approaches are capable of measuring the rate of charge carrier recombination only at open-circuit. To enable a better understanding of polaron dynamics in thin films, two new approaches are presented which are capable of measuring both the charge carrier recombination and transit rates at any OPV operating voltage. These techniques pave the way for a more complete understanding of charge carrier kinetics in molecular thin films.

  2. Ultrafast formation of interlayer hot excitons in atomically thin MoS2/WS2 heterostructures

    Science.gov (United States)

    Chen, Hailong; Wen, Xiewen; Zhang, Jing; Wu, Tianmin; Gong, Yongji; Zhang, Xiang; Yuan, Jiangtan; Yi, Chongyue; Lou, Jun; Ajayan, Pulickel M.; Zhuang, Wei; Zhang, Guangyu; Zheng, Junrong

    2016-08-01

    Van der Waals heterostructures composed of two-dimensional transition-metal dichalcogenides layers have recently emerged as a new family of materials, with great potential for atomically thin opto-electronic and photovoltaic applications. It is puzzling, however, that the photocurrent is yielded so efficiently in these structures, despite the apparent momentum mismatch between the intralayer/interlayer excitons during the charge transfer, as well as the tightly bound nature of the excitons in 2D geometry. Using the energy-state-resolved ultrafast visible/infrared microspectroscopy, we herein obtain unambiguous experimental evidence of the charge transfer intermediate state with excess energy, during the transition from an intralayer exciton to an interlayer exciton at the interface of a WS2/MoS2 heterostructure, and free carriers moving across the interface much faster than recombining into the intralayer excitons. The observations therefore explain how the remarkable charge transfer rate and photocurrent generation are achieved even with the aforementioned momentum mismatch and excitonic localization in 2D heterostructures and devices.

  3. Exploration of Porphyrin-based Semiconductors for Negative Charge Transport Applications Using Synthetic, Spectroscopic, Potentiometric, Magnetic Resonance, and Computational Methods

    Science.gov (United States)

    Rawson, Jeffrey Scott

    Organic pi-conjugated materials are emerging as commercially relevant components in electronic applications that include transistors, light-emitting diodes, and solar cells. One requirement common to all of these functions is an aptitude for accepting and transmitting charges. It is generally agreed that the development of organic semiconductors that favor electrons as the majority carriers (n-type) lags behind the advances in hole transporting (p-type) materials. This shortcoming suggests that the design space for n-type materials is not yet well explored, presenting researchers with the opportunity to develop unconventional architectures. In this regard, it is worth noting that discrete molecular materials are demonstrating the potential to usurp the preeminent positions that pi-conjugated polymers have held in these areas of organic electronics research. This dissertation describes how an extraordinary class of molecules, meso-to-meso ethyne-bridged porphyrin arrays, has been bent to these new uses. Chapter one describes vis-NIR spectroscopic and magnetic resonance measurements revealing that these porphyrin arrays possess a remarkable aptitude for the delocalization of negative charge. In fact, the miniscule electron-lattice interactions exhibited in these rigid molecules allow them to host the most vast electron-polarons ever observed in a pi-conjugated material. Chapter two describes the development of an ethyne-bridged porphyrin-isoindigo hybrid chromophore that can take the place of fullerene derivatives in the conventional thin film solar cell architecture. Particularly noteworthy is the key role played by the 5,15-bis(heptafluoropropyl)porphyrin building block in the engineering of a chromophore that, gram for gram, is twice as absorptive as poly(3-hexyl)thiophene, exhibits a lower energy absorption onset than this polymer, and yet possesses a photoexcited singlet state sufficiently energetic to transfer a hole to this polymer. Chapter three describes

  4. C-reactive protein and annexin A5 bind to distinct sites of negatively charged phospholipids present in oxidized low-density lipoprotein.

    NARCIS (Netherlands)

    Tits, L.J.H. van; Graaf, J. de; Toenhake, H.; Heerde, W.L. van; Stalenhoef, A.F.H.

    2005-01-01

    OBJECTIVE: To investigate binding of C-reactive protein (CRP) and annexin A5, 2 proteins with high affinity for negatively charged phospholipids, to oxidized low-density lipoprotein (LDL) and the consequences of these interactions for subsequent binding of oxidized LDL to monocyte/macrophage-like

  5. Excitonic fine structure and binding energies of excitonic complexes in single InAs quantum dashes

    Science.gov (United States)

    Mrowiński, P.; Zieliński, M.; Świderski, M.; Misiewicz, J.; Somers, A.; Reithmaier, J. P.; Höfling, S.; Sek, G.

    2016-09-01

    The fundamental electronic and optical properties of elongated InAs nanostructures embedded in quaternary InGaAlAs barrier are investigated by means of high-resolution optical spectroscopy and many-body atomistic tight-binding theory. These wire-like shaped, self-assembled nanostructures are known as quantum dashes and are typically formed during the molecular beam epitaxial growth on InP substrates. In this paper, we study properties of excitonic complexes confined in quantum dashes emitting in a broad spectral range from below 1.2 to 1.55 μm. We find peculiar trends for the biexciton and negative trion binding energies, with pronounced trion binding in smaller size quantum dashes. These experimental findings are then compared and qualitatively explained by atomistic theory. The theoretical analysis shows a fundamental role of correlation effects for the absolute values of excitonic binding energies. Eventually, we determine the bright exciton fine structure splitting (FSS), where both the experiment and theory predict a broad distribution of the splitting varying from below 50 to almost 180 μeV. We identify several key factors determining the FSS values in such nanostructures, including quantum dash size variation and composition fluctuations.

  6. Anharmonicity of lattice vibrations induced by charged nickel additions in A sup 2 B sup 6 semiconductors

    CERN Document Server

    Sokolov, V I; Shirokov, E A; Kislov, A N

    2002-01-01

    Paper presents the results of investigations into lattice vibrations induced by nickel impurities charged negatively as to the lattice in ZnSe:Ni, ZnO:Ni, ZnS:Ni, CdS:Ni semiconductors. To investigate into vibrations one applies a sensitive technique of field exciton-oscillation spectroscopy. One observes experimentally oscillating reiterations of the impurity exciton head line including the intensive peaks of combined repetitions up to the 8-th order. The experimental results are discussed on the basis of the model estimations of oscillations of a lattice with a charged impurity centre, as well as, on the ground of calculations for oscillations of monoatomic chain with high anharmonicity. Charged impurity centres are shown to induce new oscillations of lattice - impurity anharmonic modes

  7. Linear free energy relationships for metal-ligand complexation: Bidentate binding to negatively-charged oxygen donor atoms

    Science.gov (United States)

    Carbonaro, Richard F.; Atalay, Yasemin B.; Di Toro, Dominic M.

    2011-05-01

    Stability constants for metal complexation to bidentate ligands containing negatively-charged oxygen donor atoms can be estimated from the following linear free energy relationship (LFER): log KML = χOO( αO log KHL,1 + αO log KHL,2) where KML is the metal-ligand stability constant for a 1:1 complex, KHL,1 and KHL,2 are the proton-ligand stability constants (the ligand p Ka values), and αO is the Irving-Rossotti slope. The parameter χOO is metal specific and has slightly different values for five and six membered chelate rings. LFERs are presented for 21 different metal ions and are accurate to within approximately 0.30 log units in predictions of log KML values. Ligands selected for use in LFER development include dicarboxylic acids, carboxyphenols, and ortho-diphenols. For ortho-hydroxybenzaldehydes, α-hydroxycarboxylic acids, and α-ketocarboxylic acids, a modification of the LFER where log KHL,2 is set equal to zero is required. The chemical interpretation of χOO is that it accounts for the extra stability afforded to metal complexes by the chelate effect. Cu-NOM binding constants calculated from the bidentate LFERs are similar in magnitude to those used in WHAM 6. This LFER can be used to make log KML predictions for small organic molecules. Since natural organic matter (NOM) contains many of the same functional groups (i.e. carboxylic acids, phenols, alcohols), the LFER log KML predictions shed light on the range of appropriate values for use in modeling metal partitioning in natural systems.

  8. Exciton luminescence in BaFCl crystal

    Energy Technology Data Exchange (ETDEWEB)

    Radzhabov, E

    1998-05-01

    The luminescence spectra and decay characteristics of both 5.45 and 3.4 eV bands in BaFCl oxygen-free crystals were investigated at 5-300 K temperature range using vacuum ultraviolet excitation as well as X-ray excitation. The similarities with excitons in alkali halides allow us to consider both excitons in BaFCl as on-center excitons and strong off-center excitons.

  9. Plasmon-Exciton-Polariton Lasing

    CERN Document Server

    Ramezani, Mohammad; Fernández-Domínguez, Antonio I; Feist, Johannes; Rodriguez, Said Rahimzadeh-Kalaleh; Garcia-Vidal, Francisco J; Gómez-Rivas, Jaime

    2016-01-01

    Strong coupling of Frenkel excitons with surface plasmons leads to the formation of bosonic quasi-particles known as plasmon-exciton-polaritons (PEPs).Localized surface plasmons in nanoparticles are lossy due to radiative and nonradiative decays, which has hampered the realization of polariton lasing in a plasmonic system, i.e., PEP lasing. These losses can be reduced in collective plasmonic resonances supported by arrays of nanoparticles. Here we demonstrate PEP lasing in arrays of silver nanoparticles by showing the emergence of a threshold in the photoluminescence accompanied by both a superlinear increase of the emission and spectral narrowing. We also observe a reduction of the threshold by increasing the coupling between the molecular excitons and the resonances supported by the array despite the reduction of the quantum efficiency of the emitters. The coexistence of bright and dark collective modes in this plasmonic system allows for a 90?-change of polarization in the emission beyond the threshold.

  10. Excitonic polaritons in Fibonacci quasicrystals.

    Science.gov (United States)

    Hendrickson, J; Richards, B C; Sweet, J; Khitrova, G; Poddubny, A N; Ivchenko, E L; Wegener, M; Gibbs, H M

    2008-09-29

    The fabrication and characterization of light-emitting one-dimensional photonic quasicrystals based on excitonic resonances is reported. The structures consist of high-quality GaAs/AlGaAs quantum wells grown by molecular-beam epitaxy with wavelength-scale spacings satisfying a Fibonacci sequence. The polaritonic (resonant light-matter coupling) effects and light emission originate from the quantum well excitonic resonances. Measured reflectivity spectra as a function of detuning between emission and Bragg wavelength are in good agreement with excitonic polariton theory. Photoluminescence experiments show that active photonic quasicrystals, unlike photonic crystals, can be good light emitters: While their long-range order results in a stopband similar to that of photonic crystals, the lack of periodicity results in strong emission.

  11. Differential effects of DEAE negative mode chromatography and gel-filtration chromatography on the charge status of Helicobacter pylori neutrophil-activating protein.

    Science.gov (United States)

    Hong, Zhi-Wei; Yang, Yu-Chi; Pan, Timothy; Tzeng, Huey-Fen; Fu, Hua-Wen

    2017-01-01

    Helicobacter pylori neutrophil-activating protein (HP-NAP) is involved in H. pylori-associated gastric inflammation. HP-NAP is also a vaccine candidate, a possible drug target, and a potential diagnostic marker for H. pylori-associated diseases. Previously, we purified recombinant HP-NAP by one-step diethylaminoethyl (DEAE) negative mode chromatography by collecting the unbound fraction at pH 8.0 at 4°C. It remains unclear why HP-NAP does not bind to DEAE resins at the pH above its isoelectric point during the purification. To investigate how pH affects the surface net charge of HP-NAP and its binding to DEAE resins during the purification, recombinant HP-NAP expressed in Escherichia coli was subjected to DEAE negative mode chromatography at pH ranging from 7.0 to 9.0 at 25°C and the surface charge of purified HP-NAP was determined by capillary electrophoresis. A minimal amount of HP-NAP was detected in the elution fraction of DEAE Sepharose resin at pH 8.5, whereas recombinant HP-NAP was detected in the elution fraction of DEAE Sephadex resin only at pH 7.0 and 8.0. The purified recombinant HP-NAP obtained from the unbound fractions was not able to bind to DEAE resins at pH 7.0 to 9.0. In addition, the surface charge of the purified HP-NAP was neutral at pH 7.0 to 8.0 and was either neutral or slightly negative at pH 8.5 and 9.0. However, recombinant HP-NAP purified from gel-filtration chromatography was able to bind to DEAE Sepharose resin at pH 7.0 to 9.0 and DEAE Sephadex resin at pH 7.0. At pH 8.5 and 9.0, only the negatively charged species of HP-NAP were found. Thus, recombinant HP-NAP with different charge status can be differentially purified by DEAE negative mode chromatography and gel-filtration chromatography. Furthermore, the charge distribution on the surface of HP-NAP, the presence of impure proteins, and the overall net charge of the resins all affect the binding of HP-NAP to DEAE resins during the negative purification.

  12. Interwell excitons in GaAs superlattices

    DEFF Research Database (Denmark)

    Birkedal, Dan; Sayed, Karim El; Sanders, G.;

    1997-01-01

    The formation of spatially indirect excitons in superlattices with narrow minibands is investigated experimentally. The interwell exciton is similar to the first Wannier-Stark localized exciton of an electrically biased superlattice. However, in the present case the localization is mediated by th...

  13. Femtosecond Hydrogen Bond Dynamics of Bulk-like and Bound Water at Positively and Negatively Charged Lipid Interfaces Revealed by 2D HD-VSFG Spectroscopy.

    Science.gov (United States)

    Singh, Prashant Chandra; Inoue, Ken-Ichi; Nihonyanagi, Satoshi; Yamaguchi, Shoichi; Tahara, Tahei

    2016-08-26

    Interfacial water in the vicinity of lipids plays an important role in many biological processes, such as drug delivery, ion transportation, and lipid fusion. Hence, molecular-level elucidation of the properties of water at lipid interfaces is of the utmost importance. We report the two-dimensional heterodyne-detected vibrational sum frequency generation (2D HD-VSFG) study of the OH stretch of HOD at charged lipid interfaces, which shows that the hydrogen bond dynamics of interfacial water differ drastically, depending on the lipids. The data indicate that the spectral diffusion of the OH stretch at a positively charged lipid interface is dominated by the ultrafast (dynamics, while the dynamics at a negatively charged lipid interface exhibit sub-picosecond dynamics almost exclusively, implying that fast hydrogen bond fluctuation is prohibited. These results reveal that the ultrafast hydrogen bond dynamics at the positively charged lipid-water interface are attributable to the bulk-like property of interfacial water, whereas the slow dynamics at the negatively charged lipid interface are due to bound water, which is hydrogen-bonded to the hydrophilic head group.

  14. Probing Exciton Diffusion and Dissociation in Single-Walled Carbon Nanotube-C60 Heterojunctions

    Energy Technology Data Exchange (ETDEWEB)

    Dowgiallo, Anne-Marie; Mistry, Kevin S.; Johnson, Justin C.; Reid, Obadiah G.; Blackburn, Jeffrey L.

    2016-05-19

    The efficiency of thin-film organic photovoltaic (OPV) devices relies heavily upon the transport of excitons to type-II heterojunction interfaces, where there is sufficient driving force for exciton dissociation and ultimately the formation of charge carriers. Semiconducting single-walled carbon nanotubes (SWCNTs) are strong near-infrared absorbers that form type-II heterojunctions with fullerenes such as C60. Although the efficiencies of SWCNT-fullerene OPV devices have climbed over the past few years, questions remain regarding the fundamental factors that currently limit their performance. In this study, we determine the exciton diffusion length in the C60 layer of SWCNT-C60 bilayer active layers using femtosecond transient absorption measurements. We demonstrate that hole transfer from photoexcited C60 molecules to SWCNTs can be tracked by the growth of narrow spectroscopic signatures of holes in the SWCNT 'reporter layer'. In bilayers with thick C60 layers, the SWCNT charge-related signatures display a slow rise over hundreds of picoseconds, reflecting exciton diffusion through the C60 layer to the interface. A model based on exciton diffusion with a Beer-Lambert excitation profile, as well as Monte Carlo simulations, gives the best fit to the data as a function of C60 layer thickness using an exciton diffusion length of approximately 5 nm.

  15. Multiple-exciton generation in lead selenide nanorod solar cells with external quantum efficiencies exceeding 120%

    Science.gov (United States)

    Davis, Nathaniel J. L. K.; Böhm, Marcus L.; Tabachnyk, Maxim; Wisnivesky-Rocca-Rivarola, Florencia; Jellicoe, Tom C.; Ducati, Caterina; Ehrler, Bruno; Greenham, Neil C.

    2015-01-01

    Multiple-exciton generation—a process in which multiple charge-carrier pairs are generated from a single optical excitation—is a promising way to improve the photocurrent in photovoltaic devices and offers the potential to break the Shockley–Queisser limit. One-dimensional nanostructures, for example nanorods, have been shown spectroscopically to display increased multiple exciton generation efficiencies compared with their zero-dimensional analogues. Here we present solar cells fabricated from PbSe nanorods of three different bandgaps. All three devices showed external quantum efficiencies exceeding 100% and we report a maximum external quantum efficiency of 122% for cells consisting of the smallest bandgap nanorods. We estimate internal quantum efficiencies to exceed 150% at relatively low energies compared with other multiple exciton generation systems, and this demonstrates the potential for substantial improvements in device performance due to multiple exciton generation. PMID:26411283

  16. Predicting excitonic gaps of semiconducting single-walled carbon nanotubes from a field theoretic analysis

    Science.gov (United States)

    Konik, Robert M.; Sfeir, Matthew Y.; Misewich, James A.

    2015-02-01

    We demonstrate that a nonperturbative framework for the treatment of the excitations of single-walled carbon nanotubes based upon a field theoretic reduction is able to accurately describe experiment observations of the absolute values of excitonic energies. This theoretical framework yields a simple scaling function from which the excitonic energies can be read off. This scaling function is primarily determined by a single parameter, the charge Luttinger parameter of the tube, which is in turn a function of the tube chirality, dielectric environment, and the tube's dimensions, thus expressing disparate influences on the excitonic energies in a unified fashion. We test this theory explicitly on the data reported by Dukovic et al. [Nano Lett. 5, 2314 (2005), 10.1021/nl0518122] and Sfeir et al. [Phys. Rev. B 82, 195424 (2010), 10.1103/PhysRevB.82.195424] and so demonstrate the method works over a wide range of reported excitonic spectra.

  17. Near-infrared exciton-polaritons in strongly coupled single-walled carbon nanotube microcavities

    Science.gov (United States)

    Graf, Arko; Tropf, Laura; Zakharko, Yuriy; Zaumseil, Jana; Gather, Malte C.

    2016-10-01

    Exciton-polaritons form upon strong coupling between electronic excitations of a material and photonic states of a surrounding microcavity. In organic semiconductors the special nature of excited states leads to particularly strong coupling and facilitates condensation of exciton-polaritons at room temperature, which may lead to electrically pumped organic polariton lasers. However, charge carrier mobility and photo-stability in currently used materials is limited and exciton-polariton emission so far has been restricted to visible wavelengths. Here, we demonstrate strong light-matter coupling in the near infrared using single-walled carbon nanotubes (SWCNTs) in a polymer matrix and a planar metal-clad cavity. By exploiting the exceptional oscillator strength and sharp excitonic transition of (6,5) SWCNTs, we achieve large Rabi splitting (>110 meV), efficient polariton relaxation and narrow band emission (devices operating at telecommunication wavelengths.

  18. Triplet excitons as sensitive spin probes for structure analysis of extended defects in microcrystalline silicon

    Science.gov (United States)

    Meier, Christoph; Teutloff, Christian; Behrends, Jan; Bittl, Robert; Astakhov, Oleksandr; Lips, Klaus

    2016-07-01

    Electrically detected magnetic resonance (EDMR) spectroscopy is employed to study the influence of triplet excitons on the photocurrent in state-of-the-art microcrystalline silicon thin-film solar cells. These triplet excitons are used as sensitive spin probes for the investigation of their electronic and nuclear environment in this mixed-phase material. According to low-temperature EDMR results obtained from solar cells with different excitons reside at extended defects in the crystallites of microcrystalline silicon that give rise to shallow states in the silicon band gap. The excitons possess a rather delocalized wave function, couple to electron spins in conduction band tail states nearby, and take part in a spin-dependent recombination process. Our study shows that extended defects such as grain boundaries or stacking faults in the crystalline part of the material act as charge carrier traps that can influence the material conductivity.

  19. Multiple-exciton generation in lead selenide nanorod solar cells with external quantum efficiencies exceeding 120.

    Science.gov (United States)

    Davis, Nathaniel J L K; Böhm, Marcus L; Tabachnyk, Maxim; Wisnivesky-Rocca-Rivarola, Florencia; Jellicoe, Tom C; Ducati, Caterina; Ehrler, Bruno; Greenham, Neil C

    2015-09-28

    Multiple-exciton generation-a process in which multiple charge-carrier pairs are generated from a single optical excitation-is a promising way to improve the photocurrent in photovoltaic devices and offers the potential to break the Shockley-Queisser limit. One-dimensional nanostructures, for example nanorods, have been shown spectroscopically to display increased multiple exciton generation efficiencies compared with their zero-dimensional analogues. Here we present solar cells fabricated from PbSe nanorods of three different bandgaps. All three devices showed external quantum efficiencies exceeding 100% and we report a maximum external quantum efficiency of 122% for cells consisting of the smallest bandgap nanorods. We estimate internal quantum efficiencies to exceed 150% at relatively low energies compared with other multiple exciton generation systems, and this demonstrates the potential for substantial improvements in device performance due to multiple exciton generation.

  20. Magnetic exciton dispersion in praseodymium

    DEFF Research Database (Denmark)

    Rainford, B. D.; Houmann, Jens Christian Gylden

    1971-01-01

    Measurements of the dispersion of magnetic excitons have been made in a single crystal of praseodymium metal using inelastic neutron scattering. A preliminary analysis of the data yields the first detailed information about the exchange interactions and the crystal field splittings in the light...

  1. Exciton dynamics in molecular aggregates

    NARCIS (Netherlands)

    Augulis, R.; Pugžlys, A.; Loosdrecht, P.H.M. van; Pugzlys, A

    2006-01-01

    The fundamental aspects of exciton dynamics in double-wall cylindrical aggregates of cyanine dyes are studied by means of frequency resolved femtosecond pump-probe spectroscopy. The collective excitations of the aggregates, resulting from intermolecular dipole-dipole interactions have the characteri

  2. Exciton dynamics in molecular aggregates

    NARCIS (Netherlands)

    Augulis, R.; Pugžlys, A.; Loosdrecht, P.H.M. van; Pugzlys, A

    2006-01-01

    The fundamental aspects of exciton dynamics in double-wall cylindrical aggregates of cyanine dyes are studied by means of frequency resolved femtosecond pump-probe spectroscopy. The collective excitations of the aggregates, resulting from intermolecular dipole-dipole interactions have the

  3. Exciton size and quantum transport in nanoplatelets

    Energy Technology Data Exchange (ETDEWEB)

    Pelzer, Kenley M., E-mail: kpelzer@anl.gov; Gray, Stephen K. [Center for Nanoscale Materials, Argonne National Laboratory, 9700 Cass Ave., Argonne, Illinois 60439 (United States); Darling, Seth B. [Center for Nanoscale Materials, Argonne National Laboratory, 9700 Cass Ave., Argonne, Illinois 60439 (United States); Institute for Molecular Engineering, University of Chicago, 5747 S. Ellis Ave., Chicago, Illinois 60637 (United States); Schaller, Richard D. [Center for Nanoscale Materials, Argonne National Laboratory, 9700 Cass Ave., Argonne, Illinois 60439 (United States); Department of Chemistry, Northwestern University, 2145 Sheridan Rd., Evanston, Illinois 60208 (United States)

    2015-12-14

    Two-dimensional nanoplatelets (NPLs) are an exciting class of materials with promising optical and energy transport properties. The possibility of efficient energy transport between nanoplatelets raises questions regarding the nature of energy transfer in these thin, laterally extended systems. A challenge in understanding exciton transport is the uncertainty regarding the size of the exciton. Depending on the material and defects in the nanoplatelet, an exciton could plausibly extend over an entire plate or localize to a small region. The variation in possible exciton sizes raises the question how exciton size impacts the efficiency of transport between nanoplatelet structures. Here, we explore this issue using a quantum master equation approach. This method goes beyond the assumptions of Förster theory to allow for quantum mechanical effects that could increase energy transfer efficiency. The model is extremely flexible in describing different systems, allowing us to test the effect of varying the spatial extent of the exciton. We first discuss qualitative aspects of the relationship between exciton size and transport and then conduct simulations of exciton transport between NPLs for a range of exciton sizes and environmental conditions. Our results reveal that exciton size has a strong effect on energy transfer efficiency and suggest that manipulation of exciton size may be useful in designing NPLs for energy transport.

  4. Exciton size and quantum transport in nanoplatelets.

    Science.gov (United States)

    Pelzer, Kenley M; Darling, Seth B; Gray, Stephen K; Schaller, Richard D

    2015-12-14

    Two-dimensional nanoplatelets (NPLs) are an exciting class of materials with promising optical and energy transport properties. The possibility of efficient energy transport between nanoplatelets raises questions regarding the nature of energy transfer in these thin, laterally extended systems. A challenge in understanding exciton transport is the uncertainty regarding the size of the exciton. Depending on the material and defects in the nanoplatelet, an exciton could plausibly extend over an entire plate or localize to a small region. The variation in possible exciton sizes raises the question how exciton size impacts the efficiency of transport between nanoplatelet structures. Here, we explore this issue using a quantum master equation approach. This method goes beyond the assumptions of Förster theory to allow for quantum mechanical effects that could increase energy transfer efficiency. The model is extremely flexible in describing different systems, allowing us to test the effect of varying the spatial extent of the exciton. We first discuss qualitative aspects of the relationship between exciton size and transport and then conduct simulations of exciton transport between NPLs for a range of exciton sizes and environmental conditions. Our results reveal that exciton size has a strong effect on energy transfer efficiency and suggest that manipulation of exciton size may be useful in designing NPLs for energy transport.

  5. Light propagation in tunable exciton-polariton one-dimensional photonic crystals

    CERN Document Server

    Sedov, E S; Arakelian, S M; Kavokin, A V

    2016-01-01

    Simulations of propagation of light beams in specially designed multilayer semiconductor structures (one-dimensional photonic crystals) with embedded quantum wells reveal characteristic optical properties of resonant hyperbolic metamaterials. A strong dependence of the refraction angle and the optical beam spread on the exciton radiative lifetime is revealed. We demonstrate the strong negative refraction of light and the control of the group velocity of light by an external bias through its effect upon the exciton radiative properties.

  6. Exposure to positively- and negatively-charged plasma cluster ions impairs IgE-binding capacity of indoor cat and fungal allergens

    OpenAIRE

    NISHIKAWA, Kazuo; Fujimura, Takashi; Ota, Yasuhiro; Abe, Takuya; ElRamlawy, Kareem Gamal; Nakano, Miyako; Takado, Tomoaki; Uenishi, Akira; Kawazoe, Hidechika; Sekoguchi, Yoshinori; Tanaka, Akihiko; Ono, Kazuhisa; Kawamoto, Seiji

    2016-01-01

    Background Environmental control to reduce the amount of allergens in a living place is thought to be important to avoid sensitization to airborne allergens. However, efficacy of environmental control on inactivation of airborne allergens is not fully investigated. We have previously reported that positively- and negatively-charged plasma cluster ions (PC-ions) reduce the IgE-binding capacity of crude allergens from Japanese cedar pollen as important seasonal airborne allergens. Cat (Felis do...

  7. Exciton localization in solution-processed organolead trihalide perovskites

    Science.gov (United States)

    He, Haiping; Yu, Qianqian; Li, Hui; Li, Jing; Si, Junjie; Jin, Yizheng; Wang, Nana; Wang, Jianpu; He, Jingwen; Wang, Xinke; Zhang, Yan; Ye, Zhizhen

    2016-03-01

    Organolead trihalide perovskites have attracted great attention due to the stunning advances in both photovoltaic and light-emitting devices. However, the photophysical properties, especially the recombination dynamics of photogenerated carriers, of this class of materials are controversial. Here we report that under an excitation level close to the working regime of solar cells, the recombination of photogenerated carriers in solution-processed methylammonium-lead-halide films is dominated by excitons weakly localized in band tail states. This scenario is evidenced by experiments of spectral-dependent luminescence decay, excitation density-dependent luminescence and frequency-dependent terahertz photoconductivity. The exciton localization effect is found to be general for several solution-processed hybrid perovskite films prepared by different methods. Our results provide insights into the charge transport and recombination mechanism in perovskite films and help to unravel their potential for high-performance optoelectronic devices.

  8. Spatially indirect excitons in coupled quantum wells

    Energy Technology Data Exchange (ETDEWEB)

    Lai, Chih-Wei Eddy [Univ. of California, Berkeley, CA (United States)

    2004-03-01

    Microscopic quantum phenomena such as interference or phase coherence between different quantum states are rarely manifest in macroscopic systems due to a lack of significant correlation between different states. An exciton system is one candidate for observation of possible quantum collective effects. In the dilute limit, excitons in semiconductors behave as bosons and are expected to undergo Bose-Einstein condensation (BEC) at a temperature several orders of magnitude higher than for atomic BEC because of their light mass. Furthermore, well-developed modern semiconductor technologies offer flexible manipulations of an exciton system. Realization of BEC in solid-state systems can thus provide new opportunities for macroscopic quantum coherence research. In semiconductor coupled quantum wells (CQW) under across-well static electric field, excitons exist as separately confined electron-hole pairs. These spatially indirect excitons exhibit a radiative recombination time much longer than their thermal relaxation time a unique feature in direct band gap semiconductor based structures. Their mutual repulsive dipole interaction further stabilizes the exciton system at low temperature and screens in-plane disorder more effectively. All these features make indirect excitons in CQW a promising system to search for quantum collective effects. Properties of indirect excitons in CQW have been analyzed and investigated extensively. The experimental results based on time-integrated or time-resolved spatially-resolved photoluminescence (PL) spectroscopy and imaging are reported in two categories. (i) Generic indirect exciton systems: general properties of indirect excitons such as the dependence of exciton energy and lifetime on electric fields and densities were examined. (ii) Quasi-two-dimensional confined exciton systems: highly statistically degenerate exciton systems containing more than tens of thousands of excitons within areas as small as (10 micrometer)2 were

  9. Exciton analysis of many-body wave functions: Bridging the gap between the quasiparticle and molecular orbital pictures

    Science.gov (United States)

    Bäppler, Stefanie A.; Plasser, Felix; Wormit, Michael; Dreuw, Andreas

    2014-11-01

    Exciton sizes and electron-hole binding energies, which are central properties of excited states in extended systems and crucial to the design of modern electronic devices, are readily defined within a quasiparticle framework but are quite challenging to understand in the molecular-orbital picture. The intent of this work is to bridge this gap by providing a general way of extracting the exciton wave function out of a many-body wave function obtained by a quantum chemical excited-state computation. This methodology, which is based on the one-particle transition density matrix, is implemented within the ab initio algebraic diagrammatic construction scheme for the polarization propagator and specifically the evaluation of exciton sizes, i.e., dynamic charge separation distances, is considered. A number of examples are presented. For stacked dimers it is shown that the exciton size for charge separated states corresponds to the intermolecular separation, while it only depends on the monomer size for locally excited states or Frenkel excitons. In the case of conjugated organic polymers, the tool is applied to analyze exciton structure and dynamic charge separation. Furthermore, it is discussed how the methodology may be used for the construction of a charge-transfer diagnostic for time-dependent density-functional theory.

  10. Photon echo study of excitons and excitonic complexes in self-assembled quantum dots

    Energy Technology Data Exchange (ETDEWEB)

    Ikezawa, Michio [Institute of Physics, University of Tsukuba, Tsukuba 305-8571 (Japan)]. E-mail: mikezawa@sakura.cc.tsukuba.ac.jp; Nair, Selvakumar [Centre for Nanotechnology, University of Toronto, Toronto M5S 3E3 (Canada); Suto, Fumitaka [Institute of Physics, University of Tsukuba, Tsukuba 305-8571 (Japan); Masumoto, Yasuaki [Institute of Physics, University of Tsukuba, Tsukuba 305-8571 (Japan); Uchiyama, Chikako [Interdisciplinary Graduate School of Medicine and Engineering, University of Yamanashi, 4-3-11, Takeda, Kofu, Yamanashi 400-8511 (Japan); Aihara, Masaki [Graduate School of Materials Science, Nara Institute of Science and Technology, 8916-5, Takayama-cho, Ikoma, Nara 630-0101 (Japan); Ruda, Harry [Centre for Nanotechnology, University of Toronto, Toronto M5S 3E3 (Canada)

    2007-01-15

    The authors have studied the excitons and excitonic complexes in two kinds of self-assembled quantum dots (QDs) using photon echo measurements. In GaAs strain-induced quantum dots (SIQDs), a pronounced biexcitonic beat with a period of 1 ps is observed. The biexciton binding energy in SIQDs is obtained from the beat period, and its magnetic field dependence is investigated. It is found that the biexciton binding energy is remarkably increased by the lateral confinement and they are almost independent of the applied magnetic field up to 8 T. A theoretical calculation of the biexciton binding energy in SIQDs is presented to explain the observed magnetic field dependence. In charge-tunable InP QDs, the photon echo signal shows dramatic changes depending on the electric bias. The decay profile of the echo intensity is not a single exponential but Gaussian-like function, which indicates non-Markovian nature of the dephasing process in this system. Theoretical calculation is done assuming tunneling induced dephasing mechanism, and it reproduces the experimental results quite well.

  11. Immobilization of bilirubin oxidase on graphene oxide flakes with different negative charge density for oxygen reduction. The effect of GO charge density on enzyme coverage, electron transfer rate and current density.

    Science.gov (United States)

    Filip, Jaroslav; Andicsová-Eckstein, Anita; Vikartovská, Alica; Tkac, Jan

    2017-03-15

    Previously we showed that an effective bilirubin oxidase (BOD)-based biocathode using graphene oxide (GO) could be prepared in 2 steps: 1. electrostatic adsorption of BOD on GO; 2. electrochemical reduction of the BOD-GO composite to form a BOD-ErGO (electrochemically reduced GO) film on the electrode. In order to identify an optimal charge density of GO for BOD-ErGO composite preparation, several GO fractions differing in an average flake size and ζ-potential were prepared using centrifugation and consequently employed for BOD-ErGO biocathode preparation. A simple way to express surface charge density of these particular GO nanosheets was developed. The values obtained were then correlated with biocatalytic and electrochemical parameters of the prepared biocathodes, i.e. electrocatalytically active BOD surface coverage (Γ), heterogeneous electron transfer rate (kS) and a maximum biocatalytic current density. The highest bioelectrocatalytic current density of (597±25)μAcm(-2) and the highest Γ of (23.6±0.9)pmolcm(-2) were obtained on BOD-GO composite having the same moderate negative charge density, but the highest kS of (79.4±4.6)s(-1) was observed on BOD-GO composite having different negative charge density. This study is a solid foundation for others to consider the influence of a charge density of GO on direct bioelectrochemistry/bioelectrocatalysis of other redox enzymes applicable for construction of biosensors, bioanodes, biocathodes or biofuel cells. Copyright © 2016 Elsevier B.V. All rights reserved.

  12. Positively and Negatively Charged Ionic Modifications to Cellulose Assessed as Cotton-Based Protease-Lowering and Haemostatic Wound Agents

    Science.gov (United States)

    Recent developments in cellulose wound dressings targeted to different stages of wound healing have been based on structural and charge modifications that function to modulate events in the complex inflammatory and hemostatic phases of wound healing. Hemostasis and inflammation comprise two overlapp...

  13. Coherent exciton-polariton devices

    Science.gov (United States)

    Fraser, Michael D.

    2017-09-01

    The Bose-Einstein condensate of exciton-polaritons has emerged as a unique, coherent system for the study of non-equilibrium, macroscopically coherent Bose gases, while the full confinement of this coherent state to a semiconductor chip has also generated considerable interest in developing novel applications employing the polariton condensate, possibly even at room temperature. Such devices include low-threshold lasers, precision inertial sensors, and circuits based on superfluidity with ultra-fast non-linear elements. While the demonstration and development of such devices are at an early stage, rapid progress is being made. In this review, an overview of the exciton-polariton condensate system and the established and emerging material systems and fabrication techniques are presented, followed by a critical, in-depth assessment of the ability of the coherent polariton system to deliver on its promise of devices offering either new functionality and/or room-temperature operation.

  14. Nanoscale mapping of excitonic processes in single-layer MoS2 using tip-enhanced photoluminescence microscopy.

    Science.gov (United States)

    Su, Weitao; Kumar, Naresh; Mignuzzi, Sandro; Crain, Jason; Roy, Debdulal

    2016-05-19

    In two-dimensional (2D) semiconductors, photoluminescence originating from recombination processes involving neutral electron-hole pairs (excitons) and charged complexes (trions) is strongly affected by the localized charge transfer due to inhomogeneous interactions with the local environment and surface defects. Herein, we demonstrate the first nanoscale mapping of excitons and trions in single-layer MoS2 using the full spectral information obtained via tip-enhanced photoluminescence (TEPL) microscopy along with tip-enhanced Raman spectroscopy (TERS) imaging of a 2D flake. Finally, we show the mapping of the PL quenching centre in single-layer MoS2 with an unprecedented spatial resolution of 20 nm. In addition, our research shows that unlike in aperture-scanning near field microscopy, preferential exciton emission mapping at the nanoscale using TEPL and Raman mapping using TERS can be obtained simultaneously using this method that can be used to correlate the structural and excitonic properties.

  15. A Thermally Activated Exciton-Exciton Collision Process in ZnO Microrods

    Institute of Scientific and Technical Information of China (English)

    ZHAO Dong-Xu; LIU Yi-Chun; SHEN De-Zhen; LU You-Ming; ZHANG Ji-Ying; FAN Xi-Wu

    2004-01-01

    @@ Room-temperature P-band emission induced by an exciton-exciton collision process was observed in ZnO microrods. Both temperature- and excitation-intensity-dependent photoluminescence (PL) measurements were conducted.

  16. Exciton Seebeck effect in molecular systems

    Energy Technology Data Exchange (ETDEWEB)

    Yan, Yun-An, E-mail: yunan@nano.gznc.edu.cn [Guizhou Provincial Key Laboratory of Computational Nanomaterial Science, Guizhou Normal College, Guiyang, Guizhou 550018 (China); Cai, Shaohong [Guizhou Key Laboratory of Economic System Simulation, Guizhou University of Finance and Economics, Guiyang 550004 (China)

    2014-08-07

    We investigate the exciton dynamics under temperature difference with the hierarchical equations of motion. Through a nonperturbative simulation of the transient absorption of a heterogeneous trimer model, we show that the temperature difference causes exciton population redistribution and affects the exciton transfer time. It is found that one can reproduce not only the exciton population redistribution but also the change of the exciton transfer time induced by the temperature difference with a proper tuning of the site energies of the aggregate. In this sense, there exists a site energy shift equivalence for any temperature difference in a broad range. This phenomenon is similar to the Seebeck effect as well as spin Seebeck effect and can be named as exciton Seebeck effect.

  17. Exciton Seebeck effect in molecular systems.

    Science.gov (United States)

    Yan, Yun-An; Cai, Shaohong

    2014-08-07

    We investigate the exciton dynamics under temperature difference with the hierarchical equations of motion. Through a nonperturbative simulation of the transient absorption of a heterogeneous trimer model, we show that the temperature difference causes exciton population redistribution and affects the exciton transfer time. It is found that one can reproduce not only the exciton population redistribution but also the change of the exciton transfer time induced by the temperature difference with a proper tuning of the site energies of the aggregate. In this sense, there exists a site energy shift equivalence for any temperature difference in a broad range. This phenomenon is similar to the Seebeck effect as well as spin Seebeck effect and can be named as exciton Seebeck effect.

  18. Localized Excitons in Carbon Nanotubes.

    Science.gov (United States)

    Adamska, Lyudmyla; Doorn, Stephen K.; Tretiak, Sergei

    2015-03-01

    It has been historically known that unintentional defects in carbon nanotubes (CNTs) may fully quench the fluorescence. However, some dopants may enhance the fluorescence by one order of magnitude thus turning the CNTs, which are excellent light absorbers, in good emitters. We have correlated the experimentally observed photoluminescence spectra to the electronic structure simulations. Our experiment reveals multiple sharp asymmetric emission peaks at energies 50-300 meV red-shifted from that of the lowest bright exciton peak. Our simulations suggest an association of these peaks with deep trap states tied to different specific chemical adducts. While the wave functions of excitons in undoped CNTs are delocalized, those of the deep-trap states are strongly localized and pinned to the dopants. These findings are consistent with the experimental observation of asymmetric broadening of the deep trap emission peaks, which can result from scattering of acoustic phonons on localized excitons. Our work lays the foundation to utilize doping as a generalized route for wave function engineering and direct control of carrier dynamics in SWCNTs toward enhanced light emission properties for photonic applications.

  19. Reverse Polarization of a High-Energy Exciton in Conjugated Polymers

    Institute of Scientific and Technical Information of China (English)

    李晓雪; 董宪峰; 高琨; 解士杰

    2011-01-01

    Polarization of a high-energy exciton in conjugated polymers is investigated theoretically by using an extended one-dimensional tight-binding Su-Schrieffer-Heeger(SSH)model.Under an external electric field,the reverse polarization of a high-energy exciton is obtained and the corresponding physical mechanism is analyzed.A critical field Ec is obtained,over which the polarization of the high-energy exciton will switch from negative to positive.In addition,by taking into account the effect of the non-degenerate confinement,we find that it is possible to realize reverse polarization through high energy photoexcitation in non-degenerate polymers.%Polarization of a high-energy exciton in conjugated polymers is investigated theoretically by using an extended one-dimensional tight-binding Su-Schrieffer-Heeger (SSH) model. Under an external electric field, the reverse polarization of a high-energy exciton is obtained and the corresponding physical mechanism is analyzed. A critical Held Ec is obtained, over which the polarization of the high-energy exciton will switch from negative to positive. In addition, by taking into account the effect of the non-degenerate confinement, we find that it is possible to realize reverse polarization through high energy photoexcitation in non-degenerate polymers.

  20. Magnetic brightening and control of dark excitons in monolayer WSe2

    Science.gov (United States)

    Zhang, Xiao-Xiao; Cao, Ting; Lu, Zhengguang; Lin, Yu-Chuan; Zhang, Fan; Wang, Ying; Li, Zhiqiang; Hone, James C.; Robinson, Joshua A.; Smirnov, Dmitry; Louie, Steven G.; Heinz, Tony F.

    2017-09-01

    Monolayer transition metal dichalcogenide crystals, as direct-gap materials with strong light-matter interactions, have attracted much recent attention. Because of their spin-polarized valence bands and a predicted spin splitting at the conduction band edges, the lowest-lying excitons in WX2 (X = S, Se) are expected to be spin-forbidden and optically dark. To date, however, there has been no direct experimental probe of these dark excitons. Here, we show how an in-plane magnetic field can brighten the dark excitons in monolayer WSe2 and permit their properties to be observed experimentally. Precise energy levels for both the neutral and charged dark excitons are obtained and compared with ab initio calculations using the GW-BSE approach. As a result of their spin configuration, the brightened dark excitons exhibit much-increased emission and valley lifetimes. These studies directly probe the excitonic spin manifold and reveal the fine spin-splitting at the conduction band edges.

  1. Probing dark excitons in atomically thin semiconductors via near-field coupling to surface plasmon polaritons

    Science.gov (United States)

    Zhou, You; Scuri, Giovanni; Wild, Dominik S.; High, Alexander A.; Dibos, Alan; Jauregui, Luis A.; Shu, Chi; de Greve, Kristiaan; Pistunova, Kateryna; Joe, Andrew Y.; Taniguchi, Takashi; Watanabe, Kenji; Kim, Philip; Lukin, Mikhail D.; Park, Hongkun

    2017-09-01

    Transition metal dichalcogenide (TMD) monolayers with a direct bandgap feature tightly bound excitons, strong spin-orbit coupling and spin-valley degrees of freedom. Depending on the spin configuration of the electron-hole pairs, intra-valley excitons of TMD monolayers can be either optically bright or dark. Dark excitons involve nominally spin-forbidden optical transitions with a zero in-plane transition dipole moment, making their detection with conventional far-field optical techniques challenging. Here, we introduce a method for probing the optical properties of two-dimensional materials via near-field coupling to surface plasmon polaritons (SPPs). This coupling selectively enhances optical transitions with dipole moments normal to the two-dimensional plane, enabling direct detection of dark excitons in TMD monolayers. When a WSe2 monolayer is placed on top of a single-crystal silver film, its emission into near-field-coupled SPPs displays new spectral features whose energies and dipole orientations are consistent with dark neutral and charged excitons. The SPP-based near-field spectroscopy significantly improves experimental capabilities for probing and manipulating exciton dynamics of atomically thin materials, thus opening up new avenues for realizing active metasurfaces and robust optoelectronic systems, with potential applications in information processing and communication.

  2. Negatively charged residues of the segment linking the enzyme and cytolysin moieties restrict the membrane-permeabilizing capacity of adenylate cyclase toxin

    Science.gov (United States)

    Masin, Jiri; Osickova, Adriana; Sukova, Anna; Fiser, Radovan; Halada, Petr; Bumba, Ladislav; Linhartova, Irena; Osicka, Radim; Sebo, Peter

    2016-01-01

    The whooping cough agent, Bordetella pertussis, secretes an adenylate cyclase toxin-hemolysin (CyaA) that plays a crucial role in host respiratory tract colonization. CyaA targets CR3-expressing cells and disrupts their bactericidal functions by delivering into their cytosol an adenylate cyclase enzyme that converts intracellular ATP to cAMP. In parallel, the hydrophobic domain of CyaA forms cation-selective pores that permeabilize cell membrane. The invasive AC and pore-forming domains of CyaA are linked by a segment that is unique in the RTX cytolysin family. We used mass spectrometry and circular dichroism to show that the linker segment forms α-helical structures that penetrate into lipid bilayer. Replacement of the positively charged arginine residues, proposed to be involved in target membrane destabilization by the linker segment, reduced the capacity of the toxin to translocate the AC domain across cell membrane. Substitutions of negatively charged residues then revealed that two clusters of negative charges within the linker segment control the size and the propensity of CyaA pore formation, thereby restricting the cell-permeabilizing capacity of CyaA. The ‘AC to Hly-linking segment’ thus appears to account for the smaller size and modest cell-permeabilizing capacity of CyaA pores, as compared to typical RTX hemolysins. PMID:27581058

  3. Relation between surface properties, pore structure and first-cycle charge loss of graphite as negative electrode in lithium-ion batteries

    Science.gov (United States)

    Joho, Felix; Rykart, Beat; Blome, Andreas; Novák, Petr; Wilhelm, Henri; Spahr, Michael E.

    Cycling of graphite in lithium-ion batteries is reversible except for the first-cycle, where some charge is "lost" due to irreversible side reactions. The irreversible charge loss of different TIMREX ® graphites was found to be a linear function, both of their specific BET surface areas and of the double-layer capacitance of electrodes manufactured from these graphites. Nitrogen-adsorption measurements and differential-porosity calculations indicate that the pore structure of the graphite particles mainly consists of mesopores (2-50 nm). The surface area of these mesopores is part of the electroactive surface area determined by impedance spectroscopy, and contributes to the irreversible capacity of the graphite negative electrode in the first-cycle.

  4. Influence of expander components on the processes at the negative plates of lead-acid cells on high-rate partial-state-of-charge cycling. Part II. Effect of carbon additives on the processes of charge and discharge of negative plates

    Energy Technology Data Exchange (ETDEWEB)

    Pavlov, D.; Nikolov, P.; Rogachev, T. [Institute of Electrochemistry and Energy Systems, Bulgarian Academy of Sciences, Acad. Georgi Bonchev Street, bl. 10, Sofia 1113 (Bulgaria)

    2010-07-15

    Lead-acid batteries operated in the high-rate partial-state-of-charge (HRPSoC) duty rapidly lose capacity on cycling, because of sulfation of the negative plates. As the battery operates from a partially discharged state, the small PbSO{sub 4} crystals dissolve and precipitate onto the bigger crystals. The latter have low solubility and hence PbSO{sub 4} accumulates progressively in the negative plates causing capacity loss. In order to suppress this process, the rate of the charge process should be increased. In a previous publication of ours we have established that reduction of Pb{sup 2+} ions to Pb may proceed on the surface of both Pb and carbon black particles. Hence, the reversibility of the charge-discharge processes improves, which leads to improved cycle life performance of the batteries in the HRPSoC mode. However, not all carbon forms accelerate the charge processes. The present paper discusses the electrochemical properties of two groups of carbon blacks: Printex and active carbons. The influence of Vaniseprse A and BaSO{sub 4} (the other two components of the expander added to the negative plates) on the reversibility of the charge-discharge processes on the negative plates is also considered. It has been established that lignosulfonates are adsorbed onto the lead surface and retard charging of the battery. BaSO{sub 4} has the opposite effect, which improves the reversibility of the processes on cycling and hence prolongs battery life in the HRPSoC duty. It has been established that the cycle life of lead-acid cells depends on the type of carbon black or active carbon added to the negative plates. When the carbon particles are of nano-sizes (<180 nm), the HRPSoC cycle life is between 10,000 and 20,000 cycles. Lignosulfonates suppress this beneficial effect of carbon black and activated carbon additives to about 10,000 cycles. Cells with active carbons have the longest cycle life when they contain also BaSO{sub 4} but no lignosulfonate. A summary of

  5. Origin of space-separated charges in photoexcited organic heterojunctions on ultrafast time scales

    CERN Document Server

    Janković, Veljko

    2016-01-01

    We present detailed investigation of ultrafast (sub-ps) exciton dynamics in the lattice model of a donor/acceptor heterojunction. Exciton generation by means of a photoexcitation, exciton dissociation, and further charge separation are treated on equal footing. The experimentally observed presence of space-separated charges at $\\lesssim 100$ fs after the photoexcitation is usually attributed to ultrafast transitions from excitons in the donor to charge transfer and charge separated states. Here, we show, however, that space-separated charges appearing on $\\lesssim 100$-fs time scales are predominantly directly optically generated. Our theoretical insights into the ultrafast pump-probe spectroscopy challenge usual interpretations of pump-probe spectra in terms of ultrafast population transfer from donor excitons to space-separated charges.

  6. Near-infrared exciton-polaritons in strongly coupled single-walled carbon nanotube microcavities

    Science.gov (United States)

    Graf, Arko; Tropf, Laura; Zakharko, Yuriy; Zaumseil, Jana; Gather, Malte C.

    2016-01-01

    Exciton-polaritons form upon strong coupling between electronic excitations of a material and photonic states of a surrounding microcavity. In organic semiconductors the special nature of excited states leads to particularly strong coupling and facilitates condensation of exciton-polaritons at room temperature, which may lead to electrically pumped organic polariton lasers. However, charge carrier mobility and photo-stability in currently used materials is limited and exciton-polariton emission so far has been restricted to visible wavelengths. Here, we demonstrate strong light-matter coupling in the near infrared using single-walled carbon nanotubes (SWCNTs) in a polymer matrix and a planar metal-clad cavity. By exploiting the exceptional oscillator strength and sharp excitonic transition of (6,5) SWCNTs, we achieve large Rabi splitting (>110 meV), efficient polariton relaxation and narrow band emission (<15 meV). Given their high charge carrier mobility and excellent photostability, SWCNTs represent a promising new avenue towards practical exciton-polariton devices operating at telecommunication wavelengths. PMID:27721454

  7. Exciton delocalization incorporated drift-diffusion model for bulk-heterojunction organic solar cells

    Science.gov (United States)

    Wang, Zi Shuai; Sha, Wei E. I.; Choy, Wallace C. H.

    2016-12-01

    Modeling the charge-generation process is highly important to understand device physics and optimize power conversion efficiency of bulk-heterojunction organic solar cells (OSCs). Free carriers are generated by both ultrafast exciton delocalization and slow exciton diffusion and dissociation at the heterojunction interface. In this work, we developed a systematic numerical simulation to describe the charge-generation process by a modified drift-diffusion model. The transport, recombination, and collection of free carriers are incorporated to fully capture the device response. The theoretical results match well with the state-of-the-art high-performance organic solar cells. It is demonstrated that the increase of exciton delocalization ratio reduces the energy loss in the exciton diffusion-dissociation process, and thus, significantly improves the device efficiency, especially for the short-circuit current. By changing the exciton delocalization ratio, OSC performances are comprehensively investigated under the conditions of short-circuit and open-circuit. Particularly, bulk recombination dependent fill factor saturation is unveiled and understood. As a fundamental electrical analysis of the delocalization mechanism, our work is important to understand and optimize the high-performance OSCs.

  8. Features of exciton dynamics in molecular nanoclusters (J-aggregates): Exciton self-trapping (Review Article)

    Science.gov (United States)

    Malyukin, Yu. V.; Sorokin, A. V.; Semynozhenko, V. P.

    2016-06-01

    We present thoroughly analyzed experimental results that demonstrate the anomalous manifestation of the exciton self-trapping effect, which is already well-known in bulk crystals, in ordered molecular nanoclusters called J-aggregates. Weakly-coupled one-dimensional (1D) molecular chains are the main structural feature of J-aggregates, wherein the electron excitations are manifested as 1D Frenkel excitons. According to the continuum theory of Rashba-Toyozawa, J-aggregates can have only self-trapped excitons, because 1D excitons must adhere to barrier-free self-trapping at any exciton-phonon coupling constant g = ɛLR/2β, wherein ɛLR is the lattice relaxation energy, and 2β is the half-width of the exciton band. In contrast, very often only the luminescence of free, mobile excitons would manifest in experiments involving J-aggregates. Using the Urbach rule in order to analyze the low-frequency region of the low-temperature exciton absorption spectra has shown that J-aggregates can have both a weak (g 1) exciton-phonon coupling. Moreover, it is experimentally demonstrated that under certain conditions, the J-aggregate excited state can have both free and self-trapped excitons, i.e., we establish the existence of a self-trapping barrier for 1D Frenkel excitons. We demonstrate and analyze the reasons behind the anomalous existence of both free and self-trapped excitons in J-aggregates, and demonstrate how exciton-self trapping efficiency can be managed in J-aggregates by varying the values of g, which is fundamentally impossible in bulk crystals. We discuss how the exciton-self trapping phenomenon can be used as an alternate interpretation of the wide band emission of some J-aggregates, which has thus far been explained by the strongly localized exciton model.

  9. Charge/discharge characteristics of the coal-tar pitch carbon as negative electrode in Li-ion batteries

    Science.gov (United States)

    Kim, Jung-Sik

    The charge/discharge characteristics were studied for the coal-tar pitch-based carbon (CTPC), which was pyrolyzed under the condition to form anisotropic mesophase pitch and then heat treated at temperatures ranging from 500 to 1300°C in N 2 atmosphere. As the heat treatment temperature increased, the reversible capacity for the CTPC increased progressively up to 1000°C, while the irreversible capacity decreased continuously. Carbons synthesized through the extraction of anisotropic mesophases showed higher reversible and lower irreversible capacities than the directly pyrolyzed ones.

  10. Influence of expander components on the processes at the negative plates of lead-acid cells on high-rate partial-state-of-charge cycling. Part I: Effect of lignosulfonates and BaSO{sub 4} on the processes of charge and discharge of negative plates

    Energy Technology Data Exchange (ETDEWEB)

    Pavlov, D.; Nikolov, P.; Rogachev, T. [Institute of Electrochemistry and Energy Systems, Bulgarian Academy of Sciences, Acad. Georgi Bonchev Street, bl. 10, Sofia 1113 (Bulgaria)

    2010-07-15

    This study investigates the influence of the organic expander component (Vanisperse A) and of BaSO{sub 4} on the performance of negative lead-acid battery plates on high-rate partial-state-of-charge (HRPSoC) cycling. Batteries operating in the HRPSoC mode should be classified as a separate type of lead-acid batteries. Hence, the additives to the negative plates should differ from the conventional expander composition. It has been established that lignosulfonates are adsorbed onto the lead surface and thus impede the charge processes, which results in impaired reversibility of the charge-discharge processes and hence shorter cycle life on HRPSoC operation, limited by sulfation of the negative plates. BaSO{sub 4} exerts the opposite effect: it improves the reversibility of the processes in the HRPSoC mode and hence prolongs the cycle life of the cells. The most pronounced effect of BaSO{sub 4} has been registered when it is added in concentration of 1.0 wt.% versus the leady oxide (LO) used for paste preparation. It has also been established that BaSO{sub 4} lowers the overpotential of PbSO{sub 4} nucleation. The results of the present investigation indicate that BaSO{sub 4} affects also the crystallization process of Pb during cell charging. Thus, BaSO{sub 4} eventually improves the performance characteristics of lead-acid cells on HRPSoC cycling. (author)

  11. Evaluation of defects in cuprous oxide through exciton luminescence imaging

    Energy Technology Data Exchange (ETDEWEB)

    Frazer, Laszlo, E-mail: jl@laszlofrazer.com [Department of Physics, Northwestern University, 2145 Sheridan Road, Evanston, IL 60208 (United States); Lenferink, Erik J. [Department of Physics, Northwestern University, 2145 Sheridan Road, Evanston, IL 60208 (United States); Chang, Kelvin B. [Department of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, IL 60208 (United States); Poeppelmeier, Kenneth R. [Department of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, IL 60208 (United States); Chemical Sciences and Engineering Division, Argonne National Laboratory, 9700 South Cass Avenue, Argonne, IL 60439 (United States); Stern, Nathaniel P. [Department of Physics, Northwestern University, 2145 Sheridan Road, Evanston, IL 60208 (United States); Ketterson, John B. [Department of Physics, Northwestern University, 2145 Sheridan Road, Evanston, IL 60208 (United States); Department of Electrical Engineering and Computer Science, Northwestern University, 2145 Sheridan Road, Evanston, IL 60208 (United States)

    2015-03-15

    The various decay mechanisms of excitons in cuprous oxide (Cu{sub 2}O) are highly sensitive to defects which can relax selection rules. Here we report cryogenic hyperspectral imaging of exciton luminescence from cuprous oxide crystals grown via the floating zone method showing that the samples have few defects. Some locations, however, show strain splitting of the 1s orthoexciton triplet polariton luminescence. Strain is reduced by annealing. In addition, annealing causes annihilation of oxygen and copper vacancies, which leads to a negative correlation between luminescence of unlike vacancies. - Highlights: • We use luminescence to observe defects in high quality cuprous oxide crystals. • Strain is reduced by annealing. • Annealing causes annihilation of oxygen and copper vacancies.

  12. Unpaired Composite Fermion, Topological Exciton, and Zero Mode

    Science.gov (United States)

    Sreejith, G. J.; Wójs, A.; Jain, J. K.

    2011-09-01

    The paired state of composite fermions is expected to support two kinds of excitations: vortices and unpaired composite fermions. We construct an explicit microscopic description of the unpaired composite fermions, which we demonstrate to be accurate for a 3-body model interaction and, possibly, adiabatically connected to the Coulomb solution. This understanding reveals that an unpaired composite fermion carries with it a charge-neutral “topological” exciton, which, in turn, helps provide microscopic insight into the origin of zero modes, fusion rules, and energetics.

  13. Exploring ultrafast dynamics of excitons and multiexcitons in "giant" nanocrystal quantum dots

    Science.gov (United States)

    Sampat, Siddharth

    In this work, we have performed extensive time resolved photoluminescence (PL) studies to further the understanding of charge dynamics in semiconductor nanocrystal quantum dots (QDs). Recent developments in QD synthesis have introduced a new set of QD known as "giant" quantum dots (gQDs) that consist of a CdSe core coated with up to 19 monolayers of a CdS shell. The thick shell layer is grown using a SILAR method resulting in a defect free, alloyed CdSe/CdS interface. This has been attributed to gQDs exhibiting excellent optical properties such as high excitonic quantum yield (QY), prolonged photostability and inhibition of flourescence intermittency ("blinking"), which is regularly observed in conventional QDs. In gQDs, however, owing to unique fabrication methods and material selection, the Auger process is strongly suppressed resulting in efficient radiative recombination of photogenerated excitons as well as high PL QY of charged excitonic and multiexcitonic species. We perform extensive single gQDs studies that establish the role played by gQD shell thickness and core size in governing their optical properties. It is found that both the core and shell dimensions can be tuned in order to achieve the smallest gQDs with the highest vii Auger suppression resulting in photostable dots with high QYs. Next, we perform a study of multiexcitonic species in gQDs that are encapsulated in an insulating SiO2shell. These silica-coated gQDs exhibit strong PL from charged excitons, biexcitons as well as triexcitons. This observation has led to an accurate description of excitonic and multiexcitonic behavior which is modeled using a statistical scaling approach. As a demonstration of the practical applicability of gQDs, energy transfer of excitons as well as multiexcitons to different substrates is studied. Finally, a back gated silicon nanomembrane FET device is discussed that exhibits a large photocurrent increase when sensitized with QDs.

  14. Exciton-polaritons in Bragg gratings

    Energy Technology Data Exchange (ETDEWEB)

    Creatore, C [Department of Physics ' A. Volta' , Universita di Pavia, via Bassi 6, I-27100, Pavia (Italy); Mouchliadis, L; Langbein, W [School of Physics and Astronomy, Cardiff University, The Parade, CF24 3AA, Cardiff (United Kingdom); Biancalana, F [Max Planck Institute for the Science of Light, Guenther-Scharowsky-Str. 1/Bau 24, 91058 Erlangen (Germany); Osborne, S, E-mail: creatore@fisicavolta.unipv.i [Tyndall National Institute, Lee Maltings, Prospect Row, Cork (Ireland)

    2010-02-01

    We study the strong coupling between photons and bulk excitons in a one-dimensional Bragg grating. The dispersion of the resulting Bragg-polariton states resembles the dispersion of quantum-well microcavity polaritons. We report on a parametric scattering process at two 'magic frequencies' occurring due to the strong excitonic nonlinearity.

  15. Radiative recombination of excitons in amorphous semiconductors

    Energy Technology Data Exchange (ETDEWEB)

    Singh, Jai [School of Engineering and Logistics, Faculty Technology, B-41, Charles Darwin University, Darwin, NT 0909 (Australia)]. E-mail: jai.singh@cdu.edu.au

    2005-04-15

    A theory for calculating the radiative lifetime of excitons in amorphous semiconductors is presented. Four possibilities of excitonic radiative recombination are considered and the corresponding rates are derived at thermal equilibrium. The radiative lifetime is calculated from the inverse of the maximum rate for all the four possibilities. Results agree very well with experiments.

  16. Photosynthetic light harvesting: excitons and coherence.

    Science.gov (United States)

    Fassioli, Francesca; Dinshaw, Rayomond; Arpin, Paul C; Scholes, Gregory D

    2014-03-06

    Photosynthesis begins with light harvesting, where specialized pigment-protein complexes transform sunlight into electronic excitations delivered to reaction centres to initiate charge separation. There is evidence that quantum coherence between electronic excited states plays a role in energy transfer. In this review, we discuss how quantum coherence manifests in photosynthetic light harvesting and its implications. We begin by examining the concept of an exciton, an excited electronic state delocalized over several spatially separated molecules, which is the most widely available signature of quantum coherence in light harvesting. We then discuss recent results concerning the possibility that quantum coherence between electronically excited states of donors and acceptors may give rise to a quantum coherent evolution of excitations, modifying the traditional incoherent picture of energy transfer. Key to this (partially) coherent energy transfer appears to be the structure of the environment, in particular the participation of non-equilibrium vibrational modes. We discuss the open questions and controversies regarding quantum coherent energy transfer and how these can be addressed using new experimental techniques.

  17. The reduction rates of DEPC-modified mutant Thermus thermophilus Rieske proteins differ when there is a negative charge proximal to the cluster.

    Science.gov (United States)

    Karagas, Nicholas E; Jones, Christie N; Osborn, Deborah J; Dzierlenga, Anika L; Oyala, Paul; Konkle, Mary E; Whitney, Emily M; David Britt, R; Hunsicker-Wang, Laura M

    2014-10-01

    Rieske and Rieske-type proteins are electron transport proteins involved in key biological processes such as respiration, photosynthesis, and detoxification. They have a [2Fe-2S] cluster ligated by two cysteines and two histidines. A series of mutations, L135E, L135R, L135A, and Y158F, of the Rieske protein from Thermus thermophilus has been produced which probe the effects of the neighboring residues, in the second sphere, on the dynamics of cluster reduction and the reactivity of the ligating histidines. These properties were probed using titrations and modifications with diethyl pyrocarbonate (DEPC) at various pH values monitored using UV-Visible and circular dichroism spectrophotometry. These results, along with results from EPR studies, provide information on ligating histidine modification and rate of reduction of each of the mutant proteins. L135R, L135A, and Y158F react with DEPC similarly to wild type, resulting in modified protein with a reduced [2Fe-2S] cluster in 15 h under the same conditions. Thus, the negative charge slows down the rate of reduction and provides an explanation as to why negatively charged residues are rarely, if ever, found in the equivalent position of other Rieske and Rieske-type proteins.

  18. Study of the characteristics of a gas-discharge counter with a negatively charged wire in the air

    Energy Technology Data Exchange (ETDEWEB)

    Kalinnikov, V.A.; Kravchuk, N.P. E-mail: kravchuk@nusun.jinr.dubna.su; Kuchinsky, N.A

    1999-11-11

    Gas-discharge counters with a negative potential at the thin central electrode are studied. In a counter with thus applied high-voltage, electron avalanches develop in the direction away from the centre in a greatly decreasing electric field. The mechanism for this process and the effect of various factors are described. The counting and amplitude characteristics are given for one of the counters. The geometrically sensitive region and the dependence of its performance on the type of primary ionization is studied. The counter was tested in the air under normal conditions.

  19. Visualization of molecular excitons diffusion

    Science.gov (United States)

    Salamatova, Evgeniia; Kozlov, Oleg V.; Luponosov, Yuriy N.; Solodukhin, Alexander N.; Toropynina, Viktoria Y.; Ponomarenko, Sergei A.; Pshenichnikov, Maxim S.

    2016-09-01

    Small organic molecules of the push-pull architecture are rapidly gaining their status in the organic electronics applications. In densely packed molecular films, both intra- and intermolecular interactions play an essential role for the device performance. Here we study two different molecules, a highly symmetric star-shaped one and its newly synthesized single arm analogue, for their photophysical properties. Both chromophores were dissolved in a solid matrix at different concentrations to vary their separation and therefore intermolecular coupling. We show that in both molecules the population relaxation accelerates by more than a factor of 10 at shorter intermolecular distances due to self-quenching thereby reducing the exciton survival time. The transient anisotropy dynamics are also quite similar, with their substantial acceleration at shorter interchromophore distances due to exciton diffusion caused by the Förster-like resonance energy transfer. However, the anisotropy values are noticeably lower for the star-shaped molecule because of intramolecular mixing of different polarization states. Finally, a model is presented that accounts for the observed results.

  20. Dissociating excitons photogenerated in semiconducting carbon nanotubes at polymeric photovoltaic heterojunction interfaces.

    Science.gov (United States)

    Bindl, Dominick J; Safron, Nathaniel S; Arnold, Michael S

    2010-10-26

    Semiconducting single-walled carbon nanotubes (s-SWCNTs) have strong near-infrared and visible absorptivity and exceptional charge transport characteristics, rendering them highly attractive semiconductor absorbers for photovoltaic and photodetector technologies. However, these applications are limited by a poor understanding of how photogenerated charges, which are bound as excitons in s-SWCNTs, can be dissociated in large-area solid-state devices. Here, we measure the dissociation of excitons in s-SWCNT thin films that form planar heterojunction interfaces with polymeric photovoltaic materials using an exciton dissociation-sensitive photocapacitor measurement technique that is advantageously insensitive to optically induced thermal photoconductive effects. We find that fullerene and polythiophene derivatives induce exciton dissociation, resulting in electron and hole transfer, respectively, away from optically excited s-SWCNTs. Significantly weaker or no charge transfer is observed using wider gap polymers due to insufficient energy offsets. These results are expected to critically guide the development of thin film s-SWCNT-based photosensitive devices.

  1. Charge Carrier Dynamics at Silver Nanocluster-Molecular Acceptor Interfaces

    KAUST Repository

    Almansaf, Abdulkhaleq

    2017-07-01

    A fundamental understanding of interfacial charge transfer at donor-acceptor interfaces is very crucial as it is considered among the most important dynamical processes for optimizing performance in many light harvesting systems, including photovoltaics and photo-catalysis. In general, the photo-generated singlet excitons in photoactive materials exhibit very short lifetimes because of their dipole-allowed spin radiative decay and short diffusion lengths. In contrast, the radiative decay of triplet excitons is dipole forbidden; therefore, their lifetimes are considerably longer. The discussion in this thesis primarily focuses on the relevant parameters that are involved in charge separation (CS), charge transfer (CT), intersystem crossing (ISC) rate, triplet state lifetime, and carrier recombination (CR) at silver nanocluster (NCs) molecular-acceptors interfaces. A combination of steady-state and femto- and nanosecond broadband transient absorption spectroscopies were used to investigate the charge carrier dynamics in various donor-acceptor systems. Additionally, this thesis was prolonged to investigate some important factors that influence the charge carrier dynamics in Ag29 silver NCs donor-acceptor systems, such as the metal doping and chemical structure of the nanocluster and molecular acceptors. Interestingly, clear correlations between the steady-state measurements and timeresolved spectroscopy results are found. In the first study, we have investigated the interfacial charge transfer dynamics in positively charged meso units of 5, 10, 15, 20-tetra (1- methyl-4-pyridino)-porphyrin tetra (p-toluene sulfonate) (TMPyP) and neutral charged 5, 10, 15, 20-tetra (4-pyridyl)-porphyrin (TPyP), with negatively charged undoped and gold (Au)- doped silver Ag29 NCs. Moreover, this study showed the impact of Au doping on the charge carrier dynamics of the system. In the second study, we have investigated the interfacial charge transfer dynamics in [Pt2 Ag23 Cl7 (PPh3

  2. Bound states of a negative test charge due to many-body effects in the two-dimensional electron gas

    Science.gov (United States)

    Ghazali, A.; Gold, A.

    1995-12-01

    Bound states of a negative test electron in the low-density regime of the two-dimensional electron gas are obtained when many-body effects (exchange and correlation) are incorporated in the screening function via the local-field correction. Using the Green's-function method and a variational method we determine the energies and the wave functions of the ground state and the excited states as functions of the electron density. For high electron density no bound state is found. Below a critical density the number and the energy of bound states increase with decreasing electron density. The ground state is described by the wave function ψ2s~r exp(-r/α).

  3. Electronic structure of Ta2NiSe5 as a candidate for excitonic insulators

    Science.gov (United States)

    Kaneko, T.; Toriyama, T.; Konishi, T.; Ohta, Y.

    2012-12-01

    We make the electronic structure calculations of Ta2NiSe5 known as a candidate for excitonic insulators where the semiconducting or semi-metallic ground state becomes unstable against the coherent formation of excitons. We use the generalized gradient approximation (GGA) in the density functional theory, where the Hubbard-type repulsive interaction U is taken into account (GGA+U). We find that the material has a very simple quasi-one-dimensional (1D) electronic structure which relates to the formation of excitons. From the calculated partial density of states, band dispersion and spatial distribution of charge densities, we find in the first approximation that the conduction band is configured by the Ta 1D chain and the valence band is configured by the Ni-Se 1D chain.

  4. Influence of free carriers on exciton ground states in quantum wells

    Energy Technology Data Exchange (ETDEWEB)

    Klochikhin, A.A. [Ioffe Physical Technical Institute, 194021 St. Petersburg (Russian Federation); Nuclear Physics Institute, 350000 St. Petersburg (Russian Federation); Kochereshko, V.P., E-mail: vladimir.kochereshko@mail.ioffe.ru [Ioffe Physical Technical Institute, 194021 St. Petersburg (Russian Federation); Spin Optics Laboratory, St. Petersburg State University, 198904 St. Petersburg (Russian Federation); Tatarenko, S. [CEA-CNRS Group “Nanophysique et Semiconducteurs”, Institut Néel, CNRS and Universite Joseph Fourier, 25 Avenue des Martyrs, 38042 Grenoble (France)

    2014-10-15

    The influence of free carriers on the ground state of the exciton at zero magnetic field in a quasi-two-dimensional quantum well that contains a gas of free electrons is considered in the framework of the random phase approximation. The effects of the exciton–charge-density interaction and the inelastic scattering processes due to the electron–electron exchange interaction are taken into account. The effect of phase-space filling is considered using an approximate approach. The results of the calculation are compared with the experimental data. - Highlights: • We discussed the effect of free carriers on the exciton ground state in quantum wells. • The processes of exciton–electron scattering become the most important for excitons in doped QWs. • The direct Coulomb scattering can be neglected. • The most important becomes the exchange inelastic exciton–electron scattering.

  5. Time-resolved photoluminescence study of excitonic relaxation in one-dimensional systems

    Science.gov (United States)

    Tanino, H.; Rühle, W. W.; Takahashi, K.

    1988-12-01

    Self-trapped exciton luminescence of quasi-one-dimensional (1D) halogen-bridged mixed-valence platinum complexes [Pt(II) (EA)4][Pt(IV)Cl2(EA)4] Cl4.4H2O (EA=ethylamine) and [Pt(II)(en)2] [Pt(IV)Cl2(en)2](ClO4)4 (en=1,2-diaminoethane) are studied by time-resolved photoluminescence experiments. The lifetimes of the luminescence of self-trapped exciton are exceptionally short, of the order of 100 psec. We interpret the short lifetime by a ``giant oscillator strength'' caused by a strong coupling between the electron and hole of the 1D charge transfer exciton and an extended polaronlike character of the 1D state. The lifetimes of the broad luminescence and of the resonant Raman lines during the barrier-free relaxation process are both faster than 7 psec.

  6. Singlet-triplet annihilation limits exciton yield in poly(3-hexylthiophene)

    CERN Document Server

    Steiner, Florian; Lupton, John M

    2014-01-01

    Control of chain length and morphology in combination with single-molecule spectroscopy techniques provide a comprehensive photophysical picture of excited-state losses in the prototypical conjugated polymer poly(3-hexylthiophene) (P3HT). A universal self-quenching mechanism is revealed, based on singlet-triplet exciton annihilation, which accounts for the dramatic loss in fluorescence quantum yield of a single P3HT chain between its solution (unfolded) and bulk-like (folded) state. Triplet excitons fundamentally limit the fluorescence of organic photovoltaic materials, which impacts on the conversion of singlet excitons to separated charge carriers, decreasing the efficiency of energy harvesting at high excitation densities. Interexcitonic interactions are so effective that a single P3HT chain of >100 kDa weight behaves like a two-level system, exhibiting perfect photon-antibunching.

  7. Excitonic polaritons of zinc diarsenide single crystals

    Science.gov (United States)

    Syrbu, N. N.; Stamov, I. G.; Zalamai, V. V.; Dorogan, A.

    2017-02-01

    Excitonic polaritons of ZnAs2 single crystals had been investigated. Parameters of singlet excitons with D2bar(z) symmetry and orthoexcitons 2D1bar(y)+D2bar(x) had been determined. Spectral dependencies of ordinary and extraordinary dispersion of refractive index had been calculated using interferential reflection and transmittance spectra. It was shown, that A excitonic series were due to hole (V1) and electron (C1) bands. The values of effective masses of electrons (mc*=0.10 m0) and holes (mv1*=0.89 m0) had been estimated. It was revealed that the hole mass mv1* changes from 1.03 m0 to 0.55 m0 at temperature increasing from 10 K up to 230 K and that the electron mass mc* does not depend on temperature. The integral absorption A (eV cm-1) of the states n=1, 2 and 3 of D2bar(z) excitons depends on the An≈n-3 equality, which it is characteristic for S-type excitonic functions. Temperature dependences of the integral absorption of ground states for D2bar(z) and D2bar(D) excitons differ. The ground states of B and C excitons formed by V3 - C1 and V4 - C1 bands and its parameters had been determined.

  8. Instantaneous Rayleigh scattering from excitons localized in monolayer islands

    DEFF Research Database (Denmark)

    Langbein, Wolfgang; Leosson, Kristjan; Jensen, Jacob Riis;

    2000-01-01

    We show that the initial dynamics of Rayleigh scattering from excitons in quantum wells can be either instantaneous or delayed, depending on the exciton ensemble studied. For excitation of the entire exciton resonance, a finite rise time given by the inverse inhomogeneous broadening: of the exciton...... resonance is observed. Instead, when exciting only a subsystem of the exciton resonance, in our case excitons localized in quantum well regions of a specific monolayer thickness, the rise has an instantaneous component. This is due to the spatial nonuniformity of the initially excited exciton polarization...

  9. Efficiency of Blue Organic Light-emitting Diodes Enhanced by Employing an Exciton Feedback Layer

    Institute of Scientific and Technical Information of China (English)

    Qian-Qian Yu; Xu Zhang; Jing-Xuan Bi; Guan-Ting Liu; Qi-Wen Zhang; Xiao-Ming Wu; Yu-Lin Hua

    2016-01-01

    We report that a novel exciton feedback effect is observed by introducing the bis(2-methyl-8-quinolinolato)(4-phenylphenolato)aluminum (BAlq) inserted between the emitting layer (EML) and the electron transporting layer in blue organic light emitting diodes.As an exciton feedback layer (EFL),the BAlq does not act as a traditional hole blocking effect.The design of this kind of device structure can greatly reduce excitons' quenching due to accumulated space charge at the exciton formation interface.Meanwhile,the non-radiative energy transfer from EFL to the EML can also be utilized to enhance the excitons' formation,which is confirmed by the test of photolumimescent transient lifetime decay and electroluminescence enhancement of these devices.Accordingly,the optimal device presents the improved performances with the maximum current e~ciency of 4.2 cd/A and the luminance of 24600cd/m2,which are about 1.45 times and 1.75 times higher than those of device A (control device) without the EFL,respectively.Simultaneously,the device shows an excellent color stability with a tiny offset of the CIE coordinates (Ax =±0.003,Ay =±0.004) and a relatively lower efficiency roll-off of 26.2% under the driving voltage varying from 3 V to 10 V.

  10. Crystalline Nanoporous Frameworks: a Nanolaboratory for Probing Excitonic Device Concepts.

    Energy Technology Data Exchange (ETDEWEB)

    Allendorf, Mark D.; Azoulay, Jason; Ford, Alexandra Caroline; Foster, Michael E.; El Gabaly Marquez, Farid; Leonard, Francois Leonard; Leong-Hau, Kirsty; Stavila, Vitalie; Talin, Albert Alec; Wong, Brian M.; Brumbach, Michael T.; Van Gough, D.; Lambert, Timothy N.; Rodriguez, Mark A.; Spoerke, Erik David; Wheeler, David Roger; Deaton, Joseph C.; Centrone, Andrea; Haney, Paul; Kinney, R.; Szalai, Veronika; Yoon, Heayoung P.

    2014-09-01

    Electro-optical organic materials hold great promise for the development of high-efficiency devices based on exciton formation and dissociation, such as organic photovoltaics (OPV) and organic light-emitting devices (OLEDs). However, the external quantum efficiency (EQE) of both OPV and OLEDs must be improved to make these technologies economical. Efficiency rolloff in OLEDs and inability to control morphology at key OPV interfaces both reduce EQE. Only by creating materials that allow manipulation and control of the intimate assembly and communication between various nanoscale excitonic components can we hope to first understand and then engineer the system to allow these materials to reach their potential. The aims of this proposal are to: 1) develop a paradigm-changing platform for probing excitonic processes composed of Crystalline Nanoporous Frameworks (CNFs) infiltrated with secondary materials (such as a complimentary semiconductor); 2) use them to probe fundamental aspects of excitonic processes; and 3) create prototype OPVs and OLEDs using infiltrated CNF as active device components. These functional platforms will allow detailed control of key interactions at the nanoscale, overcoming the disorder and limited synthetic control inherent in conventional organic materials. CNFs are revolutionary inorganic-organic hybrid materials boasting unmatched synthetic flexibility that allow tuning of chemical, geometric, electrical, and light absorption/generation properties. For example, bandgap engineering is feasible and polyaromatic linkers provide tunable photon antennae; rigid 1-5 nm pores provide an oriented, intimate host for triplet emitters (to improve light emission in OLEDs) or secondary semiconducting polymers (creating a charge-separation interface in OPV). These atomically engineered, ordered structures will enable critical fundamental questions to be answered concerning charge transport, nanoscale interfaces, and exciton behavior that are inaccessible

  11. Daylight-driven photocatalytic degradation of ionic dyes with negatively surface-charged In{sub 2}S{sub 3} nanoflowers: dye charge-dependent roles of reactive species

    Energy Technology Data Exchange (ETDEWEB)

    Ge, Suxiang [Xuchang University, Key Laboratory of Micro-Nano Materials for Energy Storage and Conversion of Henan Province, Institute of Surface Micro and Nano Materials, and School of Chemistry and Chemical Engineering (China); Cai, Lejuan, E-mail: 494169965@qq.com [Central China Normal University, Key Laboratory of Pesticide and Chemical Biology of Ministry of Education, College of Chemistry (China); Li, Dapeng, E-mail: lidapengabc@126.com; Fa, Wenjun; Zhang, Yange; Zheng, Zhi [Xuchang University, Key Laboratory of Micro-Nano Materials for Energy Storage and Conversion of Henan Province, Institute of Surface Micro and Nano Materials, and School of Chemistry and Chemical Engineering (China)

    2015-12-15

    Even though dye degradation is a successful application of semiconductor photocatalysis, the roles of reactive species in dye degradation have not received adequate attention. In this study, we systematically investigated the degradation of two cationic dyes (rhodamine B and methylene blue) and two anionic dyes (methyl orange and orange G) over negatively surface-charged In{sub 2}S{sub 3} nanoflowers synthesized at 80 °C under indoor daylight lamp irradiation. It is notable to find In{sub 2}S{sub 3} nanoflowers were more stable in anionic dyes degradation compared to that in cationic dyes removal. The active species trapping experiments indicated photogenerated electrons were mainly responsible for cationic dyes degradation, but holes were more important in anionic dyes degradation. A surface-charge-dependent role of reactive species in ionic dye degradation was proposed for revealing such interesting phenomenon. This study would provide a new insight for preparing highly efficient daylight-driven photocatalyst for ionic dyes degradation.

  12. Ground-state oxygen holes and the metal-insulator transition in the negative charge-transfer rare-earth nickelates

    Science.gov (United States)

    Bisogni, Valentina; Catalano, Sara; Green, Robert J.; Gibert, Marta; Scherwitzl, Raoul; Huang, Yaobo; Strocov, Vladimir N.; Zubko, Pavlo; Balandeh, Shadi; Triscone, Jean-Marc; Sawatzky, George; Schmitt, Thorsten

    2016-10-01

    The metal-insulator transition and the intriguing physical properties of rare-earth perovskite nickelates have attracted considerable attention in recent years. Nonetheless, a complete understanding of these materials remains elusive. Here we combine X-ray absorption and resonant inelastic X-ray scattering (RIXS) spectroscopies to resolve important aspects of the complex electronic structure of rare-earth nickelates, taking NdNiO3 thin film as representative example. The unusual coexistence of bound and continuum excitations observed in the RIXS spectra provides strong evidence for abundant oxygen holes in the ground state of these materials. Using cluster calculations and Anderson impurity model interpretation, we show that distinct spectral signatures arise from a Ni 3d8 configuration along with holes in the oxygen 2p valence band, confirming suggestions that these materials do not obey a conventional positive charge-transfer picture, but instead exhibit a negative charge-transfer energy in line with recent models interpreting the metal-insulator transition in terms of bond disproportionation.

  13. Optical nutation in the exciton range of spectrum

    Energy Technology Data Exchange (ETDEWEB)

    Khadzhi, P. I. [Academy of Sciences of Moldova, Institute of Applied Physics (Moldova, Republic of); Vasiliev, V. V., E-mail: vasscorp@mail.ru [Taras Shevchenko Transnistria State University (Moldova, Republic of)

    2013-08-15

    Optical nutation in the exciton range of spectrum is studied in the mean field approximation taking into account exciton-photon and elastic exciton-exciton interactions. It is shown that the features of nutation development are determined by the initial exciton and photon densities, the resonance detuning, the nonlinearity parameter, and the initial phase difference. For nonzero initial exciton and photon concentrations, three regimes of temporal evolution of excitons and photons exist: periodic conversion of excitons to photons and vice versa, aperiodic conversion of photons to excitons, and the rest regime. In the rest regime, the initial exciton and photon densities are nonzero and do not change with time. The oscillation amplitudes and periods of particle densities determined by the system parameters are found. The exciton self-trapping and photon trapping appearing in the system at threshold values of the nonlinearity parameter were predicted. As this parameter increases, the oscillation amplitudes of the exciton and photon densities sharply change at the critical value of the nonlinearity parameter. These two phenomena are shown to be caused by the elastic exciton-exciton interaction, resulting in the dynamic concentration shift of the exciton level.

  14. Enormous excitonic effects in bulk, mono- and bi- layers of cuprous halides using many-body perturbation technique

    Science.gov (United States)

    Azhikodan, Dilna; Nautiyal, Tashi

    2017-10-01

    Cuprous halides (CuX with X = Cl, Br, I), intensely studied about four decades ago by experimentalists for excitons, are again drawing attention of researchers recently. Potential of cuprous halide systems for device applications has not yet been fully explored. We go beyond the one-particle picture to capture the two-particle physics (electron-hole interaction to form excitons). We have deployed the full tool kit of many-body perturbation technique, GW approximation + Bethe Salpeter equation, to unfurl the rich excitonic physics of the bulk as well as layers of CuX. The negative spin-orbit contribution at the valence band top in CuCl, compared to CuBr and CuI, is in good agreement with experiments. We note that CuX have exceptionally strong excitons, defying the linear fit (between the excitonic binding energy and band gap) encompassing many semiconductors. The mono- and bi- layers of cuprous halides are predicted to be rich in excitons, with exceptionally large binding energies and the resonance energies in UV/visible region. Hence this work projects CuX layers as good candidates for optoelectronic applications. With advancement of technology, we look forward to experimental realization of CuX layers and harnessing of their rich excitonic potential.

  15. Can disorder enhance incoherent exciton diffusion?

    CERN Document Server

    Lee, Elizabeth M Y; Willard, Adam P

    2015-01-01

    Recent experiments aimed at probing the dynamics of excitons have revealed that semiconducting films composed of disordered molecular subunits, unlike expectations for their perfectly ordered counterparts, can exhibit a time-dependent diffusivity in which the effective early time diffusion constant is larger than that of the steady state. This observation has led to speculation about what role, if any, microscopic disorder may play in enhancing exciton transport properties. In this article, we present the results of a model study aimed at addressing this point. Specifically, we present a general model, based upon F\\"orster theory, for incoherent exciton diffusion in a material composed of independent molecular subunits with static energetic disorder. Energetic disorder leads to heterogeneity in molecule-to-molecule transition rates which we demonstrate has two important consequences related to exciton transport. First, the distribution of local site-specific diffusivity is broadened in a manner that results i...

  16. Exciton absorption in narrow armchair graphene nanoribbons

    Science.gov (United States)

    Monozon, B. S.; Schmelcher, P.

    2016-11-01

    We develop an analytical approach to the exciton optical absorption for narrow gap armchair graphene nanoribbons (AGNR). We focus on the regime of dominant size quantization in combination with the attractive electron-hole interaction. An adiabatic separation of slow and fast motions leads via the two-body Dirac equation to the isolated and coupled subband approximations. Discrete and continuous exciton states are in general coupled and form quasi-Rydberg series of purely discrete and resonance type character. The corresponding oscillator strengths and widths are derived. We show that the exciton peaks are blue-shifted, become broader and increase in magnitude upon narrowing the ribbon. At the edge of a subband the singularity related to the 1D density of states is transformed into finite absorption via the presence of the exciton. Our analytical results are in good agreement with those obtained by other methods including numerical approaches. Estimates of the expected experimental values are provided for realistic AGNR.

  17. Quantum-dot excitons in nanostructured environments

    DEFF Research Database (Denmark)

    Hvam, Jørn Märcher; Stobbe, Søren; Lodahl, Peter

    2011-01-01

    The interaction between light and quantum-dot (QD) excitons is strongly influenced by the environment in which the QD is placed. We have investigated the interaction by measuring the time-resolved spontaneous-emission rate of QD excitons in different nanostructured environments. Thereby, we have...... is demonstrated and the influence of disorder is discussed. The findings have a strong bearing on future nanophotonic devices....

  18. Quantum-dot excitons in nanostructured environments

    DEFF Research Database (Denmark)

    Hvam, Jørn Märcher; Stobbe, Søren; Lodahl, Peter

    2010-01-01

    The interaction between light and quantum-dot (QD) excitons is strongly influenced by the environment in which the QD is placed. We have investigated the interaction by measuring the time-resolved spontaneous-emission rate of QD excitons in different nanostructured environments. Thereby, we have...... is demonstrated and the influence of disorder is discussed. The findings have a strong bearing on future nanophotonic devices....

  19. Beneficial effects of activated carbon additives on the performance of negative lead-acid battery electrode for high-rate partial-state-of-charge operation

    Science.gov (United States)

    Xiang, Jiayuan; Ding, Ping; Zhang, Hao; Wu, Xianzhang; Chen, Jian; Yang, Yusheng

    2013-11-01

    Experiments are made with negative electrode of 2 V cell and 12 V lead-acid battery doped with typical activated carbon additives. It turns out that the negative electrode containing tens-of-micron-sized carbon particles in NAM exhibits markedly increased HRPSoC cycle life than the one containing carbon particles with much smaller size of several microns or the one containing no activated carbon. The improved performance is mainly attributed to the optimized NAM microstructure and the enhanced electrode reaction kinetics by introducing appropriate activated carbon. The beneficial effects can be briefly summarized from three aspects. First, activated carbon acts as new porous-skeleton builder to increase the porosity and active surface of NAM, and thus facilitates the electrolyte diffusion from surface to inner and provides more sites for crystallization/dissolution of lead sulfate; second, activated carbon plays the role of electrolyte supplier to provide sufficient H2SO4 in the inner of plate when the diffusion of H2SO4 from plate surface cannot keep pace of the electrode reaction; Third, activated carbon acts as capacitive buffer to absorb excess charge current which would otherwise lead to insufficient NAM conversion and hydrogen evolution.

  20. Excitonic nonlinearities in single-wall carbon nanotubes

    Energy Technology Data Exchange (ETDEWEB)

    Nguyen, D.T.; Voisin, C.; Roussignol, P. [Laboratoire Pierre Aigrain, Ecole Normale Superieure, UPMC, Universite Paris Diderot, CNRS UMR8551, Paris (France); Roquelet, C.; Lauret, J.S. [Laboratoire de Photonique Quantique et Moleculaire de l' Ecole Normale Superieure de Cachan (France); Cassabois, G. [Laboratoire Pierre Aigrain, Ecole Normale Superieure, UPMC, Universite Paris Diderot, CNRS UMR8551, Paris (France); Laboratoire Charles Coulomb, UMR5221, Universite Montpellier 2, Montpellier (France); CNRS, Laboratoire Charles Coulomb, UMR5221, Montpellier (France)

    2012-05-15

    Excitons are composite bosons that allow a fair description of the optical properties in solid state systems. The quantum confinement in nanostructures enhances the excitonic effects and impacts the exciton-exciton interactions, which tailor the performances of classical and quantum optoelectronic devices, such as lasers or single-photon emitters. The excitonic nonlinearities exhibit significant differences between organic and inorganic compounds. Tightly bound Frenkel excitons in molecular crystals are for instance affected by an efficient exciton-exciton annihilation (EEA). This Auger process also governs the population relaxation dynamics in carbon nanotubes that share many physical properties with organic materials. Here, we show that this similarity breaks down for the excitonic decoherence in carbon nanotubes. Original nonlinear spectral-hole burning experiments bring evidence of pure dephasing induced by exciton-exciton scattering (EES) in the k-space. This mechanism controls the exciton collision-induced broadening, as for Wannier excitons in inorganic semiconductors. We demonstrate that this singular behavior originates from the intrinsic one-dimensionality of excitons in carbon nanotubes, which display unique hybrid features of organic and inorganic systems. (Copyright copyright 2012 WILEY-VCH Verlag GmbH and Co. KGaA, Weinheim)

  1. Low-Energy Charge and Spin Dynamics in Quantum Confined Systems

    Science.gov (United States)

    Rice, William D.

    Condensed matter systems exhibit a variety of dynamical phenomena at low energy scales, from gigahertz (GHz) to terahertz (THz) frequencies in particular, arising from complex interplay between charge, spin, and lattice. A large number of collective and elementary excitations in solids occur in this frequency range, which are further modified and enriched by scattering, interactions, and disorder. Recent advancements in spectroscopic methods for probing low-energy dynamics allow us to investigate novel aspects of charge and spin dynamics in solids. In this dissertation work, we used direct current (DC) conductivity, GHz, THz, and mid-infrared (MIR) techniques to provide significant new insights into interaction and disorder effects in low-dimensional systems. Specifically, we have studied temperature-dependent magnetoresistance (MR) and electron spin resonance (ESR) in single-wall carbon nanotubes (SWCNTs), intra-exciton scattering in InGaAs quantum wells, and high-field MIR-induced band gaps in graphene. Temperature-dependent resistance and MR were measured in an ensemble of SWCNTs from 0.3 to 350 K. The resistance temperature behavior followed a 3D variable range hopping (VRH) behavior from 0.3 to ˜100 K. A positive MR was observed at temperatures above 25 K and could be fit with a spin-dependent VRH model; negative MR was seen at low temperatures. In the GHz regime, the ESR linewidth for SWCNTs was observed to narrow by as much as 50% as the temperature was increased from 3 to 300 K, a phenomenon known as motional narrowing, suggesting that we are detecting the ESR of hopping spins. From the linewidth change versus temperature, we find the hopping frequency to be 285 GHz. For excitons in InGaAs quantum wells, we demonstrate the manipulation of intra-excitonic populations using intense, narrow-band THz pulses. The THz radiation temporarily quenches the 1s emission, which is then followed by an enhancement and subsequent decay of 2s emission. After the quenching

  2. Exciton correlations and input-output relations in non-equilibrium exciton superfluids

    Energy Technology Data Exchange (ETDEWEB)

    Ye, Jinwu, E-mail: jy306@ccs.msstate.edu [Key Laboratory of Terahertz Optoelectronics, Ministry of Education, Department of Physics, Capital Normal University, Beijing 100048 (China); Department of Physics and Astronomy, Mississippi State University, MS 39762 (United States); Sun, Fadi; Yu, Yi-Xiang [Department of Physics and Astronomy, Mississippi State University, MS 39762 (United States); Institute of Physics, Chinese Academy of Sciences, Beijing, 100080 (China); Liu, Wuming [Institute of Physics, Chinese Academy of Sciences, Beijing, 100080 (China)

    2013-02-15

    The photoluminescence (PL) measurements on photons and the transport measurements on excitons are the two types of independent and complementary detection tools to search for possible exciton superfluids in electron-hole semi-conductor bilayer systems. In fact, it was believed that the transport measurements can provide more direct evidences on superfluids than the spectroscopic measurements. It is important to establish the relations between the two kinds of measurements. In this paper, using quantum Heisenberg-Langevin equations, we establish such a connection by calculating various exciton correlation functions in the putative exciton superfluids. These correlation functions include both normal and anomalous greater, lesser, advanced, retarded, and time-ordered exciton Green functions and also various two exciton correlation functions. We also evaluate the corresponding normal and anomalous spectral weights and the Keldysh distribution functions. We stress the violations of the fluctuation and dissipation theorem among these various exciton correlation functions in the non-equilibrium exciton superfluids. We also explore the input-output relations between various exciton correlation functions and those of emitted photons such as the angle resolved photon power spectrum, phase sensitive two mode squeezing spectrum and two photon correlations. Applications to possible superfluids in the exciton-polariton systems are also mentioned. For a comparison, using conventional imaginary time formalism, we also calculate all the exciton correlation functions in an equilibrium dissipative exciton superfluid in the electron-electron coupled semi-conductor bilayers at the quantum Hall regime at the total filling factor {nu}{sub T}=1. We stress the analogies and also important differences between the correlations functions in the two exciton superfluid systems. - Highlights: Black-Right-Pointing-Pointer Establish the relations between photoluminescence and transport

  3. Exciton interference revealed by energy dependent exciton transfer rate for ring-structured molecular systems

    Energy Technology Data Exchange (ETDEWEB)

    Yan, Yun-An, E-mail: yunan@gznc.edu.cn [Guizhou Provincial Key Laboratory of Computational Nanomaterial Science, Guizhou Education University, Guiyang, Guizhou 550018 (China)

    2016-01-14

    The quantum interference is an intrinsic phenomenon in quantum physics for photon and massive quantum particles. In principle, the quantum interference may also occur with quasi-particles, such as the exciton. In this study, we show how the exciton quantum interference can be significant in aggregates through theoretical simulations with hierarchical equations of motion. The systems under investigation are generalized donor-bridge-acceptor model aggregates with the donor consisting of six homogeneous sites assuming the nearest neighbor coupling. For the models with single-path bridge, the exciton transfer time only shows a weak excitation energy dependence. But models with double-path bridge have a new short transfer time scale and the excitation energy dependence of the exciton transfer time assumes clear peak structure which is detectable with today’s nonlinear spectroscopy. This abnormality is attributed to the exciton quantum interference and the condition for a clear observation in experiment is also explored.

  4. Exciton Absorption Spectra by Linear Response Methods: Application to Conjugated Polymers.

    Science.gov (United States)

    Mosquera, Martín A; Jackson, Nicholas E; Fauvell, Thomas J; Kelley, Matthew S; Chen, Lin X; Schatz, George C; Ratner, Mark A

    2017-03-15

    The theoretical description of the time-evolution of excitons requires, as an initial step, the calculation of their spectra, which has been inaccessible to most users due to the high computational scaling of conventional algorithms and accuracy issues caused by common density functionals. Previously (J. Chem. Phys. 2016, 144, 204105), we developed a simple method that resolves these issues. Our scheme is based on a two-step calculation in which a linear-response TDDFT calculation is used to generate orbitals perturbed by the excitonic state, and then a second linear-response TDDFT calculation is used to determine the spectrum of excitations relative to the excitonic state. Herein, we apply this theory to study near-infrared absorption spectra of excitons in oligomers of the ubiquitous conjugated polymers poly(3-hexylthiophene) (P3HT), poly(2-methoxy-5-(2-ethylhexyloxy)-1,4-phenylenevinylene) (MEH-PPV), and poly(benzodithiophene-thieno[3,4-b]thiophene) (PTB7). For P3HT and MEH-PPV oligomers, the calculated intense absorption bands converge at the longest wavelengths for 10 monomer units, and show strong consistency with experimental measurements. The calculations confirm that the exciton spectral features in MEH-PPV overlap with those of the bipolaron formation. In addition, our calculations identify the exciton absorption bands in transient absorption spectra measured by our group for oligomers (1, 2, and 3 units) of PTB7. For all of the cases studied, we report the dominant orbital excitations contributing to the optically active excited state-excited state transitions, and suggest a simple rule to identify absorption peaks at the longest wavelengths. We suggest our methodology could be considered for further developments in theoretical transient spectroscopy to include nonadiabatic effects, coherences, and to describe the formation of species such as charge-transfer states and polaron pairs.

  5. Attosecond Electron Processes in Materials: Excitons, Plasmons, and Charge Dynamics

    Science.gov (United States)

    2015-05-19

    plasmon electric field will introduce several features in both velocity map images ( VMI ) and time-of-flight (TOF) photoelectron velocity traces that...dipole moment of 80 nm silver nanospheres excited by a resonant 5-fs, 376 nm laser pulse using VMI (a) and ToF (b) techniques. (a) Plot of the...dynamical dipole moment amplitude (green, right axis). The analysis showed that conventional VMI analysis by means of Legendre polynomial decomposition is

  6. Excitonic polaritons of zinc diarsenide single crystals

    Energy Technology Data Exchange (ETDEWEB)

    Syrbu, N.N., E-mail: sirbunn@yahoo.com [Technical University of Moldova, Chisinau, Republic of Moldova (Moldova, Republic of); Stamov, I.G. [T.G. Shevchenko State University of Pridnestrovie, Tiraspol, Republic of Moldova (Moldova, Republic of); Zalamai, V.V. [Institute of Applied Physics, Academy of Sciences of Moldova, Chisinau, Republic of Moldova (Moldova, Republic of); Dorogan, A. [Technical University of Moldova, Chisinau, Republic of Moldova (Moldova, Republic of)

    2017-02-01

    Excitonic polaritons of ZnAs{sub 2} single crystals had been investigated. Parameters of singlet excitons with Г{sub 2}¯(z) symmetry and orthoexcitons 2Г{sub 1}¯(y)+Г{sub 2}¯(x) had been determined. Spectral dependencies of ordinary and extraordinary dispersion of refractive index had been calculated using interferential reflection and transmittance spectra. It was shown, that A excitonic series were due to hole (V{sub 1}) and electron (C{sub 1}) bands. The values of effective masses of electrons (m{sub c}{sup *}=0.10 m{sub 0}) and holes (m{sub v1}{sup *}=0.89 m{sub 0}) had been estimated. It was revealed that the hole mass m{sub v1}{sup *} changes from 1.03 m{sub 0} to 0.55 m{sub 0} at temperature increasing from 10 K up to 230 K and that the electron mass m{sub c}{sup *} does not depend on temperature. The integral absorption A (eV cm{sup −1}) of the states n=1, 2 and 3 of Г{sub 2}¯(z) excitons depends on the A{sub n}≈n{sup −3} equality, which it is characteristic for S-type excitonic functions. Temperature dependences of the integral absorption of ground states for Г{sub 2}¯(z) and Г{sub 2}¯(Ñ…) excitons differ. The ground states of B and C excitons formed by V{sub 3} – C{sub 1} and V{sub 4} – C{sub 1} bands and its parameters had been determined.

  7. Negatively charged Ir(iii) cyclometalated complexes containing a chelating bis-tetrazolato ligand: synthesis, photophysics and the study of reactivity with electrophiles.

    Science.gov (United States)

    Fiorini, Valentina; Zacchini, Stefano; Raiteri, Paolo; Mazzoni, Rita; Zanotti, Valerio; Massi, Massimiliano; Stagni, Stefano

    2016-08-09

    The bis-tetrazolate dianion [1,2 BTB](2-), which is the deprotonated form of 1,2 bis-(1H-tetrazol-5-yl)benzene [1,2-H2BTB], is for the first time exploited as an ancillary N^N ligand for negatively charged [Ir(C^N)2(N^N)](-)-type complexes, where C^N is represented by cyclometalated 2-phenylpyridine (ppy) or 2-(2,4-difluorophenyl)pyridine (F2ppy). The new Ir(iii) complexes [Ir(ppy)2(1,2 BTB)]- and [Ir(F2ppy)2(1,2 BTB)]- have been fully characterised and the analysis of the X-ray structure of [Ir(ppy)2(1,2 BTB)]- confirmed the coordination of the [1,2 BTB](2-) dianion in a bis chelated fashion through the N-atoms adjacent to each of the tetrazolic carbons. Both of the new anionic Ir(iii) complexes displayed phosphorescence in the visible region, with intense sky-blue (λmax = 460-490 nm) or aqua (λmax = 490-520 nm) emissions originating from [Ir(F2ppy)2(1,2 BTB)]- and [Ir(ppy)2(1,2 BTB)]-, respectively. In comparison with our very recent examples of anionic Ir(iii)tetrazolate cyclometalates, the new Ir(iii) tris chelate complexes [Ir(F2ppy)2(1,2 BTB)]- and [Ir(ppy)2(1,2 BTB)]-, display an improved robustness, allowing the study of their reactivity toward the addition of electrophiles such as H(+) and CH3(+). In all cases, the electrophilic attacks occurred at the coordinated tetrazolate rings, involving the reversible - by a protonation deprotonation mechanism - or permanent - upon addition of a methyl moiety - switching of their global net charge from negative to positive and, in particular, the concomitant variation of their photoluminescence output. The combination of the anionic complexes [Ir(F2ppy)2(1,2 BTB)]- or [Ir(ppy)2(1,2 BTB)]- with a deep red emitting (λmax = 686 nm) cationic Ir(iii) tetrazole complex such as [IrTPYZ-Me]+, where TPYZ-Me is 2-(2-methyl-2H-tetrazol-5-yl)pyrazine, gave rise to two fully Ir(iii)-based soft salts capable of displaying additive and O2-sensitive emission colours, with an almost pure white light obtained by the appropriate

  8. Direct measurement of exciton valley coherence in monolayer WSe2

    KAUST Repository

    Hao, Kai

    2016-02-29

    In crystals, energy band extrema in momentum space can be identified by a valley index. The internal quantum degree of freedom associated with valley pseudospin indices can act as a useful information carrier, analogous to electronic charge or spin. Interest in valleytronics has been revived in recent years following the discovery of atomically thin materials such as graphene and transition metal dichalcogenides. However, the valley coherence time—a crucial quantity for valley pseudospin manipulation—is difficult to directly probe. In this work, we use two-dimensional coherent spectroscopy to resonantly generate and detect valley coherence of excitons (Coulomb-bound electron–hole pairs) in monolayer WSe2 (refs ,). The imposed valley coherence persists for approximately one hundred femtoseconds. We propose that the electron–hole exchange interaction provides an important decoherence mechanism in addition to exciton population recombination. This work provides critical insight into the requirements and strategies for optical manipulation of the valley pseudospin for future valleytronics applications.

  9. Exciton-polaron quenching in organic thin-film transistors studied by fluorescence lifetime imaging microscopy

    DEFF Research Database (Denmark)

    Jensen, Per Baunegaard With; Leißner, Till; Osadnik, Andreas

    Organic semiconductors show great potential in electronic and optical applications. However, a major challenge is the degradation of the semiconductor materials that cause a reduction in device performance. Here, we present our investigations of Organic Thin Film Transistors (OTFT) based...... that correlates with the local charge density indicates a pronounced exciton quenching by the injected charges. Subsequent FLIM measurements on previously biased OTFT devices show a general decrease in fluorescence lifetime suggesting degradation of the organic semiconductor. This is correlated with the results...... on the material 5,5-bis(naphthyl)-2,20-bithiophene (NaT2). These types of OTFT have previously been shown to have light emitting properties. Fluorescence Lifetime Imaging Microscopy (FLIM) has been used to investigate the exciton-polaron quenching in biased OTFTs. A clear reduction in fluorescence lifetime...

  10. Extraction of negative charges from an ion source: Transition from an electron repelling to an electron attracting plasma close to the extraction surface

    Science.gov (United States)

    Wimmer, Christian; Fantz, Ursel

    2016-08-01

    Large-scale sources for negative hydrogen ions, capable of delivering an extracted ion current of several ten amperes, are a key component of the neutral beam injection system of the upcoming ITER fusion device. Since the created heat load of the inevitably co-extracted electrons after magnetic separation from the extracted beam limits their tolerable amount, special care must be taken for the reduction of co-extracted electrons—in particular, in deuterium operation, where the larger amount of co-extracted electrons often limits the source performance. By biasing the plasma grid (PG, first grid of the extraction system) positively with respect to the source body, the plasma sheath in front of the PG can be changed from an electron repelling towards an electron attracting sheath. In this way, the flux of charged particles onto the PG can be varied, thus changing the bias current and inverse to it the amount of co-extracted electrons. The PG bias affects also the flux of surface-produced H - towards the plasma volume as well as the plasma symmetry in front of the plasma grid, strongly influenced by an E → × B → drift. The influence of varying PG sheath potential profile on the plasma drift, the negative hydrogen ion density, and the source performance at the prototype H - source is presented, comparing hydrogen and deuterium operation. The transition in the PG sheath profile takes place in both isotopes, with a minimum of co-extracted electrons formed in case of the electron attracting PG sheath. The co-extracted electron density in deuterium operation is higher than in hydrogen operation, which is accompanied by an increased plasma density in deuterium.

  11. Multiple exciton generation in nanocrystalline solar cells (Conference Presentation)

    Science.gov (United States)

    Boehm, Marcus; Davis, Nathaniel; Greenham, Neil C.

    2016-09-01

    Multiple exciton generation (MEG) - a process in which multiple charge-carrier pairs are generated from a single optical excitation - is a promising way to improve the photocurrent in photovoltaic devices and offers the potential of breaking the Shockley-Queisser limit. It remains, however, challenging to harvest charge-carrier pairs generated by MEG in working solar cells. Initial yields of additional carrier pairs may be reduced due to ultra-fast intraband relaxation processes, which compete with MEG at early times. Quantum dots of materials, which display reduced carrier cooling rates (e.g. PbTe)[1] or one-dimensional nanostructures (e.g. nano rods)[2] which accelerate the carrier multiplication process are therefore promising candidates to increase the impact of MEG in photovoltaic devices. Here we show that both theorised strategies can lead to solar cells, which produce extractable charge carrier pairs with an external quantum efficiency above 120%, and we estimate an internal quantum efficiency exceeding 150%. Resolving the charge carrier kinetics on the ultra-fast timescale with pump-probe transient absorption and pump-push-photocurrent measurements, we identify a delayed cooling effect above the experimentally- determined threshold energy for MEG[1].

  12. Disinfection of Escherichia coli Gram negative bacteria using surface modified TiO2: optimization of Ag metallization and depiction of charge transfer mechanism.

    Science.gov (United States)

    Gomathi Devi, LakshmipathiNaik; Nagaraj, Basavalingaiah

    2014-01-01

    The antibacterial activity of silver deposited TiO2 (Ag-TiO2 ) against Gram negative Escherichia coli bacteria was investigated by varying the Ag metal content from 0.10 to 0.50% on the surface of TiO2 . Ag depositions by the photoreduction method were found to be stable. Surface silver metallization was confirmed by EDAX and XPS studies. Photoluminescence studies show that the charge carrier recombination is less for 0.1% Ag-TiO2 and this catalyst shows superior bactericidal activity under solar light irradiation compared to Sol gel TiO2 (SG-TiO2 ) due to the surface plasmon effect. The energy levels of deposited Ag are dependent on the Ag content and it varies from -4.64 eV to -1.30 eV with respect to the vacuum energy level based on atomic silver to bulk silver deposits. The ability of electron transfer from Ag deposit to O2 depends on the position of the energy levels. The 0.25% and 0.50% Ag depositions showed detrimental effect on bactericidal activity due to the mismatch of energy levels. The effect of the EROS (External generation of the Reactive Oxygen Species by 0.1% Ag-TiO2 ) and IROS (Interior generation of Reactive Oxygen Species within the bacteria) on the bactericidal inactivation is discussed in detail.

  13. Measurement of negatively charged pion spectra in inelastic p+p interactions at p{sub lab} = 20, 31, 40, 80 and 158 GeV/c

    Energy Technology Data Exchange (ETDEWEB)

    Abgrall, N.; Blondel, A.; Bravar, A.; Debieux, S.; Haesler, A.; Korzenev, A.; Murphy, S.; Ravonel, M. [University of Geneva, Geneva (Switzerland); Aduszkiewicz, A.; Dominik, W.; Kielczewska, D.; Kirejczyk, M.; Matulewicz, T.; Posiadala, M.; Skrzypczak, E. [University of Warsaw, Faculty of Physics, Warsaw (Poland); Ali, Y.; Brzychczyk, J.; Majka, Z.; Marcinek, A.; Planeta, R.; Staszel, P.; Wyszynski, O. [Jagiellonian University, Cracow (Poland); Anticic, T.; Kadija, K.; Susa, T. [Rudjer Boskovic Institute, Zagreb (Croatia); Antoniou, N.; Christakoglou, P.; Davis, N.; Diakonos, F.; Kapoyannis, A.; Panagiotou, A.D.; Vassiliou, M. [University of Athens, Athens (Greece); Baatar, B.; Bunyatov, S.A.; Kolesnikov, V.I.; Krasnoperov, A.; Lyubushkin, V.V.; Malakhov, A.I.; Melkumov, G.L.; Tereshchenko, V. [Joint Institute for Nuclear Research, Dubna (Russian Federation); Bay, F.; Luise, S.Di; Rubbia, A.; Sgalaberna, D. [ETH, Zurich (Switzerland); Blumer, J.; Dembinski, H.; Engel, R.; Mathes, H.J.; Roth, M.; Szuba, M.; Ulrich, R.; Unger, M. [Karlsruhe Institute of Technology, Karlsruhe (Germany); Bogomilov, M.; Kolev, D.; Tsenov, R. [University of Sofia, Faculty of Physics, Sofia (Bulgaria); Busygina, O.; Golubeva, M.; Guber, F.; Ivashkin, A.; Kurepin, A.; Marin, V.; Petukhov, O.; Sadovsky, A. [Institute for Nuclear Research, Moscow (Russian Federation); Czopowicz, T.; Dynowski, K.; Grebieszkow, K.; Maksiak, B.; Peryt, W.; Pluta, J.; Slodkowski, M. [Warsaw University of Technology, Warsaw (Poland); Drozhzhova, T.; Feofilov, G.A.; Igolkin, S.; Kondratiev, V.P.; Vechernin, V.V.; Vinogradov, L. [St. Petersburg State University, St. Petersburg (Russian Federation); Dumarchez, J.; Robert, A.; Zambelli, L. [LPNHE, University of Paris VI and VII, Paris (France); Ereditato, A.; Hierholzer, M.; Nirkko, M.; Pistillo, C.; Redij, A. [University of Bern, Bern (Switzerland); Fodor, Z.; Fulop, A.; Kiss, T.; Laszlo, A.; Marton, K.; Palla, G.; Sipos, R.; Tolyhi, T.; Vesztergombi, G. [KFKI Research Institute for Particle and Nuclear Physics, Budapest (Hungary); Gazdzicki, M. [Jan Kochanowski University in Kielce, Kielce (Poland); University of Frankfurt, Frankfurt (Germany); Grzeszczuk, A.; Kaptur, E.; Kisiel, J.; Kowalski, S.; Larsen, D.; Pulawski, S.; Schmidt, K.; Wilczek, A.; Zipper, W. [University of Silesia, Katowice (Poland); Hasegawa, T.; Kobayashi, T.; Nakadaira, T.; Nishikawa, K.; Sakashita, K.; Sekiguchi, T.; Shibata, M.; Tada, M. [High Energy Accelerator Research Organization (KEK), Tsukuba, Ibaraki (Japan); Idczak, R.; Kovesarki, P.; Turko, L. [University of Wroclaw, Wroclaw (Poland); Jokovic, D.; Manic, D.; Puzovic, J.; Savic, M. [University of Belgrade, Belgrade (Serbia); Kleinfelder, S. [University of California, Irvine (United States); Mackowiak-Pawlowska, M.; Renfordt, R.; Rustamov, A.; Stroebele, H. [University of Frankfurt, Frankfurt (Germany); Matveev, V. [Joint Institute for Nuclear Research, Dubna (Russian Federation); Institute for Nuclear Research, Moscow (Russian Federation); Mrowczynski, S.; Rybczynski, M.; Seyboth, P.; Stefanek, G.; Wlodarczyk, Z.; Wojtaszek-Szwarc, A. [Jan Kochanowski University in Kielce, Kielce (Poland); Palczewski, T.; Rondio, E.; Stepaniak, J. [National Centre for Nuclear Research, Warsaw (Poland); Paul, T.; Veberic, D. [University Nova Gorica, Laboratory of Astroparticle Physics, Nova Gorica (Slovenia); Popov, B.A. [Joint Institute for Nuclear Research, Dubna (Russian Federation); LPNHE, University of Paris VI and VII, Paris (France); Rauch, W. [Fachhochschule Frankfurt, Frankfurt (Germany); Roehrich, D. [University of Bergen, Bergen (Norway); Collaboration: NA61/SHINE Collaboration

    2014-03-15

    We present experimental results on inclusive spectra and mean multiplicities of negatively charged pions produced in inelastic p+p interactions at incident projectile momenta of 20, 31, 40, 80 and 158 GeV/c (√(s) = 6.3, 7.7, 8.8, 12.3 and 17.3 GeV, respectively). The measurements were performed using the large acceptance NA61/SHINE hadron spectrometer at the CERN super proton synchrotron. Two-dimensional spectra are determined in terms of rapidity and transverse momentum. Their properties such as the width of rapidity distributions and the inverse slope parameter of transverse mass spectra are extracted and their collision energy dependences are presented. The results on inelastic p+p interactions are compared with the corresponding data on central Pb+Pb collisions measured by the NA49 experiment at the CERN SPS. The results presented in this paper are part of the NA61/SHINE ion program devoted to the study of the properties of the onset of deconfinement and search for the critical point of strongly interacting matter. They are required for interpretation of results on nucleus-nucleus and proton-nucleus collisions. (orig.)

  14. Measurement of negatively charged pion spectra in inelastic p+p interactions at 20, 31, 40, 80 and 158 GeV/c

    Science.gov (United States)

    Abgrall, N.; Aduszkiewicz, A.; Ali, Y.; Anticic, T.; Antoniou, N.; Baatar, B.; Bay, F.; Blondel, A.; Blumer, J.; Bogomilov, M.; Bravar, A.; Brzychczyk, J.; Bunyatov, S. A.; Busygina, O.; Christakoglou, P.; Czopowicz, T.; Davis, N.; Debieux, S.; Dembinski, H.; Diakonos, F.; Luise, S. Di; Dominik, W.; Drozhzhova, T.; Dumarchez, J.; Dynowski, K.; Engel, R.; Ereditato, A.; Feofilov, G. A.; Fodor, Z.; Fulop, A.; Gaździcki, M.; Golubeva, M.; Grebieszkow, K.; Grzeszczuk, A.; Guber, F.; Haesler, A.; Hasegawa, T.; Hierholzer, M.; Idczak, R.; Igolkin, S.; Ivashkin, A.; Joković, D.; Kadija, K.; Kapoyannis, A.; Kaptur, E.; Kiełczewska, D.; Kirejczyk, M.; Kisiel, J.; Kiss, T.; Kleinfelder, S.; Kobayashi, T.; Kolesnikov, V. I.; Kolev, D.; Kondratiev, V. P.; Korzenev, A.; Kovesarki, P.; Kowalski, S.; Krasnoperov, A.; Kurepin, A.; Larsen, D.; László, A.; Lyubushkin, V. V.; Maćkowiak-Pawłowska, M.; Majka, Z.; Maksiak, B.; Malakhov, A. I.; Manić, D.; Marcinek, A.; Marin, V.; Marton, K.; Mathes, H.-J.; Matulewicz, T.; Matveev, V.; Melkumov, G. L.; Mrówczyński, St.; Murphy, S.; Nakadaira, T.; Nirkko, M.; Nishikawa, K.; Palczewski, T.; Palla, G.; Panagiotou, A. D.; Paul, T.; Pistillo, C.; Peryt, W.; Petukhov, O.; Płaneta, R.; Pluta, J.; Popov, B. A.; Posiadała, M.; Puławski, S.; Puzović, J.; Rauch, W.; Ravonel, M.; Redij, A.; Renfordt, R.; Robert, A.; Röhrich, D.; Rondio, E.; Roth, M.; Rubbia, A.; Rustamov, A.; Rybczyński, M.; Sadovsky, A.; Sakashita, K.; Savić, M.; Schmidt, K.; Sekiguchi, T.; Seyboth, P.; Sgalaberna, D.; Shibata, M.; Sipos, R.; Skrzypczak, E.; Słodkowski, M.; Staszel, P.; Stefanek, G.; Stepaniak, J.; Ströbele, H.; Šuša, T.; Szuba, M.; Tada, M.; Tereshchenko, V.; Tolyhi, T.; Tsenov, R.; Turko, L.; Ulrich, R.; Unger, M.; Vassiliou, M.; Veberič, D.; Vechernin, V. V.; Vesztergombi, G.; Vinogradov, L.; Wilczek, A.; Włodarczyk, Z.; Wojtaszek-Szwarc, A.; Wyszyński, O.; Zambelli, L.; Zipper, W.

    2014-03-01

    We present experimental results on inclusive spectra and mean multiplicities of negatively charged pions produced in inelastic p+p interactions at incident projectile momenta of 20, 31, 40, 80 and 158 GeV/ c ( 6.3, 7.7, 8.8, 12.3 and 17.3 GeV, respectively). The measurements were performed using the large acceptance NA61/SHINE hadron spectrometer at the CERN super proton synchrotron. Two-dimensional spectra are determined in terms of rapidity and transverse momentum. Their properties such as the width of rapidity distributions and the inverse slope parameter of transverse mass spectra are extracted and their collision energy dependences are presented. The results on inelastic p+p interactions are compared with the corresponding data on central Pb+Pb collisions measured by the NA49 experiment at the CERN SPS. The results presented in this paper are part of the NA61/SHINE ion program devoted to the study of the properties of the onset of deconfinement and search for the critical point of strongly interacting matter. They are required for interpretation of results on nucleus-nucleus and proton-nucleus collisions.

  15. Measurement of negatively charged pion spectra in inelastic p+p interactions at $p_{lab}$ = 20, 31, 40, 80 and 158 GeV/c

    CERN Document Server

    Abgrall, N; Ali, Y; Anticic, T; Antoniou, N; Baatar, B; Bay, F; Blondel, A; Blumer, J; Bogomilov, M; Bravar, A; Brzychczyk, J; Bunyatov, S A; Busygina, O; Christakoglou, P; Czopowicz, T; Davis, N; Debieux, S; Dembinski, H; Diakonos, F; Di Luise, S; Dominik, W; Drozhzhova, T; Dumarchez, J; Dynowski, K; Engel, R; Ereditato, A; Feofilov, G A; Fodor, Z; Fulop, A; Gazdzicki, M; Golubeva, M; Grebieszkow, K; Grzeszczuk, A; Guber, F; Haesler, A; Hasegawa, T; Hierholzer, M; Idczak, R; Igolkin, S; Ivashkin, A; Jokovic, D; Kadija, K; Kapoyannis, A; Katrynska, N; Kaptur, E; Kielczewska, D; Kirejczyk, M; Kisiel, J; Kiss, T; Kleinfelder, S; Kobayashi, T; Kolesnikov, V I; Kolev, D; Kondratiev, V P; Korzenev, A; Kovesarki, P; Kowalski, S; Krasnoperov, A; Kurepin, A; Larsen, D; Laszlo, A; Lyubushkin, V V; Mackowiak-Pawlowska, M; Majka, Z; Maksiak, B; Malakhov, A I; Manic, D; Marcinek, A; Marin, V; Marton, K; Mathes, H J; Matulewicz, T; Matveev, V; Melkumov, G.L; Mrowczynski, St; Murphy, S; Nakadaira, T; Nirkko, M; Nishikawa, K; Palczewski, T; Palla, G; Panagiotou, A D; Paul, T; Pistillo, C; Peryt, W; Petukhov, O; Planeta, R; Pluta, J; Popov, B A; Posiadala, M; Pulawski, S; Puzovic, J; Rauch, W; Ravonel, M; Redij, A; Renfordt, R; Robert, A; Rohrich, D; Rondio, E; Roth, M; Rubbia, A; Rustamov, A; Rybczynski, M; Sadovsky, A; Sakashita, K; Savic, M; Schmidt, K; Sekiguchi, T; Seyboth, P; Sgalaberna, D; Shibata, M; Sipos, R; Skrzypczak, E; Slodkowski, M; Staszel, P; Stefanek, G; Stepaniak, J; Strobele, H; Susa, T; Szuba, M; Tada, M; Tereshchenko, V; Tolyhi, T; Tsenov, R; Turko, L; Ulrich, R; Unger, M; Vassiliou, M; Veberic, D; Vechernin, V V; Vesztergombi, G; Vinogradov, L; Wilczek, A; Wlodarczyk, Z; Wojtaszek-Szwarc, A; Wyszynski, O; Zambelli, L; Zipper, W

    2014-01-01

    We present experimental results on inclusive spectra and mean multiplicities of negatively charged pions produced in inelastic p+p interactions at incident projectile momenta of 20, 31, 40, 80 and 158GeV/c ($\\sqrt{s}$ = 6.3, 7.7, 8.8, 12.3 and 17.3GeV, respectively). The measurements were performed using the large acceptance NA61/SHINE hadron spectrometer at the CERN super proton synchrotron. Two-dimensional spectra are determined in terms of rapidity and transverse momentum. Their properties such as the width of rapidity distributions and the inverse slope parameter of transverse mass spectra are extracted and their collision energy dependences are presented. The results on inelastic p+p interactions are compared with the corresponding data on central Pb+Pb collisions measured by the NA49 experiment at the CERN SPS. The results presented in this paper are part of the NA61/SHINE ion program devoted to the study of the properties of the onset of deconfinement and search for the critical point of strongly inter...

  16. Bose-Einstein condensation and indirect excitons: a review.

    Science.gov (United States)

    Combescot, Monique; Combescot, Roland; Dubin, François

    2017-06-01

    We review recent progress on Bose-Einstein condensation (BEC) of semiconductor excitons. The first part deals with theory, the second part with experiments. This Review is written at a time where the problem of exciton Bose-Einstein condensation has just been revived by the understanding that the exciton condensate must be dark because the exciton ground state is not coupled to light. Here, we theoretically discuss this missed understanding before providing its experimental support through experiments that scrutinize indirect excitons made of spatially separated electrons and holes. The theoretical part first discusses condensation of elementary bosons. In particular, the necessary inhibition of condensate fragmentation by exchange interaction is stressed, before extending the discussion to interacting bosons with spin degrees of freedom. The theoretical part then considers composite bosons made of two fermions like semiconductor excitons. The spin structure of the excitons is detailed, with emphasis on the crucial fact that ground-state excitons are dark: indeed, this imposes the exciton Bose-Einstein condensate to be not coupled to light in the dilute regime. Condensate fragmentations are then reconsidered. In particular, it is shown that while at low density, the exciton condensate is fully dark, it acquires a bright component, coherent with the dark one, beyond a density threshold: in this regime, the exciton condensate is 'gray'. The experimental part first discusses optical creation of indirect excitons in quantum wells, and the detection of their photoluminescence. Exciton thermalisation is also addressed, as well as available approaches to estimate the exciton density. We then switch to specific experiments where indirect excitons form a macroscopic fragmented ring. We show that such ring provides efficient electrostatic trapping in the region of the fragments where an essentially-dark exciton Bose-Einstein condensate is formed at sub-Kelvin bath

  17. Ultrafast exciton transfers in DNA and its nonlinear optical spectroscopy

    OpenAIRE

    Kim, Hyeon-Deuk; Tanimura, Yoshitaka; Cho, Minhaeng

    2008-01-01

    We have calculated the nonlinear response function of a DNA duplex helix including the contributions from the exciton population and coherence transfers by developing an appropriate exciton theory as well as by utilizing a projector operator technique. As a representative example of DNA double helices, the B-form (dA)10-(dT)10 is considered in detail. The Green functions of the exciton population and coherence transfer processes were obtained by developing the DNA exciton Hamiltonian. This en...

  18. Bose-Einstein condensation and indirect excitons: a review

    Science.gov (United States)

    Combescot, Monique; Combescot, Roland; Dubin, François

    2017-06-01

    We review recent progress on Bose-Einstein condensation (BEC) of semiconductor excitons. The first part deals with theory, the second part with experiments. This Review is written at a time where the problem of exciton Bose-Einstein condensation has just been revived by the understanding that the exciton condensate must be dark because the exciton ground state is not coupled to light. Here, we theoretically discuss this missed understanding before providing its experimental support through experiments that scrutinize indirect excitons made of spatially separated electrons and holes. The theoretical part first discusses condensation of elementary bosons. In particular, the necessary inhibition of condensate fragmentation by exchange interaction is stressed, before extending the discussion to interacting bosons with spin degrees of freedom. The theoretical part then considers composite bosons made of two fermions like semiconductor excitons. The spin structure of the excitons is detailed, with emphasis on the crucial fact that ground-state excitons are dark: indeed, this imposes the exciton Bose-Einstein condensate to be not coupled to light in the dilute regime. Condensate fragmentations are then reconsidered. In particular, it is shown that while at low density, the exciton condensate is fully dark, it acquires a bright component, coherent with the dark one, beyond a density threshold: in this regime, the exciton condensate is ‘gray’. The experimental part first discusses optical creation of indirect excitons in quantum wells, and the detection of their photoluminescence. Exciton thermalisation is also addressed, as well as available approaches to estimate the exciton density. We then switch to specific experiments where indirect excitons form a macroscopic fragmented ring. We show that such ring provides efficient electrostatic trapping in the region of the fragments where an essentially-dark exciton Bose-Einstein condensate is formed at sub-Kelvin bath

  19. Non-conservation of excitons in finite molecular chain

    Energy Technology Data Exchange (ETDEWEB)

    Tosic, Bratislav, E-mail: btosic@yahoo.co [Vojvodina Academy of Science and Arts, 21000 Novi Sad, Dunavska 37 (Serbia); Sajfert, Vjekoslav, E-mail: sajfertv@nadlanu.co [University of Novi Sad, Technical Faculty ' M. Pupin' , 23000 Zrenjanin, Djure Djakovica bb (Serbia); Maskovic, Ljiljana, E-mail: maskovicm@yahoo.co.u [Academy of Criminalistic and Police Studies, 11000 Belgrade, Zemun (Serbia); Bednar, Nikola, E-mail: bednar.nikola@gmail.co [University of Novi Sad, Faculty of Technical Sciences, 21000 Novi Sad, Trg Dositeja Obradovica 6 (Serbia)

    2010-11-15

    We have analyzed a linear molecular chain with exciton excitations when the number of excitons is not conserved. The dispersion law depends on two independent variables and it is surfaced in a 3D plot. The same conclusion is valid for the concentrations of excitons and exciton pairs. As it was expected, physical characteristics of the finite chain depend on spatial coordinates. All results are compared to the corresponding results of an infinite chain.

  20. Resonant Transfer of Excitons and Quantum Computation

    CERN Document Server

    Lovett, B; Nazir, A; Kothari, B; Briggs, A; Lovett, Brendon; Reina, John H.; Nazir, Ahsan; Kothari, Beeneet; Briggs, Andrew

    2003-01-01

    The excitation-energy transfer--the so-called Forster resonant energy transfer--plays a key role in light harvesting processes in photosynthetic organisms in nature. Here we give two methods for performing quantum logic operations by tailoring this interaction. The first implementation uses a coupled quantum dot molecule where the exciton-exciton interaction and the Forster coupling are controlled by means of the dot size, interdot separation, material composition, confinement potential and applied electric field to obtain high fidelity logic. The second proposes the use of biological systems for embodying qubits where, as a result of a stronger Forster interaction, extended exciton states are expected. These states are likely to be more immune to decoherence.

  1. Efficient exciton funneling in cascaded PbS quantum dot superstructures.

    Science.gov (United States)

    Xu, Fan; Ma, Xin; Haughn, Chelsea R; Benavides, Jamie; Doty, Matthew F; Cloutier, Sylvain G

    2011-12-27

    Benzenedithiol (BDT) and ethanedithiol (EDT) ligand-exchange treatments can be used to cross-link colloidal PbS quantum dots into nanocrystalline film structures with distinct optoelectronic properties. Such structures can provide a unique platform to study the energy transfer between layers of quantum dots with different sizes. In this report, efficient exciton funneling and recycling of surface state-bound excitons is observed in cascaded PbS quantum dot-based multilayered superstructures, where the excitons transfer from the larger band gap or donor layers to the smallest band gap or acceptor layers. In this system, both the BDT- and EDT-treated cascaded structures exhibit dramatically enhanced photoluminescence from the acceptor layers. As we show, the energy transfer mechanisms involved and their efficiencies are significantly different depending on the ligand-exchange treatment. In the future, we believe these efficient exciton recycling and funneling mechanisms could be used to improve significantly the photocurrent, charge-transport, and conversion efficiencies in low-cost nanocrystalline and hybrid solar cells and the emission efficiencies in hybrid light-emitting devices.

  2. Resonance effects of excitons and electrons. Basics and applications

    Energy Technology Data Exchange (ETDEWEB)

    Geru, Ion [Moldovan Academy of Sciences, Chisinau (Moldova, Republic of). Inst. of Chemistry; Suter, Dieter [Technische Univ. Dortmund (Germany). Fakultaet Physik

    2013-08-01

    Represents the first book on non-traditional resonance effects of excitons in semiconductors. Explains resonance phenomena of excitons and electrons in solids. Presents the Knight shift at the Bose-Einstein condensation of excitons. This book presents the various types of resonance effects on excitons, biexcitons and the local electronic centers (LEC) in solids, such as paramagnetic and paraelectric resonances on excitons, exciton acoustic resonance at intra- and interband transitions, radio-optical double resonance on excitons, hole-nuclear double resonance on localized biexcitons, ENDOR and acoustic ENDOR on LEC. The criteria for the generation of coherent photons, phonons and magnons by excitons are explained. The interactions of excitons and biexcitons with paramagnetic centers and nuclear spins, the indirect interaction between the PC through a field of excitons as well as the quasienergy spectrum of excitons and spin systems are discussed. It is proved that the interaction of paramagnetic centers with excitons increases the spin relaxation rate of paramagnetic centers in comparison with the case of their interaction with free carriers. The giant magneto-optical effects in semi-magnetic semiconductors are theoretically interpreted. In recent years, a new perspective has been added to these systems and their interactions: they can be used for storing and processing information in the form of quantum bits (qubits), the building blocks of quantum computers. The basics of this emerging technology are explained and examples of demonstration-type quantum computers based on localized spins in solids are discussed.

  3. Spin coherence and electromagnetically induced transparency via exciton correlations.

    Science.gov (United States)

    Phillips, Mark; Wang, Hailin

    2002-10-28

    We report experimental studies on exciton spin coherence induced via Coulomb correlations between excitons with opposite spins, including correlations associated with unbound as well as bound exciton pairs. Electromagnetically induced transparency resulting from the spin coherence is demonstrated in the transient optical response in GaAs quantum wells.

  4. Arsenic-bound excitons in diamond

    Science.gov (United States)

    Barjon, J.; Jomard, F.; Morata, S.

    2014-01-01

    A set of new excitonic recombinations is observed in arsenic-implanted diamond. It is composed of two groups of emissions at 5.355/5.361 eV and at 5.215/5.220/5.227 eV. They are respectively attributed to the no-phonon and transverse-optical phonon-assisted recombinations of excitons bound to neutral arsenic donors. From the Haynes rule, an ionization energy of 0.41 eV is deduced for arsenic in diamond, which shows that arsenic is a shallower donor than phosphorus (0.6 eV), in agreement with theory.

  5. Heat pumping with optically driven excitons

    CERN Document Server

    Gauger, Erik M

    2010-01-01

    We present a theoretical study showing that an optically driven excitonic two-level system in a solid state environment acts as a heat pump by means of repeated phonon emission or absorption events. We derive a master equation for the combined phonon bath and two-level system dynamics and analyze the direction and rate of energy transfer as a function of the externally accessible driving parameters. We discover that if the driving laser is detuned from the exciton transition, cooling the phonon environment becomes possible.

  6. Excitonic dynamical Franz-Keldysh effect

    DEFF Research Database (Denmark)

    Nordstrøm, K.B.; Johnsen, Kristinn; Allen, S.J.

    1998-01-01

    The dynamical Franz-Keldysh effect is exposed by exploring near-band-gap absorption in the presence of intense THz electric fields. It bridges the gap between the de Franz-Keldysh effect and multiphoton absorption and competes with the THz ac Stark effect in shifting the energy of the excitonic...... resonance. A theoretical model which includes the strong THz field nonperturbatively via a nonequilibrium Green functions technique is able to describe the dynamical Franz-Keldysh effect in the presence of excitonic absorption....

  7. Switching exciton pulses through conical intersections

    CERN Document Server

    Leonhardt, K; Rost, J -M

    2013-01-01

    Exciton pulses transport excitation and entanglement adiabatically through Rydberg aggregates, assemblies of highly excited light atoms, which are set into directed motion by resonant dipole-dipole interaction. Here, we demonstrate the coherent splitting of such pulses as well as the spatial segregation of electronic excitation and atomic motion. Both mechanisms exploit local non-adiabatic effects at a conical intersection, turning them from a decoherence source into an asset. The intersection provides a sensitive knob controlling the propagation direction and coherence properties of exciton pulses.

  8. Determination of stability constants of tauro- and glyco-conjugated bile salts with the negatively charged sulfobutylether-β-cyclodextrin: comparison of affinity capillary electrophoresis and isothermal titration calorimetry and thermodynamic analysis of the interaction

    DEFF Research Database (Denmark)

    Holm, René; Østergaard, Jesper; Schönbeck, Jens Christian Sidney;

    2014-01-01

    The aim of the present work was to investigate the interaction between bile salts present in the intestine of man, dog and rat with the negatively charged cyclodextrin (CD), sulfobutylether-β-cyclodextrin (SBEβCD). The interactions between bile salts and CDs are of importance for the release of C...

  9. Optical and spin properties of localized and free excitons in GaBi x As1-x /GaAs multiple quantum wells

    Science.gov (United States)

    Balanta, M. A. G.; Kopaczek, J.; Orsi Gordo, V.; Santos, B. H. B.; Rodrigues, A. D.; Galeti, H. V. A.; Richards, R. D.; Bastiman, F.; David, J. P. R.; Kudrawiec, R.; Galvão Gobato, Y.

    2016-09-01

    Raman spectroscopy and magneto-photoluminescence measurements under high magnetic fields were used to investigate the optical and spin properties of GaBiAs/GaAs multiple quantum wells (MQWs). An anomalous negative diamagnetic energy shift was observed at higher temperatures and higher laser intensities, which was associated to a sign inversion of hole effective mass in these structures. In addition, an enhancement of the polarization degree with decreasing of laser intensity was observed (experimental condition where the emission is dominated by localized excitons). This effect was explained by changes of spin relaxation and exciton recombination times due to exciton localization by disorder.

  10. Bright and dark excitons in semiconductor carbon nanotubes

    Energy Technology Data Exchange (ETDEWEB)

    Tretiak, Sergei [Los Alamos National Laboratory

    2008-01-01

    We report electronic structure calculations of finite-length semiconducting carbon nanotubes using the time dependent density functional theory (TD-DFT) and the time dependent Hartree Fock (TD-HF) approach coupled with semiempirical AM1 and ZINDO Hamiltonians. We specifically focus on the energy splitting, relative ordering, and localization properties of the optically active (bright) and optically forbidden (dark) states from the lowest excitonic band of the nanotubes. These excitonic states are very important in competing radiative and non-radiative processes in these systems. Our analysis of excitonic transition density matrices demonstrates that pure DFT functionals overdelocalize excitons making an electron-hole pair unbound; consequently, excitonic features are not presented in this method. In contrast, the pure HF and A111 calculations overbind excitons inaccurately predicting the lowest energy state as a bright exciton. Changing AM1 with ZINDO Hamiltonian in TD-HF calculations, predicts the bright exciton as the second state after the dark one. However, in contrast to AM1 calculations, the diameter dependence of the excitation energies obtained by ZINDO does not follow the experimental trends. Finally, the TD-DFT approach incorporating hybrid functions with a moderate portion of the long-range HF exchange, such as B3LYP, has the most generality and predictive capacity providing a sufficiently accurate description of excitonic structure in finite-size nanotubes. These methods characterize four important lower exciton bands. The lowest state is dark, the upper band is bright, and the two other dark and nearly degenerate excitons lie in-between. Although the calculated energy splittings between the lowest dark and the bright excitons are relatively large ({approx}0.1 eV), the dense excitonic manifold below the bright exciton allows for fast non-radiative relaxation leasing to the fast population of the lowest dark exciton. This rationalizes the low

  11. Free-exciton states in crystalline GaTe

    Science.gov (United States)

    Wan, J. Z.; Brebner, J. L.; Leonelli, R.

    1995-12-01

    Polarized properties of both the singlet and triplet ground exciton states in the photoluminescence and transmission spectra of crystalline GaTe are explained based on the possible symmetry properties of the energy band edge of GaTe. Some experimental results about excited exciton states in GaTe are presented and discussed. The energy positions of exciton series in GaTe follow the three-dimensional direct allowed Wannier exciton formula just as in the the other III-VI layered compounds of GaSe and InSe. The nonthermalized, ``hot'' nature of excitons inside GaTe under higher optical excitation intensities is also discussed.

  12. Coherent control of ground state excitons in the nonlinear regime within an ensemble of self-assembled InAs quantum dots

    Energy Technology Data Exchange (ETDEWEB)

    Moldaschl, Thomas; Mueller, Thomas; Golka, Sebastian; Parz, Wolfgang; Strasser, Gottfried; Unterrainer, Karl [Photonics Institute and Center for Micro- and Nanostructures, Vienna University of Technology (Austria)

    2009-04-15

    In this work femtosecond spectral hole burning spectroscopy is used to resonantly excite ground state excitons in an ensemble of self-assembled InAs/GaAs quantum dots with a strong pump pulse. Two fundamental coherent nonlinear effects are observed with the aid of the intrinsic time- and frequency resolution of the setup: The low temperature Rabi oscillation of the two-level system associated with the excitonic ground state transition and the observation of two-photon absorption in the surrounding GaAs crystal matrix. The emergence of the latter effect also infers the existence of charged excitons in the nominally undoped QD sample, backed up by the observation of additional spectral holes next to the excitonic transitions. (copyright 2009 WILEY-VCH Verlag GmbH and Co. KGaA, Weinheim) (orig.)

  13. Exciton dynamics in GaAs/(Al,Ga)As core-shell nanowires with shell quantum dots

    Science.gov (United States)

    Corfdir, Pierre; Küpers, Hanno; Lewis, Ryan B.; Flissikowski, Timur; Grahn, Holger T.; Geelhaar, Lutz; Brandt, Oliver

    2016-10-01

    We study the dynamics of excitons in GaAs/(Al,Ga)As core-shell nanowires by continuous-wave and time-resolved photoluminescence and photoluminescence excitation spectroscopy. Strong Al segregation in the shell of the nanowires leads to the formation of Ga-rich inclusions acting as quantum dots. At 10 K, intense light emission associated with these shell quantum dots is observed. The average radiative lifetime of excitons confined in the shell quantum dots is 1.7 ns. We show that excitons may tunnel toward adjacent shell quantum dots and nonradiative point defects. We investigate the changes in the dynamics of charge carriers in the shell with increasing temperature, with particular emphasis on the transfer of carriers from the shell to the core of the nanowires. We finally discuss the implications of carrier localization in the (Al,Ga)As shell for fundamental studies and optoelectronic applications based on core-shell III-As nanowires.

  14. Final Report, DOE grant DE-FG02-99ER45780, "Indirect Excitons in Coupled Quantum Wells"

    Energy Technology Data Exchange (ETDEWEB)

    Snoke, david W. [University of Pittsburgh

    2014-07-21

    The is the final technical report for this project, which was funded by the DOE from 1999 to 2012. The project focused on experimental studies of spatially indirect excitons in coupled quantum wells, with the aim of understanding the quantum physics of these particles, including such effects as pattern formation due to electron-hole charge separation, the Mott plasma-insulator transition, luminescence up-conversion through field-assisted tunneling, luminescence line shifts due to many-body renormalization and magnetic field effects on tunneling, and proposed effects such as Bose-Einstein condensation of indirect excitons and phase separation of bright and dark indirect excitons. Significant results are summarized here and the relation to other work is discussed.

  15. Electrical Control of Excitons in Semiconductor Nanostructures

    DEFF Research Database (Denmark)

    Kirsanské, Gabija

    The scope of this thesis covers investigation of the exciton Mott transition in coupled quantum wells, fabrication of photonic-crystal structures with embedded self-assembled quantum dots, and tuning of their properties by means of an external electric field. In the first part of the thesis the f...

  16. Excitons in van der Waals heterostructures

    DEFF Research Database (Denmark)

    Latini, Simone; Olsen, Thomas; Thygesen, Kristian Sommer

    2015-01-01

    The existence of strongly bound excitons is one of the hallmarks of the newly discovered atomically thin semiconductors. While it is understood that the large binding energy is mainly due to the weak dielectric screening in two dimensions, a systematic investigation of the role of screening on tw...

  17. Effective models for excitons in carbon nanotubes

    DEFF Research Database (Denmark)

    Cornean, Horia; Duclos, Pierre; Ricaud, Benjamin

    We analyse the low lying spectrum of a model of excitons in carbon nanotubes. Consider two particles with a Coulomb self-interaction, placed on an infinitely long cylinder. If the cylinder radius becomes small, the low lying spectrum is well described by a one-dimensional effective Hamiltonian...

  18. Properties of Excitons Bound to Ionized Donors

    DEFF Research Database (Denmark)

    Skettrup, Torben; Suffczynski, M.; Gorzkowski, W.

    1971-01-01

    Binding energies, interparticle distances, oscillator strengths, and exchange corrections are calculated for the three-particle complex corresponding to an exciton bound to an ionized donor. The results are given as functions of the mass ratio of the electron and hole. Binding of the complex is o...

  19. Exciton Transfer Integrals Between Polymer Chains

    CERN Document Server

    Barford, W

    2007-01-01

    The line-dipole approximation for the evaluation of the exciton transfer integral, $J$, between conjugated polymer chains is rigorously justified. Using this approximation, as well as the plane-wave approximation for the exciton center-of-mass wavefunction, it is shown analytically that $J \\sim L$ when the chain lengths are smaller than the separation between them, or $J\\sim L^{-1}$ when the chain lengths are larger than their separation, where $L$ is the polymer length. Scaling relations are also obtained numerically for the more realistic standing-wave approximation for the exciton center-of-mass wavefunction, where it is found that for chain lengths larger than their separation $J \\sim L^{-1.8}$ or $J \\sim L^{-2}$, for parallel or collinear chains, respectively. These results have important implications for the photo-physics of conjugated polymers and self-assembled molecular systems, as the Davydov splitting in aggregates and the F\\"orster transfer rate for exciton migration decreases with chain lengths l...

  20. Directional charge separation in isolated organic semiconductor crystalline nanowires

    Science.gov (United States)

    Labastide, J. A.; Thompson, H. B.; Marques, S. R.; Colella, N. S.; Briseno, A. L.; Barnes, M. D.

    2016-02-01

    One of the fundamental design paradigms in organic photovoltaic device engineering is based on the idea that charge separation is an extrinsically driven process requiring an interface for exciton fission. This idea has driven an enormous materials science engineering effort focused on construction of domain sizes commensurate with a nominal exciton diffusion length of order 10 nm. Here, we show that polarized optical excitation of isolated pristine crystalline nanowires of a small molecule n-type organic semiconductor, 7,8,15,16-tetraazaterrylene, generates a significant population of charge-separated polaron pairs along the π-stacking direction. Charge separation was signalled by pronounced power-law photoluminescence decay polarized along the same axis. In the transverse direction, we observed exponential decay associated with excitons localized on individual monomers. We propose that this effect derives from an intrinsic directional charge-transfer interaction that can ultimately be programmed by molecular packing geometry.

  1. Coherent quantum dynamics of excitons in monolayer transition metal dichalcogenides

    KAUST Repository

    Moody, Galan

    2016-03-14

    Transition metal dichalcogenides (TMDs) have garnered considerable interest in recent years owing to their layer thickness-dependent optoelectronic properties. In monolayer TMDs, the large carrier effective masses, strong quantum confinement, and reduced dielectric screening lead to pronounced exciton resonances with remarkably large binding energies and coupled spin and valley degrees of freedom (valley excitons). Coherent control of valley excitons for atomically thin optoelectronics and valleytronics requires understanding and quantifying sources of exciton decoherence. In this work, we reveal how exciton-exciton and exciton-phonon scattering influence the coherent quantum dynamics of valley excitons in monolayer TMDs, specifically tungsten diselenide (WSe2), using two-dimensional coherent spectroscopy. Excitation-density and temperature dependent measurements of the homogeneous linewidth (inversely proportional to the optical coherence time) reveal that exciton-exciton and exciton-phonon interactions are significantly stronger compared to quasi-2D quantum wells and 3D bulk materials. The residual homogeneous linewidth extrapolated to zero excitation density and temperature is ~1:6 meV (equivalent to a coherence time of 0.4 ps), which is limited only by the population recombination lifetime in this sample. © (2016) COPYRIGHT Society of Photo-Optical Instrumentation Engineers (SPIE). Downloading of the abstract is permitted for personal use only.

  2. Polaronic Effects of an Exciton in a Cylindrical Quantum Wire

    Institute of Scientific and Technical Information of China (English)

    WANG Rui-Qiang; XIE Hong-Jing; GUO Kang-Xian; YU You-Bin; DENG Yong-Qing

    2005-01-01

    The effects of exciton-optical phonon interaction on the binding energy and the total and reduced effective masses of an exciton in a cylindrical quantum wire have been investigated. We adopt a perturbative-PLL [T.D. Lee,F. Low, and D. Pines, Phys. Rev. B90 (1953) 297] technique to construct an effective Hamiltonian and then use a variational solution to deal with the exciton-phonon system. The interactions of exciton with the longitudinal-optical phonon and the surface-optical phonon have been taken into consideration. The numerical calculations for GaAs show that the influences of phonon modes on the exciton in a quasi-one-dimensional quantum wire are considerable and should not be neglected. Moreover the numerical results for heavy- and light-hole exciton are obtained, which show that the polaronic effects on two types of excitons are very different but both depend heavily on the sizes of the wire.

  3. Exciton dynamics at the heteromolecular interface between N,N′-dioctyl-3,4,9,10-perylenedicarboximide and quaterrylene, studied using time-resolved photoluminescence

    Directory of Open Access Journals (Sweden)

    Nobuya Hiroshiba

    2014-06-01

    Full Text Available To elucidate the exciton dynamics at the heteromolecular interface, the temperature dependence of time-resolved photoluminescence (TRPL spectra of neat-N,N′-dioctyl-3,4,9,10-perylenedicarboximide (PTCDI-C8 and PTCDI-C8/Quaterrylene (QT heteromolecular thin films was investigated. The lifetimes of excitons were evaluated to identify the Frenkel (FE, high energy charge-transfer (CTEhigh, low energy charge-transfer (CTElow, and excimer exciton states. The thermal activation energy (Δact of CTElow in PTCDI-C8 thin film was evaluated as 25 meV, which is 1/5 of that of FE, indicating that CTElow is more thermally sensitive than FE in PTCDI-C8 thin film. We investigated the exciton transport length (l along the vertical direction against the substrate surface in PTCDI-C8/QT thin film at 30 K, and demonstrated that lFE = 9.9 nm, lCTElow = 4.2 nm, lCTEhigh = 4.3 nm, and lexcimer = 11.9 nm. To elucidate the difference in l among these excitons, the activation energies (Ea for quenching at the heteromolecular interface were investigated. Ea values were estimated to be 13.1 meV for CTElow and 18.6 meV for CTEhigh. These values agree with the thermal sensitivity of CTEs as reported in a previous static PL study. This latter situation is different from the case of FE and excimer excitons, which are transported via a resonant process and have no temperature dependence. The small Ea values of CTEs suggest that exciton transport takes place via a thermal hopping process in CTEs. The present experimental study provides information on nano-scaled exciton dynamics in a well-defined PTCDI-C8 (2 ML/QT (2 ML system.

  4. Radiatively Limited Dephasing and Exciton Dynamics in MoSe2 Monolayers Revealed with Four-Wave Mixing Microscopy.

    Science.gov (United States)

    Jakubczyk, Tomasz; Delmonte, Valentin; Koperski, Maciej; Nogajewski, Karol; Faugeras, Clément; Langbein, Wolfgang; Potemski, Marek; Kasprzak, Jacek

    2016-09-14

    By implementing four-wave mixing (FWM) microspectroscopy, we measure coherence and population dynamics of the exciton transitions in monolayers of MoSe2. We reveal their dephasing times T2 and radiative lifetime T1 in a subpicosecond (ps) range, approaching T2 = 2T1 and thus indicating radiatively limited dephasing at a temperature of 6 K. We elucidate the dephasing mechanisms by varying the temperature and by probing various locations on the flake exhibiting a different local disorder. At the nanosecond range, we observe the residual FWM produced by the incoherent excitons, which initially disperse toward the dark states but then relax back to the optically active states within the light cone. By introducing polarization-resolved excitation, we infer intervalley exciton dynamics, revealing an initial polarization degree of around 30%, constant during the initial subpicosecond decay, followed by the depolarization on a picosecond time scale. The FWM hyperspectral imaging reveals the doped and undoped areas of the sample, allowing us to investigate the neutral exciton, the charged one, or both transitions at the same time. In the latter, we observe the exciton-trion beating in the coherence evolution indicating their coherent coupling.

  5. Nonlinear Raman Shift Induced by Exciton-to-Trion Transformation in Suspended Trilayer MoS2

    CERN Document Server

    Taghinejad, Hossein; Tarasov, Alexey; Tsai, Meng-Yen; Hosseinnia, Amir H; Campbell, Philip M; Eftekhar, Ali A; Vogel, Eric M; Adibi, Ali

    2015-01-01

    Layered two-dimensional (2D) semiconductors such as molybdenum disulfide (MoS2) have recently attracted remarkable attention because of their unique physical properties. Here, we use photoluminescence (PL) and Raman spectroscopy to study the formation of the so- called trions in a synthesized freestanding trilayer MoS2. A trion is a charged quasi-particle formed by adding one electron or hole to a neutral exciton (a bound electron-hole pair). We demonstrate accurate control over the transformation of excitons to trions by tuning the power of the optical pump (laser). Increasing the power of the excitation laser beyond a certain threshold (~ 4 mW) allows modulation of trion-to-exciton PL intensity ratio as well as the spectral linewidth of both trions and excitons. Via a systematic and complementary Raman analysis we disclose a strong coupling between laser induced exciton-to-trion transformation and the characteristic phononic vibrations of MoS2. The onset of such an optical transformation corresponds to the ...

  6. Electron transport mechanism of bathocuproine exciton blocking layer in organic photovoltaics.

    Science.gov (United States)

    Lee, Jeihyun; Park, Soohyung; Lee, Younjoo; Kim, Hyein; Shin, Dongguen; Jeong, Junkyeong; Jeong, Kwangho; Cho, Sang Wan; Lee, Hyunbok; Yi, Yeonjin

    2016-02-21

    Efficient exciton management is a key issue to improve the power conversion efficiency of organic photovoltaics (OPVs). It is well known that the insertion of an exciton blocking layer (ExBL) having a large band gap promotes the efficient dissociation of photogenerated excitons at the donor-acceptor interface. However, the large band gap induces an energy barrier which disrupts the charge transport. Therefore, building an adequate strategy based on the knowledge of the true charge transport mechanism is necessary. In this study, the true electron transport mechanism of a bathocuproine (BCP) ExBL in OPVs is comprehensively investigated by in situ ultraviolet photoemission spectroscopy, inverse photoemission spectroscopy, density functional theory calculation, and impedance spectroscopy. The chemical interaction between deposited Al and BCP induces new states within the band gap of BCP, so that electrons can transport through these new energy levels. Localized trap states are also formed upon the Al-BCP interaction. The activation energy of these traps is estimated with temperature-dependent conductance measurements to be 0.20 eV. The Al-BCP interaction induces both transport and trap levels in the energy gap of BCP and their interplay results in the electron transport observed.

  7. First-principles simulation of light propagation and exciton dynamics in metal cluster nanostructures

    Science.gov (United States)

    Lisinetskaya, Polina G.; Röhr, Merle I. S.; Mitrić, Roland

    2016-06-01

    We present a theoretical approach for the simulation of the electric field and exciton propagation in ordered arrays constructed of molecular-sized noble metal clusters bound to organic polymer templates. In order to describe the electronic coupling between individual constituents of the nanostructure we use the ab initio parameterized transition charge method which is more accurate than the usual dipole-dipole coupling. The electronic population dynamics in the nanostructure under an external laser pulse excitation is simulated by numerical integration of the time-dependent Schrödinger equation employing the fully coupled Hamiltonian. The solution of the TDSE gives rise to time-dependent partial point charges for each subunit of the nanostructure, and the spatio-temporal electric field distribution is evaluated by means of classical electrodynamics methods. The time-dependent partial charges are determined based on the stationary partial and transition charges obtained in the framework of the TDDFT. In order to treat large plasmonic nanostructures constructed of many constituents, the approximate self-consistent iterative approach presented in (Lisinetskaya and Mitrić in Phys Rev B 89:035433, 2014) is modified to include the transition-charge-based interaction. The developed methods are used to study the optical response and exciton dynamics of Ag3+ and porphyrin-Ag4 dimers. Subsequently, the spatio-temporal electric field distribution in a ring constructed of ten porphyrin-Ag4 subunits under the action of circularly polarized laser pulse is simulated. The presented methodology provides a theoretical basis for the investigation of coupled light-exciton propagation in nanoarchitectures built from molecular size metal nanoclusters in which quantum confinement effects are important.

  8. Singlet exciton condensation and bond-order-wave phase in the extended Hubbard model

    Science.gov (United States)

    Hafez-Torbati, Mohsen; Uhrig, Götz S.

    2017-09-01

    The competition of interactions implies the compensation of standard mechanisms, which leads to the emergence of exotic phases between conventional phases. The extended Hubbard model (EHM) is a fundamental example for the competition of the local Hubbard interaction and the nearest-neighbor density-density interaction, which at half-filling and in one dimension leads to a bond-order wave (BOW) between a charge-density wave (CDW) and a quasi-long-range order Mott insulator. We study the full momentum-resolved excitation spectrum of the one-dimensional EHM in the CDW phase, and we clarify the relation between different elementary energy gaps. We show that the CDW-to-BOW transition is driven by the softening of a singlet exciton at momentum π . The BOW is realized as the condensate of this singlet exciton.

  9. Charge Separation in Semicrystalline Polymeric Semiconductors by Photoexcitation: Is the Mechanism Intrinsic or Extrinsic?

    Science.gov (United States)

    Paquin, Francis; Latini, Gianluca; Sakowicz, Maciej; Karsenti, Paul-Ludovic; Wang, Linjun; Beljonne, David; Stingelin, Natalie; Silva, Carlos

    2011-05-01

    We probe charge photogeneration and subsequent recombination dynamics in neat regioregular poly(3-hexylthiophene) films over six decades in time by means of time-resolved photoluminescence spectroscopy. Exciton dissociation at 10 K occurs extrinsically at interfaces between molecularly ordered and disordered domains. Polaron pairs thus produced recombine by tunneling with distributed rates governed by the distribution of electron-hole radii. Quantum-chemical calculations suggest that hot-exciton dissociation at such interfaces results from a high charge-transfer character.

  10. Light propagation in tunable exciton-polariton one-dimensional photonic crystals

    OpenAIRE

    Sedov, E. S.; Cherotchenko, E. D.; Arakelian, S.M.; Kavokin, A. V.

    2016-01-01

    Simulations of propagation of light beams in specially designed multilayer semiconductor structures (one-dimensional photonic crystals) with embedded quantum wells reveal characteristic optical properties of resonant hyperbolic metamaterials. A strong dependence of the refraction angle and the optical beam spread on the exciton radiative lifetime is revealed. We demonstrate the strong negative refraction of light and the control of the group velocity of light by an external bias through its e...

  11. Fine structure of the exciton electroabsorption in semiconductor superlattices

    Science.gov (United States)

    Monozon, B. S.; Schmelcher, P.

    2017-02-01

    Wannier-Mott excitons in a semiconductor layered superlattice (SL) are investigated analytically for the case that the period of the superlattice is much smaller than the 2D exciton Bohr radius. Additionally we assume the presence of a longitudinal external static electric field directed parallel to the SL axis. The exciton states and the optical absorption coefficient are derived in the tight-binding and adiabatic approximations. Strong and weak electric fields providing spatially localized and extended electron and hole states, respectively, are studied. The dependencies of the exciton states and the exciton absorption spectrum on the SL parameters and the electric field strength are presented in an explicit form. We focus on the fine structure of the ground quasi-2D exciton level formed by the series of closely spaced energy levels adjacent from the high frequencies. These levels are related to the adiabatically slow relative exciton longitudinal motion governed by the potential formed by the in-plane exciton state. It is shown that the external electric fields compress the fine structure energy levels, decrease the intensities of the corresponding optical peaks and increase the exciton binding energy. A possible experimental study of the fine structure of the exciton electroabsorption is discussed.

  12. Relaxation of nonthermal hh and lh excitons in ZnSe quantum wells

    DEFF Research Database (Denmark)

    Kalt, H.; Hoffmann, J.; Umlauff, M.

    1998-01-01

    The strong exciton-LO phonon coupling in ZnSe QWs gives a direct access to the relaxation dynamics of nonthermal, free heavy-hole and light-hole excitons. Narrow hot-exciton distributions can be generated by LO-phonon assisted exciton formation. The thermalization of these excitons is monitored...

  13. Suppression of exciton-exciton annihilation in tungsten disulfide monolayers encapsulated by hexagonal boron nitrides

    Science.gov (United States)

    Hoshi, Yusuke; Kuroda, Takashi; Okada, Mitsuhiro; Moriya, Rai; Masubuchi, Satoru; Watanabe, Kenji; Taniguchi, Takashi; Kitaura, Ryo; Machida, Tomoki

    2017-06-01

    We investigates exciton-exciton annihilation (EEA) in tungsten disulfide (W S2) monolayers encapsulated by hexagonal boron nitride (hBN). It is revealed that decay signals observed by time-resolved photoluminescence (PL) are not strongly dependent on the exciton densities of hBN-encapsulated W S2 monolayers (W S2/hBN ) . In contrast, the sample without the bottom hBN layer (W S2/Si O2) exhibits a drastic decrease of decay time with increasing exciton density due to the appearance of a rapid PL decay component, signifying nonradiative EEA-mediated recombination. Furthermore, the EEA rate constant of W S2/hBN was determined as (6.3 ±1.7 ) ×10-3c m2s-1 , being about 2 orders of magnitude smaller than that of W S2/Si O2 . Thus, the observed EEA rate reduction played a key role in enhancing luminescence intensity at high exciton densities in the W S2 monolayer.

  14. Multiple Exciton Generation in Colloidal Nanocrystals

    Directory of Open Access Journals (Sweden)

    Charles Smith

    2013-12-01

    Full Text Available In a conventional solar cell, the energy of an absorbed photon in excess of the band gap is rapidly lost as heat, and this is one of the main reasons that the theoretical efficiency is limited to ~33%. However, an alternative process, multiple exciton generation (MEG, can occur in colloidal quantum dots. Here, some or all of the excess energy is instead used to promote one or more additional electrons to the conduction band, potentially increasing the photocurrent of a solar cell and thereby its output efficiency. This review will describe the development of this field over the decade since the first experimental demonstration of multiple exciton generation, including the controversies over experimental artefacts, comparison with similar effects in bulk materials, and the underlying mechanisms. We will also describe the current state-of-the-art and outline promising directions for further development.

  15. Microcavity controlled coupling of excitonic qubits

    CERN Document Server

    Albert, F; Kasprzak, J; Strauß, M; Schneider, C; Höfling, S; Kamp, M; Forchel, A; Reitzenstein, S; Muljarov, E A; Langbein, W

    2012-01-01

    Controlled non-local energy and coherence transfer enables light harvesting in photosynthesis and non-local logical operations in quantum computing. The most relevant mechanism of coherent coupling of distant qubits is coupling via the electromagnetic field. Here, we demonstrate the controlled coherent coupling of spatially separated excitonic qubits via the photon mode of a solid state microresonator. This is revealed by two-dimensional spectroscopy of the sample's coherent response, a sensitive and selective probe of the coherent coupling. The experimental results are quantitatively described by a rigorous theory of the cavity mediated coupling within a cluster of quantum dots excitons. Having demonstrated this mechanism, it can be used in extended coupling channels - sculptured, for instance, in photonic crystal cavities - to enable a long-range, non-local wiring up of individual emitters in solids.

  16. Can Natural Sunlight Induce Coherent Exciton Dynamics?

    CERN Document Server

    Olšina, Jan; Wang, Chen; Cao, Jianshu

    2014-01-01

    Excitation of a model photosynthetic molecular aggregate by incoherent sunlight is systematically examined. For a closed system, the excited state coherence induced by the sunlight oscillates with an average amplitude that is inversely proportional to the excitonic gap, and reaches a stationary amplitude that depends on the temperature and coherence time of the radiation field. For an open system, the light-induced dynamical coherence relaxes to a static coherence determined by the non-canonical thermal distribution resulting from the entanglement with the phonon bath. The decay of the excited state population to the common ground state establishes a non-equilibrium steady-state flux driven by the sunlight, and it defines a time window to observe the transition from dynamical to static coherence. For the parameters relevant to photosynthetic systems, the exciton dynamics initiated by the sunlight exhibits a non-negligible amount of dynamical coherence (quantum beats) on the sub-picosecond timescale; however, ...

  17. Excitonic and photonic processes in materials

    CERN Document Server

    Williams, Richard

    2015-01-01

    This book is expected to present state-of-the-art understanding of a selection of excitonic and photonic processes in useful materials from semiconductors to insulators to metal/insulator nanocomposites, both inorganic and organic.  Among the featured applications are components of solar cells, detectors, light-emitting devices, scintillators, and materials with novel optical properties.  Excitonic properties are particularly important in organic photovoltaics and light emitting devices, as also in questions of the ultimate resolution and efficiency of new-generation scintillators for medical diagnostics,  border security, and nuclear nonproliferation.  Novel photonic and optoelectronic applications benefit from new material combinations and structures to be discussed.

  18. Exciton Polaritons in Microcavities New Frontiers

    CERN Document Server

    Sanvitto, Daniele

    2012-01-01

    In the past decade, there has been a burst of new and fascinating physics associated to the unique properties of two-dimensional exciton polaritons, their recent demonstration of condensation under non-equilibrium conditions and all the related quantum phenomena, which have stimulated extensive research work. This monograph summarizes the current state of the art of research on exciton polaritons in microcavities: their interactions, fast dynamics, spin-dependent phenomena, temporal and spatial coherence, condensation under non-equilibrium conditions, related collective quantum phenomena and most advanced applications. The monograph is written by the most active authors who have strongly contributed to the advances in this area. It is of great interests to both physicists approaching this subject for the first time, as well as a wide audience of experts in other disciplines who want to be updated on this fast moving field.

  19. Energy spectrum of an exciton in a CdSe/ZnTe type-II core/shell spherical quantum dot

    Science.gov (United States)

    Chafai, A.; Dujardin, F.; Essaoudi, I.; Ainane, A.

    2017-01-01

    The binding energy of an exciton inside a CdSe/ZnTe core/shell spherical quantum dot was theoretically examined taking into account the dependence of the dielectric constant and charge carriers effective mass on radius, and using the envelope function approximation. Such a structure presents original optical and electronic properties because of the spatial separation of electrons and holes caused by the type-II alignment of energy states. The mean distance between the electron and hole was calculated variationally using a trial function taking into account the coulomb interaction between charge carriers. Our numerical results provide a description to the size dependence of the binding energy of an exciton inside a core/shell nanoheterostructure type-II. Indeed, by controlling the inner and outer radii, we can precisely control the energy spectrum of the exciton.

  20. Ultracold Gas of Excitons in Traps

    Science.gov (United States)

    2012-06-08

    Thomas,, G. Grosso,, M. Remeika,, A. T. Hammack,, A. D. Meyertholen,, M. M. Fogler ,, L.V. Butov,, M. Hanson,, A. C. Gossard. Trapping Indirect...M. Fogler , L. V. Butov, A. V. Kavokin, K. L. Campman, A. A. High, A. C. Gossard. Spontaneous coherence in a cold exciton gas, Nature, (03 2012...56:19 7 A. High, A. Thomas, G. Grosso, M. Remeika, A. Hammack, A. Meyertholen, M. Fogler , L. Butov, M. Hanson, A. Gossard. Trapping Indirect

  1. Multiple Exciton Generation in Colloidal Silicon Nanocrystals

    Energy Technology Data Exchange (ETDEWEB)

    Beard, M. C.; Knutsen, K. P.; Yu, P.; Luther, J. M.; Song, Q.; Metzger, W. K.; Ellingson, R. J.; Nozik, A. M.

    2007-01-01

    Multiple exciton generation (MEG) is a process whereby multiple electron-hole pairs, or excitons, are produced upon absorption of a single photon in semiconductor nanocrystals (NCs) and represents a promising route to increased solar conversion efficiencies in single-junction photovoltaic cells. We report for the first time MEG yields in colloidal Si NCs using ultrafast transient absorption spectroscopy. We find the threshold photon energy for MEG in 9.5 nm diameter Si NCs (effective band gap {identical_to} Eg = 1.20 eV) to be 2.4 {+-} 0.1E{sub g} and find an exciton-production quantum yield of 2.6 {+-} 0.2 excitons per absorbed photon at 3.4E{sub g}. While MEG has been previously reported in direct-gap semiconductor NCs of PbSe, PbS, PbTe, CdSe, and InAs, this represents the first report of MEG within indirect-gap semiconductor NCs. Furthermore, MEG is found in relatively large Si NCs (diameter equal to about twice the Bohr radius) such that the confinement energy is not large enough to produce a large blue-shift of the band gap (only 80 meV), but the Coulomb interaction is sufficiently enhanced to produce efficient MEG. Our findings are of particular importance because Si dominates the photovoltaic solar cell industry, presents no problems regarding abundance and accessibility within the Earth's crust, and poses no significant environmental problems regarding toxicity.

  2. Transport Theory for Metals with Excitonic Instabilities

    OpenAIRE

    Breitkreiz, Maxim

    2015-01-01

    Metals with excitonic instabilities are multiband systems with significant electron-electron interaction. The electronic transport in such systems is affected by collective fluctuations of the electrons, leading to anomalous features in the measured transport coefficients. Many of these anomalies have not been well understood because the transport mechanisms in these systems tend to be rather complex. The complexity arises, on the one hand, from the multiband nature and, on the other, fro...

  3. Singlet exciton fission in nanostructured organic solar cells.

    Science.gov (United States)

    Jadhav, Priya J; Mohanty, Aseema; Sussman, Jason; Lee, Jiye; Baldo, Marc A

    2011-04-13

    Singlet exciton fission is an efficient multiexciton generation process in organic molecules. But two concerns must be satisfied before it can be exploited in low-cost solution-processed organic solar cells. Fission must be combined with longer wavelength absorption in a structure that can potentially surpass the single junction limit, and its efficiency must be demonstrated in nanoscale domains within blended devices. Here, we report organic solar cells comprised of tetracene, copper phthalocyanine, and the buckyball C(60). Short wavelength light generates singlet excitons in tetracene. These are subsequently split into two triplet excitons and transported through the phthalocyanine. In addition, the phthalocyanine absorbs photons below the singlet exciton energy of tetracene. To test tetracene in nanostructured blends, we fabricate coevaporated bulk heterojunctions and multilayer heterojunctions of tetracene and C(60). We measure a singlet fission efficiency of (71 ± 18)%, demonstrating that exciton fission can efficiently compete with exciton dissociation on the nanoscale.

  4. Laser pulse induced multiple exciton kinetics in molecular ring structures

    Science.gov (United States)

    Hou, Xiao; Wang, Luxia

    2016-11-01

    Multiple excitons can be formed upon strong optical excitation of molecular aggregates and complexes. Based on a theoretical approach on exciton-exciton annihilation dynamics in supramolecular systems (May et al., 2014), exciton interaction kinetics in ring aggregates of two-level molecules are investigated. Excited by the sub-picosecond laser pulse, multiple excitons keep stable in the molecular ring shaped as a regular polygon. If the symmetry is destroyed by changing the dipole of a single molecule, the excitation of different molecules becomes not identical, and the changed dipole-dipole interaction initiates subsequent energy redistribution. Depending on the molecular distance and the dipole configuration, the kinetics undergo different types of processes, but all get stable within some hundreds of femtoseconds. The study of exciton kinetics will be helpful for further investigations of the efficiency of optical devices based on molecular aggregates.

  5. Exciton Mapping at Subwavelength Scales in Two-Dimensional Materials

    KAUST Repository

    Tizei, Luiz H. G.

    2015-03-01

    Spatially resolved electron-energy-loss spectroscopy (EELS) is performed at diffuse interfaces between MoS2 and MoSe2 single layers. With a monochromated electron source (20 meV) we successfully probe excitons near the interface by obtaining the low loss spectra at the nanometer scale. The exciton maps clearly show variations even with a 10 nm separation between measurements; consequently, the optical band gap can be measured with nanometer-scale resolution, which is 50 times smaller than the wavelength of the emitted photons. By performing core-loss EELS at the same regions, we observe that variations in the excitonic signature follow the chemical composition. The exciton peaks are observed to be broader at interfaces and heterogeneous regions, possibly due to interface roughness and alloying effects. Moreover, we do not observe shifts of the exciton peak across the interface, possibly because the interface width is not much larger than the exciton Bohr radius.

  6. Chiral topological excitons in the monolayer transition metal dichalcogenides

    Science.gov (United States)

    Gong, Z. R.; Luo, W. Z.; Jiang, Z. F.; Fu, H. C.

    2017-02-01

    We theoretically investigate the chiral topological excitons emerging in the monolayer transition metal dichalcogenides, where a bulk energy gap of valley excitons is opened up by a position dependent external magnetic field. We find two emerging chiral topological nontrivial excitons states, which exactly connects to the bulk topological properties, i.e., Chern number = 2. The dependence of the spectrum of the chiral topological excitons on the width of the magnetic field domain wall as well as the magnetic filed strength is numerically revealed. The chiral topological valley excitons are not only important to the excitonic transport due to prevention of the backscattering, but also give rise to the quantum coherent control in the optoelectronic applications.

  7. Bose-Einstein condensation of dipolar excitons in quantum wells

    Energy Technology Data Exchange (ETDEWEB)

    Timofeev, V B; Gorbunov, A V, E-mail: timofeev@issp.ac.r [Institute of Solid State Physics, Russian Academy of Sciences, 142432, Chernogolovka, Moscow region (Russian Federation)

    2009-02-01

    The experiments on Bose-Einstein condensation (BEC) of dipolar (spatially-indirect) excitons in the lateral traps in GaAs/AlGaAs Schottky-diode heterostructures with double and single quantum wells are presented. The condensed part of dipolar excitons under detection in the far zone is placed in k-space in the range which is almost two orders of magnitude less than thermal exciton wave vector. BEC occurs spontaneously in a reservoir of thermalized excitons. Luminescence images of Bose-condensate of dipolar excitons exhibit along perimeter of circular trap axially symmetrical spatial structures of equidistant bright spots which strongly depend on excitation power and temperature. By means of two-beam interference experiments with the use of cw and pulsed photoexcitation it was found that the state of dipolar exciton Bose-condensate is spatially coherent and the whole patterned luminescence configuration in real space is described by a common wave function.

  8. Excitonic Stark effect in MoS2 monolayers

    Science.gov (United States)

    Scharf, Benedikt; Frank, Tobias; Gmitra, Martin; Fabian, Jaroslav; Žutić, Igor; Perebeinos, Vasili

    2016-12-01

    We theoretically investigate excitons in MoS2 monolayers in an applied in-plane electric field. Tight-binding and Bethe-Salpeter equation calculations predict a quadratic Stark shift, of the order of a few meV for fields of 10 V/μ m , in the linear absorption spectra. The spectral weight of the main exciton peaks decreases by a few percent with an increasing electric field due to the exciton field ionization into free carriers as reflected in the exciton wave functions. Subpicosecond exciton decay lifetimes at fields of a few tens of V/μ m could be utilized in solar energy harvesting and photodetection. We find simple scaling relations of the exciton binding, radius, and oscillator strength with the dielectric environment and an electric field, which provides a path to engineering the MoS2 electro-optical response.

  9. Topological Excitonic Superfluids in Three Dimensions

    Science.gov (United States)

    Gilbert, Matthew; Hankiewicz, Ewelina; Kim, Youngseok

    2013-03-01

    We study the equilibrium and non-equilibrium properties of topological dipolar intersurface exciton condensates within time-reversal invariant topological insulators in three spatial dimensions without a magnetic field. We elucidate that, in order to correctly identify the proper pairing symmetry within the condensate order parameter, the full three-dimensional Hamiltonian must be considered. As a corollary, we demonstrate that only particles with similar chirality play a significant role in condensate formation. Furthermore, we find that the intersurface exciton condensation is not suppressed by the interconnection of surfaces in three-dimensional topological insulators as the intersurface polarizability vanishes in the condensed phase. This eliminates the surface current flow leaving only intersurface current flow through the bulk. We conclude by illustrating how the excitonic superfluidity may be identified through an examination of the terminal currents above and below the condensate critical current. Army Research Office (ARO) under contract number W911NF-09-1-0347, the Office of Naval Research (ONR) under contract number N0014-11-1-0728, and the Air Force Office of Scientific Research (AFOSR) under contract number FA9550-10-1-0459, DFG Grant HA 5893

  10. Microcavity controlled coupling of excitonic qubits.

    Science.gov (United States)

    Albert, F; Sivalertporn, K; Kasprzak, J; Strauß, M; Schneider, C; Höfling, S; Kamp, M; Forchel, A; Reitzenstein, S; Muljarov, E A; Langbein, W

    2013-01-01

    Controlled non-local energy and coherence transfer enables light harvesting in photosynthesis and non-local logical operations in quantum computing. This process is intuitively pictured by a pair of mechanical oscillators, coupled by a spring, allowing for a reversible exchange of excitation. On a microscopic level, the most relevant mechanism of coherent coupling of distant quantum bits--like trapped ions, superconducting qubits or excitons confined in semiconductor quantum dots--is coupling via the electromagnetic field. Here we demonstrate the controlled coherent coupling of spatially separated quantum dots via the photon mode of a solid state microresonator using the strong exciton-photon coupling regime. This is enabled by two-dimensional spectroscopy of the sample's coherent response, a sensitive probe of the coherent coupling. The results are quantitatively understood in a rigorous description of the cavity-mediated coupling of the quantum dot excitons. This mechanism can be used, for instance in photonic crystal cavity networks, to enable a long-range, non-local coherent coupling.

  11. Simultaneous observation of free and defect-bound excitons in CH3NH3PbI3 using four-wave mixing spectroscopy.

    Science.gov (United States)

    March, Samuel A; Clegg, Charlotte; Riley, Drew B; Webber, Daniel; Hill, Ian G; Hall, Kimberley C

    2016-12-15

    Solar cells incorporating organic-inorganic perovskite, which may be fabricated using low-cost solution-based processing, have witnessed a dramatic rise in efficiencies yet their fundamental photophysical properties are not well understood. The exciton binding energy, central to the charge collection process, has been the subject of considerable controversy due to subtleties in extracting it from conventional linear spectroscopy techniques due to strong broadening tied to disorder. Here we report the simultaneous observation of free and defect-bound excitons in CH3NH3PbI3 films using four-wave mixing (FWM) spectroscopy. Due to the high sensitivity of FWM to excitons, tied to their longer coherence decay times than unbound electron- hole pairs, we show that the exciton resonance energies can be directly observed from the nonlinear optical spectra. Our results indicate low-temperature binding energies of 13 meV (29 meV) for the free (defect-bound) exciton, with the 16 meV localization energy for excitons attributed to binding to point defects. Our findings shed light on the wide range of binding energies (2-55 meV) reported in recent years.

  12. Simultaneous observation of free and defect-bound excitons in CH3NH3PbI3 using four-wave mixing spectroscopy

    Science.gov (United States)

    March, Samuel A.; Clegg, Charlotte; Riley, Drew B.; Webber, Daniel; Hill, Ian G.; Hall, Kimberley C.

    2016-12-01

    Solar cells incorporating organic-inorganic perovskite, which may be fabricated using low-cost solution-based processing, have witnessed a dramatic rise in efficiencies yet their fundamental photophysical properties are not well understood. The exciton binding energy, central to the charge collection process, has been the subject of considerable controversy due to subtleties in extracting it from conventional linear spectroscopy techniques due to strong broadening tied to disorder. Here we report the simultaneous observation of free and defect-bound excitons in CH3NH3PbI3 films using four-wave mixing (FWM) spectroscopy. Due to the high sensitivity of FWM to excitons, tied to their longer coherence decay times than unbound electron- hole pairs, we show that the exciton resonance energies can be directly observed from the nonlinear optical spectra. Our results indicate low-temperature binding energies of 13 meV (29 meV) for the free (defect-bound) exciton, with the 16 meV localization energy for excitons attributed to binding to point defects. Our findings shed light on the wide range of binding energies (2–55 meV) reported in recent years.

  13. Exciton ionization in multilayer transition-metal dichalcogenides

    DEFF Research Database (Denmark)

    Pedersen, Thomas Garm; Latini, Simone; Thygesen, Kristian Sommer;

    2016-01-01

    Photodetectors and solar cells based on materials with strongly bound excitons rely crucially on field-assisted exciton ionization. We study the ionization process in multilayer transition-metal dichalcogenides (TMDs) within the Mott-Wannier model incorporating fully the pronounced anisotropy......-principles material parameters, an analysis of several important TMDs reveals WSe2 and MoSe2 to be superior for applications relying on ionization of direct and indirect excitons, respectively....

  14. Compensation of Dipolar-Exciton Spin Splitting in Magnetic Field

    OpenAIRE

    Gorbunov, A. V.; Timofeev, V. B.

    2012-01-01

    Magnetoluminescence of spatially indirect dipolar excitons collected in 25 nm GaAs/AlGaAs single quantum well within a lateral potential trap has been studied in perpendicular magnetic field in Faraday geometry. The paramagnetic spin splitting of the luminescence line of the heavy-hole excitons in the trap centre is completely compensated at magnetic fields below critical value, around 2 Tesla. The effect of spin-splitting compensation is caused by the exchange interaction in dense exciton Bo...

  15. Determination of Surface Exciton Energies by Velocity Resolved Atomic Desorption

    Energy Technology Data Exchange (ETDEWEB)

    Hess, Wayne P.; Joly, Alan G.; Beck, Kenneth M.; Sushko, Petr V.; Shluger, Alexander L.

    2004-08-20

    We have developed a new method for determining surface exciton band energies in alkali halides based on velocity-resolved atomic desorption (VRAD). Using this new method, we predict the surface exciton energies for K1, KBr, KC1, and NaC1 within +0.15 eV. Our data, combined with the available EELS data for alkali fluorides, demonstrate a universal linear correlation with the inverse inter-atomic distance in these materials. The results suggest that surface excitons exist in all alkali halides and their excitation energies can be predicted from the known bulk exciton energies and the obtained correlation plot.

  16. Exciton migration and quenching in poly(propylene imine) dendrimers

    Science.gov (United States)

    Minevičiūtė, I.; Gulbinas, V.; Franckevičius, M.; Vaišnoras, R.; Marcos, M.; Serrano, J. L.

    2009-05-01

    Exciton migration between chromophore groups of the poly(propylene imine) dendrimer in chloroform solution and in solid state has been investigated by means of the time-resolved fluorescence measurements. Fluorescence decay kinetics, dynamic band shift and the depolarization rate have been analyzed. Exciton migration in a single dendrimer was found to be slow in comparison with temperature-dependent chromophore reorientation time of 150-600 ps. In a solid state chromophore groups form collective excitonic states responsible for the dendrimer film fluorescence. Exciton migration and localization to the lowest energy sites within the distributed density of states take place on a subnanosecond-nanosecond time scale.

  17. Revealing and Characterizing Dark Excitons Through Coherent Multidimensional Spectroscopy

    CERN Document Server

    Tollerud, Jonathan O; Davis, Jeffrey A

    2016-01-01

    Dark excitons are of fundamental importance in a broad range of contexts, but are difficult to study using conventional optical spectroscopy due to their weak interaction with light. We show how coherent multidimensional spectroscopy can reveal and characterize dark states. Using this approach, we identify different types of dark excitons in InGaAs/GaAs quantum wells and determine details regarding lifetimes, homogeneous and inhomogeneous linewidths, broadening mechanisms and coupling strengths. The observations of coherent coupling between bright and dark excitons hint at a role for a multi-step process by which excitons in the barrier can relax into the quantum wells.

  18. Exciton management in organic photovoltaic multidonor energy cascades.

    Science.gov (United States)

    Griffith, Olga L; Forrest, Stephen R

    2014-05-14

    Multilayer donor regions in organic photovoltaics show improved power conversion efficiency when arranged in decreasing exciton energy order from the anode to the acceptor interface. These so-called "energy cascades" drive exciton transfer from the anode to the dissociating interface while reducing exciton quenching and allowing improved overlap with the solar spectrum. Here we investigate the relative importance of exciton transfer and blocking in a donor cascade employing diphenyltetracene (D1), rubrene (D2), and tetraphenyldibenzoperiflanthene (D3) whose optical gaps monotonically decrease from D1 to D3. In this structure, D1 blocks excitons from quenching at the anode, D2 accepts transfer of excitons from D1 and blocks excitons at the interface between D2 and D3, and D3 contributes the most to the photocurrent due to its strong absorption at visible wavelengths, while also determining the open circuit voltage. We observe singlet exciton Förster transfer from D1 to D2 to D3 consistent with cascade operation. The power conversion efficiency of the optimized cascade OPV with a C60 acceptor layer is 7.1 ± 0.4%, which is significantly higher than bilayer devices made with only the individual donors. We develop a quantitative model to identify the dominant exciton processes that govern the photocurrent generation in multilayer organic structures.

  19. Molecular dissection of the contribution of negatively and positively charged residues in S2, S3, and S4 to the final membrane topology of the voltage sensor in the K+ channel, KAT1.

    Science.gov (United States)

    Sato, Yoko; Sakaguchi, Masao; Goshima, Shinobu; Nakamura, Tatsunosuke; Uozumi, Nobuyuki

    2003-04-11

    Voltage-dependent ion channels control changes in ion permeability in response to membrane potential changes. The voltage sensor in channel proteins consists of the highly positively charged segment, S4, and the negatively charged segments, S2 and S3. The process involved in the integration of the protein into the membrane remains to be elucidated. In this study, we used in vitro translation and translocation experiments to evaluate interactions between residues in the voltage sensor of a hyperpolarization-activated potassium channel, KAT1, and their effect on the final topology in the endoplasmic reticulum (ER) membrane. A D95V mutation in S2 showed less S3-S4 integration into the membrane, whereas a D105V mutation allowed S4 to be released into the ER lumen. These results indicate that Asp(95) assists in the membrane insertion of S3-S4 and that Asp(105) helps in preventing S4 from being releasing into the ER lumen. The charge reversal mutation, R171D, in S4 rescued the D105R mutation and prevented S4 release into the ER lumen. A series of constructs containing different C-terminal truncations of S4 showed that Arg(174) was required for correct integration of S3 and S4 into the membrane. Interactions between Asp(105) and Arg(171) and between negative residues in S2 or S3 and Arg(174) may be formed transiently during membrane integration. These data clarify the role of charged residues in S2, S3, and S4 and identify posttranslational electrostatic interactions between charged residues that are required to achieve the correct voltage sensor topology in the ER membrane.

  20. Matrix assisted ionization: new aromatic and nonaromatic matrix compounds producing multiply charged lipid, peptide, and protein ions in the positive and negative mode observed directly from surfaces.

    Science.gov (United States)

    Li, Jing; Inutan, Ellen D; Wang, Beixi; Lietz, Christopher B; Green, Daniel R; Manly, Cory D; Richards, Alicia L; Marshall, Darrell D; Lingenfelter, Steven; Ren, Yue; Trimpin, Sarah

    2012-10-01

    Matrix assisted inlet ionization (MAII) is a method in which a matrix:analyte mixture produces mass spectra nearly identical to electrospray ionization without the application of a voltage or the use of a laser as is required in laserspray ionization (LSI), a subset of MAII. In MAII, the sample is introduced by, for example, tapping particles of dried matrix:analyte into the inlet of the mass spectrometer and, therefore, permits the study of conditions pertinent to the formation of multiply charged ions without the need of absorption at a laser wavelength. Crucial for the production of highly charged ions are desolvation conditions to remove matrix molecules from charged matrix:analyte clusters. Important factors affecting desolvation include heat, vacuum, collisions with gases and surfaces, and even radio frequency fields. Other parameters affecting multiply charged ion production is sample preparation, including pH and solvent composition. Here, findings from over 100 compounds found to produce multiply charged analyte ions using MAII with the inlet tube set at 450 °C are presented. Of the compounds tested, many have -OH or -NH(2) functionality, but several have neither (e.g., anthracene), nor aromaticity or conjugation. Binary matrices are shown to be applicable for LSI and solvent-free sample preparation can be applied to solubility restricted compounds, and matrix compounds too volatile to allow drying from common solvents. Our findings suggest that the physical properties of the matrix such as its morphology after evaporation of the solvent, its propensity to evaporate/sublime, and its acidity are more important than its structure and functional groups.

  1. Binding energy of exciton in a nanowire superlattice in magnetic and electric fields

    Energy Technology Data Exchange (ETDEWEB)

    Galvan-Moya, J E; Gutierrez, W [Escuela de Fisica, Universidad Industrial de Santander, Bucaramanga, Colombia A.A. 678 (Colombia); Moscoso, C, E-mail: edogalvan@gmail.co [Departamento de Fisica, Universidad Nacional de Colombia, Bogota, Colombia A.A. 5997 (Colombia)

    2010-02-01

    We study the binding energy of excitons in a cylindrical GaAs/Ga{sub 1-x}Al{sub x}As nanowire superlattice, embedded in Ga{sub 1-y}Al{sub y}As matrix, in the presence of magnetic and electric fields applied parallel to the growth direction. We express the exciton trial function as a product of one-particle wave functions of the electron and the hole with variationally determined envelope function, which describes the exciton intrinsic properties and depends only on the electron-hole separation. By using a functional derivative technique, we derive a differential equation for this envelope function, which we solve numerically. By varying the wire radius, interwell barrier width and well sizes we obtain binding energies ranging in character from one for strongly coupled superlattice to that for a system of stack of isolated disks. The behaviour of the binding energies and the charge distributions as functions of the interwell coupling, well sizes, and the external fields is consistently described with our simple formalism.

  2. Intermolecular Singlet and Triplet Exciton Transfer Integrals from Many-Body Green's Functions Theory.

    Science.gov (United States)

    Wehner, Jens; Baumeier, Björn

    2017-03-08

    A general approach to determine orientation and distance-dependent effective intermolecular exciton transfer integrals from many-body Green's functions theory is presented. On the basis of the GW approximation and the Bethe-Salpeter equation (BSE), a projection technique is employed to obtain the excitonic coupling by forming the expectation value of a supramolecular BSE Hamiltonian with electron-hole wave functions for excitations localized on two separated chromophores. Within this approach, accounting for the effects of coupling mediated by intermolecular charge transfer (CT) excitations is possible via perturbation theory or a reduction technique. Application to model configurations of pyrene dimers shows an accurate description of short-range exchange and long-range Coulomb interactions for the coupling of singlet and triplet excitons. Computational parameters, such as the choice of the exchange-correlation functional in the density-functional theory (DFT) calculations that underly the GW-BSE steps and the convergence with the number of included CT excitations, are scrutinized. Finally, an optimal strategy is derived for simulations of full large-scale morphologies by benchmarking various approximations using pairs of dicyanovinyl end-capped oligothiophenes (DCV5T), which are used as donor material in state-of-the-art organic solar cells.

  3. Next Generation Photovoltaics Based on Multiple Exciton Generation in Quantum Dot Solar Cells

    Science.gov (United States)

    Nozik, Arthur J.

    Next Generation solar cells based onMultiple Exciton Generation (MEG) in semiconductorquantum dots (QDs) are described. This application of QDs depends upon efficient MEG in QDs incorporated into PV cells, followed by efficient exciton splitting into free electrons and holes and their efficient separation and collection in the cell contacts to produce multiple free carriers per absorbed photon. Using time-resolved transient absorption, bleaching, photoluminescence and THz spectroscopy, MEG has been initially confirmed in several Group IV-VI, III-V, II-VI, and IV colloidal semiconductor QDs. Some controversy using these techniques have now been attributed to effects of the variable of the QD surface chemisty and under certain conditions to artifacts arising from long-lived trapping of photoinduced charge; in our opinion these controversies have been resolved and are discussed here. Furthermore, various photovoltaic cell architectures utilizing QDs have recently been constructed and the photocurrent and photovoltage characterisitics have been studied. These photocurrent measurements provide a more direct measurement of MEG since the photogenerated carriers are counted directly via the current, and they are very consistent with the QYs of MEG reported using the proper spectroscopic techniques; thus, these new photocurrent measurements confirm the existence of enhanced exciton and carrier multiplication in QDs. The past work and prognosis for QD-based Next Generation PV cells based on MEG are discussed.

  4. Assessment of Density Functional Methods for Exciton Binding Energies and Related Optoelectronic Properties

    CERN Document Server

    Lee, Jui-Che; Lin, Shiang-Tai

    2015-01-01

    The exciton binding energy, the energy required to dissociate an excited electron-hole pair into free charge carriers, is one of the key factors to the optoelectronic performance of organic materials. However, it remains unclear whether modern quantum-mechanical calculations, mostly based on Kohn-Sham density functional theory (KS-DFT) and time-dependent density functional theory (TDDFT), are reliably accurate for exciton binding energies. In this study, the exciton binding energies and related optoelectronic properties (e.g., the ionization potentials, electron affinities, fundamental gaps, and optical gaps) of 121 small- to medium-sized molecules are calculated using KS-DFT and TDDFT with various density functionals. Our KS-DFT and TDDFT results are compared with those calculated using highly accurate CCSD and EOM-CCSD methods, respectively. The omegaB97, omegaB97X, and omegaB97X-D functionals are shown to generally outperform (with a mean absolute error of 0.36 eV) other functionals for the properties inve...

  5. Hole-exciton interaction induced high field decay of magneto-electroluminescence in Alq{sub 3}-based organic light-emitting diodes at room temperature

    Energy Technology Data Exchange (ETDEWEB)

    Zhang, Tingting; Holford, D. F.; Gu, Hang; Kreouzis, T. [Materials Research Institute and School of Physics and Astronomy, Queen Mary University of London, Mile End Road, London E1 4NS (United Kingdom); Zhang, Sijie, E-mail: Sijie.zhang@scu.edu.cn, E-mail: w.gillin@qmul.ac.uk [College of Physical Science and Technology, Sichuan University, Chengdu 610064 (China); Gillin, W. P., E-mail: Sijie.zhang@scu.edu.cn, E-mail: w.gillin@qmul.ac.uk [Materials Research Institute and School of Physics and Astronomy, Queen Mary University of London, Mile End Road, London E1 4NS (United Kingdom); College of Physical Science and Technology, Sichuan University, Chengdu 610064 (China)

    2016-01-11

    The magnetic field effects on the electroluminescence of aluminium tris-(8-hydroxyqinoline) (Alq{sub 3}) based organic light emitting diodes have been investigated by varying the electron/hole ratio in the emissive layer. Experimental results reveal that a negative high field effect in the magneto-electroluminescence (MEL) can be found in devices with very low triplet exciton concentration at room temperature. This suggests triplet-triplet annihilation cannot be used to explain the negative high field MEL in the Alq{sub 3} system. Our results suggest that hole-exciton interaction may be the origin of the negative high field MEL and also, in parallel with this interaction, there is also the more common positive high field process occurring which has been tentatively attributed to electron-exciton interactions. The competition between these different processes decides the final shape of the MEL at high fields.

  6. Optics of plasmon-exciton nanomaterials.

    Science.gov (United States)

    Sukharev, Maxim; Nitzan, Abraham

    2017-08-14

    This review provides a brief introduction to the physics of coupled exciton-plasmon systems, the theoretical description and experimental manifestation of such phenomena, followed by an account of the state-of-the-art methodology for the numerical simulations of such phenomena and supplemented by a number of FORTRAN codes, by which the interested reader can introduce himself/herself to the practice of such simulations. Applications to CW light scattering as well as transient response and relaxation are described. Particular attention is given to so-called strong coupling limit, where the hybrid exciton-plasmon nature of the system response is strongly expressed. While traditional descriptions of such phenomena usually rely on analysis of the electromagnetic response of inhomogeneous dielectric environments that individually support plasmon and exciton excitations, here we explore also the consequences of a more detailed description of the molecular environment in terms of its quantum density matrix (applied in a mean field approximation level). Such a description makes it possible to account for characteristics that cannot be described by the dielectric response model: the effects of dephasing on the molecular response on one hand, and nonlinear response on the other. It also highlights the still missing important ingredients in the numerical approach, in particular its limitation to a classical description of the radiation field and its reliance on a mean field description of the many-body molecular system. We end our review with an outlook to the near future, where these limitations will be addressed and new novel applications of the numerical approach will be pursued. © 2017 IOP Publishing Ltd.

  7. The P9 pocket of HLA-DQ2 (non-Aspbeta57) has no particular preference for negatively charged anchor residues found in other type 1 diabetes-predisposing non-Aspbeta57 MHC class II molecules

    DEFF Research Database (Denmark)

    Quarsten, H; Paulsen, G; Johansen, B H;

    1998-01-01

    residues at P9 and that there is no particular preference for binding peptides with negatively charged residues at this position. The specificity of the P9 pocket in the mutated DQ molecule is altered, indicating that the beta57 residue contributes to determining the specificity of the P9 pocket. Our data...... anchor residues. We have investigated the specificity of the P9 pocket of the type 1 diabetes-associated DQ2 molecule and in particular examined for charge effects at this anchor position. Different approaches were undertaken. We analyzed binding of a high-affinity binding ligand and P9-substituted...... variants of this peptide, and we analyzed the binding of a set of synthetic random peptide libraries. The binding analyses were performed with wild-type DQ2 and a mutated DQ2 with Ala at beta57 substituted with Asp. Our results indicate that the wild-type DQ2 (non-Aspbeta57) prefers large hydrophobic...

  8. Optical properties of localized excitons in semiconductor nanostructures

    DEFF Research Database (Denmark)

    Leosson, Kristjan; Hvam, Jørn Märcher; Langbein, Wolfgang Werner;

    2002-01-01

    Denne afhandling beskriver optiske undersøgelser af lokaliserede excitoner i III-V halvleder nanostrukturer. Det drejer sig især om tredimensional lokalisering af excitoner i to typer af selvorganiserede systemer, nemlig kvantebrønde med fluktuerende lagtykkelse og såkaldte selv-dannede kvantepun...

  9. Exciton dephasing in ZnSe quantum wires

    DEFF Research Database (Denmark)

    Wagner, Hans Peter; Langbein, Wolfgang Werner; Hvam, Jørn Märcher

    1998-01-01

    The homogeneous linewidths of excitons in wet-etched ZnSe quantum wires of lateral sizes down to 23 nm are studied by transient four-wave mixing. The low-density dephasing time is found to increase with decreasing wire width. This is attributed mainly to a reduction of electron-exciton scattering...

  10. Molecular weight dependence of exciton diffusion in poly(3-hexylthiophene)

    DEFF Research Database (Denmark)

    Masri, Zarifi; Ruseckas, Arvydas; Emelianova, Evguenia V.

    2013-01-01

    A joint experimental and theoretical study of singlet exciton diffusion in spin-coated poly(3-hexylthiophene) (P3HT) films and its dependence on molecular weight is presented. The results show that exciton diffusion is fast along the co-facial π–π aggregates of polymer chromophores and about 100...

  11. Coherent secondary emission from resonantly excited two-exciton states

    DEFF Research Database (Denmark)

    Birkedal, Dan

    2000-01-01

    to the nonlinear susceptibility. The method exploits that emission from two-exciton coherences can occur in non-specular directions, with the recoil momentum taken up by an exciton left behind in the sample. Using ultrafast spectral interferometry we demonstrate the presence of this new coherent component...

  12. Coherent excitonic nonlinearity versus inhomogeneous broadening in single quantum wells

    DEFF Research Database (Denmark)

    Langbein, Wolfgang Werner; Borri, Paola; Hvam, Jørn Märcher;

    1998-01-01

    The coherent response of excitons in semiconductor nanostructures, as measured in four wave mixing (FWM) experiments, depends strongly on the inhomogeneous broadening of the exciton transition. We investigate GaAs-AlGaAs single quantum wells (SQW) of 4 nm to 25 nm well width. Two main mechanisms...

  13. Bose Condensation of Interwell Excitons in Double Quantum Wells

    DEFF Research Database (Denmark)

    Larionov, A. V.; Timofeev, V. B.; Ni, P. A.

    2002-01-01

    in the domain. With a rise in temperature, this line disappears from the spectrum (Tc 3.4 K). The observed phenomenon is attributed to Bose–Einstein condensation in a quasi-two-dimensional system of interwell excitons. In the temperature range studied (1.5–3.4 K), the critical exciton density and temperature...

  14. Magnetic excitons in singlet-ground-state ferromagnets

    DEFF Research Database (Denmark)

    Birgeneau, R.J.; Als-Nielsen, Jens Aage; Bucher, E.

    1971-01-01

    The authors report measurements of the dispersion of singlet-triplet magnetic excitons as a function of temperature in the singlet-ground-state ferromagnets fcc Pr and Pr3Tl. Well-defined excitons are observed in both the ferromagnetic and paramagnetic regions, but with energies which are nearly...

  15. Bose Condensation of Interwell Excitons in Double Quantum Wells

    DEFF Research Database (Denmark)

    Larionov, A. V.; Timofeev, V. B.; Ni, P. A.

    2002-01-01

    The luminescence of interwell excitons in double quantum wells GaAs/AlGaAs (n–i–n heterostructures) with large-scale fluctuations of random potential in the heteroboundary planes was studied. The properties of excitons whose photoexcited electron and hole are spatially separated in the neighboring...

  16. Weakly disordered two-dimensional Frenkel excitons

    Science.gov (United States)

    Boukahil, A.; Zettili, Nouredine

    2004-03-01

    We report the results of studies of the optical properties of weakly disordered two- dimensional Frenkel excitons in the Coherent Potential Approximation (CPA). An approximate complex Green's function for a square lattice with nearest neighbor interactions is used in the self-consistent equation to determine the coherent potential. It is shown that the Density of States is very much affected by the logarithmic singularities in the Green's function. Our CPA results are in excellent agreement with previous investigations by Schreiber and Toyozawa using the Monte Carlo simulation.

  17. Excitons in conjugated polymers from first principles

    Science.gov (United States)

    van der Horst, J.-W.; Bobbert, P. A.; Pasveer, W. F.; Michels, M. A. J.; Brocks, G.; Kelly, P. J.

    2002-08-01

    By a combination of ab-initio computational techniques, based on density-functional theory, GW theory, and the Bethe-Salpeter equation, we study the opto-electronic properties of several conjugated polymers and in particular the properties of excitons. We study three different situations: (I) an isolated polymer chain, (II) a chain embedded in a dielectric medium, and (III) a polymer crystal. Surprisingly, the results obtained for situation (II) generally agree best with experiment. We discuss possible reasons for this rule and an interesting exception.

  18. Directing energy transport in organic photovoltaic cells using interfacial exciton gates.

    Science.gov (United States)

    Menke, S Matthew; Mullenbach, Tyler K; Holmes, Russell J

    2015-04-28

    Exciton transport in organic semiconductors is a critical, mediating process in many optoelectronic devices. Often, the diffusive and subdiffusive nature of excitons in these systems can limit device performance, motivating the development of strategies to direct exciton transport. In this work, directed exciton transport is achieved with the incorporation of exciton permeable interfaces. These interfaces introduce a symmetry-breaking imbalance in exciton energy transfer, leading to directed motion. Despite their obvious utility for enhanced exciton harvesting in organic photovoltaic cells (OPVs), the emergent properties of these interfaces are as yet uncharacterized. Here, directed exciton transport is conclusively demonstrated in both dilute donor and energy-cascade OPVs where judicious optimization of the interface allows exciton transport to the donor-acceptor heterojunction to occur considerably faster than when relying on simple diffusion. Generalized systems incorporating multiple exciton permeable interfaces are also explored, demonstrating the ability to further harness this phenomenon and expeditiously direct exciton motion, overcoming the diffusive limit.

  19. Superfluid phase transition in two-dimensional excitonic systems

    Energy Technology Data Exchange (ETDEWEB)

    Apinyan, V.; Kopeć, T.K., E-mail: kopec@int.pan.wroc.pl

    2014-03-01

    We study the superfluid phase transition in the two-dimensional (2D) excitonic system. Employing the extended Falicov–Kimball model (EFKM) and considering the local quantum correlations in the system composed of conduction band electrons and valence band holes we demonstrate the existence of the excitonic insulator (EI) state in the system. We show that at very low temperatures, the particle phase stiffness in the pure-2D excitonic system, governed by the non-local cross correlations, is responsible for the vortex–antivortex binding phase-field state, known as the Berezinskii–Kosterlitz–Thouless (BKT) superfluid state. We demonstrate that the existence of excitonic insulator phase is a necessary prerequisite, leading to quasi-long-range order in the 2D excitonic system.

  20. Optically induced rotation of a quantum dot exciton spin

    CERN Document Server

    Poem, E; Kodriano, Y; Benny, Y; Khatsevich, S; Avron, J E; Gershoni, D

    2011-01-01

    We demonstrate control over the spin state of a semiconductor quantum dot exciton using a polarized picosecond laser pulse slightly detuned from a biexciton resonance. The control pulse follows an earlier pulse, which generates an exciton and initializes its spin state as a coherent superposition of its two non-degenerate eigenstates. The control pulse preferentially couples one component of the exciton state to the biexciton state, thereby rotating the exciton's spin direction. We detect the rotation by measuring the polarization of the exciton spectral line as a function of the time-difference between the two pulses. We show experimentally and theoretically how the angle of rotation depends on the detuning of the second pulse from the biexciton resonance.

  1. Excitons in quantum-dot quantum-well nanoparticles

    Institute of Scientific and Technical Information of China (English)

    史俊杰

    2002-01-01

    A variational calculation is presented for the ground-state properties of excitons confined in spherical core-shell quantum-dot quantum-well (QDQW) nanoparticles. The relationship between the exciton states and structure parameters of QDQW nanoparticles is investigated, in which both the heavy-hole and the light-hole exciton states are considered. The results show that the confinement energies of the electron and hole states and the exciton binding energies depend sensitively on the well width and core radius of the QDQW structure. A detailed comparison between the heavy-hole and light-hole exciton states is given. Excellent agreement is found between experimental results and our calculated 1se-1sh transition energies.

  2. Excitons in conjugated polymers: wavefunctions, symmetries, and quantum numbers.

    Science.gov (United States)

    Barford, William; Paiboonvorachat, Nattapong

    2008-10-28

    We introduce a mapping from configuration interaction singles wavefunctions, expressed as linear combinations of particle-hole excitations between Hartree-Fock molecular orbitals, to real-space exciton wavefunctions, expressed as linear combinations of particle-hole excitations between localized Wannier functions. The exciton wavefunction is a two-dimensional amplitude for the exciton center-of-mass coordinate, R, and the electron-hole separation (or relative coordinate), r, having an exact analogy to one-dimensional hydrogenlike wavefunctions. We describe the excitons by their appropriate quantum numbers, namely, the principle quantum number, n, associated with r and the center-of-mass pseudomomentum quantum number, j, associated with R. In addition, for models with particle-hole symmetry, such as the Pariser-Parr-Pople model, we emphasize the connection between particle-hole symmetry and particle-hole parity. The method is applied to the study of excitons in trans-polyacetylene and poly(para-phenylene).

  3. Exciton-Phonon Dynamics with Long-Range Interaction

    CERN Document Server

    Laskin, Nick

    2011-01-01

    Exciton-phonon dynamics on a 1D lattice with long-range exciton-exciton interaction have been introduced and elaborated. Long-range interaction leads to a nonlocal integral term in the motion equation of the exciton subsystem if we go from discrete to continuous space. In some particular cases for power-law interaction, the integral term can be expressed through a fractional order spatial derivative. A system of two coupled equations has been obtained, one is a fractional differential equation for the exciton subsystem, the other is a standard differential equation for the phonon subsystem. These two equations present a new fundamental framework to study nonlinear dynamics with long-range interaction. New approaches to model the impact of long-range interaction on nonlinear dynamics are: fractional generalization of Zakharov system, Hilbert-Zakharov system, Hilbert-Ginzburg-Landau equation and nonlinear Hilbert-Schrodinger equation. Nonlinear fractional Schrodinger equation and fractional Ginzburg-Landau equa...

  4. Speciation and fractionation of heavy metals in soil experimentally contaminated with Pb, Cd, Cu and Zn together and effects on soil negative surface charge

    Institute of Scientific and Technical Information of China (English)

    2002-01-01

    Speciation of heavy metals in soil subsamplesexperimentally loaded with Pb, Cd, Cu and Zn in orthogonal designwas investigated by sequential extraction, and operationallydefined as water-soluble and exchangeable(SE), weakly specificadsorbed(WSA), Fe and Mn oxides-bound(OX) and organic-bound(ORG).The results show that speciation of heavy metals in the soilsubsamples depended on their kinds. About 90% of Cd and 75% of Znexisted in soil subsamples in the SE fraction. Lead and Cu existedin soil subsamples as SE, WSA and OX fractions simultaneously,although SE was still the major fraction. Organic-bound heavymetals were not clearly apparent in all the soil subsamples. Theconcentration of some heavy metal speciation in soil subsamplesshowed good correlation with ionic impulsion of soil, especiallyfor the SE fraction. Continuous saturation of soil subsamples with0.20 mol/L NH4Cl, which is the first step for determination of thenegative surface charge of soil by the ion retention method, resulted in desorption of certain heavy metals from the soil. Itwas found that the percentage desorption of heavy metals from soilsubsamples depended greatly on pH, the composition and originalheavy metal content of the soil subsamples. However, most of theheavy metals in the soil subsamples were still retained aftermultiple saturation. Compared with the parent soil, the negativesurface charge of soil subsamples loaded with heavy metals did notshow differ significantly from that of the parent one bystatistical analysis. Heavy metals existed in the soil subsamplesmainly as exchangeable and precipitated simultaneously.

  5. Exciton Dynamics in Semiconducting Carbon Nanotubes

    Energy Technology Data Exchange (ETDEWEB)

    Graham, Matt [University of California, Berkeley; Chmeliov, Javgenij [Vilnius University, Lithuania; Ma, Yingzhong [ORNL; Shinohara, Nori [Nagoya University, Japan; Green, Alexander A. [Northwestern University, Evanston; Hersam, Mark C. [Northwestern University, Evanston; Valkunas, Leonas [Vilnius University, Lithuania; Fleming, Graham [University of California, Berkeley

    2010-01-01

    We report femtosecond transient absorption spectroscopic study on the (6, 5) single-walled carbon nanotubes and the (7, 5) inner tubes of a dominant double-walled carbon nanotube species. We found that the dynamics of exciton relaxation probed at the first transition-allowed state (E11) of a given tube type exhibits a markedly slower decay when the second transition-allowed state (E22) is excited than that measured by exciting its first transition-allowed state (E11). A linear intensity dependence of the maximal amplitude of the transient absorption signal is found for the E22 excitation, whereas the corresponding amplitude scales linearly with the square root of the E11 excitation intensity. Theoretical modeling of these experimental findings was performed by developing a continuum model and a stochastic model with explicit consideration of the annihilation of coherent excitons. Our detailed numerical simulations show that both models can reproduce reasonably well the initial portion of decay kinetics measured upon the E22 and E11 excitation of the chosen tube species, but the stochastic model gives qualitatively better agreement with the intensity dependence observed experimentally than those obtained with the continuum model.

  6. Exciton Correlations in Intramolecular Singlet Fission.

    Science.gov (United States)

    Sanders, Samuel N; Kumarasamy, Elango; Pun, Andrew B; Appavoo, Kannatassen; Steigerwald, Michael L; Campos, Luis M; Sfeir, Matthew Y

    2016-06-15

    We have synthesized a series of asymmetric pentacene-tetracene heterodimers with a variable-length conjugated bridge that undergo fast and efficient intramolecular singlet fission (iSF). These compounds have distinct singlet and triplet energies, which allow us to study the spatial dynamics of excitons during the iSF process, including the significant role of exciton correlations in promoting triplet pair generation and recombination. We demonstrate that the primary photoexcitations in conjugated dimers are delocalized singlets that enable fast and efficient iSF. However, in these asymmetric dimers, the singlet becomes more localized on the lower energy unit as the length of the bridge is increased, slowing down iSF relative to analogous symmetric dimers. We resolve the recombination kinetics of the inequivalent triplets produced via iSF, and find that they primarily decay via concerted processes. By identifying different decay channels, including delayed fluorescence via triplet-triplet annihilation, we can separate transient species corresponding to both correlated triplet pairs and uncorrelated triplets. Recombination of the triplet pair proceeds rapidly despite our experimental and theoretical demonstration that individual triplets are highly localized and unable to be transported across the conjugated linker. In this class of compounds, the rate of formation and yield of uncorrelated triplets increases with bridge length. Overall, these constrained, asymmetric systems provide a unique platform to isolate and study transient species essential for singlet fission, which are otherwise difficult to observe in symmetric dimers or condensed phases.

  7. Unraveling the exciton quenching mechanism of quantum dots on antimony-doped SnO₂ films by transient absorption and single dot fluorescence spectroscopy.

    Science.gov (United States)

    Song, Nianhui; Zhu, Haiming; Liu, Zheng; Huang, Zhuangqun; Wu, David; Lian, Tianquan

    2013-02-26

    Integrating quantum dots (QDs) into modern optoelectronic devices requires an understanding of how a transparent conducting substrate affects the properties of QDs, especially their excited-state dynamics. Here, the exciton quenching dynamics of core/multishell (CdSe/CdS(3ML)ZnCdS(2ML)ZnS(2ML)) quantum dots deposited on glass, tin oxide (SnO₂), and antimony (Sb)-doped tin oxide (ATO) films are studied by transient absorption and single QD fluorescence spectroscopic methods. By comparing ensemble-averaged fluorescence decay and transient absorption kinetics, we show that, for QDs on SnO₂, the exciton is quenched by electron transfer from the QD to SnO₂. At the QD-ATO interface, much faster exciton quenching rates are observed and attributed to fast Auger recombination in charged QDs formed by Fermi level equilibration between the QD and n-doped ATO. Single QDs on SnO₂ and ATO show similar blinking dynamics with correlated fluctuations of emission intensities and lifetimes. Compared to QDs on SnO₂, QDs on ATO films show larger variation of average exciton quenching rates, which is attributed to a broad distribution of the number of charges and nature of charging sites on the QD surface.

  8. Normal mode analysis of the spectral density of the Fenna-Matthews-Olson light-harvesting protein: how the protein dissipates the excess energy of excitons.

    Science.gov (United States)

    Renger, Thomas; Klinger, Alexander; Steinecker, Florian; Schmidt am Busch, Marcel; Numata, Jorge; Müh, Frank

    2012-12-20

    We report a method for the structure-based calculation of the spectral density of the pigment-protein coupling in light-harvesting complexes that combines normal-mode analysis with the charge density coupling (CDC) and transition charge from electrostatic potential (TrEsp) methods for the computation of site energies and excitonic couplings, respectively. The method is applied to the Fenna-Matthews-Olson (FMO) protein in order to investigate the influence of the different parts of the spectral density as well as correlations among these contributions on the energy transfer dynamics and on the temperature-dependent decay of coherences. The fluctuations and correlations in excitonic couplings as well as the correlations between coupling and site energy fluctuations are found to be 1 order of magnitude smaller in amplitude than the site energy fluctuations. Despite considerable amplitudes of that part of the spectral density which contains correlations in site energy fluctuations, the effect of these correlations on the exciton population dynamics and dephasing of coherences is negligible. The inhomogeneous charge distribution of the protein, which causes variations in local pigment-protein coupling constants of the normal modes, is responsible for this effect. It is seen thereby that the same building principle that is used by nature to create an excitation energy funnel in the FMO protein also allows for efficient dissipation of the excitons' excess energy.

  9. Excitons and trions in single and vertically coupled quantum dots under an electric field

    Science.gov (United States)

    Zhai, Li-Xue; Wang, Yan; An, Zhong

    2017-08-01

    We present a theoretical study of the exciton (X0), the positive and negative trions (X+ and X-) in single and vertically coupled configurations of self-assembled InGaAs quantum dots under an electric field. The quantum states of X0, X+ and X- have been investigated using a quasi-one-dimensional (Q1D) model within the effective-mass approximation. For the single quantum dots, the electric-field dependent energy levels and the average inter-particle distances for the exciton and trions have been calculated. For the coupled quantum dots, the ground and the excited states for X0, X+ and X- have also been calculated and discussed. It is found that either the hole or the electron can be tuned into resonance states by the electric field and that the transition energy spectra for both trions consequently show crossing and anticrossing patterns. The recombination probabilities of the exciton and trion optical transitions are also calculated. The theoretical results have been compared with previously reported photoluminescence data and qualitative agreement is obtained. The trion conditional wave functions are also plotted under different electric field intensities, and it is found that a molecular orbital can be formed at a critical electric field intensity. The evolution of the energy levels of the trions in coupled quantum dots can be explained by the interplay of particle transfer and the electric field.

  10. Theory of exciton transfer and diffusion in conjugated polymers

    Energy Technology Data Exchange (ETDEWEB)

    Barford, William, E-mail: william.barford@chem.ox.ac.uk [Department of Chemistry, Physical and Theoretical Chemistry Laboratory, University of Oxford, Oxford OX1 3QZ (United Kingdom); Tozer, Oliver Robert [Department of Chemistry, Physical and Theoretical Chemistry Laboratory, University of Oxford, Oxford OX1 3QZ (United Kingdom); University College, University of Oxford, Oxford OX1 4BH (United Kingdom)

    2014-10-28

    We describe a theory of Förster-type exciton transfer between conjugated polymers. The theory is built on three assumptions. First, we assume that the low-lying excited states of conjugated polymers are Frenkel excitons coupled to local normal modes, and described by the Frenkel-Holstein model. Second, we assume that the relevant parameter regime is ℏω < J, i.e., the adiabatic regime, and thus the Born-Oppenheimer factorization of the electronic and nuclear degrees of freedom is generally applicable. Finally, we assume that the Condon approximation is valid, i.e., the exciton-polaron wavefunction is essentially independent of the normal modes. The resulting expression for the exciton transfer rate has a familiar form, being a function of the exciton transfer integral and the effective Franck-Condon factors. The effective Franck-Condon factors are functions of the effective Huang-Rhys parameters, which are inversely proportional to the chromophore size. The Born-Oppenheimer expressions were checked against DMRG calculations, and are found to be within 10% of the exact value for a tiny fraction of the computational cost. This theory of exciton transfer is then applied to model exciton migration in conformationally disordered poly(p-phenylene vinylene). Key to this modeling is the assumption that the donor and acceptor chromophores are defined by local exciton ground states (LEGSs). Since LEGSs are readily determined by the exciton center-of-mass wavefunction, this theory provides a quantitative link between polymer conformation and exciton migration. Our Monte Carlo simulations indicate that the exciton diffusion length depends weakly on the conformation of the polymer, with the diffusion length increasing slightly as the chromophores became straighter and longer. This is largely a geometrical effect: longer and straighter chromophores extend over larger distances. The calculated diffusion lengths of ∼10 nm are in good agreement with experiment. The spectral

  11. Influences of strong exciton-phonon interaction on two coupled quantum dots within cavity QED

    Energy Technology Data Exchange (ETDEWEB)

    Yuan Xiaozhong [Department of Physics, Institute of Quantum Optics and Quantum Information, Shanghai Jiao Tong University, Shanghai 200240 (China)]. E-mail: yxz@sjtu.edu.cn; Zhu Kadi [Department of Physics, Institute of Quantum Optics and Quantum Information, Shanghai Jiao Tong University, Shanghai 200240 (China); Li Waisang [Department of Electronic and Information Engineering, Hong Kong Polytechnic University, Hong Kong (China)

    2004-08-30

    For two coupled quantum dots within cavity QED, we show that the exciton-phonon interaction reduces the Rabi frequency and Foerster interaction even at absolute zero temperature. The exciton-phonon interaction also makes an additional contribution to the static exciton-exciton dipole interaction energy.

  12. Influences of strong exciton-phonon interaction on two coupled quantum dots within cavity QED

    Science.gov (United States)

    Yuan, Xiao-Zhong; Zhu, Ka-Di; Li, Wai-Sang

    2004-08-01

    For two coupled quantum dots within cavity QED, we show that the exciton-phonon interaction reduces the Rabi frequency and Förster interaction even at absolute zero temperature. The exciton-phonon interaction also makes an additional contribution to the static exciton-exciton dipole interaction energy.

  13. Modelling space-charge limited transport in discotic liquid crystals

    Science.gov (United States)

    Lever, L.; Bushby, R. J.; Kelsall, R. W.

    2006-05-01

    Using a self-consistent Monte Carlo/Poisson algorithm, we investigate space-charge limited conduction in discotic liquid crystal time of flight (TOF) experiments. The charge transport mechanism is via a semi-delocalised banding process, and two mechanisms of photo-generation of charge carriers are considered: excitons generated by the laser pulse, which quench at the anode, and processes, such as the Onsager mechanism, that lead to direct generation of free electron/hole pairs within the bulk. The nature of the space-charge limited TOF transient is investigated as a function of quantum yield of charge carriers and as a function of applied potential.

  14. Exciton Transfer in Carbon Nanotube Aggregates for Energy Harvesting Applications

    Science.gov (United States)

    Davoody, Amirhossein; Karimi, Farhad; Knezevic, Irena

    Carbon nanotubes (CNTs) are promising building blocks for organic photovoltaic devices, owing to their tunable band gap, mechanical and chemical stability. We study intertube excitonic energy transfer between pairs of CNTs with different orientations and band gaps. The optically bright and dark excitonic states in CNTs are calculated by solving the Bethe-Salpeter equation. We calculate the exciton transfer rates due to the direct and exchange Coulomb interactions, as well as the second-order phonon-assisted processes. We show the importance of phonons in calculating the transfer rates that match the measurements. In addition, we discuss the contribution of optically inactive excited states in the exciton transfer process, which is difficult to determine experimentally. Furthermore, we study the effects of sample inhomogeneity, impurities, and temperature on the exciton transfer rate. The inhomogeneity in the CNT sample dielectric function can increase the transfer rate by about a factor of two. We show that the exciton confinement by impurities has a detrimental effect on the transfer rate between pairs of similar CNTs. The exciton transfer rate increases monotonically with increasing temperature. Support by the U.S. Department of Energy, Office of Basic Energy Sciences, Division of Materials Sciences and Engineering under Award DE-SC0008712.

  15. Ultrafast dynamics of exciton fission in polycrystalline pentacene.

    Science.gov (United States)

    Wilson, Mark W B; Rao, Akshay; Clark, Jenny; Kumar, R Sai Santosh; Brida, Daniele; Cerullo, Giulio; Friend, Richard H

    2011-08-10

    We use ultrafast transient absorption spectroscopy with sub-20 fs time resolution and broad spectral coverage to directly probe the process of exciton fission in polycrystalline thin films of pentacene. We observe that the overwhelming majority of initially photogenerated singlet excitons evolve into triplet excitons on an ∼80 fs time scale independent of the excitation wavelength. This implies that exciton fission occurs at a rate comparable to phonon-mediated exciton localization processes and may proceed directly from the initial, delocalized, state. The singlet population is identified due to the brief presence of stimulated emission, which is emitted at wavelengths which vary with the photon energy of the excitation pulse, a violation of Kasha's Rule that confirms that the lowest-lying singlet state is extremely short-lived. This direct demonstration that triplet generation is both rapid and efficient establishes multiple exciton generation by exciton fission as an attractive route to increased efficiency in organic solar cells. © 2011 American Chemical Society

  16. Synthesis and Exciton Dynamics of Triplet Sensitized Conjugated Polymers

    KAUST Repository

    Andernach, Rolf

    2015-07-22

    We report the synthesis of a novel polythiophene-based host-guest copolymer incorporating a Pt-porphyrin complex (TTP-Pt) into the backbone for efficient singlet to triplet polymer exciton sensitization. We elucidated the exciton dynamics in thin films of the material by means of Transient Absorption Spectrosopcy (TAS) on multiple timescales and investigated the mechanism of triplet exciton formation. During sensitization, single exciton diffusion is followed by exciton transfer from the polymer backbone to the complex where it undergoes intersystem crossing to the triplet state of the complex. We directly monitored the triplet exciton back transfer from the Pt-porphyrin to the polymer and find that 60% of the complex triplet excitons are transferred with a time constant of 1087 ps. We propose an equilibrium between polymer and porphyrin triplet states as a result of the low triplet diffusion length in the polymer backbone and hence an increased local triplet population resulting in increased triplet-triplet annihilation. This novel system has significant implications for the design of novel materials for triplet sensitized solar cells and up-conversion layers.

  17. Exciton condensation and its influence on the specific heat

    Energy Technology Data Exchange (ETDEWEB)

    Wachter, P., E-mail: wachter@solid.phys.ethz.ch [Laboratorium fuer Festkoerperphysik, ETH Zuerich, 8093 Zuerich (Switzerland); Bucher, B. [HSR Hochschule fuer Technik, 8640 Rapperswil (Switzerland)

    2013-01-01

    In rare earth compounds with localized 4f states the observation of bound 4f-hole-5d-electron states, excitons, is questionable. On the other hand the same compounds exhibit p-d excitons, which are derived from itinerant bands. In rare earth compounds, which exhibit intermediate valence, 4f-5d hybridization produces a narrow, several 10 meV wide 4f band. Now 4f-5d excitons are possible and have been observed in TmSe{sub 0.45}Te{sub 0.55} and similar compositions. The special band structure of these materials permits an enormous amount of excitons ( Almost-Equal-To 10{sup 21} cm{sup -3}), which condense in a first order transition at low temperatures and high pressure. This static and immense concentration of excitons dominates the heat conductivity and the thermal diffusivity and even exhibits the phenomenon of superfluidity in a solid. The measured specific heat shows that phonons couple to these excitons forming exciton polarons.

  18. Energy Transfer of Excitons Between Quantum Wells Separated by a Wide Barrier

    Energy Technology Data Exchange (ETDEWEB)

    LYO,SUNGKWUN K.

    1999-12-06

    We present a microscopic theory of the excitonic Stokes and anti-Stokes energy transfer mechanisms between two widely separated unequal quantum wells with a large energy mismatch ({Delta}) at low temperatures (T). Exciton transfer through dipolar coupling, photon-exchange coupling and over-barrier ionization of the excitons through exciton-exciton Auger processes are examined. The energy transfer rate is calculated as a function of T and the center-to-center distance d between the two wells. The rates depend sensitively on T for plane-wave excitons. For located excitons, the rates depend on T only through the T-dependence of the localization radius.

  19. Multiple excitons and the electron phonon bottleneck in semiconductor quantum dots: An ab initio perspective

    Science.gov (United States)

    Prezhdo, Oleg V.

    2008-07-01

    regarding the phonon bottleneck and the generation of multiple excitons in semiconductor QDs. Both the electron-hole and charge-phonon interactions are strong and, therefore, optical excitations can directly generate multiple excitons, while the electron-phonon relaxation exhibits no bottlenecks, except at low excitation energies and in very small QDs.

  20. Renormalization group study of excitonic and superconducting order in doped honeycomb bilayer

    Science.gov (United States)

    Murray, James; Vafek, Oskar

    2014-03-01

    We explore the competition between spin-charge order and unconventional superconductivity in the context of the AB stacked bilayer honeycomb lattice, realized experimentally as bilayer graphene, which features approximately parabolically touching electron bands. Using a weak-coupling renormalization group theory, we show that unconventional superconductivity arises generically for repulsively interacting fermions as excitonic order is suppressed by adding charge carriers to the system. We investigate the effects of finite temperature and further-neighbor hopping, the latter of which leads to so-called ``trigonal warping'' and destroys the perfect circular symmetry of the Fermi surfaces. We show that superconductivity survives for a finite range of trigonal warping, and that the nature of the superconducting phase may change as a function of further neighbor hopping. Depending on the range of interactions and the degree of trigonal warping, we find that the most likely superconducting instabilities are to f-wave, chiral d-wave, and pair density wave phases. It is shown that unconventional superconductivity is significantly enhanced by fluctuations in particle-hole channels, with the critical temperature reaching a maximum near the excitonic phase. Supported by the NSF CAREER award under Grant No. DMR-0955561, NSF Cooperative Agreement No. DMR-0654118, and the State of Florida, as well as by ICAM-I2CAM (NSF grant DMR-0844115) and by DoE, Office of Basic Energy Sciences (Award DE-FG02-08ER46544).

  1. Image charge effects in single-molecule junctions: Breaking of symmetries and negative-differential resistance in a benzene single-electron transistor

    DEFF Research Database (Denmark)

    Kaasbjerg, Kristen; Flensberg, K.

    2011-01-01

    blockade regime. This results in the appearance of a so-called blocking state, which gives rise to negative-differential resistance (NDR). We show that the appearance of NDR and its magnitude in the symmetry-broken benzene SET depends in a complicated way on the interplay between the many-body matrix...... elements, the lead tunnel coupling asymmetry, and the bias polarity. In particular, the current reducing property of the blocking state causing the NDR is shown to vanish under strongly asymmetric tunnel couplings, when the molecule is coupled stronger to the drain electrode. The calculated I-V...

  2. The influence of the interband Coulomb interaction and the f-electron hopping on excitonic correlations in the extended Falicov-Kimball model

    Science.gov (United States)

    Farkašovský, Pavol

    2015-05-01

    The density matrix renormalization group (DMRG) method is used to examine the effects of the interband Coulomb interaction U between f and d electrons as well as the f-electron hopping on the stability of the excitonic phase in the one-dimensional Falicov-Kimball model (FKM) with local hybridization V. It is found that the interband Coulomb interaction significantly enhances the excitonic Pdf= average and that this effect is especially strong in the limit of small hybridization, where the interacting Pdf(U) excitonic value is enhanced several hundred times in comparison to its non-interacting Pdf(U=0) value. The further increase in P df is observed due to the non-zero f-electron hopping, but these changes are considerable only if the d and f bands have opposite parity. In addition, the examination of the interplay between the excitonic effects and the charge density wave (CDW) instability showed that the CDW and excitonic phase coexist up to relatively large values of local hybridization (V ∼ 0.13) . The ground-state phase diagram of the model in the V\\text-U plane is discussed.

  3. Limits of Exciton-Exciton Annihilation for Light Emission in Transition Metal Dichalcogenide Monolayers

    CERN Document Server

    Yu, Yiling; Xu, Chao; Barrette, Andy; Gundogdu, Kenan; Cao, Linyou

    2015-01-01

    We quantitatively evaluate the exciton-exciton annihilation (EEA) and its effect on light emission properties in monolayer TMDC materials, including WS2, MoS2, and WSe2. The EEA rate is found to be 0.3 cm2/s and 0.1 cm2/s for suspended WS2 and MoS2 monolayers, respectively, and subject to the influence from substrates, being 0.1 cm2/s and 0.05 cm2/s for the supported WS2 and MoS2 on sapphire substrates. It can substantially affect the luminescence efficiency of suspended monolayers even at an exciton concentration as low as 109 cm-2, but plays a milder role for supported monolayers due to the effect of the substrate. However, regardless the presence of substrates or not, the lasing threshold of the monolayer is always predominantly determined by the EEA, which is estimated to be 12-18 MW/cm2 if using 532 nm as the pumping wavelength.

  4. Hot exciton cooling and multiple exciton generation in PbSe quantum dots.

    Science.gov (United States)

    Kumar, Manoj; Vezzoli, Stefano; Wang, Zilong; Chaudhary, Varun; Ramanujan, Raju V; Gurzadyan, Gagik G; Bruno, Annalisa; Soci, Cesare

    2016-11-16

    Multiple exciton generation (MEG) is a promising process to improve the power conversion efficiency of solar cells. PbSe quantum dots (QDs) have shown reasonably high MEG quantum yield (QY), although the photon energy threshold for this process is still under debate. One of the reasons for this inconsistency is the complicated competition of MEG and hot exciton cooling, especially at higher excited states. Here, we investigate MEG QY and the origin of the photon energy threshold for MEG in PbSe QDs of three different sizes by studying the transient absorption (TA) spectra, both at the band gap (near infrared, NIR) and far from the band gap energy (visible range). The comparison of visible TA spectra and dynamics for different pump wavelengths, below, around and above the MEG threshold, provides evidence of the role of the Σ transition in slowing down the exciton cooling process that can help MEG to take over the phonon relaxation process. The universality of this behavior is confirmed by studying QDs of three different sizes. Moreover, our results suggest that MEG QY can be determined by pump-probe experiments probed above the band gap.

  5. Exciton optical transitions in a hexagonal boron nitride single crystal

    Energy Technology Data Exchange (ETDEWEB)

    Museur, L. [Laboratoire de Physique des Lasers - LPL, CNRS UMR 7538, Institut Galilee, Universite Paris 13, 93430 Villetaneuse (France); Brasse, G.; Maine, S.; Ducastelle, F.; Loiseau, A. [ONERA - Laboratoire d' Etude des Microstructures - LEM, ONERA-CNRS, UMR 104, BP 72, 92322 Chatillon Cedex (France); Pierret, A. [ONERA - Laboratoire d' Etude des Microstructures - LEM, ONERA-CNRS, UMR 104, BP 72, 92322 Chatillon Cedex (France); CEA-CNRS, Institut Neel/CNRS, Universite J. Fourier, CEA/INAC/SP2M, 17 rue des Martyrs, 38 054 Grenoble Cedex 9 (France); Attal-Tretout, B. [ONERA - Departement Mesures Physiques - DMPh, 27 Chemin de la Huniere, 91761 Palaiseau Cedex (France); Barjon, J. [GEMaC, Universite de Versailles St Quentin, CNRS Bellevue, 1 Place Aristide Briand, 92195 Meudon Cedex (France); Watanabe, K.; Taniguchi, T. [National Institute for Materials Science, Namiki 1-1, Tsukuba, Ibaraki 305-0044 (Japan); Kanaev, A. [Laboratoire des Sciences des Procedes et des Materiaux - LSPM, CNRS UPR 3407, Universite Paris 13, 93430 Villetaneuse (France)

    2011-06-15

    Near band gap photoluminescence (PL) of a hexagonal boron nitride single crystal has been studied at cryogenic temperatures with synchrotron radiation excitation. The PL signal is dominated by trapped-exciton optical transitions, while the photoluminescence excitation (PLE) spectra show features assigned to free excitons. Complementary photoconductivity and PLE measurements set the band gap transition energy to 6.4 eV and the Frenkel exciton binding energy larger than 380 meV. (copyright 2011 WILEY-VCH Verlag GmbH and Co. KGaA, Weinheim) (orig.)

  6. Excitonic AND Logic Gates on DNA Brick Nanobreadboards

    Science.gov (United States)

    2015-01-01

    A promising application of DNA self-assembly is the fabrication of chromophore-based excitonic devices. DNA brick assembly is a compelling method for creating programmable nanobreadboards on which chromophores may be rapidly and easily repositioned to prototype new excitonic devices, optimize device operation, and induce reversible switching. Using DNA nanobreadboards, we have demonstrated each of these functions through the construction and operation of two different excitonic AND logic gates. The modularity and high chromophore density achievable via this brick-based approach provide a viable path toward developing information processing and storage systems. PMID:25839049

  7. Quantized Vortices and Four-Component Superfluidity of Semiconductor Excitons.

    Science.gov (United States)

    Anankine, Romain; Beian, Mussie; Dang, Suzanne; Alloing, Mathieu; Cambril, Edmond; Merghem, Kamel; Carbonell, Carmen Gomez; Lemaître, Aristide; Dubin, François

    2017-03-24

    We study spatially indirect excitons of GaAs quantum wells, confined in a 10  μm electrostatic trap. Below a critical temperature of about 1 K, we detect macroscopic spatial coherence and quantized vortices in the weak photoluminescence emitted from the trap. These quantum signatures are restricted to a narrow range of density, in a dilute regime. They manifest the formation of a four-component superfluid, made by a low population of optically bright excitons coherently coupled to a dominant fraction of optically dark excitons.

  8. Excitonic AND Logic Gates on DNA Brick Nanobreadboards.

    Science.gov (United States)

    Cannon, Brittany L; Kellis, Donald L; Davis, Paul H; Lee, Jeunghoon; Kuang, Wan; Hughes, William L; Graugnard, Elton; Yurke, Bernard; Knowlton, William B

    2015-03-18

    A promising application of DNA self-assembly is the fabrication of chromophore-based excitonic devices. DNA brick assembly is a compelling method for creating programmable nanobreadboards on which chromophores may be rapidly and easily repositioned to prototype new excitonic devices, optimize device operation, and induce reversible switching. Using DNA nanobreadboards, we have demonstrated each of these functions through the construction and operation of two different excitonic AND logic gates. The modularity and high chromophore density achievable via this brick-based approach provide a viable path toward developing information processing and storage systems.

  9. Ordered Dissipative Structures in Exciton Systems in Semiconductor Quantum Wells

    Directory of Open Access Journals (Sweden)

    Andrey A. Chernyuk

    2006-02-01

    Full Text Available A phenomenological theory of exciton condensation in conditions of inhomogeneous excitation is proposed. The theory is applied to the study of the development of an exciton luminescence ring and the ring fragmentation at macroscopical distances from the central excitation spot in coupled quantum wells. The transition between the fragmented and the continuous ring is considered. With assumption of a defect in the structure, a possibility of a localized island of the condensed phase in a fixed position is shown. Exciton density distribution is also analyzed in the case of two spatially separated spots of the laser excitation.

  10. Generalized master equation for modular exciton density transfer

    CERN Document Server

    Jang, Seogjoo; Fleming, Graham; Whaley, K Birgitta

    2013-01-01

    A generalized master equation (GME) governing quantum evolution of modular exciton density (MED) is derived for large scale light harvesting systems composed of weakly interacting modules of multiple chromophores. The GME-MED offers a practical framework to incorporate real time coherent quantum dynamics calculations at small length scales into dynamics over large length scales, without assumptions of time scale separation or specific forms of intra-module quantum dynamics. A test of the GME-MED for four sites of the Fenna-Matthews-Olson complex demonstrates how coherent dynamics of excitonic populations over many coupled chromophores can be accurately described by transitions between subgroups (modules) of delocalized excitons.

  11. Photogenerated Exciton Dissociation in Highly Coupled Lead Salt Nanocrystal Assemblies

    KAUST Repository

    Choi, Joshua J.

    2010-05-12

    Internanocrystal coupling induced excitons dissociation in lead salt nanocrystal assemblies is investigated. By combining transient photoluminescence spectroscopy, grazing incidence small-angle X-ray scattering, and time-resolved electric force microscopy, we show that excitons can dissociate, without the aid of an external bias or chemical potential gradient, via tunneling through a potential barrier when the coupling energy is comparable to the exciton binding energy. Our results have important implications for the design of nanocrystal-based optoelectronic devices. © 2010 American Chemical Society.

  12. Confocal shift interferometry of coherent emission from trapped dipolar excitons

    Energy Technology Data Exchange (ETDEWEB)

    Repp, J. [Walter Schottky Institut and Physik-Department, Am Coulombwall 4a, Technische Universität München, D-85748 Garching (Germany); Nanosystems Initiative Munich (NIM), Schellingstr. 4, 80799 München (Germany); Center for NanoScience and Fakultät für Physik, Ludwig-Maximilians-Universität, Geschwister-Scholl-Platz 1, 80539 München (Germany); Schinner, G. J.; Schubert, E. [Nanosystems Initiative Munich (NIM), Schellingstr. 4, 80799 München (Germany); Center for NanoScience and Fakultät für Physik, Ludwig-Maximilians-Universität, Geschwister-Scholl-Platz 1, 80539 München (Germany); Rai, A. K.; Wieck, A. D. [Angewandte Festkörperphysik, Ruhr-Universität Bochum, Universitätsstraße 150, 44780 Bochum (Germany); Reuter, D. [Angewandte Festkörperphysik, Ruhr-Universität Bochum, Universitätsstraße 150, 44780 Bochum (Germany); Department Physik, Universität Paderborn, 33098 Paderborn (Germany); Wurstbauer, U.; Holleitner, A. W. [Walter Schottky Institut and Physik-Department, Am Coulombwall 4a, Technische Universität München, D-85748 Garching (Germany); Nanosystems Initiative Munich (NIM), Schellingstr. 4, 80799 München (Germany); and others

    2014-12-15

    We introduce a confocal shift-interferometer based on optical fibers. The presented spectroscopy allows measuring coherence maps of luminescent samples with a high spatial resolution even at cryogenic temperatures. We apply the spectroscopy onto electrostatically trapped, dipolar excitons in a semiconductor double quantum well. We find that the measured spatial coherence length of the excitonic emission coincides with the point spread function of the confocal setup. The results are consistent with a temporal coherence of the excitonic emission down to temperatures of 250 mK.

  13. Ubiquity of Exciton Localization in Cryogenic Carbon Nanotubes.

    Science.gov (United States)

    Hofmann, Matthias S; Noé, Jonathan; Kneer, Alexander; Crochet, Jared J; Högele, Alexander

    2016-05-11

    We present photoluminescence studies of individual semiconducting single-wall carbon nanotubes at room and cryogenic temperatures. From the analysis of spatial and spectral features of nanotube photoluminescence, we identify characteristic signatures of unintentional exciton localization. Moreover, we quantify the energy scale of exciton localization potentials as ranging from a few to a few tens of millielectronvolts and stemming from both environmental disorder and shallow covalent side-wall defects. Our results establish disorder-induced crossover from the diffusive to the localized regime of nanotube excitons at cryogenic temperatures as a ubiquitous phenomenon in micelle-encapsulated and as-grown carbon nanotubes.

  14. Evidence of Excitonic Optical Tamm States using Molecular Materials

    CERN Document Server

    Núñez-Sánchez, S; Murshidy, M M; Abdel-Hady, A G; Serry, M Y; Adawi, A M; Rarity, J G; Oulton, R; Barnes, W L

    2015-01-01

    We report the first experimental observation of an Excitonic Optical Tamm State supported at the interface between a periodic multilayer dielectric structure and an organic dye-doped polymer layer. The existence of such states is enabled by the metal-like optical properties of the excitonic layer based on aggregated dye molecules. Experimentally determined dispersion curves, together with simulated data, including field profiles, allow us to identify the nature of these new modes. Our results demonstrate the potential of organic excitonic materials as a powerful means to control light at the nanoscale, offering the prospect of a new alternative type of nanophotonics based on molecular materials.

  15. Predicting polarizabilities and lifetimes of excitons on conjugated polymer chains

    Science.gov (United States)

    van der Horst, J.-W.; Bobbert, P. A.; de Jong, P. H. L.; Michels, M. A. J.; Siebbeles, L. D. A.; Warman, J. M.; Gelinck, G. H.; Brocks, G.

    2001-02-01

    The properties of excitons on three different conjugated polymers in solution are investigated both experimentally and theoretically. The theoretical description of the excitons is obtained by solving the electron-hole Bethe-Salpeter equation (BSE) for the polymers, starting from a calculation within density-functional theory. The calculated radiative lifetimes and polarizabilities of the excitons are compared with experimental results from time-resolved fluorescence decay and flash-photolysis microwave conductivity measurements. The quantitative agreement demonstrates the predictive power of the theoretical approach.

  16. Excitation of exciton states on a curved surface

    Science.gov (United States)

    Silotia, Poonam; Prasad, Vinod

    2016-05-01

    Excitonic transitions on the surface of a sphere have been studied in he presence of external static electric and laser fields. The spectrum and the various coupling matrix elements, (for n = 1 , 2 , 3), between few states of exciton have been evaluated in the absence and presence of excitonic Coulombic interaction with different values of dielectric constant. Variation of various physical quantities: energy eigenvalues, transition probability, orientational and alignment parameter, has been shown to have strong dependence on the laser field and static electric field.

  17. Optical Absorption Spectra and Excitons of Dye-Substrate Interfaces: Catechol on TiO2(110).

    Science.gov (United States)

    Mowbray, Duncan John; Migani, Annapaola

    2016-06-14

    Optimizing the photovoltaic efficiency of dye-sensitized solar cells (DSSC) based on staggered gap heterojunctions requires a detailed understanding of sub-band gap transitions in the visible from the dye directly to the substrate's conduction band (CB) (type-II DSSCs). Here, we calculate the optical absorption spectra and spatial distribution of bright excitons in the visible region for a prototypical DSSC, catechol on rutile TiO2(110), as a function of coverage and deprotonation of the OH anchoring groups. This is accomplished by solving the Bethe-Salpeter equation (BSE) based on hybrid range-separated exchange and correlation functional (HSE06) density functional theory (DFT) calculations. Such a treatment is necessary to accurately describe the interfacial level alignment and the weakly bound charge transfer transitions that are the dominant absorption mechanism in type-II DSSCs. Our HSE06 BSE spectra agree semiquantitatively with spectra measured for catechol on anatase TiO2 nanoparticles. Our results suggest deprotonation of catechol's OH anchoring groups, while being nearly isoenergetic at high coverages, shifts the onset of the absorption spectra to lower energies, with a concomitant increase in photovoltaic efficiency. Further, the most relevant bright excitons in the visible region are rather intense charge transfer transitions with the electron and hole spatially separated in both the [110] and [001] directions. Such detailed information on the absorption spectra and excitons is only accessible via periodic models of the combined dye-substrate interface.

  18. Theory and it ab initio calculation of radiative lifetime of excitons in semiconducting carbon nanotubes

    OpenAIRE

    Spataru, Catalin D.; Ismail-Beigi, Sohrab; Capaz, Rodrigo B.; Louie, Steven G.

    2005-01-01

    We present theoretical analysis and first-principles calculation of the radiative lifetime of excitons in semiconducting carbon nanotubes. An intrinsic lifetime of the order of 10 ps is computed for the lowest optically active bright excitons. The intrinsic lifetime is however a rapid increasing function of the exciton momentum. Moreover, the electronic structure of the nanotubes dictates the existence of dark excitons nearby in energy to each bright exciton. Both effects strongly influence m...

  19. Exciton and multi-exciton dynamics in CdSe/Cd1-xZnxS quantum dots

    Science.gov (United States)

    Righetto, Marcello; Minotto, Alessandro; Bozio, Renato

    2016-04-01

    The outstanding optical properties of Semiconductor Quantum Dots (QDs) have attracted much interest for over two decades. The development of synthetic methods for the production of core-shell QDs has opened the way to attaining almost ideal emitting properties. Their implementation in opto-electronic devices, such as light emitting diodes (LEDs) and lasers, requires a full understanding of the fine details of their photophysics. The exciton dynamics of core and coreshell QDs was extensively studied by means of pump and probe (P and P) and transient photoluminescence (TRPL) spectroscopies. Nevertheless, the wealth of possible exciton and multi-exciton decay mechanisms, operating on comparable time-scales, results in complex signals. In this work, the exciton dynamics of a complete CdSe/Cd1-xZnxS series is investigated, with a focus on exciton trapping processes. Insights into the energy distribution of exciton traps are unveiled by wavelength resolve QY measurements. Multicolor P and P measurements give a deeper insight into the dynamics of exciton trapping and Auger recombinations. An inversion method is proposed as a powerful tool for separating different contribution in complex P and P transients. The outcomes of this work clarify the role of core/shell interfaces and surfaces in modulating the optical properties and suggest possible routes for their improvement.

  20. Control of Exciton Photon Coupling in Nano-structures

    Science.gov (United States)

    Liu, Xiaoze

    In this thesis, we study the interaction of excitons with photons and plasmons and methods to control and enhance this interaction. This study is categorized in three parts: light-matter interaction in microcavity structures, direct dipole-dipole interactions, and plasmon-exciton interaction in metal-semiconductor systems. In the microcavity structures, the light-matter interactions become significant when the excitonic energy is in resonance with microcavity photons. New hybrid quantum states named polariton states will be formed if the strong coupling regime is achieved, where the interaction rate is faster than the average decay rate of the excitons and photons. Polaritons have been investigated in zinc oxide (ZnO) nanoparticles based microcavity at room temperature and stimulated emission of the polaritons has also been observed with a low optical pump threshold. Exictons in organic semiconductors (modeled as Frenkel excitons) are tightly bound to molecular sites, and differ considerably from loosely bound hydrogen atom-like inorganic excitons (modeled as Wannier-Mott excitons). This fundamental difference results in distinct optoelectronic properties. Not only strongly coupled to Wannier-Mott excitons in ZnO, the microcavity photons have also been observed to be simultaneously coupled to Frenkel excitons in 3,4,7,8-naphthalene tetracarboxylic dianhydride (NTCDA). The photons here act like a glue combining Wannier-Mott and Frenkel excitons into new hybrid polaritons taking the best from both constituents. Two-dimensional (2D) excitons in monolayer transition metal dichalcogenides (TMDs) have emerged as a new and fascinating type of Wannier-Mott-like excitons due to direct bandgap transition, huge oscillator strength and large binding energy. Monolayer molybdenum disulfide (MoS2) has been incorporated into the microcavity structure and 2D exciton-polaritons have been observed for the first time with directional emission in the strong coupling regime. Valley

  1. Benchmarking calculations of excitonic couplings between bacteriochlorophylls

    CERN Document Server

    Kenny, Elise P

    2015-01-01

    Excitonic couplings between (bacterio)chlorophyll molecules are necessary for simulating energy transport in photosynthetic complexes. Many techniques for calculating the couplings are in use, from the simple (but inaccurate) point-dipole approximation to fully quantum-chemical methods. We compared several approximations to determine their range of applicability, noting that the propagation of experimental uncertainties poses a fundamental limit on the achievable accuracy. In particular, the uncertainty in crystallographic coordinates yields an uncertainty of about 20% in the calculated couplings. Because quantum-chemical corrections are smaller than 20% in most biologically relevant cases, their considerable computational cost is rarely justified. We therefore recommend the electrostatic TrEsp method across the entire range of molecular separations and orientations because its cost is minimal and it generally agrees with quantum-chemical calculations to better than the geometric uncertainty. We also caution ...

  2. Excitons in topological Kondo insulators: Theory of thermodynamic and transport anomalies in SmB_{6}.

    Science.gov (United States)

    Knolle, Johannes; Cooper, Nigel R

    2017-03-03

    Kondo insulating materials lie outside the usual dichotomy of weakly versus correlated-band versus Mott-insulators. They are metallic at high temperatures but resemble band insulators at low temperatures because of the opening of an interaction-induced band gap. The first discovered Kondo insulator (KI) SmB_{6} has been predicted to form a topological KI (TKI). However, since its discovery thermodynamic and transport anomalies have been observed that have defied a theoretical explanation. Enigmatic signatures of collective modes inside the charge gap are seen in specific heat, thermal transport, and quantum oscillation experiments in strong magnetic fields. Here, we show that TKIs are susceptible to the formation of excitons and magnetoexcitons. These charge neutral composite particles can account for long-standing anomalies in SmB_{6}.

  3. Amine reactivity with charged sulfuric acid clusters

    OpenAIRE

    Bzdek, B. R.; D. P. Ridge; Johnston, M. V.

    2011-01-01

    The distribution of charged species produced by electrospray of an ammonium sulfate solution in both positive and negative polarities is examined using Fourier transform ion cyclotron resonance mass spectrometry (FTICR-MS). Positively-charged ammonium bisulfate cluster composition differs significantly from negatively-charged cluster composition. For positively-charged clusters all sulfuric acid is neutralized to bisulfate, whereas for negatively-charged clusters the degree of sulfuric acid n...

  4. Multiplicity distribution and spectra of negatively charged hadrons in Au+Au collisions at square root of (sNN) = 130 GeV.

    Science.gov (United States)

    Adler, C; Ahammed, Z; Allgower, C; Amonett, J; Anderson, B D; Anderson, M; Averichev, G S; Balewski, J; Barannikova, O; Barnby, L S; Baudot, J; Bekele, S; Belaga, V V; Bellwied, R; Berger, J; Bichsel, H; Bland, L C; Blyth, C O; Bonner, B E; Bossingham, R; Boucham, A; Brandin, A; Caines, H; Calderón De La Barca Sánchez, M; Cardenas, A; Carroll, J; Castillo, J; Castro, M; Cebra, D; Chattopadhyay, S; Chen, M L; Chen, Y; Chernenko, S P; Cherney, M; Chikanian, A; Choi, B; Christie, W; Coffin, J P; Conin, L; Cormier, T M; Cramer, J G; Crawford, H J; DeMello, M; Deng, W S; Derevschikov, A A; Didenko, L; Draper, J E; Dunin, V B; Dunlop, J C; Eckardt, V; Efimov, L G; Emelianov, V; Engelage, J; Eppley, G; Erazmus, B; Fachini, P; Finch, E; Fisyak, Y; Flierl, D; Foley, K J; Fu, J; Gagunashvili, N; Gans, J; Gaudichet, L; Germain, M; Geurts, F; Ghazikhanian, V; Grabski, J; Grachov, O; Greiner, D; Grigoriev, V; Guedon, M; Gushin, E; Hallman, T J; Hardtke, D; Harris, J W; Heffner, M; Heppelmann, S; Herston, T; Hippolyte, B; Hirsch, A; Hjort, E; Hoffmann, G W; Horsley, M; Huang, H Z; Humanic, T J; Hümmler, H; Igo, G; Ishihara, A; Ivanshin, Y I; Jacobs, P; Jacobs, W W; Janik, M; Johnson, I; Jones, P G; Judd, E; Kaneta, M; Kaplan, M; Keane, D; Kisiel, A; Klay, J; Klein, S R; Klyachko, A; Konstantinov, A S; Kotchenda, L; Kovalenko, A D; Kramer, M; Kravtsov, P; Krueger, K; Kuhn, C; Kulikov, A I; Kunde, G J; Kunz, C L; Kutuev, R K; Kuznetsov, A A; Lakehal-Ayat, L; Lamas-Valverde, J; Lamont, M A; Landgraf, J M; Lange, S; Lansdell, C P; Lasiuk, B; Laue, F; Lebedev, A; LeCompte, T; Lednický, R; Leontiev, V M; Leszczynski, P; LeVine, M J; Li, Q; Li, Q; Lindenbaum, S J; Lisa, M A; Ljubicic, T; Llope, W J; LoCurto, G; Long, H; Longacre, R S; Lopez-Noriega, M; Love, W A; Lynn, D; Majka, R; Maliszewski, A; Margetis, S; Martin, L; Marx, J; Matis, H S; Matulenko, Y A; McShane, T S; Meissner, F; Melnick, Y; Meschanin, A; Messer, M; Miller, M L; Milosevich, Z; Minaev, N G; Mitchell, J; Moiseenko, V A; Moltz, D; Moore, C F; Morozov, V; de Moura, M M; Munhoz, M G; Mutchler, G S; Nelson, J M; Nevski, P; Nikitin, V A; Nogach, L V; Norman, B; Nurushev, S B; Odyniec, G; Ogawa, A; Okorokov, V; Oldenburg, M; Olson, D; Paic, G; Pandey, S U; Panebratsev, Y; Panitkin, S Y; Pavlinov, A I; Pawlak, T; Perevoztchikov, V; Peryt, W; Petrov, V A; Pinganaud, W; Platner, E; Pluta, J; Porile, N; Porter, J; Poskanzer, A M; Potrebenikova, E; Prindle, D; Pruneau, C; Radomski, S; Rai, G; Ravel, O; Ray, R L; Razin, S V; Reichhold, D; Reid, J G; Retiere, F; Ridiger, A; Ritter, H G; Roberts, J B; Rogachevski, O V; Romero, J L; Roy, C; Russ, D; Rykov, V; Sakrejda, I; Sandweiss, J; Saulys, A C; Savin, I; Schambach, J; Scharenberg, R P; Schweda, K; Schmitz, N; Schroeder, L S; Schüttauf, A; Seger, J; Seliverstov, D; Seyboth, P; Shahaliev, E; Shestermanov, K E; Shimanskii, S S; Shvetcov, V S; Skoro, G; Smirnov, N; Snellings, R; Sowinski, J; Spinka, H M; Srivastava, B; Stephenson, E J; Stock, R; Stolpovsky, A; Strikhanov, M; Stringfellow, B; Stroebele, H; Struck, C; Suaide, A A; Sugarbaker, E; Suire, C; Sumbera, M; Symons, T J; Szanto De Toledo, A; Szarwas, P; Takahashi, J; Tang, A H; Thomas, J H; Tikhomirov, V; Trainor, T A; Trentalange, S; Tokarev, M; Tonjes, M B; Trofimov, V; Tsai, O; Turner, K; Ullrich, T; Underwood, D G; Van Buren, G; VanderMolen, A M; Vanyashin, A; Vasilevski, I M; Vasiliev, A N; Vigdor, S E; Voloshin, S A; Wang, F; Ward, H; Watson, J W; Wells, R; Wenaus, T; Westfall, G D; Whitten, C; Wieman, H; Willson, R; Wissink, S W; Witt, R; Xu, N; Xu, Z; Yakutin, A E; Yamamoto, E; Yang, J; Yepes, P; Yokosawa, A; Yurevich, V I; Zanevski, Y V; Zborovský, I; Zhang, W M; Zoulkarneev, R; Zubarev, A N

    2001-09-10

    The minimum-bias multiplicity distribution and the transverse momentum and pseudorapidity distributions for central collisions have been measured for negative hadrons ( h(-)) in Au+Au interactions at square root of ([s(NN)]) = 130 GeV. The multiplicity density at midrapidity for the 5% most central interactions is dN(h(-))/d(eta)/(eta = 0) = 280+/-1(stat)+/-20(syst), an increase per participant of 38% relative to pp collisions at the same energy. The mean transverse momentum is 0.508+/-0.012 GeV/c and is larger than in central Pb+Pb collisions at lower energies. The scaling of the h(-) yield per participant is a strong function of p( perpendicular). The pseudorapidity distribution is almost constant within /eta/<1.

  5. Negative magnetoresistivity in holography

    CERN Document Server

    Sun, Ya-Wen

    2016-01-01

    Negative magnetoresistivity is a special magnetotransport property associated with chiral anomaly in four dimensional chiral anomalous systems, which refers to the transport behavior that the DC longitudinal magnetoresistivity decreases with increasing magnetic field. We calculate the longitudinal magnetoconductivity in the presence of backreactions of the magnetic field to gravity in holographic zero charge and axial charge density systems with and without axial charge dissipation. In the absence of axial charge dissipation, we find that the quantum critical conductivity grows with increasing magnetic field when the backreaction strength is larger than a critical value, in contrast to the monotonically decreasing behavior of quantum critical conductivity in the probe limit. With axial charge dissipation, we find the negative magnetoresistivity behavior. The DC longitudinal magnetoconductivity scales as $B$ in the large magnetic field limit, which deviates from the exact $B^2$ scaling of the probe limit resul...

  6. Vibrational exciton-mediated quantum state transfert: a simple model

    CERN Document Server

    Pouthier, Vincent J C

    2012-01-01

    A communication protocol is proposed in which quantum state transfer is mediated by a vibrational exciton. We consider two distant molecular groups grafted on the sides of a lattice. These groups behave as two quantum computers where the information in encoded and received. The lattice plays the role of a communication channel along which the exciton propagates and interacts with a phonon bath. Special attention is paid for describing the system involving an exciton dressed by a single phonon mode. The Hamiltonian is thus solved exactly so that the relevance of the perturbation theory is checked. Within the nonadiabatic weak-coupling limit, it is shown that the system supports three quasi-degenerate states that define the relevant paths followed by the exciton to tunnel between the computers. When the model parameters are judiciously chosen, constructive interferences take place between these paths. Phonon-induced decoherence is minimized and a high-fidelity quantum state transfer occurs over a broad temperat...

  7. Fate of the excitonic insulator in the presence of phonons

    Science.gov (United States)

    Zenker, B.; Fehske, H.; Beck, H.

    2014-11-01

    The influence of phonons on the formation of the excitonic insulator has hardly been analyzed so far. Recent experiments on Ta2NiSe5 ,1 T -TiSe2, and TmSe0.45Te0.55 , being candidates for realizing the excitonic-insulator state, suggest, however, that the underlying lattice plays a significant role. Employing the Kadanoff-Baym approach we address this issue theoretically. We show that owing to the electron-phonon coupling a static lattice distortion may arise at the excitonic instability. Most importantly such a distortion will destroy the acoustic phase mode being present if the electron-hole pairing and condensation is exclusively driven by the Coulomb interaction. The absence of off-diagonal long-range order, when lattice degrees of freedom are involved, challenges that excitons in these materials form a superfluid condensate of Bose particles or Cooper pairs composed of electrons and holes.

  8. Ghost Fano Resonance of Excitons in Twisted Bilayer Graphene

    Science.gov (United States)

    Liang, Yufeng

    2014-03-01

    Metallic systems are generally considered to be unable to harbor tightly bound excitons because of the strong screening effect as well as the absence of a finite band gap. Previously, exception has only been found in one-dimensional metallic carbon nanotubes due to the depressed screening effects and the symmetry gap. We explore the exciton spectra of twisted bilayer graphene (tBLG) and predict the existence of even more strongly bound exciton (with binding energy as large as 0.5eV) in this system despite of its higher dimensionality. Based on our results from first-principles simulations and effective model calculations, a mechanism known as the ghost Fano resonance is proposed for the bound exciton formation in metallic systems beyond the dimensonality-related argument. Our results shed light on engineering the e-h excitations in the few-layer van der Waals heterojunction. NSF Grant No. DMR-1207141.

  9. Long-range exciton dissociation in organic solar cells

    National Research Council Canada - National Science Library

    Domenico Caruso; Alessandro Troisi

    2012-01-01

    It is normally assumed that electrons and holes in organic solar cells are generated by the dissociation of excitons at the interface between donor and acceptor materials in strongly bound hole-electron pairs...

  10. Exciton-Dependent Pre-formation Probability of Composite Particles

    Institute of Scientific and Technical Information of China (English)

    ZHANG Jing-Shang; WANG Ji-Min; DUAN Jun-Feng

    2007-01-01

    In Iwamoto-Harada model the whole phase space is full of fermions. When the momentum distributions of the exciton states are taken into account, the pre-formation probability of light composite particles could be improved,and the exciton state-dependent pre-formation probability has been proposed. The calculated results indicate that the consideration of the momentum distribution enhances the pre-formation probability of [1,m] configuration, and suppresses that of [l > 1, m] configurations seriously.

  11. Tuning of Exciton States in a Magnetic Quantum Ring

    OpenAIRE

    Ghazaryan, Areg; Manaselyan, Aram; Chakraborty, Tapash

    2014-01-01

    We have studied the exciton states in a CdTe quantum ring in an external magnetic field containing a single magnetic impurity. We have used the multiband approximation which includes the heavy hole - light hole coupling effects. The electron-hole spin interactions and the s, p-d interactions between the electron, hole and the magnetic impurity are also included. The exciton energy levels and optical transitions are evaluated using the exact diagonalization scheme. We show that due to the spin...

  12. Quantum confinement of excitons in wurtzite InP nanowires

    Science.gov (United States)

    Pemasiri, K.; Jackson, H. E.; Smith, L. M.; Wong, B. M.; Paiman, S.; Gao, Q.; Tan, H. H.; Jagadish, C.

    2015-05-01

    Exciton resonances are observed in photocurrent spectra of 80 nm wurtzite InP nanowire devices at low temperatures, which correspond to transitions between the A, B, and C valence bands and the lower conduction band. Photocurrent spectra for 30 nm WZ nanowires exhibit shifts of the exciton resonances to higher energy, which are consistent with finite element calculations of wavefunctions of the confined electrons and holes for the various bands.

  13. Control of Exciton Dynamics in Nanodots for Quantum Operations

    Science.gov (United States)

    Chen, Pochung; Piermarocchi, C.; Sham, L. J.

    2001-08-01

    We present a theory to further a new perspective of proactive control of exciton dynamics in the quantum limit. Circularly polarized optical pulses in a semiconductor nanodot are used to control the dynamics of two interacting excitons of opposite polarizations. Shaping of femtosecond laser pulses keeps the quantum operation within the decoherence time. Computation of the fidelity of the operations and application to the complete solution of a minimal quantum computing algorithm demonstrate in theory the feasibility of quantum control.

  14. Coherence and Optical Emission from Bilayer Exciton Condensates

    Directory of Open Access Journals (Sweden)

    D. W. Snoke

    2011-01-01

    Full Text Available Experiments aimed at demonstrating Bose-Einstein condensation of excitons in two types of experiments with bilayer structures (coupled quantum wells are reviewed, with an emphasis on the basic effects. Bose-Einstein condensation implies the existence of a macroscopic coherence, also known as off-diagonal long-range order, and proposed tests and past claims for coherence in these excitonic systems are discussed.

  15. Bose condensation of interwell excitons in double quantum wells

    CERN Document Server

    Larionov, A V; Ni, P A; Dubonos, S V; Hvam, I; Soerensen, K

    2002-01-01

    The luminescence of the interwell excitons in the GaAs/AlGaAs double quantum wells, containing large-scale fluctuations of the random potential in the heteroboundary planes, is studied. The properties of the excitons, wherein the excited electron and hole are spatially separated between the neighboring quantum wells by the density and temperature variation within the domain limits of the scale below one micron, are investigated. The interwell excitons by low pumping (below 50 mW) are strongly localized due to the small-scale fluctuations of the random potential. The localized excitons line grows by increase in the resonance excitation capacity through the threshold method. With the temperature growth this line disappears in the spectrum (T sub c <= 3.4 K). The above phenomenon is related to the Bose-Einstein condensation in the quasi-two-dimensional system of the interwell excitons. The critical values of the exciton density and temperature in the studied temperature range (1.5-3.4 K) grow according to the...

  16. Acousto-exciton interaction in a gas of 2D indirect dipolar excitons in the presence of disorder

    Energy Technology Data Exchange (ETDEWEB)

    Kovalev, V. M.; Chaplik, A. V., E-mail: chaplik@isp.nsc.ru [Russian Academy of Sciences, Rzhanov Institute of Semiconductor Physics, Siberian Branch (Russian Federation)

    2016-03-15

    A theory for the linear and quadratic responses of a 2D gas of indirect dipolar excitons to an external surface acoustic wave perturbation in the presence of a static random potential is considered. The theory is constructed both for high temperatures, definitely greater than the exciton gas condensation temperature, and at zero temperature by taking into account the Bose–Einstein condensation effects. The particle Green functions, the density–density correlation function, and the quadratic response function are calculated by the “cross” diagram technique. The results obtained are used to calculate the absorption of Rayleigh surface waves and the acoustic exciton gas drag by a Rayleigh wave. The damping of Bogoliubov excitations in an exciton condensate due to theirs scattering by a random potential has also been determined.

  17. Phase coherence and spectral functions in the two-dimensional excitonic systems

    Energy Technology Data Exchange (ETDEWEB)

    Apinyan, V., E-mail: V.Apinyan@int.pan.wroc.pl; Kopeć, T.K.

    2015-09-15

    The nonlocal correlation mechanism between excitonic pairs is considered for a two dimensional exciton system. On the base of the unitary decomposition of the usual electron operator, we include the electron phase degrees of freedom into the problem of interacting excitons. Applying the path integral formalism, we treat the excitonic insulator state (EI) and the Bose–Einstein condensation (BEC) of preformed excitonic pairs as two independent problems. For the BEC of excitons the phase field variables play a crucial role. We derive the expression of the local EI order parameter by integrating out the phase variables. Then, considering the zero temperature limit, we obtain the excitonic BEC transition probability function, by integrating out the fermions. We calculate the normal excitonic Green functions for the conduction and valence band electrons and we derive the excitonic spectral functions, both analytically and numerically. Different values of the Coulomb interaction parameter are considered.

  18. Ligand-dependent exciton dynamics and photovoltaic properties of PbS quantum dot heterojunction solar cells.

    Science.gov (United States)

    Chang, Jin; Ogomi, Yuhei; Ding, Chao; Zhang, Yao Hong; Toyoda, Taro; Hayase, Shuzi; Katayama, Kenji; Shen, Qing

    2017-03-01

    The surface chemistry of colloidal quantum dots (QDs) plays an important role in determining the photoelectric properties of QD films and the corresponding quantum dot heterojunction solar cells (QDHSCs). To investigate the effects of the ligand structure on the photovoltaic performance and exciton dynamics of QDHSCs, PbS QDHSCs were fabricated by the solid state ligand exchange method with mercaptoalkanoic acid as the cross-linking ligand. Temperature-dependent photoluminescence and ultrafast transient absorption spectra show that the electronic coupling and charge transfer rate within QD ensembles were monotonically enhanced as the ligand length decreased. However, in practical QDHSCs, the second shortest ligand 3-mercaptopropionic acid (MPA) showed higher power conversion efficiency than the shortest ligand thioglycolic acid (TGA). This could be attributed to the difference in their surface trap states, supported by thermally stimulated current measurements. Moreover, compared with the non-conjugated ligand MPA, the conjugated ligand 4-mercaptobenzoic acid (MBA) introduces less trap states and has a similar charge transfer rate in QD ensembles, but has poor photovoltaic properties. This unexpected result could be contributed by the QD-ligand orbital mixing, leading to the charge transfer from QDs to ligands instead of charge transfer between adjacent QDs. This work highlights the significant effects of ligand structures on the photovoltaic properties and exciton dynamics of QDHSCs, which would shed light on the further development of QD-based photoelectric devices.

  19. 1,3-Bis(nitroimido)-1,2,3-triazolate anion, the N-nitroimide moiety, and the strategy of alternating positive and negative charges in the design of energetic materials.

    Science.gov (United States)

    Klapötke, Thomas M; Petermayer, Christian; Piercey, Davin G; Stierstorfer, Jörg

    2012-12-26

    This unique study reports on the 1,3-bis(nitroimido)-1,2,3-triazolate anion. This compound provides unique insight into both academic and practical considerations surrounding high-nitrogen systems. The bonding in this energetic anion can be represented multiple ways, one of which includes a chain of alternating positive/negative charges nine atoms long. The validity of this resonance structure is discussed in terms of experimental, computational, and valence bond results. The prepared materials based on this energetic anion were also characterized chemically (infrared, Raman, NMR, X-ray) and as high explosives in terms of their energetic performances (detonation velocity, pressure, etc.) and sensitivities (impact, friction, electrostatic), and the 1,3-bis(nitroimido)-1,2,3-triazolate anion is found to be very high performing with high thermal stabilities while being quite sensitive to mechanical stimuli.

  20. Coupling of Excitons and Discrete Acoustic Phonons in Vibrationally Isolated Quantum Emitters.

    Science.gov (United States)

    Werschler, Florian; Hinz, Christopher; Froning, Florian; Gumbsheimer, Pascal; Haase, Johannes; Negele, Carla; de Roo, Tjaard; Mecking, Stefan; Leitenstorfer, Alfred; Seletskiy, Denis V

    2016-09-14

    The photoluminescence emission by mesoscopic condensed matter is ultimately dictated by the fine-structure splitting of the fundamental exciton into optically allowed and dipole-forbidden states. In epitaxially grown semiconductor quantum dots, nonradiative equilibration between the fine-structure levels is mediated by bulk acoustic phonons, resulting in asymmetric spectral broadening of the excitonic luminescence. In isolated colloidal quantum dots, spatial confinement of the vibrational motion is expected to give rise to an interplay between the quantized electronic and phononic degrees of freedom. In most cases, however, zero-dimensional colloidal nanocrystals are strongly coupled to the substrate such that the charge relaxation processes are still effectively governed by the bulk properties. Here we show that encapsulation of single colloidal CdSe/CdS nanocrystals into individual organic polymer shells allows for systematic vibrational decoupling of the semiconductor nanospheres from the surroundings. In contrast to epitaxially grown quantum dots, simultaneous quantization of both electronic and vibrational degrees of freedom results in a series of strong and narrow acoustic phonon sidebands observed in the photoluminescence. Furthermore, an individual analysis of more than 200 compound particles reveals that enhancement or suppression of the radiative properties of the fundamental exciton is controlled by the interaction between fine-structure states via the discrete vibrational modes. For the first time, pronounced resonances in the scattering rate between the fine-structure states are directly observed, in good agreement with a quantum mechanical model. The unambiguous assignment of mediating acoustic modes to the observed scattering resonances complements the experimental findings. Thus, our results form an attractive basis for future studies on subterahertz quantum opto-mechanics and efficient laser cooling at the nanoscale.

  1. Simulated nucleon–nucleon and nucleon–nucleus reactions in the frame of the cascade exciton model at high and intermediate energies

    Indian Academy of Sciences (India)

    A Abdel-Hafiez; Shaker El-Shater; M F Zaki

    2015-04-01

    In this study, we have used the cascade exciton model (CEM) to investigate different characteristics of nuclear reactions. Number of nucleon–nucleon collisions in Pb+Pb collisions as a function of impact parameter and rapidity distributions of negative particles from p+Ar and p+Xe interactions at lab = 200 GeV/c have been studied. We could create inclusive spectra of pions for separate charged states from reactions and total neutron multiplicities per primary reaction at 1000 MeV for different thin targets. Also, cross-sections for the reactions 209Bi(p, f) and 209Bi(n, f) were studied. Interactions of 1.0 GeV protons with C, Al, Cu, Sn, and Pb are presented in this study. All the calculated characteristics are compared with other theoretical calculations and compared with the experimental data. CEM shows good agreement with both theoretical and experimental results. In this study, we have used quantum molecular dynamic (QMD) as a theoretical model to compare our results.

  2. Impurity trapped excitons under high hydrostatic pressure

    Science.gov (United States)

    Grinberg, Marek

    2013-09-01

    Paper summarizes the results on pressure effect on energies of the 4fn → 4fn and 4fn-15d1 → 4fn transitions as well as influence of pressure on anomalous luminescence in Lnα+ doped oxides and fluorides. A model of impurity trapped exciton (ITE) was developed. Two types of ITE were considered. The first where a hole is localized at the Lnα+ ion (creation of Ln(α+1)+) and an electron is attracted by Coulomb potential at Rydberg-like states and the second where an electron captured at the Lnα+ ion (creation of Ln(α-1)+) and a hole is attracted by Coulomb potential at Rydberg-like states. Paper presents detailed analysis of nonlinear changes of energy of anomalous luminescence of BaxSr1-xF2:Eu2+ (x > 0.3) and LiBaF3:Eu2+, and relate them to ITE-4f65d1 states mixing.

  3. Linear, third- and fifth-order nonlinear spectroscopy of a charge transfer system coupled to an underdamped vibration

    CERN Document Server

    Dijkstra, Arend G

    2015-01-01

    We study hole, electron and exciton transport in a charge transfer system in the presence of underdamped vibrational motion. We analyze the signature of these processes in the linear and third-, and fifth-order nonlinear electronic spectra. Calculations are performed with a numerically exact hierarchical equations of motion method for an underdamped Brownian oscillator spectral density. We find that combining electron, hole and exciton transfer can lead to non-trivial spectra with more structure than with excitonic coupling alone. Traces taken during the waiting time of a two-dimensional spectrum are dominated by vibrational motion and do not reflect the electron, hole, and exciton dynamics directly. We find that the fifth-order nonlinear response is particularly sensitive to the charge transfer process. While third-order 2D spectroscopy detects the correlation between two coherences, fifth-order 2D spectroscopy (2D population spectroscopy) is here designed to detect correlations between the excited states du...

  4. Excitonic Phase Transition in the Extended Three-Dimensional Falicov-Kimball Model

    Science.gov (United States)

    Apinyan, V.; Kopeć, T. K.

    2014-07-01

    We study the excitonic phase transition in a system of the conduction band electrons and valence band holes described by the three-dimensional (3D) extended Falicov-Kimball (EFKM) model with the tunable Coulomb interaction between both species. By lowering the temperature, the electron-hole system may become unstable with respect to the formation of the excitons, i.e, electron-hole pairs at temperature , exhibiting a gap in the particle excitation spectrum. To this end we implement the functional integral formulation of the EFKM, where the Coulomb interaction term is expressed in terms of U(1) phase variables conjugate to the local particle number, providing a useful representation of strongly correlated system. The effective action formalism allows us to formulate a problem in the phase-only action in the form of the quantum rotor model and to obtain analytical formulas for the critical lines and other quantities of physical interest like charge gap, chemical potential and the correlation length.

  5. Analysis of Triplet Exciton Loss Pathways in PTB7:PC71BM Bulk Heterojunction Solar Cells

    Science.gov (United States)

    Kraus, Hannes; Heiber, Michael C.; Väth, Stefan; Kern, Julia; Deibel, Carsten; Sperlich, Andreas; Dyakonov, Vladimir

    2016-07-01

    A strategy for increasing the conversion efficiency of organic photovoltaics has been to increase the VOC by tuning the energy levels of donor and acceptor components. However, this opens up a new loss pathway from an interfacial charge transfer state to a triplet exciton (TE) state called electron back transfer (EBT), which is detrimental to device performance. To test this hypothesis, we study triplet formation in the high performing PTB7:PC71BM blend system and determine the impact of the morphology-optimizing additive 1,8-diiodoctane (DIO). Using photoluminescence and spin-sensitive optically detected magnetic resonance (ODMR) measurements at low temperature, we find that TEs form on PC71BM via intersystem crossing from singlet excitons and on PTB7 via EBT mechanism. For DIO blends with smaller fullerene domains, an increased density of PTB7 TEs is observed. The EBT process is found to be significant only at very low temperature. At 300 K, no triplets are detected via ODMR, and electrically detected magnetic resonance on optimized solar cells indicates that TEs are only present on the fullerenes. We conclude that in PTB7:PC71BM devices, TE formation via EBT is impacted by fullerene domain size at low temperature, but at room temperature, EBT does not represent a dominant loss pathway.

  6. Energy characteristics of excitons in InGaN/GaN heterostructures

    Science.gov (United States)

    Usov, S. O.; Tsatsul'nikov, A. F.; Lundin, W. V.; Sakharov, A. V.; Zavarin, E. E.; Sinitsyn, M. A.; Ledentsov, N. N.

    2008-04-01

    The structure and optical properties of the heterostructures, which contain an ultra-thin InGaN layers with GaN or AlGaN barriers, grown by MOCVD method were investigated by photoluminescence and high resolution X-ray diffraction (HRXRD) tehnigue. The exciton localization energy, Urbah energy and charge carries activation energies were obtained from analysis of the temperature dependences of the photoluminescence spectra for the In-rich areas (QDs). In these structures the In-rich areas are shown to appear in ultrathin InGaN layers due to phase decomposition. That leads to exciton and carrier localization in fluctuation minima, which prevents them from tranport to nonradiative recombination centres. The indium composition in the InGaN QDs were obtained using theoretical model, which describes the electron transition energy as a function of In-rich areas parameters. The parameters such as deformation of InGaN/GaN region and layer thickness were determined from HRXRD. The suggested approach is supposed to be effective method for analysis of the optical properties of InGaN/GaN heterostructures.

  7. Correlated Pair States Formed by Singlet Fission and Exciton-Exciton Annihilation.

    Science.gov (United States)

    Scholes, Gregory D

    2015-12-24

    Singlet fission to form a pair of triplet excitations on two neighboring molecules and the reverse process, triplet-triplet annihilation to upconvert excitation, have been extensively studied. Comparatively little work has sought to examine the properties of the intermediate state in both of these processes-the bimolecular pair state. Here, the eigenstates constituting the manifold of 16 bimolecular pair excitations and their relative energies in the weak-coupling regime are reported. The lowest-energy states obtained from the branching diagram method are the triplet pairs with overall singlet spin |X1⟩ ≈ (1)[TT] and quintet spin |Q⟩ ≈ (5)[TT]. It is shown that triplet pair states can be separated by a triplet-triplet energy-transfer mechanism to give a separated, yet entangled triplet pair (1)[T···T]. Independent triplets are produced by decoherence of the separated triplet pair. Recombination of independent triplets by exciton-exciton annihilation to form the correlated triplet pair (i.e., nongeminate recombination) happens with 1/3 of the rate of either triplet migration or recombination of the separated correlated triplet pair (geminate recombination).

  8. Ultrafast Optical Studies of Multiple Exciton Generation in Lead Chalcogenide Quantum Dots

    Science.gov (United States)

    Midgett, Aaron G.

    2011-12-01

    Providing affordable, clean energy is one of the major challenges facing society today, and one of the promising solutions is third generation solar energy conversion. Present day, first and second-generation solar cells can at most convert each absorbed photon into a single electron hole pair, thereby establishing a theoretical limit to the power conversion efficiency. The process of multiple exciton generation (MEG) in semiconductor quantum dots increases that theoretical efficiency from 33% to 42% by utilizing the excess energy of high energy photons that is otherwise wasted as heat to excite a second electron-hole pair, thereby boosting the potential photocurrent. This thesis explores the benefits of MEG in quantum confined systems and shows that quantum dots are more efficient at generating multiple excitons from a single photon than bulk semiconductors. The variations in optical measurements of MEG have raised skepticism and brought into question the validity of these experiments. The two important questions that this thesis attempts to address are (1) what are the enhanced QYs in isolated PbSe QDs and (2) does quantum confinement enhance MEG over bulk semiconductors. Experimental variations in the enhanced QYs are partially explained by the production of a long-lived photocharged state that increases the apparent photon-to-exciton QYs. A procedure is detailed that decreases the possibility of producing this charged state. By studying the production of these states, conditions are found that minimize their effect and produce less variation in the reported QYs. Variations in the MEG efficiency were studied in films of chemically treated PbSe quantum dots where a different mechanism was responsible for an apparent decrease of the measured QYs. Finally, for the first time, a quantum dot size-dependence in the MEG efficiency was found in colloidal PbSe, PbS, and PbSxSe1-x quantum dot solutions and is attributed to the increased Coulomb interaction in materials

  9. Combined effects of local and nonlocal hybridization on formation and condensation of excitons in the extended Falicov-Kimball model

    Science.gov (United States)

    Farkašovský, Pavol

    2017-04-01

    We study the combined effects of local and nonlocal hybridization on the formation and condensation of the excitonic bound states in the extended Falicov-Kimball model by the density-matrix-renormalization-group (DMRG) method. Analysing the resultant behaviours of the excitonic momentum distribution N(q) we found, that unlike the local hybridization V, which supports the formation of the q=0 momentum condensate, the nonlocal hybridization Vn supports the formation of the q = π momentum condensate. The combined effect of local and nonlocal hybridization further enhances the excitonic correlations in q=0 as well as q = π state, especially for V and Vn values from the charge-density-wave (CDW) region. Strong effects of local and nonlocal hybridization are observed also for other ground-state quantities of the model such as the f-electron density, or the density of unbound d-electrons, which are generally enhanced with increasing V and Vn. The same calculations performed for nonzero values of f-level energy Ef revealed that this model can yield a reasonable explanation for the pressure-induced resistivity anomaly observed experimentally in TmSe0.45Te0.55 compound.

  10. Reconfigurable exciton-plasmon interconversion for nanophotonic circuits

    Science.gov (United States)

    Lee, Hyun Seok; Luong, Dinh Hoa; Kim, Min Su; Jin, Youngjo; Kim, Hyun; Yun, Seokjoon; Lee, Young Hee

    2016-11-01

    The recent challenges for improving the operation speed of nanoelectronics have motivated research on manipulating light in on-chip integrated circuits. Hybrid plasmonic waveguides with low-dimensional semiconductors, including quantum dots and quantum wells, are a promising platform for realizing sub-diffraction limited optical components. Meanwhile, two-dimensional transition metal dichalcogenides (TMDs) have received broad interest in optoelectronics owing to tightly bound excitons at room temperature, strong light-matter and exciton-plasmon interactions, available top-down wafer-scale integration, and band-gap tunability. Here, we demonstrate principal functionalities for on-chip optical communications via reconfigurable exciton-plasmon interconversions in ~200-nm-diameter Ag-nanowires overlapping onto TMD transistors. By varying device configurations for each operation purpose, three active components for optical communications are realized: field-effect exciton transistors with a channel length of ~32 μm, field-effect exciton multiplexers transmitting multiple signals through a single NW and electrical detectors of propagating plasmons with a high On/Off ratio of~190. Our results illustrate the unique merits of two-dimensional semiconductors for constructing reconfigurable device architectures in integrated nanophotonic circuits.

  11. Interband Optical Transitions due to Donor Bound Excitons in Wurtzite InGaN Strained Coupled Quantum Dots: Strong Built-in Electric Field Effects

    Institute of Scientific and Technical Information of China (English)

    CHI Yue-Meng; SHI Jun-Jie

    2006-01-01

    @@ Considering the three-dimensional confinement of the electrons and holes and the strong built-in electric field (BEF) in the wurtzite InGaN strained coupled quantum dots (QDs), the positively charged donor bound exciton states and interband optical transitions are investigated theoretically by means of a variational method. Our calculations indicate that the emission wavelengths sensitively depend on the donor position, the strong BEF,and the structure parameters of the QD system.

  12. Amine reactivity with charged sulfuric acid clusters

    OpenAIRE

    Bzdek, B. R.; D. P. Ridge; Johnston, M. V.

    2011-01-01

    The distribution of ionic species produced by electrospray of an ammonium sulfate solution in both positive and negative polarities is examined using Fourier transform ion cyclotron resonance mass spectrometry (FTICR-MS). Positively-charged ammonium bisulfate cluster composition differs significantly from negatively-charged cluster composition. For positively-charged clusters all sulfuric acid is neutralized to bisulfate, whereas for negatively-charged clusters the degree of sulfuric acid neu...

  13. Exciton effective mass enhancement in coupled quantum wells in electric and magnetic fields

    Science.gov (United States)

    Wilkes, J.; Muljarov, E. A.

    2016-02-01

    We present a calculation of exciton states in semiconductor coupled quantum wells in the presence of electric and magnetic fields applied perpendicular to the QW plane. The exciton Schrödinger equation is solved in real space in three-dimensions to obtain the Landau levels of both direct and indirect excitons. Calculation of the exciton energy levels and oscillator strengths enables mapping of the electric and magnetic field dependence of the exciton absorption spectrum. For the ground state of the system, we evaluate the Bohr radius, optical lifetime, binding energy and dipole moment. The exciton mass renormalization due to the magnetic field is calculated using a perturbative approach. We predict a non-monotonous dependence of the exciton ground state effective mass on magnetic field. Such a trend is explained in a classical picture, in terms of the ground state tending from an indirect to a direct exciton with increasing magnetic field.

  14. Single Molecule Photobleaching Probes the Exciton Wavefunction in a Multichromophoric System

    NARCIS (Netherlands)

    Hernando, J.; Hoogenboom, J.P.; Dijk, van E.M.H.P.; Garcia-Lopez, J.J.; Crego Calama, M.; Reinhoudt, D.N.; Hulst, van N.F.; Garcia-Parajo, M.F.

    2004-01-01

    The exciton wave function of a trichromophoric system is investigated by means of single molecule spectroscopy at room temperature. Individual trimers exhibit superradiance and loss of vibronic structure in emission spectrum, features proving exciton delocalization. We identify two distinct photodeg

  15. Systematic study of exciton diffusion length in organic semiconductors by six experimental methods

    NARCIS (Netherlands)

    Lin, Jason D. A.; Mikhnenko, Oleksandr V.; Chen, Jingrun; Masri, Zarifi; Ruseckas, Arvydas; Mikhailovsky, Alexander; Raab, Reilly P.; Liu, Jianhua; Blom, Paul W. M.; Loi, Maria Antonietta; Garcia-Cervera, Carlos J.; Samuel, Ifor D. W.; Thuc-Quyen Nguyen, [No Value

    Six experimental methods have been used to investigate the exciton diffusion length in materials with systematic chemical modifications. We find that exciton diffusion length correlates with molecular ordering. We discuss situations in which certain experimental techniques are more appropriate.

  16. Charge-driven feedback loop in the resonance fluorescence of a single quantum dot

    Science.gov (United States)

    Merkel, B.; Kurzmann, A.; Schulze, J.-H.; Strittmatter, A.; Geller, M.; Lorke, A.

    2017-03-01

    We demonstrate a feedback loop that manifests itself in a strong hysteresis and bistability of the exciton resonance fluorescence signal. Field ionization of photogenerated quantum dot excitons leads to the formation of a charged interface layer that drags the emission line along over a frequency range of more than 30 GHz . These measurements are well described by a rate equation model. With a time-resolved resonance fluorescence measurement we determined the buildup times for the hole gas in the orders of milliseconds. This internal charge-driven feedback loop could be used to reduce the spectral wandering in the emission spectra of single self-assembled quantum dots.

  17. Communication: Exciton analysis in time-dependent density functional theory: How functionals shape excited-state characters.

    Science.gov (United States)

    Mewes, Stefanie A; Plasser, Felix; Dreuw, Andreas

    2015-11-01

    Excited-state descriptors based on the one-particle transition density matrix referring to the exciton picture have been implemented for time-dependent density functional theory. State characters such as local, extended ππ(∗), Rydberg, or charge transfer can be intuitively classified by simple comparison of these descriptors. Strong effects of the choice of the exchange-correlation kernel on the physical nature of excited states can be found and decomposed in detail leading to a new perspective on functional performance and the design of new functionals.

  18. Large Range Manipulation of Exciton Species in Monolayer WS2

    CERN Document Server

    Wei, Ke; Yang, Hang; Cheng, Xiangai; Jiang, Tian

    2016-01-01

    Unconventional emissions from exciton and trion in monolayer WS2 are studied by photoexcitation. Excited by 532nm laser beam, the carrier species in the monolayer WS2 are affected by the excess electrons escaping from photoionization of donor impurity, the concentration of which varies with different locations of the sample. Simply increasing the excitation power at room temperature, the excess electron and thus the intensity ratio of excited trion and exciton can be continuously tuned over a large range from 0.1 to 7.7. Furthermore, this intensity ratio can also be manipulated by varying temperature. However, in this way the resonance energy of the exciton and trion show red-shifts with increasing temperature due to electron-phonon coupling. The binding energy of the trion is determined to be ~23meV and independent to temperature, indicating strong Coulomb interaction of carriers in such 2D materials.

  19. Exciton coupling induces vibronic hyperchromism in light-harvesting complexes

    CERN Document Server

    Schulze, Jan; Kühn, Oliver; Pullerits, Tõnu

    2013-01-01

    The recently suggested possibility that weak vibronic transitions can be excitonically enhanced in light-harvesting complexes is studied in detail. A vibronic exciton dimer model which includes ground state vibrations is investigated using multi-configuration time-dependent Hartree method with a parameter set typical to photosynthetic light-harvesting complexes. Absorption spectra are discussed in dependence on the Coulomb coupling, the detuning of site energies, and the number of vibrational mode. Calculations of the fluorescence spectra show that the spectral densities obtained from the low temperature fluorescence line narrowing measurements of light-harvesting systems need to be corrected for the exciton effects. For the J-aggregate configuration, as in most of the light-harvesting complexes, the true spectral density has larger amplitude than what is obtained from the measurement.

  20. Tuning the driving force for exciton dissociation in single-walled carbon nanotube heterojunctions

    Science.gov (United States)

    Ihly, Rachelle; Mistry, Kevin S.; Ferguson, Andrew J.; Clikeman, Tyler T.; Larson, Bryon W.; Reid, Obadiah; Boltalina, Olga V.; Strauss, Steven H.; Rumbles, Garry; Blackburn, Jeffrey L.

    2016-06-01

    Understanding the kinetics and energetics of interfacial electron transfer in molecular systems is crucial for the development of a broad array of technologies, including photovoltaics, solar fuel systems and energy storage. The Marcus formulation for electron transfer relates the thermodynamic driving force and reorganization energy for charge transfer between a given donor/acceptor pair to the kinetics and yield of electron transfer. Here we investigated the influence of the thermodynamic driving force for photoinduced electron transfer (PET) between single-walled carbon nanotubes (SWCNTs) and fullerene derivatives by employing time-resolved microwave conductivity as a sensitive probe of interfacial exciton dissociation. For the first time, we observed the Marcus inverted region (in which driving force exceeds reorganization energy) and quantified the reorganization energy for PET for a model SWCNT/acceptor system. The small reorganization energies (about 130 meV, most of which probably arises from the fullerene acceptors) are beneficial in minimizing energy loss in photoconversion schemes.