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Sample records for carbon nanorings excitonic

  1. Optoelectronic Properties of Carbon Nanorings: Excitonic Effects from Time-Dependent Density Functional Theory

    CERN Document Server

    Wong, Bryan M

    2009-01-01

    The electronic structure and size-scaling of optoelectronic properties in cycloparaphenylene carbon nanorings are investigated using time-dependent density functional theory (TDDFT). The TDDFT calculations on these molecular nanostructures indicate that the lowest excitation energy surprisingly becomes larger as the carbon nanoring size is increased, in contradiction with typical quantum confinement effects. In order to understand their unusual electronic properties, I performed an extensive investigation of excitonic effects by analyzing electron-hole transition density matrices and exciton binding energies as a function of size in these nanoring systems. 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 the nanorings. Based on overall trends in exciton binding energies and their spatial delocalization, I find that excitonic effects play a vital role...

  2. Excitonic Absorption of Semiconductor Nanorings under Terahertz Fields

    Institute of Scientific and Technical Information of China (English)

    ZHANG Tong-Yi; ZHAO Wei; ZHU Shao-Lan

    2005-01-01

    @@ The optical absorption of GaAs nanorings (NRs) under a dc electric field and a terahertz (THz) ac electric field applied in the plane containing the NRs is investigated theoretically. The NRs may enclose some magnetic flux in the presence of a magnetic field perpendicular to the NRs plane. Numerical calculation shows that the excitonic effects are essential to correctly describe the optical absorption in NRs. The applied lateral THz electric field, as well as the dc field leads to reduction, broadening and splitting of the exciton peak. In contrast to the presence of a dc field, significant optical absorption peak arises below the zero-field bandgap in the presence of a THz electric field at a certain frequency. The optical absorption spectrum depends evidently on the frequency and amplitude of the applied THz field and on the magnetic flux threading the NRs. This promises potential applications of NRs for magneto-optical and THz electro-optical sensing.

  3. Carbon nanotube-nucleobase hybrids: nanorings from uracil-modified single-walled carbon nanotubes.

    Science.gov (United States)

    Singh, Prabhpreet; Toma, Francesca Maria; Kumar, Jitendra; Venkatesh, V; Raya, Jesus; Prato, Maurizio; Verma, Sandeep; Bianco, Alberto

    2011-06-06

    Single-walled carbon nanotubes (SWCNTs) have been covalently functionalized with uracil nucleobase. The hybrids have been characterized by using complementary spectroscopic and microscopic techniques including solid-state NMR spectroscopy. The uracil-functionalized SWCNTs are able to self-assemble into regular nanorings with a diameter of 50-70 nm, as observed by AFM and TEM. AFM shows that the rings do not have a consistent height and thickness, which indicates that they may be formed by separate bundles of CNTs. The simplest model for the nanoring formation likely involves two bundles of CNTs interacting with each other via uracil-uracil base-pairing at both CNT ends. These nanorings can be envisaged for the development of advanced electronic circuits.

  4. Carbon nanorings with inserted acenes: breaking symmetry in excited state dynamics

    Science.gov (United States)

    Franklin-Mergarejo, R.; Alvarez, D. Ondarse; Tretiak, S.; Fernandez-Alberti, S.

    2016-08-01

    Conjugated cycloparaphenylene rings have unique electronic properties being the smallest segments of carbon nanotubes. Their conjugated backbones support delocalized electronic excitations, which dynamics is strongly influenced by cyclic geometry. Here we present a comparative theoretical study of the electronic and vibrational energy relaxation and redistribution in photoexcited cycloparaphenylene carbon nanorings with inserted naphthalene, anthracene, and tetracene units using non-adiabatic excited-state molecular dynamics simulations. Calculated excited state structures reflect modifications of optical selection rules and appearance of low-energy electronic states localized on the acenes due to gradual departure from a perfect circular symmetry. After photoexcitation, an ultrafast electronic energy relaxation to the lowest excited state is observed on the time scale of hundreds of femtoseconds in all molecules studied. Concomitantly, the efficiency of the exciton trapping in the acene raises when moving from naphthalene to anthracene and to tetracene, being negligible in naphthalene, and ~60% and 70% in anthracene and tetracene within the first 500 fs after photoexcitation. Observed photoinduced dynamics is further analyzed in details using induced molecular distortions, delocatization properties of participating electronic states and non-adiabatic coupling strengths. Our results provide a number of insights into design of cyclic molecular systems for electronic and light-harvesting applications.

  5. 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.

  6. 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...

  7. 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...

  8. 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)

  9. 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.

  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. Multiparticle Exciton Ionization in Shallow Doped Carbon Nanotubes.

    Science.gov (United States)

    Sau, Jay D; Crochet, Jared J; Doorn, Stephen K; Cohen, Marvin L

    2013-03-21

    Shallow hole doping in small-diameter semiconducting carbon nanotubes with a valley degeneracy is predicted to result in the resonant ionization of excitons into free electron-hole pairs. This mechanism, which relies on the chirality of the electronic states, causes excitons to decay with high efficiencies where the rate scales as the square of the dopant density. Moreover, multiparticle exciton ionization can account for delocalized fluorescence quenching when a few holes per micrometer of tube length are present.

  12. 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.

  13. 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....

  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. Electrochemical performance and structure evolution of core-shell nano-ring α-Fe2O3@Carbon anodes for lithium-ion batteries

    Science.gov (United States)

    Sun, Yan-Hui; Liu, Shan; Zhou, Feng-Chen; Nan, Jun-Min

    2016-12-01

    Core-shell nano-ring α-Fe2O3@Carbon (CSNR) composites with different carbon content (CSNR-5%C and CSNR-13%C) are synthesized using a hydrothermal method by controlling different amounts of glucose and α-Fe2O3 nano-rings with further annealing. The CSNR electrodes exhibit much improved specific capacity, cycling stability and rate capability compared with that of bare nano-ring α-Fe2O3 (BNR), which is attributed to the core-shell nano-ring structure of CSNR. The carbon shell in the inner and outer surface of CSNR composite can increase electron conductivity of the electrode and inhibit the volume change of α-Fe2O3 during discharge/charge processes, and the nano-ring structure of CSNR can buffer the volume change too. The CSNR-5%C electrode shows super high initial discharge/charge capacities of 1570/1220 mAh g-1 and retains 920/897 mAh g-1 after 200 cycles at 500 mA g-1 (0.5C). Even at 2000 mA g-1 (2C), the electrode delivers the initial capacities of 1400/900 mAh g-1, and still maintains 630/610 mAh g-1 after 200 cycles. The core-shell nano-rings opened during cycling and rebuilt a new flower-like structure consisting of α-Fe2O3@Carbon nano-sheets. The space among the nano-sheet networks can further buffer the volume expansion of α-Fe2O3 and facilitate the transportation of electrons and Li+ ions during the charge/discharge processes, which increases the capacity and rate capability of the electrode. It is the first time that the evolution of core-shell α-Fe2O3@Carbon changing to flower-like networks during lithiation/de-lithiation has been reported.

  16. 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....

  17. Electrodynamic and excitonic intertube interactions in semiconducting carbon nanotube aggregates.

    Science.gov (United States)

    Crochet, Jared J; Sau, Jay D; Duque, Juan G; Doorn, Stephen K; Cohen, Marvin L

    2011-04-26

    The optical properties of selectively aggregated, nearly single chirality single-wall carbon nanotubes were investigated by both continuous-wave and time-resolved spectroscopies. With reduced sample heterogeneities, we have resolved aggregation-dependent reductions of the excitation energy of the S(1) exciton and enhanced electron-hole pair absorption. Photoluminescence spectra revealed a spectral splitting of S(1) and simultaneous reductions of the emission efficiencies and nonradiative decay rates. The observed strong deviations from isolated tube behavior are accounted for by enhanced screening of the intratube Coulomb interactions, intertube exciton tunneling, and diffusion-driven exciton quenching. We also provide evidence that density gradient ultracentrifugation can be used to structurally sort single-wall carbon nanotubes by aggregate size as evident by a monotonic dependence of the aforementioned optical properties on buoyant density.

  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. 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...

  20. Disorder limited exciton transport in colloidal single-wall carbon nanotubes.

    Science.gov (United States)

    Crochet, Jared J; Duque, Juan G; Werner, James H; Lounis, Brahim; Cognet, Laurent; Doorn, Stephen K

    2012-10-10

    We present measurements of S(1) exciton transport in (6,5) carbon nanotubes at room temperature in a colloidal environment. Exciton diffusion lengths associated with end quenching paired with photoluminescence lifetimes provide a direct basis for determining a median diffusion constant of approximately 7.5 cm(2)s(-1). Our experimental results are compared to model diffusion constants calculated using a realistic exciton dispersion accounting for a logarithmic correction due to the exchange self-energy and a nonequilibrium distribution between bright and dark excitons. The intrinsic diffusion constant associated with acoustic phonon scattering is too large to explain the observed diffusion length, and as such, we attribute the observed transport to disorder-limited diffusional transport associated with the dynamics of the colloidal interface. In this model an effective surface potential limits the exciton mean free path to the same size as that of the exciton wave function, defined by the strength of the electron-hole Coulomb interaction.

  1. Excitonic signatures in the optical response of single-wall carbon nanotubes

    Energy Technology Data Exchange (ETDEWEB)

    Voisin, Christophe; Berger, Sebastien; Cassabois, Guillaume; Roussignol, Philippe [Laboratoire Pierre Aigrain, Ecole Normale Superieure, CNRS UMR8551, UPMC, Universite Paris Diderot, 24 rue Lhomond, 75005 Paris (France); Berciaud, Stephane [IPCMS, UMR 7504, CNRS Universite de Strasbourg, 23 rue du Loess, 67034 Strasbourg (France); Yan, Hugen; Hone, James; Heinz, Tony F. [Physics, Mechanical Engineering and Electrical Engineering Departments, Columbia University, New York, NY (United States); Lauret, Jean-Sebastien [Laboratoire de Photonique Quantique et Moleculaire, Ecole Normale Superieure de Cachan, CNRS UMR 8537, Institut Dalembert, 61 Avenue Wilson, Cachan (France)

    2012-05-15

    The optical properties of single-wall carbon nanotubes (SWNTs) are dominated by the excitonic character of the transitions even at room temperature. The very peculiar properties of these excitons arise from both the one-dimensional (1D) nature of carbon nanotubes and from the electronic properties of graphene from which nanotubes are made. We first propose a brief qualitative review of the structure of the excitonic manifold and emphasize the role of dark states. We describe recent experimental investigations of this excitonic structure by means of temperature dependent PL measurements. We investigate the case of upper sub-bands and show that high-order optical transitions remain excitonic for large diameter nanotubes. A careful investigation of Rayleigh scattering spectra at the single nanotube level reveals clear exciton-phonon side-bands and Lorentzian line profiles for all semi-conducting nanotubes. In contrast, metallic nanotubes show an ambivalent behavior which is related to the reduced excitonic binding energy. Schematic of the exciton manifold in single-wall carbon nanotubes. (Copyright copyright 2012 WILEY-VCH Verlag GmbH and Co. KGaA, Weinheim)

  2. Quantum dot-like excitonic behavior in individual single walled-carbon nanotubes

    Science.gov (United States)

    Wang, Xu; Alexander-Webber, Jack A.; Jia, Wei; Reid, Benjamin P. L.; Stranks, Samuel D.; Holmes, Mark J.; Chan, Christopher C. S.; Deng, Chaoyong; Nicholas, Robin J.; Taylor, Robert A.

    2016-11-01

    Semiconducting single-walled carbon nanotubes are one-dimensional materials with great prospects for applications such as optoelectronic and quantum information devices. Yet, their optical performance is hindered by low fluorescent yield. Highly mobile excitons interacting with quenching sites are attributed to be one of the main non-radiative decay mechanisms that shortens the exciton lifetime. In this paper we report on time-integrated photoluminescence measurements on individual polymer wrapped semiconducting carbon nanotubes. An ultra narrow linewidth we observed demonstrates intrinsic exciton dynamics. Furthermore, we identify a state filling effect in individual carbon nanotubes at cryogenic temperatures as previously observed in quantum dots. We propose that each of the CNTs is segmented into a chain of zero-dimensional states confined by a varying local potential along the CNT, determined by local environmental factors such as the amount of polymer wrapping. Spectral diffusion is also observed, which is consistent with the tunneling of excitons between these confined states.

  3. Exciton diffusion in air-suspended single-walled carbon nanotubes

    OpenAIRE

    Moritsubo, S.; Murai, T; Shimada, T.; Murakami, Y.; Chiashi, S.; Maruyama, S; Kato, Y. K.

    2010-01-01

    Direct measurements of the diffusion length of excitons in air-suspended single-walled carbon nanotubes are reported. Photoluminescence microscopy is used to identify individual nanotubes and to determine their lengths and chiral indices. Exciton diffusion length is obtained by comparing the dependence of photoluminescence intensity on the nanotube length to numerical solutions of diffusion equations. We find that the diffusion length in these clean, as-grown nanotubes is significantly longer...

  4. Control of quantum interference of an excitonic wave in a chlorophyll chain with a chlorophyll ring

    Energy Technology Data Exchange (ETDEWEB)

    Hong, Suc-Kyoung; Nam, Seog-Woo [Korea University, Jochiwon, Chungnam (Korea, Republic of); Yeon, Kyu-Hwang [Chungbuk National University, Cheonju (Korea, Republic of)

    2010-06-15

    The quantum interference of an excitonic wave and its coherent control in a nanochain with a nanoring are studied. The nanochain is comprised of six chlorophylls, where four chlorophylls compose the nanoring and two chlorophylls are attached at two opposite sites on the nanoring. The exciton dynamics and the correlation of the excitation between chlorophylls are analyzed for a given configurational arrangement and dipolar orientation of the chlorophylls. The results of this study show that the excitation at specified chlorophylls is suppressed or enhanced by destructive or constructive interference of the excitonic wave in the chlorophyll nanochain.

  5. 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.

  6. Prolonged spontaneous emission and dephasing of localized excitons in air-bridged carbon nanotubes

    Science.gov (United States)

    Sarpkaya, Ibrahim; Zhang, Zhengyi; Walden-Newman, William; Wang, Xuesi; Hone, James; Wong, Chee W.; Strauf, Stefan

    2013-07-01

    The bright exciton emission of carbon nanotubes is appealing for optoelectronic devices and fundamental studies of light-matter interaction in one-dimensional nanostructures. However, to date, the photophysics of excitons in carbon nanotubes is largely affected by extrinsic effects. Here we perform time-resolved photoluminescence measurements over 14 orders of magnitude for ultra-clean carbon nanotubes bridging an air gap over pillar posts. Our measurements demonstrate a new regime of intrinsic exciton photophysics with prolonged spontaneous emission times up to T1=18 ns, about two orders of magnitude better than prior measurements and in agreement with values hypothesized by theorists about a decade ago. Furthermore, we establish for the first time exciton decoherence times of individual nanotubes in the time domain and find fourfold prolonged values up to T2=2.1 ps compared with ensemble measurements. These first observations motivate new discussions about the magnitude of the intrinsic dephasing mechanism while the prolonged exciton dynamics is promising for applications.

  7. 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.

  8. Photoluminescence imaging of electronic-impurity-induced exciton quenching in single-walled carbon nanotubes.

    Science.gov (United States)

    Crochet, Jared J; Duque, Juan G; Werner, James H; Doorn, Stephen K

    2012-02-01

    The electronic properties of single-walled carbon nanotubes can be altered by surface adsorption of electronic impurities or dopants. However, fully understanding the influence of these impurities is difficult because of the inherent complexity of the solution-based colloidal chemistry of nanotubes, and because of a lack of techniques for directly imaging dynamic processes involving these impurities. Here, we show that photoluminescence microscopy can be used to image exciton quenching in semiconducting single-walled carbon nanotubes during the early stages of chemical doping with two different species. The addition of AuCl(3) leads to localized exciton-quenching sites, which are attributed to a mid-gap electronic impurity level, and the adsorbed species are also found sometimes to be mobile on the surface of the nanotubes. The addition of H(2)O(2) leads to delocalized exciton-quenching hole states, which are responsible for long-range photoluminescence blinking, and are also mobile.

  9. Excitonic effects on coherent phonon dynamics in single-wall carbon nanotubes

    Science.gov (United States)

    Nugraha, A. R. T.; Rosenthal, E. I.; Hasdeo, E. H.; Sanders, G. D.; Stanton, C. J.; Dresselhaus, M. S.; Saito, R.

    2013-08-01

    We discuss how excitons can affect the generation of coherent radial breathing modes in the ultrafast spectroscopy of single-wall carbon nanotubes. Photoexcited excitons can be localized spatially and give rise to a spatially distributed driving force in real space which involves many phonon wave vectors of the exciton-phonon interaction. The equation of motion for the coherent phonons is modeled phenomenologically by the Klein-Gordon equation, which we solve for the oscillation amplitudes as a function of space and time. By averaging the calculated amplitudes per nanotube length, we obtain time-dependent coherent phonon amplitudes that resemble the homogeneous oscillations that are observed in some pump-probe experiments. We interpret this result to mean that the experiments are only able to see a spatial average of coherent phonon oscillations over the wavelength of light in carbon nanotubes and the microscopic details are averaged out. Our interpretation is justified by calculating the time-dependent absorption spectra resulting from the macroscopic atomic displacements induced by the coherent phonon oscillations. The calculated coherent phonon spectra including excitonic effects show the experimentally observed symmetric peaks at the nanotube transition energies, in contrast to the asymmetric peaks that would be obtained if excitonic effects were not included.

  10. Exciton Distribution between the Bright and Dark States in Single Carbon Nanotubes Studied by Magneto-Photoluminescence Spectroscopy

    Science.gov (United States)

    Matsunaga, Ryusuke; Matsuda, Kazunari; Kanemitsu, Yoshihiko

    2009-03-01

    We have performed micro-photoluminescence (PL) spectroscopy for single carbon nanotubes under magnetic fields at various temperatures. Sharp PL spectra of single carbon nanotubes allow us to directly observe the dark exciton PL peak a few meV below the bright exciton PL peak due to the Aharonov-Bohm effect [1]. From the PL intensity ratio of the dark to the bright excitons under magnetic fields, we found that the non-equilibrium (non-Boltzmann) distribution occurs between the bright and dark states, because phonons cannot scatter excitons between the two states with different parities [2]. Furthermore, we discuss the diameter dependence of the exciton population of the bright and dark states in single carbon nanotubes. [1] R. Matsunaga, K. Matsuda, and Y. Kanemitsu, Phys. Rev. Lett. 101, 147404 (2008). [2] V. Perebeinos, J. Tersoff, and Ph. Avouris, Nano Lett. 5, 2495 (2005).

  11. Exciton Radiative Lifetimes and Their Temperature Dependence in Single-Walled Carbon Nanotubes

    Science.gov (United States)

    Miyauchi, Yuhei; Matsunaga, Ryusuke; Hirori, Hideki; Matsuda, Kazunari; Kanemitsu, Yoshihiko

    2009-03-01

    We have investigated the radiative lifetimes of excitons in single-walled carbon nanotubes (SWNTs) from simultaneous measurements of the photoluminescence (PL) lifetimes [1] and the PL quantum yields. A high-quality sample of PFO dispersed-SWNTs was used for the PL measurements. The evaluated radiative lifetimes were ˜5-15 ns for SWNTs with diameters ˜0.8-1.1 nm at room temperature. The radiative lifetimes increased with the tube diameter. The exciton spatial coherence volume (length) was of the order 10 ^2 nm along the tube axis, as deduced from the radiative lifetimes. Furthermore, we discuss the dynamics of bright and dark excitons [2] from the temperature dependence of the radiative lifetime (10 to 300 K).[3pt] [1] H. Hirori, K. Matsuda, Y. Miyauchi, S. Maruyama, and Y. Kanemitsu, Phys. Rev. Lett. 97, 257401 (2006). [0pt] [2] R. Matsunaga, K. Matsuda, and Y. Kanemitsu, Phys. Rev. Lett. 101, 147404 (2008).

  12. 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

  13. Excitonic effects in third-harmonic generation: The case of carbon nanotubes and nanoribbons

    Science.gov (United States)

    Attaccalite, C.; Cannuccia, E.; Grüning, M.

    2017-03-01

    Linear and nonlinear optical properties of low-dimensional nanostructures have attracted great interest from the scientific community as tools to probe the strong confinement of electrons and for possible applications in optoelectronic devices. In particular it has been shown that the linear optical response of carbon nanotubes [F. Wang et al., Science 308, 838 (2005), 10.1126/science.1110265] and graphene nanoribbons [Nat. Commun. 5 4253 (2014), 10.1038/ncomms5253] is dominated by bounded electron-hole pairs, excitons. The role of excitons in linear response has been widely studied, but still, little is known about their effect on nonlinear susceptibilities. Using a recently developed methodology [Phys. Rev. B 88, 235113 (2013), 10.1103/PhysRevB.88.235113] based on well-established ab initio many-body perturbation theory approaches, we find that quasiparticle shifts and excitonic effects significantly modify the third-harmonic generation in carbon nanotubes and graphene nanoribbons. For both systems the net effect of many-body effects is to reduce the intensity of the main peak in the independent-particle spectrum and redistribute the spectral weight among several excitonic resonances.

  14. Experimental determination of excitonic band structures of single-walled carbon nanotubes using circular dichroism spectra

    Science.gov (United States)

    Wei, Xiaojun; Tanaka, Takeshi; Yomogida, Yohei; Sato, Naomichi; Saito, Riichiro; Kataura, Hiromichi

    2016-10-01

    Experimental band structure analyses of single-walled carbon nanotubes have not yet been reported, to the best of our knowledge, except for a limited number of reports using scanning tunnelling spectroscopy. Here we demonstrate the experimental determination of the excitonic band structures of single-chirality single-walled carbon nanotubes using their circular dichroism spectra. In this analysis, we use gel column chromatography combining overloading selective adsorption with stepwise elution to separate 12 different single-chirality enantiomers. Our samples show higher circular dichroism intensities than the highest values reported in previous works, indicating their high enantiomeric purity. Excitonic band structure analysis is performed by assigning all observed Eii and Eij optical transitions in the circular dichroism spectra. The results reproduce the asymmetric structures of the valence and conduction bands predicted by density functional theory. Finally, we demonstrate that an extended empirical formula can estimate Eij optical transition energies for any (n,m) species.

  15. 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.

  16. Ultrafast vibrations of gold nanorings

    DEFF Research Database (Denmark)

    Kelf, T; Tanaka, Y; Matsuda, O;

    2011-01-01

    elucidate the corresponding mode shapes and find that the substrate plays an important role in determining the mode damping. This study demonstrates the need for a plasmonic nano-optics approach to understand the optical excitation and detection mechanisms for the vibrations of plasmonic nanostructures.......We investigate the vibrational modes of gold nanorings on a silica substrate with an ultrafast optical technique. By comparison with numerical simulations, we identify several resonances in the gigahertz range associated with axially symmetric deformations of the nanoring and substrate. We...

  17. Photoluminescence Imaging of Polyfluorene Surface Structures on Semiconducting Carbon Nanotubes: Implications for Thin Film Exciton Transport.

    Science.gov (United States)

    Hartmann, Nicolai F; Pramanik, Rajib; Dowgiallo, Anne-Marie; Ihly, Rachelle; Blackburn, Jeffrey L; Doorn, Stephen K

    2016-12-27

    Single-walled carbon nanotubes (SWCNTs) have potential to act as light-harvesting elements in thin film photovoltaic devices, but performance is in part limited by the efficiency of exciton diffusion processes within the films. Factors contributing to exciton transport can include film morphology encompassing nanotube orientation, connectivity, and interaction geometry. Such factors are often defined by nanotube surface structures that are not yet well understood. Here, we present the results of a combined pump-probe and photoluminescence imaging study of polyfluorene (PFO)-wrapped (6,5) and (7,5) SWCNTs that provide additional insight into the role played by polymer structures in defining exciton transport. Pump-probe measurements suggest exciton transport occurs over larger length scales in films composed of PFO-wrapped (7,5) SWCNTs, compared to those prepared from PFO-bpy-wrapped (6,5) SWCNTs. To explore the role the difference in polymer structure may play as a possible origin of differing transport behaviors, we performed a photoluminescence imaging study of individual polymer-wrapped (6,5) and (7,5) SWCNTs. The PFO-bpy-wrapped (6,5) SWCNTs showed more uniform intensity distributions along their lengths, in contrast to the PFO-wrapped (7,5) SWCNTs, which showed irregular, discontinuous intensity distributions. These differences likely originate from differences in surface coverage and suggest the PFO wrapping on (7,5) nanotubes produces a more open surface structure than is available with the PFO-bpy wrapping of (6,5) nanotubes. The open structure likely leads to improved intertube coupling that enhances exciton transport within the (7,5) films, consistent with the results of our pump-probe measurements.

  18. Photoluminescence Imaging of Polyfluorene Surface Structures on Semiconducting Carbon Nanotubes: Implications for Thin Film Exciton Transport

    Energy Technology Data Exchange (ETDEWEB)

    Hartmann, Nicolai F.; Pramanik, Rajib; Dowgiallo, Anne-Marie; Ihly, Rachelle; Blackburn, Jeffrey L.; Doorn, Stephen K.

    2016-12-27

    Single-walled carbon nanotubes (SWCNTs) have potential to act as light-harvesting elements in thin film photovoltaic devices, but performance is in part limited by the efficiency of exciton diffusion processes within the films. Factors contributing to exciton transport can include film morphology encompassing nanotube orientation, connectivity, and interaction geometry. Such factors are often defined by nanotube surface structures that are not yet well understood. Here, we present the results of a combined pump-probe and photoluminescence imaging study of polyfluorene (PFO)-wrapped (6,5) and (7,5) SWCNTs that provide additional insight into the role played by polymer structures in defining exciton transport. Pump-probe measurements suggest exciton transport occurs over larger length scales in films composed of PFO-wrapped (7,5) SWCNTs, compared to those prepared from PFO-bpy-wrapped (6,5) SWCNTs. To explore the role the difference in polymer structure may play as a possible origin of differing transport behaviors, we performed a photoluminescence imaging study of individual polymer-wrapped (6,5) and (7,5) SWCNTs. The PFO-bpy-wrapped (6,5) SWCNTs showed more uniform intensity distributions along their lengths, in contrast to the PFO-wrapped (7,5) SWCNTs, which showed irregular, discontinuous intensity distributions. These differences likely originate from differences in surface coverage and suggest the PFO wrapping on (7,5) nanotubes produces a more open surface structure than is available with the PFO-bpy wrapping of (6,5) nanotubes. The open structure likely leads to improved intertube coupling that enhances exciton transport within the (7,5) films, consistent with the results of our pump-probe measurements.

  19. Exciton States and Linear Optical Spectra of Semiconducting Carbon Nanotubes under Uniaxial Strain

    Institute of Scientific and Technical Information of China (English)

    YU Gui-Li; JIA Yong-Lei

    2009-01-01

    Considering the exciton effect,the linear optical spectra of semiconducting single-walled carbon nanotubes (SWNTs) under uniaxial strain are theoretically studied by using the standard formulae of Orr and Ward [Mol.Phys.20(1971)513].It is found that due to the wrapping effect existing in the semiconducting zigzag tubes,the excitation energies of the linear optical spectra show two different kinds of variations with increasing uniaxial strain,among which one decreases such as tube (11,0),and the other increases firstly and then decreases such as tube (10,0).These variations of the linear optical spectra are consistent with the changes of the exciton binding energies or the (quasi)continuum edge of these SWNTs calculated in our previous work,which can be used as a supplemented tool to detect the deformation degree of an SWNT under uniaxiai strain.

  20. 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

  1. Free-Standing Bimetallic Nanorings and Nanoring Arrays Made by On-Wire Lithography

    Energy Technology Data Exchange (ETDEWEB)

    Liusman, C.; Li, S. Z.; Chen, X. D.; Wei, W.; Zhang, H.; Schatz, George C.; Boey, F.; Mirkin, Chad

    2010-12-28

    This paper describes a new strategy for synthesizing free-standing bimetallic nanorings and nanoring arrays based upon on-wire lithography and a galvanic replacement reaction. The strategy allows one to tune the diameter, length, and therefore aspect ratio of the nanorings. In addition, it can be used to produce arrays of nanorings in high yield with control over number and spacing. Spectroscopic studies and discrete dipole approximation calculations show that nanoring dimers exhibit greater surface enhanced Raman scattering than the analogous nanodisk dimers.

  2. α-Fe{sub 2}O{sub 3}@C nanorings as anode materials for high performance lithium ion batteries

    Energy Technology Data Exchange (ETDEWEB)

    Li, Le; Li, Zhenzhen; Fu, Wenming; Li, Fagen [Department of Physics, Faculty of Science, Ningbo University, Ningbo (China); Wang, Jun, E-mail: wjnaf@ustc.edu [Department of Physics, Faculty of Science, Ningbo University, Ningbo (China); Wang, Wenzhong [School of Science, Minzu University of China, Beijing 100081 (China)

    2015-10-25

    α-Fe{sub 2}O{sub 3}@C core–shell nanorings are prepared by a facile large-scale two-step route incorporating a hydrothermal method and a carbon coated progress. Its structure and morphology are characterized by X-ray diffraction, scanning electron microscopy, transmission electron microscope, and thermogravimetry. It is found that the as-prepared composite is composed of α-Fe{sub 2}O{sub 3}@C nanorings of about 148 nm in outer diameter, 50 nm in thickness, and 115 nm in length. These α-Fe{sub 2}O{sub 3}@C nanorings are enwrapped with ∼3 nm thick carbon shell. And the electrodes exhibit longer cycle life (815 mAhg{sup −1} after cycling 160 times) at high current rate (1000 mAg{sup −1}) compared with that of bare α-Fe{sub 2}O{sub 3} nanorings (810 mAhg{sup −1} after cycling 30 times). The improved performance of the composite is attributed to the bondage from carbon shell, which can enhance the electronic conductivity and structural stability of α-Fe{sub 2}O{sub 3} nanorings. - Highlights: • α-Fe{sub 2}O{sub 3}@C core–shell nanorings are prepared by a facile two-step route. • The α-Fe{sub 2}O{sub 3}@C nanorings are firstly reported as anode materials for LIBs. • The nanorings show a high capacity of 815 mAhg{sup −1} at 1 Ag{sup -1} after 160 cycles.

  3. Self-assembled polyelectrolyte nanorings observed by liquid-cell AFM

    Energy Technology Data Exchange (ETDEWEB)

    Menchaca, J-Luis [Instituto de Fisica, Universidad Autonoma de San Luis Potosi, Alvaro Obregon 64, San Luis Potosi (Mexico); Flores, Hector [Facultad de Estomatologia, Universidad Autonoma de San Luis Potosi, Alvaro Obregon 64, San Luis Potosi (Mexico); Cuisinier, Frederic [INSERM U 595, Federation de Recherche Odontologiques, Universite Louis Pasteur, 11 rue Humann, 67085 Strasbourg Cedex (France); Perez, ElIas [Instituto de Fisica, Universidad Autonoma de San Luis Potosi, Alvaro Obregon 64, San Luis Potosi (Mexico)

    2004-06-09

    Self-assembled polyelectrolyte nanorings formed by polyelectrolytes are presented for the first time in this work. They are formed by poly(ethylenimine) (PEI) and poly(sodium 4-styrenesulfanate) (PSS) during the two first steps of the formation of the self-assembled polyelectrolyte films (SAPFs). These are formed on a negatively charged glass surface and observed by an in situ liquid-cell AFM technique, which has recently been introduced as an alternative technique to follow polyelectrolyte multilayer formation without drying effects (Menchaca et al 2003 Colloids Surf. A 222 185). Nanoring formation strongly depends on the preparation method and parameters such as polyelectrolyte filtration, air and CO{sub 2} presence during SAPFs formation and buffer solution. A necessary condition to obtain nanorings is that polyelectrolyte solutions have to be filtered prior to injection into the liquid-cell AFM. The outer diameter of nanorings can be varied from hundreds of nanometres to microns by changing these parameters. Nanorings are stable in the liquid cell for hours but they disappear on contact with air. Additionally, carbonate ions seem to be mainly responsible for the formation of this novel structure.

  4. Tuning the driving force for exciton dissociation in single-walled carbon nanotube heterojunctions

    Energy Technology Data Exchange (ETDEWEB)

    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.

    2016-04-25

    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.

  5. 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.

  6. One-Pot Silver Nanoring Synthesis

    Directory of Open Access Journals (Sweden)

    Drogat Nicolas

    2009-01-01

    Full Text Available Abstract Silver colloidal nanorings have been synthesized by reducing silver ions with NaBH4 in trisodium citrate buffers. pH increase, by addition of NaOH, was used to speed up reduction reaction. The UV–vis absorption spectra of resulting silver nanorings showed two peaks accounting for transverse and longitudinal surface plasmon resonance, at ≈400 nm, and between 600 and 700 nm, respectively. The shapes of these silver nanoparticles (nanorings depended on AgNO3/NaBH4 ratio, pH and reaction temperature. Particles were analysed by transmission electron microscopy, scanning electron microscopy and X-ray diffraction. A reaction pathway is proposed to explain silver nanoring formation.

  7. Excitonic energy transfer in polymer wrapped carbon nanotubes in gradually grown nanoassemblies.

    Science.gov (United States)

    Karachevtsev, Victor A; Plokhotnichenko, Alexander M; Glamazda, Alexander Yu; Leontiev, Victor S; Levitsky, Igor A

    2014-06-14

    We investigate the exciton energy transfer (ET) in nanoassemblies (nanotube based aggregates) formed by polymer wrapped single-walled carbon nanotubes (SWNTs) using photoluminescence (PL) spectroscopy and simulation. The distinctive feature of this study is the gradual growth of such nanostructures in aqueous medium induced by increasing the concentration of porphyrin molecules stitching nanotube-polymer complexes in densely packed assemblies. Experimental dependencies of PL intensity on the porphyrin concentration for different types of semiconducting SWNTs demonstrate step-like behavior controlled by the amount of bound nanotubes and are in good agreement with the simulating model. The simulation algorithm determines the criterion of the aggregate formation depending on the number of porphyrin molecules per tube and the cascade exciton energy transfer between neighboring semiconducting nanotubes of different chiralities. Aggregates of small sizes (up to six-eight individual tubes) contain mostly semiconducting species, while aggregates of a larger size (up to several tens of tubes) incorporate metallic SWNTs, inducing strong PL quenching. From the fitting procedure, an ET rate of 0.6 × 10(10) s(-1) has been determined which is consistent with the center to center distance (∼2.3 nm) between adjacent tubes separated by polymer and porphyrin molecules. The threshold of the dimer formation corresponds to one porphyrin molecule per ∼20 nm of tube lengths that was supported by molecular dynamics simulation. These findings provide insight into the ET mechanism in SWNT nanoassemblies of variable sizes, which can be gradually controlled by the external factor (the concentration of porphyrin molecules).

  8. Plasmon mode excitation and photoluminescence enhancement on silver nanoring

    CERN Document Server

    Kuchmizhak, A A; Kulchin, Yu N; Vitrik, O B

    2015-01-01

    We demonstrate a simple and high-performance laser-assisted technique for silver nanoring fabrication, which includes the ablation of the Ag film by focused nanosecond pulses and subsequent reactive ion polishing. The nanoring diameter and thickness can be controlled by optimizing both the pulse energy and the metal film thickness at laser ablation step, while the subsequent reactive ion polishing provides the ability to fabricate the nanoring with desirable height. Scattering patterns of s-polarized collimated laser beam obliquely illuminating the nanoring demonstrate the focal spot inside the nanoring shifted from its center at a distance of ~ 0.57Rring. Five-fold enhancement of the photoluminescence signal from the Rhodamine 6G organic dye near the Ag nanoring was demonstrated. This enhancement was attributed to the increase of the electromagnetic field amplitude near the nanoring surface arising from excitation of the multipole plasmon modes traveling along the nanoring. This assumption was confirmed by d...

  9. Photophysics of quasi-one-dimensional excitons in pi-conjugated polymers and semiconducting single-walled carbon nanotubes

    Science.gov (United States)

    Sheng, Chuanxiang

    In this work we studied the ultrafast dynamics of photoexcitations in pi-conjugated organic semiconductors and semiconducting single-walled carbon nanotubes (S-NTs), using a low-intensity high-repetition rate laser system in the spectral range from 0.13 to 1.05 eV, and high-intensity low-repletion rate laser system in the spectral range from 1.2 to 2.5 eV, in the time domain from 100 fs to 1 ns. We also measured cw photomodulation (PM) spectroscopy of pi-conjugated polymers and photoluminescence (PL) spectra of both polymers and isolated nanotubes. In polymers, we found that excitons are the primary photoexcitations in single polymer chains. However, polarons and polaron pairs may also be photogenerated at early time in films. We consider this process to be extrinsic in nature, namely, dependent on materials properties, temperatures, excitation photon energies, as well as the quality of films. Both annealed and unannealed thin NT films and D2O solutions of isolated NTs were investigated. Various transient photoinduced bleaching (PB) and photoinduced absorption (PA) bands were observed, which also showed photoinduced dichroism and decay together after taking into account the PB spectral shift. The PL emission shows polarization degree. We therefore conclude that the primary photoexcitations in S-NT are excitons that are confined along the NTs. Prom the average PL polarization degree and the transient polarization memory decay, we estimate the PL lifetime in isolated NTs in solution to be of the order of 500 ps, coupling with the minute PL emission quantum efficiency, which indicates weak radiative transition strength. In S-NTs and pi-polymers, the emission spectra relative to the absorption bands are very similar, as well as transient photoinduced absorption bands (PA) with a low-energy PA1 and a higher-energy PA2 in all cases. Theoretical calculations of excited state absorptions within a correlated pi-electron Hamiltonian show the same excitonic energy spectrum

  10. Ultrafast energy transfer of one-dimensional excitons between carbon nanotubes: a femtosecond time-resolved luminescence study.

    Science.gov (United States)

    Koyama, Takeshi; Miyata, Yasumitsu; Asaka, Koji; Shinohara, Hisanori; Saito, Yahachi; Nakamura, Arao

    2012-01-21

    Excitation energy transfer has long been an intriguing subject in the fields of photoscience and materials science. Along with the recent progress of photovoltaics, photocatalysis, and photosensors using nanoscale materials, excitation energy transfer between a donor and an acceptor at a short distance (≤1-10 nm) is of growing importance in both fundamental research and technological applications. This Perspective highlights our recent studies on exciton energy transfer between carbon nanotubes with interwall (surface-to-surface) distances of less than ∼1 nm, which are equivalent to or shorter than the size of one-dimensional excitons in carbon nanotubes. We show exciton energy transfer in bundles of single-walled carbon nanotubes with the interwall distances of ∼0.34 and 0.9 nm (center-to-center distances ∼1.3-1.4 and 1.9 nm). For the interwall distance of ∼0.34 nm (center-to-center distance ∼1.3-1.4 nm), the transfer rate per tube from a semiconducting tube to adjacent semiconducting tubes is (1.8-1.9) × 10(12) s(-1), and that to adjacent metallic tubes is 1.1 × 10(12) s(-1). For the interwall distance of ∼0.9 nm (center-to-center distance ∼1.9 nm), the transfer rate per tube from a semiconducting tube to adjacent semiconducting tubes is 2.7 × 10(11) s(-1). These transfer rates are much lower than those predicted by the Förster model calculation based on a point dipole approximation, indicating the failure of the conventional Förster model calculations. In double-walled carbon nanotubes, which are equivalent to ideal nanoscale coaxial cylinders, we show exciton energy transfer from the inner to the outer tubes. The transfer rate between the inner and the outer tubes with an interwall distance of ∼0.38 nm is 6.6 × 10(12) s(-1). Our findings provide an insight into the energy transfer mechanisms of one-dimensional excitons.

  11. Magnetoresistive system with concentric ferromagnetic asymmetric nanorings

    Energy Technology Data Exchange (ETDEWEB)

    Avila, J. I., E-mail: javila@ulg.ac.be; Tumelero, M. A.; Pasa, A. A.; Viegas, A. D. C. [Laboratório de Filmes Finos e Superfícies (LFFS), Departamento de Física, Universidade Federal de Santa Catarina, CP 476 Florianópolis (Brazil)

    2015-03-14

    A structure consisting of two concentric asymmetric nanorings, each displaying vortex remanent states, is studied with micromagnetic calculations. By orienting in suitable directions, both the asymmetry of the rings and a uniform magnetic field, the vortices chiralities can be switched from parallel to antiparallel, obtaining in this way the analogue of the ferromagnetic and antiferromagnetic configurations found in bar magnets pairs. Conditions on the thickness of single rings to obtain vortex states, as well as formulas for their remanent magnetization are given. The concentric ring structure enables the creation of magnetoresistive systems comprising the qualities of magnetic nanorings, such as low stray fields and high stability. A possible application is as contacts in spin injection in semiconductors, and estimations obtained here of magnetoresistance change for a cylindrical spin injection based device show significant variations comparable to linear geometries.

  12. Size-Independent Energy Transfer in Biomimetic Nanoring Complexes

    Science.gov (United States)

    2016-01-01

    Supramolecular antenna-ring complexes are of great interest due to their presence in natural light-harvesting complexes. While such systems are known to provide benefits through robust and efficient energy funneling, the relationship between molecular structure, strain (governed by nuclear coordinates and motion), and energy dynamics (arising from electronic behavior) is highly complex. We present a synthetic antenna-nanoring system based on a series of conjugated porphyrin chromophores ideally suited to explore such effects. By systematically varying the size of the acceptor nanoring, we reveal the interplay between antenna-nanoring binding, local strain, and energy dynamics on the picosecond time scale. Binding of the antenna unit creates a local strain in the nanoring, and this strain was measured as a function of the size of the nanoring, by UV–vis-NIR titration, providing information on the conformational flexibility of the system. Strikingly, the energy-transfer rate is independent of nanoring size, indicating the existence of strain-localized acceptor states, spread over about six porphyrin units, arising from the noncovalent antenna-nanoring association. PMID:27176553

  13. Size-Independent Energy Transfer in Biomimetic Nanoring Complexes.

    Science.gov (United States)

    Parkinson, Patrick; Kamonsutthipaijit, Nuntaporn; Anderson, Harry L; Herz, Laura M

    2016-06-28

    Supramolecular antenna-ring complexes are of great interest due to their presence in natural light-harvesting complexes. While such systems are known to provide benefits through robust and efficient energy funneling, the relationship between molecular structure, strain (governed by nuclear coordinates and motion), and energy dynamics (arising from electronic behavior) is highly complex. We present a synthetic antenna-nanoring system based on a series of conjugated porphyrin chromophores ideally suited to explore such effects. By systematically varying the size of the acceptor nanoring, we reveal the interplay between antenna-nanoring binding, local strain, and energy dynamics on the picosecond time scale. Binding of the antenna unit creates a local strain in the nanoring, and this strain was measured as a function of the size of the nanoring, by UV-vis-NIR titration, providing information on the conformational flexibility of the system. Strikingly, the energy-transfer rate is independent of nanoring size, indicating the existence of strain-localized acceptor states, spread over about six porphyrin units, arising from the noncovalent antenna-nanoring association.

  14. Equilibrium magnetisation structures in ferromagnetic nanorings

    Energy Technology Data Exchange (ETDEWEB)

    Kravchuk, Volodymyr P. [National Taras Shevchenko, University of Kiev, 03127 Kiev (Ukraine); Sheka, Denis D. [National Taras Shevchenko, University of Kiev, 03127 Kiev (Ukraine)]. E-mail: denis_sheka@univ.kiev.ua; Gaididei, Yuri B. [Institute for Theoretical Physics, 03143 Kiev (Ukraine)

    2007-03-15

    The ground state of the ring-shape magnetic nanoparticle is studied. Depending on the geometrical and magnetic parameters of the nanoring, there exist different magnetisation configurations (magnetic phases): two phases with homogeneous magnetisation (easy-axis and easy-plane phases) and two inhomogeneous (planar vortex phase and out-of-plane one). The existence of a new intermediate out-of-plane vortex phase, where the inner magnetisation is not strongly parallel to the easy axis, is predicted. Possible transitions between different phases are analysed using the combination of analytical calculations and micromagnetic simulations.

  15. Plasmonic shock waves and solitons in a nanoring

    OpenAIRE

    2016-01-01

    We apply the hydrodynamic theory of electron liquid to demonstrate that a circularly polarized radiation induces the diamagnetic, helicity-sensitive dc current in a ballistic nanoring. This current is dramatically enhanced in the vicinity of plasmonic resonances. The resulting magnetic moment of the nanoring represents a giant increase of the inverse Faraday effect. With increasing radiation intensity, linear plasmonic excitations evolve into the strongly non-linear plasma shock waves. These ...

  16. Controlled-synthesis of ZnO nanorings

    Institute of Scientific and Technical Information of China (English)

    Yin PENG; Ling BAO

    2008-01-01

    ZnO nanorings were synthesized on a large scale by an easy solution-based method at 70℃ for 5 h using hexamethylenetramine (C6H12N4, HMT) and Zn ant poly(acrylamide-co-diallyldimethylammonium chlor-ide) (PAM-CTAC). The structure and morphology of the products were characterized by X-ray powder diffraction (XRD) and scanning electron microscopy (SEM). The influence of experimental conditions such as concentra-tion of surfactant and reactants, reaction temperature on the structure and morphology of the products were inves-tigated. A probable formation mechanism of ZnO nanor-ings in the presence of surfactant PAM-CTAC was discussed. The results show that the products are wurtzite hexagonal ZnO nanorings with an inner diameter of 220 nm and a wall thickness of 70 nm. Reaction temper-ature and concentration of reactants influence the shape and size ofZnO nanorings but PAM-CTAC plays the key role in the formation of ZnO nanorings. Through adjust-ing the concentration of PAM-CTAC, controlled-syn-thesis of ZnO nanorings can be realized. A room temperature photoluminescence (PL) spectrum of ZnO obtained shows that the full width at half maximum (FWHM) of the UV emission (~7 nm) is much narrower than that of commercial ZnO bulk crystals (~18 nm). The narrow FWHM confirms the uniformity and narrow size distribution of the synthesized ZnO crystals.

  17. Template-directed synthesis of flexible porphyrin nanocage and nanorings via one-step olefin metathesis.

    Science.gov (United States)

    Zhu, Bin; Chen, Huanxin; Lin, Wei; Ye, Yang; Wu, Jing; Li, Shijun

    2014-10-29

    We describe the fabrication of a suite of flexible porphyrin cages and nanorings from a simple tetraalkene-derived zinc porphyrin monomer via a highly efficient template-directed strategy. The zinc porphyrin monomers were preorganized together by coordination with N atoms of multidentate ligands. Subsequent one-step olefin metathesis furnished a bisporphyrin cage, a triporphyrin nanoring, and a hexaporphyrin nanoring. In the case of the hexaporphyrin nanoring, 24 terminal olefins from six porphyrin monomers reacted with each other to form 12 new double bonds, delivering the final product. The triporphyrin and hexaporphyrin nanorings were further employed as hosts to encapsulate C60 and C70.

  18. Dynamic susceptibility of onion in ferromagnetic elliptical nanoring

    Directory of Open Access Journals (Sweden)

    Congpu Mu

    2016-06-01

    Full Text Available Micromagnetic simulation was performed to investigate the equilibrium state and dynamic susceptibility spectra of magnetic elliptical nanoring. There are two equilibrium states (onion and vortex obtained in elliptical nanoring. The onion state can be used to record information in MRAM. And it is important to investigate the dynamic susceptibility spectra of onion state, which is closely related to writing and reading speed of magnetic memory devices. Those results show that two or three resonance peaks are found under different thickness of elliptical nanoring with onion state, respectively. The low resonance frequency of two resonance peaks is increasing with the arm width of the elliptical ring, but is decreasing with the thickness. However, the high frequency of two resonance peaks is decreasing with the arm width of the elliptical ring.

  19. Dynamic susceptibility of onion in ferromagnetic elliptical nanoring

    Science.gov (United States)

    Mu, Congpu; Song, Jiefang; Xu, Jianghong; Wen, Fusheng

    2016-06-01

    Micromagnetic simulation was performed to investigate the equilibrium state and dynamic susceptibility spectra of magnetic elliptical nanoring. There are two equilibrium states (onion and vortex) obtained in elliptical nanoring. The onion state can be used to record information in MRAM. And it is important to investigate the dynamic susceptibility spectra of onion state, which is closely related to writing and reading speed of magnetic memory devices. Those results show that two or three resonance peaks are found under different thickness of elliptical nanoring with onion state, respectively. The low resonance frequency of two resonance peaks is increasing with the arm width of the elliptical ring, but is decreasing with the thickness. However, the high frequency of two resonance peaks is decreasing with the arm width of the elliptical ring.

  20. Control of spin-polarised currents in graphene nanorings

    Energy Technology Data Exchange (ETDEWEB)

    Saiz-Bretín, M.; Munárriz, J. [GISC, Departamento de Física de Materiales, Universidad Complutense, E-28040 Madrid (Spain); Malyshev, A.V. [GISC, Departamento de Física de Materiales, Universidad Complutense, E-28040 Madrid (Spain); Ioffe Physical–Technical Institute, St-Petersburg (Russian Federation); Domínguez-Adame, F., E-mail: adame@fis.ucm.es [GISC, Departamento de Física de Materiales, Universidad Complutense, E-28040 Madrid (Spain); Department of Physics, University of Warwick, Coventry, CV4 7AL (United Kingdom)

    2015-09-25

    We study electronic transport in systems comprising square graphene nanorings with a ferromagnetic insulator layer on top of them. The rings are connected symmetrically or asymmetrically to contacts. The proximity exchange interaction of electrons with magnetic ions results in spin-dependent transport properties. When a nanoring is connected asymmetrically, the occurrence of Fano-like antiresonances in the transmission coefficient can induce abrupt changes in the spin polarisation under minute variations of the Fermi energy. We also demonstrate that the spin polarisation can be efficiently controlled by a side-gate voltage. This opens a possibility to use these effects for fabricating tunable sources of polarised electrons.

  1. Dynamically configurable hybridization of plasmon modes in nanoring dimer arrays

    Science.gov (United States)

    Zhang, Lei; Dong, Zhaogang; Wang, Ying Min; Liu, Yan Jun; Zhang, Shuang; Yang, Joel Kwang Wei; Qiu, Cheng-Wei

    2015-07-01

    We present a novel strategy capable of dynamically configuring the plasmon-induced transparency (PIT) effect with a polarization-dependent controllability based on a nanoring dimer array. The controllable coupling strength between the superradiant and subradiant modes is due to the polarization-dependent field distributions. It is shown that this dynamically controlled PIT is realized with a modulation depth as high as 95%, and a linear dependence of the coupling strength on polarization angle is deduced using a coupled-oscillator model. We believe that our results will inspire further exciting achievements that utilize various polarization states of the electromagnetic wave and pave a way towards applications using PIT with dynamic controllability such as slow light, optical nonlinearities and chemical/bio-sensing.We present a novel strategy capable of dynamically configuring the plasmon-induced transparency (PIT) effect with a polarization-dependent controllability based on a nanoring dimer array. The controllable coupling strength between the superradiant and subradiant modes is due to the polarization-dependent field distributions. It is shown that this dynamically controlled PIT is realized with a modulation depth as high as 95%, and a linear dependence of the coupling strength on polarization angle is deduced using a coupled-oscillator model. We believe that our results will inspire further exciting achievements that utilize various polarization states of the electromagnetic wave and pave a way towards applications using PIT with dynamic controllability such as slow light, optical nonlinearities and chemical/bio-sensing. Electronic supplementary information (ESI) available: Method, mode supported by single nanoring, transmittance spectrum of single nanoring, comparison of transmittance spectra simulated under different illumination angles, diffraction coupling in the proposed nanoring dimer system, and the coupled Lorentz oscillator model and parameters

  2. Plasmonic shock waves and solitons in a nanoring

    Science.gov (United States)

    Koshelev, K. L.; Kachorovskii, V. Yu.; Titov, M.; Shur, M. S.

    2017-01-01

    We apply the hydrodynamic theory of electron liquid to demonstrate that a circularly polarized radiation induces the diamagnetic, helicity-sensitive dc current in a ballistic nanoring. This current is dramatically enhanced in the vicinity of plasmonic resonances. The resulting magnetic moment of the nanoring represents a giant increase of the inverse Faraday effect. With increasing radiation intensity, linear plasmonic excitations evolve into the strongly nonlinear plasma shock waves. These excitations produce a series of the well-resolved peaks at the THz frequencies. We demonstrate that the plasmonic wave dispersion transforms the shock waves into solitons. The predicted effects should enable multiple applications in a wide frequency range (from the microwave to terahertz band) using optically controlled ultralow-loss electric, photonic, and magnetic devices.

  3. Topology induced anomalous plasmon modes in metallic Mobius nanorings

    CERN Document Server

    Yin, Yin; Engemaier, Vivienne; Naz, Ehsan Saei Ghareh; Giudicatti, Silvia; Ma, Libo; Schmidt, Oliver G

    2016-01-01

    We report on the investigation of plasmonic resonances in metallic M\\"obius nanorings. Half-integer numbers of resonant modes are observed due to the presence of an extra phase {\\pi} provided by the topology of the M\\"obius nanostrip. Anomalous plasmon modes located at the non-orientable surface of the M\\"obius nanoring break the symmetry that exist in conventional ring cavities, thus enable far-field excitation and emission as bright modes. The far-field resonant wavelength as well as the feature of half-integer mode numbers is invariant to the change of charge distribution on the M\\"obius nanoring due to the nontrivial topology. Owing to the ultra-small mode volume induced by the remaining dark feature, an extremely high sensitivity as well as a remarkable figure of merit is obtained in sensing performance. The topological metallic nanostructure provides a novel platform for the investigation of localized surface plasmon modes exhibiting unique phenomena in plasmonic applications such as high sensitive dete...

  4. Large-Scale Synthesis of Single-Crystalline Iron Oxide Magnetic Nanorings

    DEFF Research Database (Denmark)

    Jia, Chun-Jiang; Sun, Ling-Dong; Luo, Feng

    2008-01-01

    We present an innovative approach to the production of single-crystal iron oxide nanorings employing a solution-based route. Single-crystal hematite (alpha-Fe2O3) nanorings were synthesized using a double anion-assisted hydrothermal method (involving phosphate and sulfate ions), which can...... be divided into two stages: (1) formation of capsule-shaped alpha-Fe2O3 nanoparticles and (2) preferential dissolution along the long dimension of the elongated nanoparticles (the c axis of alpha-Fe2O3) to form nanorings. The shape of the nanorings is mainly regulated by the adsorption of phosphate ions...... an intriguing three-dimensional magnetic configuration. This work provides an easily scaled-up method for preparing tailor-made iron oxide nanorings that could meet the demands of a variety of applications ranging from medicine to magnetoelectronics....

  5. 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.

  6. Wavelet analisys and HHG in nanorings Their applications in logic gates and memory mass devices

    CERN Document Server

    Cricchio, Dario

    2015-01-01

    We study the application of one nanoring driven by a laser field in different states of polarization in logic circuits. In particular we show that assigning boolean values to different state of the incident laser field and to the emitted signals, we can create logic gates such as OR, XOR and AND. We also show the possibility to make logic circuits such as half-adder and full-adder using one and two nanoring respectively. Using two nanorings we made the Toffoli gate. Finally we use the final angular momentum acquired by the electron to store information and hence show the possibility to use an array of nanorings as a mass memory device.

  7. Magnetization states and switching in narrow-gapped ferromagnetic nanorings

    Directory of Open Access Journals (Sweden)

    Jie Li

    2012-03-01

    Full Text Available We study permalloy nanorings that are lithographically fabricated with narrow gaps that break the rotational symmetry of the ring while retaining the vortex ground state, using both micromagnetic simulations and magnetic force microscopy (MFM. The vortex chirality in these structures can be readily set with an in-plane magnetic field and easily probed by MFM due to the field associated with the gap, suggesting such rings for possible applications in storage technologies. We find that the gapped ring edge characteristics (i.e., edge profile and gap shape are critical in determining the magnetization switching field, thus elucidating an essential parameter in the controls of devices that might incorporate such structures.

  8. Persistent currents in three-dimensional shell-doped nanorings

    Institute of Scientific and Technical Information of China (English)

    Xu Ning; Ding Jian-Wen; Chen Hong-Bo; Ma Ming-Ming

    2009-01-01

    The persistent current in three-dimensional (P×N2) nanorings as a function of the unit cell number (P), the channel number (M = N2), surface disorder (ξ), and temperature (T) is theoretically investigated in terms of rotational symmetry. On the whole, the typical current increases linearly with (<3) but decreases exponentially with P, while wide fluctuations exist therein. In the presence of surface disorder, the persistent current decreases with ξ in the regime of weak disorder but increases in the regime of strong disorder. In addition, it is found that the persistent current in perfect rings decreases exponentially with temperature even at T < T*, while in most disorder rings, the typical current decreases slightly with temperature at T < T*.

  9. Polarization dependent switching of asymmetric nanorings with a circular field

    Directory of Open Access Journals (Sweden)

    Nihar R. Pradhan

    2016-01-01

    Full Text Available We experimentally investigated the switching from onion to vortex states in asymmetric cobalt nanorings by an applied circular field. An in-plane field is applied along the symmetric or asymmetric axis of the ring to establish domain walls (DWs with symmetric or asymmetric polarization. A circular field is then applied to switch from the onion state to the vortex state, moving the DWs in the process. The asymmetry of the ring leads to different switching fields depending on the location of the DWs and direction of applied field. For polarization along the asymmetric axis, the field required to move the DWs to the narrow side of the ring is smaller than the field required to move the DWs to the larger side of the ring. For polarization along the symmetric axis, establishing one DW in the narrow side and one on the wide side, the field required to switch to the vortex state is an intermediate value.

  10. Lithographically patterned electrodeposition of gold, silver, and nickel nanoring arrays with widely tunable near-infrared plasmonic resonances.

    Science.gov (United States)

    Halpern, Aaron R; Corn, Robert M

    2013-02-26

    A novel low-cost nanoring array fabrication method that combines the process of lithographically patterned nanoscale electrodeposition (LPNE) with colloidal lithography is described. Nanoring array fabrication was accomplished in three steps: (i) a thin (70 nm) sacrificial nickel or silver film was first vapor-deposited onto a plasma-etched packed colloidal monolayer; (ii) the polymer colloids were removed from the surface, a thin film of positive photoresist was applied, and a backside exposure of the photoresist was used to create a nanohole electrode array; (iii) this array of nanoscale cylindrical electrodes was then used for the electrodeposition of gold, silver, or nickel nanorings. Removal of the photoresist and sacrificial metal film yielded a nanoring array in which all of the nanoring dimensions were set independently: the inter-ring spacing was fixed by the colloidal radius, the radius of the nanorings was controlled by the plasma etching process, and the width of the nanorings was controlled by the electrodeposition process. A combination of scanning electron microscopy (SEM) measurements and Fourier transform near-infrared (FT-NIR) absorption spectroscopy were used to characterize the nanoring arrays. Nanoring arrays with radii from 200 to 400 nm exhibited a single strong NIR plasmonic resonance with an absorption maximum wavelength that varied linearly from 1.25 to 3.33 μm as predicted by a simple standing wave model linear antenna theory. This simple yet versatile nanoring array fabrication method was also used to electrodeposit concentric double gold nanoring arrays that exhibited multiple NIR plasmonic resonances.

  11. 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...... spectrum of the exciton, via a remarkably transparent expression for the susceptibility, and show that the effects of strongly avoided quasienergy crossings manifest themselves directly, both in the absorption and transmitted sidebands....

  12. 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 ...

  13. Far-field Fano resonance in nanoring lattices modeled from extracted, point dipole polarizability

    Energy Technology Data Exchange (ETDEWEB)

    DeJarnette, Drew; Forcherio, Gregory T. [Microelectronics and Photonics Graduate Program, University of Arkansas, Fayetteville, Arkansas 72701 (United States); Blake, Phillip [Department of Chemical Engineering, University of Arkansas, Fayetteville, Arkansas 72701 (United States); Keith Roper, D., E-mail: dkroper@uark.edu [Microelectronics and Photonics Graduate Program, University of Arkansas, Fayetteville, Arkansas 72701 (United States); Department of Chemical Engineering, University of Arkansas, Fayetteville, Arkansas 72701 (United States)

    2014-01-14

    Coupling and extinction of light among particles representable as point dipoles can be characterized using the coupled dipole approximation (CDA). The analytic form for dipole polarizability of spheroidal particles supports rapid electrodynamic analysis of nanoparticle lattices using CDA. However, computational expense increases for complex shapes with non-analytical polarizabilities which require discrete dipole (DDA) or higher order approximations. This work shows fast CDA analysis of assembled nanorings is possible using a single dipole nanoring polarizability extrapolated from a DDA calculation by summing contributions from individual polarizable volume elements. Plasmon resonance wavelengths of nanorings obtained using extracted polarizabilities blueshift as wall dimensions-to-inner radius aspect ratio increases, consistent with published theory and experiment. Calculated far-field Fano resonance energy maximum and minimum wavelengths were within 1% of full volume element results. Considering polarizability allows a more complete physical picture of predicting plasmon resonance location than metal dielectric alone. This method reduces time required for calculation of diffractive coupling more than 40 000-fold in ordered nanoring systems for 400–1400 nm incident wavelengths. Extension of this technique beyond nanorings is possible for more complex shapes that exhibit dipolar or quadrupole radiation patterns.

  14. 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...

  15. 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...

  16. Topological structure effect on far-infrared spectra in a GaAs/InAs nanoring

    Institute of Scientific and Technical Information of China (English)

    Gu Li-Ying; Li Yan-Fang; Chu Wei-Dong; Wei Ying-Hui

    2012-01-01

    On the basis of the growth mechanism of a GaAs/InAe nanoring,we propose a fine model which reflects the confinement details of real nanoring.Through calculations of the two-electron energy and far-infrared (FIR) spectra,we find that the ring topological structure and electron-electron interaction have great influence on the FIR spectra.The two unknown transition peaks in the experiment are determined theoretically.The theoretical results are in good agreement with the experiments.

  17. Simulation of optical soliton control in micro- and nanoring resonator systems

    CERN Document Server

    Daud, Suzairi; Ali, Jalil

    2015-01-01

    This book introduces optical soliton control in micro- and nanoring resonator systems. It describes how the ring resonator systems can be optimized as optical tweezers for photodetection by controlling the input power, ring radii and coupling coefficients of the systems. Numerous arrangements and configurations of micro and nanoring resonator systems are explained. The analytical formulation and optical transfer function for each model and the interaction of the optical signals in the systems are discussed. This book shows that the models designed are able to control the dynamical behaviour of generated signals.

  18. Highly tunable plasmonic nanoring arrays for nanoparticle manipulation and detection

    Science.gov (United States)

    Sergides, M.; Truong, V. G.; Chormaic, S. Nic

    2016-09-01

    The advancement of trapping and detection of nano-objects at very low laser powers in the near-infra-red region (NIR) is crucial for many applications. Singular visible-light nano-optics based on abrupt phase changes have recently demonstrated a significant improvement in molecule detection. Here, we propose and demonstrate tunable plasmonic nanodevices, which can improve both the trapping field enhancement and detection of nano-objects using singular phase drops in the NIR range. The plasmonic nanostructures, which consist of gaps with dimensions 50 nm × 50 nm connecting nanorings in arrays is discussed. These gaps act as individual detection and trapping sites. The tunability of the system is evident from extinction and reflection spectra while increasing the aperture size in the arrays. Additionally, in the region where the plasmonic nano-array exhibits topologically-protected, near-zero reflection behaviour, the phase displays a rapid change. Our experimental data predict that, using this abrupt phase changes, one can improve the detection sensitivity by 10 times compared to the extinction spectra method. We finally report experimental evidence of 100 nm polystyrene beads trapping using low incident power on these devices. The overall design demonstrates strong capability as an optical, label-free, non-destructive tool for single molecule manipulation where low trapping intensity, minimal photo bleaching and high sensitivity is required.

  19. Self-assembled formation and transformation of In/CdZnTe(110) nano-rings into camel-humps

    Energy Technology Data Exchange (ETDEWEB)

    Cohen-Taguri, G. [School of Mechanical Engineering and Materials and Nanotechnologies Program, Faculty of Engineering, Tel Aviv University, Tel Aviv 69978 (Israel); Ruzin, A. [School of Electrical Engineering, Faculty of Engineering, Tel Aviv University, Tel Aviv 69978 (Israel); Goldfarb, I. [School of Mechanical Engineering and Materials and Nanotechnologies Program, Faculty of Engineering, Tel Aviv University, Tel Aviv 69978 (Israel); Research Center for Nanoscience and Nanotechnology, Tel Aviv University, Tel Aviv 69978 (Israel)

    2012-05-21

    We used in situ scanning tunneling microscopy to monitor in real time the formation of nano-rings at the molecular beam epitaxially grown In/CdZnTe(110) surface, and Auger electron spectroscopy to explore the corresponding compositional changes. In-diffusion of In and segregation of Cd to the surface in course of annealing lead to a formation of elliptically distorted nano-rings, elongated along the fast [110] diffusion direction. Exacerbated diffusion anisotropy in the liquid state, at temperatures above the melting point of In, further distorts the nano-rings into a camel-hump shape.

  20. Vernier-templated synthesis, crystal structure, and supramolecular chemistry of a 12-porphyrin nanoring.

    Science.gov (United States)

    Kondratuk, Dmitry V; Sprafke, Johannes K; O'Sullivan, Melanie C; Perdigao, Luis M A; Saywell, Alex; Malfois, Marc; O'Shea, James N; Beton, Peter H; Thompson, Amber L; Anderson, Harry L

    2014-09-26

    Vernier templating exploits a mismatch between the number of binding sites in a template and a reactant to direct the formation of a product that is large enough to bind several template units. Here, we present a detailed study of the Vernier-templated synthesis of a 12-porphyrin nanoring. NMR and small-angle X-ray scattering (SAXS) analyses show that Vernier complexes are formed as intermediates in the cyclo-oligomerization reaction. UV/Vis/NIR titrations show that the three-component assembly of the 12-porphyrin nanoring figure-of-eight template complex displays high allosteric cooperativity and chelate cooperativity. This nanoring-template 1:2 complex is among the largest synthetic molecules to have been characterized by single-crystal analysis. It crystallizes as a racemate, with an angle of 27° between the planes of the two template units. The crystal structure reveals many unexpected intramolecular C-H⋅⋅⋅N contacts involving the tert-butyl side chains. Scanning tunneling microscopy (STM) experiments show that molecules of the 12-porphyrin template complex can remain intact on the gold surface, although the majority of the material unfolds into the free nanoring during electrospray deposition.

  1. Enhanced electrochemical nanoring electrode for analysis of cytosol in single cells.

    Science.gov (United States)

    Zhuang, Lihong; Zuo, Huanzhen; Wu, Zengqiang; Wang, Yu; Fang, Danjun; Jiang, Dechen

    2014-12-02

    A microelectrode array has been applied for single cell analysis with relatively high throughput; however, the cells were typically cultured on the microelectrodes under cell-size microwell traps leading to the difficulty in the functionalization of an electrode surface for higher detection sensitivity. Here, nanoring electrodes embedded under the microwell traps were fabricated to achieve the isolation of the electrode surface and the cell support, and thus, the electrode surface can be modified to obtain enhanced electrochemical sensitivity for single cell analysis. Moreover, the nanometer-sized electrode permitted a faster diffusion of analyte to the surface for additional improvement in the sensitivity, which was evidenced by the electrochemical characterization and the simulation. To demonstrate the concept of the functionalized nanoring electrode for single cell analysis, the electrode surface was deposited with prussian blue to detect intracellular hydrogen peroxide at a single cell. Hundreds of picoamperes were observed on our functionalized nanoring electrode exhibiting the enhanced electrochemical sensitivity. The success in the achievement of a functionalized nanoring electrode will benefit the development of high throughput single cell electrochemical analysis.

  2. Eco-friendly synthesis of colloidal silver nanospheres, nanorings and nanonetworks

    NARCIS (Netherlands)

    Singh, A.K.; Rai, A.K.; Bicanic, D.D.

    2009-01-01

    Colloidal silver nanospheres, nanorings, and nanonetworks were synthesized by the nanosecond pulsed laser ablation of a silver metal plate in a pure distilled water (at room temperature) using the fundamental (1064 nm), second harmonic (532 nm), and third harmonic (355 nm) wavelengths of the Nd:YAG

  3. Synthesis and Characterization of NiCr Self-assembled Nanorings

    NARCIS (Netherlands)

    Serdio, Victor M.; Gracia-Pinilla, Miguel A.; Velumani, S.; Perez-Tijerina, Eduardo G.; Wiel, van der Wilfred G.

    2010-01-01

    Formation of NiCr nanorings out of 2-3 nm NiCr nanoparticles prepared by DC magnetron sputtering with inert gas condensation is reported. An RF quadrupole mass filter has been used to get the particle size distribution and control the particle size in the plasma stream of grown material. The deposit

  4. Interband magneto-optical transitions in a layer of semiconductor nano-rings

    NARCIS (Netherlands)

    Voskoboynikov, O.; Wijers, C.M.J.; Liu, J.L.; Lee, C.P.

    2005-01-01

    We have developed a quantitative theory of the collective electromagnetic response of layers of semiconductor nano-rings. The response can be controlled by means of an applied magnetic field through the optical Aharonov-Bohm effect and is ultimately required for the design of composite materials. We

  5. Charge ordering and exchange bias behaviors in Co3O4 porous nanoplatelets and nanorings

    Science.gov (United States)

    Debnath, J. C.; Wang, Jianli; Zeng, R.

    2017-01-01

    We present the synthesis of α-Co3O4 porous nanoplatelets and hexagonal nanorings using microwave-assisted hydrothermal and conventional chemical reaction methods. The x-ray diffraction (XRD) and refinement analyses indicate the α-Co3O4 crystal structure, and the x-ray photoelectron spectrum (XPS) indicates the high purity of the samples. The M-T (including 1/χ-T) curves indicate an antiferromagnetic transition at about 35 K in both kind of samples but the interesting finding was made that a charge-ordered (CO) state appears at 250 K for the nanoplatelets sample whereas it is inattentive for the nanorings. The antiferromagnetic transition temperature TN is lower than that of the bulk α-Co3O4 single crystal due to the nanosized structures. We observed quite significant exchange bias for nanorings. The exchange bias behavior of the α-Co3O4 hexagonal nanorings is consistent with an antiferromagnetic (AFM) Co3O4 core and spin-glass like shell.

  6. 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.

  7. 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.

  8. 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.

  9. Aromatic and antiaromatic ring currents in a molecular nanoring

    Science.gov (United States)

    Peeks, Martin D.; Claridge, Timothy D. W.; Anderson, Harry L.

    2016-12-01

    Aromatic and antiaromatic molecules—which have delocalized circuits of [4n + 2] or [4n] electrons, respectively—exhibit ring currents around their perimeters. The direction of the ring current in an aromatic molecule is such as to generate a magnetic field that opposes the external field inside the ring (a ‘diatropic’ current), while the ring current in an antiaromatic molecule flows in the reverse direction (‘paratropic’). Similar persistent currents occur in metal or semiconductor rings, when the phase coherence of the electronic wavefunction is preserved around the ring. Persistent currents in non-molecular rings switch direction as a function of the magnetic flux passing through the ring, so that they can be changed from diatropic (‘aromatic’) to paratropic (‘antiaromatic’) simply by changing the external magnetic field. As in molecular systems, the direction of the persistent current also depends on the number of electrons. The relationship between ring currents in molecular and non-molecular rings is poorly understood, partly because they are studied in different size regimes: the largest aromatic molecules have diameters of about one nanometre, whereas persistent currents are observed in microfabricated rings with diameters of 20-1,000 nanometres. Understanding the connection between aromaticity and quantum-coherence effects in mesoscopic rings provides a motivation for investigating ring currents in molecules of an intermediate size. Here we show, using nuclear magnetic resonance spectroscopy and density functional theory, that a six-porphyrin nanoring template complex, with a diameter of 2.4 nanometres, is antiaromatic in its 4+ oxidation state (80 π electrons) and aromatic in its 6+ oxidation state (78 π electrons). The antiaromatic state has a huge paramagnetic susceptibility, despite having no unpaired electrons. This work demonstrates that a global ring current can be promoted in a macrocycle by adjusting its oxidation state

  10. 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...

  11. Synthesis of Platinum Nanotubes and Nanorings via Simultaneous Metal Alloying and Etching

    KAUST Repository

    Huang, Zhiqi

    2016-04-19

    Metallic nanotubes represent a class of hollow nanostructures with unique catalytic properties. However, the wet-chemical synthesis of metallic nanotubes remains a substantial challenge, especially for those with dimensions below 50 nm. This communication describes a simultaneous alloying-etching strategy for the synthesis of Pt nanotubes with open ends by selective etching Au core from coaxial Au/Pt nanorods. This approach can be extended for the preparation of Pt nanorings when Saturn-like Au core/Pt shell nanoparticles are used. The diameter and wall thickness of both nanotubes and nanorings can be readily controlled in the range of 14-37 nm and 2-32 nm, respectively. We further demonstrated that the nanotubes with ultrathin side walls showed superior catalytic performance in oxygen reduction reaction. © 2016 American Chemical Society.

  12. Manipulation of Magnetization States of Permalloy Nanorings by an External Azimuthal Field

    Science.gov (United States)

    Yang, Tianyu; Pradhan, Nihar; Goldman, Abby; Kemei, Moureen; Licht, Abbey; Li, Yihan; Tuominen, Mark; Aidala, Katherine

    2011-03-01

    This experimental research investigates a new method of manipulating the magnetic states of ferromagnetic nanorings using a circular magnetic field directed along the ring circumference. This type of azimuthal field can naturally select a vortex magnetization of desired chirality. The understanding of the magnetization switching behavior in an azimuthal field could lead to new designs of practical magnetic data storage devices. Symmetric and asymmetric nanorings made of permalloy are fabricated by a standard technique using electron-beam lithography and e-beam evaporation. Azimuthal fields are generated by passing current through an atomic force microscope tip, which is positioned at the center of the ring. The magnetic field direction and magnitude are controlled by the current. We demonstrate control over switching from an onion state to a vortex state, and also between two vortex states, using magnetic force microscopy to image the resulting magnetic states. This work was supported by NSF grants DMR-0907201 CMMI-0531171.

  13. Quantum mechanical investigation of bond gaps of π-acceptor complex alone and affected nanoring field

    Directory of Open Access Journals (Sweden)

    Mehrnoosh Khaleghian

    2014-06-01

    Full Text Available We studied non-bonded interaction of the [Co(CN6]3- complex Situated B24N24 nanoring. Early, the geometry of [Co(CN6]3- and B24N24 have been optimized at B3LYP method with Def2-SV(P/ LANL2DZ(ECP and EPR-II basis set respectively. To confirmation the structural stability of the B24N24-[Co(CN6]3- nano system, delocalization of electrons between donor and acceptor bonds and LUMO and HOMO for the lowest energy have been computed by DFT/ B3LYP method. Then we investigated NBO data such as coefficients and hybrids of orbitals, second order perturbation theory analysis of fock matrix, and ΔE in different loops of the nanoring have been calculated at B3LYP method.

  14. Nucleation kinetics of SrTiO3 3D islands and nanorings on Si substrates.

    Science.gov (United States)

    Tejedor, Paloma; Benedicto, Marcos; Vázquez, Luis; Galiana, Beatriz

    2014-11-07

    The nucleation of SrTiO3 three-dimensional (3D) islands and nanorings on Si substrates via a novel metalorganic decomposition (MOD) process has been investigated as a function of temperature and solution concentration of the SrTi(OC3H7)6 precursor. Quantitative analysis of island density and size distribution by atomic force microscopy (AFM) has revealed the existence of a nucleation regime at solution concentrations below 5 × 10(-3) M, in which the critical nucleus is a trimer and a coalescence regime at higher concentrations, dominated by growth of immobile clusters. Nanorings form preferentially under high supersaturation conditions and their size distribution is consistent with a dynamic coalescence. On the basis of recent theoretical models (Gill, 2012), we have proposed that the island-to-nanoring transition in the SrTiO3/Si system occurs above a critical size as a result of a competition between energetic and kinetic factors. The combination of high-resolution transmission electron microscopy (HRTEM) and attenuated total reflectance Fourier transform infrared spectroscopy (ATR-FTIR) has shown that the monocrystalline SrTiO3 nanoclusters grow pseudomorphically on the Si substrate and exhibit a strain-induced tetragonal lattice distortion.

  15. Nanoring formation via in situ photoreduction of silver on a virus scaffold

    Science.gov (United States)

    Bayram, Serene S.; Zahr, Omar K.; Del Re, Julia; Szuchmacher Blum, Amy

    2016-12-01

    The fabrication of plasmonic nanorings remains of substantial interest by virtue of their enhanced electric and magnetic response to light fields which can be subsequently exploited in diverse applications. Scaling down the size of nanorings holds promise in creating artificial magnetism at wavelengths matching the solar spectrum. Nanosized bioscaffolds can be utilized to tackle the challenge of size reduction of metallic rings owing to their miniature features as well as their well-known biomineralization capacity. Herein, we use the tobacco mosaic virus coat protein as a command surface to grow and assemble silver nanoparticles into sub-30 nm rings. The versatility of TMV allows the formation of both solid rings and rings consisting of discrete nanoparticles that are characterized by UV-vis and TEM. The pH-dependent coulombic surface map along with the annular geometry of the protein aggregate allow the generation of rings with or without a central nanoparticle. Our silver rings are believed to be the smallest to date, and they can offer a test material for existing theories on metallic nanorings of this heretofore unreached size scale.

  16. Nanobubble and nanodroplet template growth of particle nanorings versus nanoholes in drying nanofluids and polymer films.

    Science.gov (United States)

    Darwich, S; Mougin, K; Vidal, L; Gnecco, E; Haidara, H

    2011-03-01

    Here we demonstrate how confined nanobubbles and nanodroplets, which can either form spontaneously at the suspension/substrate interface, or can more interestingly be purposely introduced in the system, allow assembly of nanoparticles (NPs) into nanoring-like structures with a flexible control of both the size and distribution. As with most wetting-mediated nanopatterning methods, this approach provides an alternative to direct replication from templates. The formation of two-dimensional ring-shaped nanostructures was obtained by drying a nanocolloidal gold (Au) suspension drop confining nanobubbles (or nanodroplets) that are settled at a solid substrate. AFM investigation of the dry nanostructures showed the formation of isolated Au NPs rings having diameters ranging from 200 nm to 500 nm along the dewetting-drying path of the suspension drop. The flexibility of these wetting processes for the variation of the spatial features of the nanoring (size and shape resolution) essentially depends on physical parameters such as the nanobubble/nanodroplet size and concentration, the wettability, and the evaporation rate of the nanofluid drop on the substrate. Furthermore, we show that the underpinning mechanism of this evaporation-assisted assembly of Au NPs into supported functional nanoring patterns is fairly similar to that at work in the spontaneous formation of nanoholes in drying polymer thin films. Finally, the method proves to be a simple and flexible nanofabrication tool to be extended to various nanosize objects, towards specific optical and sensing applications.

  17. 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

  18. Electromagnetic plasmon propagation and coupling through gold nanoring heptamers: a route to design optimized telecommunication photonic nanostructures.

    Science.gov (United States)

    Ahmadivand, Arash; Golmohammadi, Saeed

    2014-06-20

    In this work, a configuration of bulk gold nanorings with certain geometrical sizes has been utilized for designing efficient photonic subwavelength nanostructures. We verify that adjacent heptamers based on gold nanorings are able to couple and transport magnetic plasmon resonance along a nanoring array in chrysene and triphenylene molecule orientations. This magnetic resonance transmission is caused by an antiphase circular current through the heptamer arrays. An orientation model of nanoring heptamers helps us to provide efficient optical structures with a remarkable decay length and a trivial ratio of destructive interferences. Exploiting the robust magnetic plasmon resonance coupling effect between heptamers arrays, we would be able to propose a practical plasmonic waveguide, a Y-shaped optical power divider (splitter), and an ON/OFF router that is operating based on destructive and constructive interferences. The quality of power splitting has been discussed comprehensively and also, the effect of undesirable occasions on the functioning performance of the proposed router has been investigated numerically. Ultimately, we verify that employing heptamers based on gold nanorings leads us to propose efficient plasmonic nanostructures and devices that are able to work in the telecommunication spectrum.

  19. 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.

  20. 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.

  1. Asymmetric split nanorings for Fano induced plasmonic sensor in visible region

    Energy Technology Data Exchange (ETDEWEB)

    Ding, Yao, E-mail: dingyao@cqcet.com [General Education College, Chongqing College of Electronic Engineering, Chongqing 401331 (China); Liao, Zhongwei, E-mail: liaozw@cqu.edu.cn [Soft Matter and Interdisciplinary Research Institute, College of Physics, Chongqing University, Chongqing 401331 (China)

    2015-05-01

    Fano resonance exhibits high sensitivity and promising applications in the field of ultra-sensitive plasmonic sensor. In this work, the Fano lineshape in spectra of gold rectangular split nanorings (RSNRs) is investigated using the finite element method. The simulation results figure out the Fano lineshape could be modulated by the positions of split gap in RSNRs for symmetry breaking, which is explained by the plasmonic hybridization theory. Furthermore, the high order bonding plasmon mode H in absorption spectra exhibits high sensitivity in visible region. Our investigations here are beneficial for the design and application of ultra-sensitive LSPR sensor in visible region.

  2. Lithography-Free Fabrication of Silica Nanocylinders with Suspended Gold Nanorings for LSPR-Based Sensing

    DEFF Research Database (Denmark)

    Thilsted, Anil Haraksingh; Pan, Jesper Yue; Wu, Kaiyu;

    2016-01-01

    areas, such as 8 in. wafers. The authors demonstrate that gold coated nanocylinders support localized surface plasmon resonances (LSPR) from visible to near infrared wavelengths. The plasmonic platform can be characterized as suspended gold nanorings and exhibits a sensitivity of 658 nm RIU-1...... with a figure-of-merit of 10, comparable to other state-of-the-art LSPR sensing platforms that utilize more complex nanofabrication pathways. It was observed that the LSPR peak positions can be controlled by varying the geometry of the nanocylinders. The authors illustrate surface functionalization, biosensing...

  3. 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.

  4. 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.

  5. 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...

  6. 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

  7. 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...... rare-earth metals....

  8. 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.

  9. 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.

  10. 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

  11. Printable nanoscale metal ring arrays via vertically aligned carbon nanotube platforms.

    Science.gov (United States)

    Lee, Sang Ho; Yoon, Seungha; Jeong, Huisu; Han, Mingu; Choi, Sung Mook; Kim, Jong Guk; Park, Ji-Woong; Jung, Gun Young; Cho, Beong Ki; Kim, Won Bae

    2013-11-01

    This paper reports a novel and efficient strategy for fabricating sub-100 nm metal ring arrays using a simple printing process. Vertically aligned carbon nanotubes that are supported by hexagonally ordered channels of alumina matrices are used as a stamp to print nanoscale ring patterns, which is a very unique stamping platform that has never been reported. Using this strategy, uniform nanoring patterns of various metals can be directly printed onto a wide range of substrate surfaces under ambient conditions. Significantly, the size and interval of the printed nanorings can be systematically tuned by controlling the ring-shaped tip dimensions of the pristine stamps. An advanced example of these printable nanoscale metal ring arrays is explicitly embodied in this work by investigation of the plasmon resonances of metal nanorings with different sizes and intervals.

  12. 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.

  13. 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.

  14. 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.

  15. Constructive quantum interference in a bis-copper six-porphyrin nanoring

    Science.gov (United States)

    Richert, Sabine; Cremers, Jonathan; Kuprov, Ilya; Peeks, Martin D.; Anderson, Harry L.; Timmel, Christiane R.

    2017-03-01

    The exchange interaction, J, between two spin centres is a convenient measure of through bond electronic communication. Here, we investigate quantum interference phenomena in a bis-copper six-porphyrin nanoring by electron paramagnetic resonance spectroscopy via measurement of the exchange coupling between the copper centres. Using an analytical expression accounting for both dipolar and exchange coupling to simulate the time traces obtained in a double electron electron resonance experiment, we demonstrate that J can be quantified to high precision even in the presence of significant through-space coupling. We show that the exchange coupling between two spin centres is increased by a factor of 4.5 in the ring structure with two parallel coupling paths as compared to an otherwise identical system with just one coupling path, which is a clear signature of constructive quantum interference.

  16. Zinc oxide nanoring embedded lacey graphene nanoribbons in symmetric/asymmetric electrochemical capacitive energy storage

    Science.gov (United States)

    Sahu, Vikrant; Goel, Shubhra; Sharma, Raj Kishore; Singh, Gurmeet

    2015-12-01

    This article describes the synthesis and characterization of ZnO nanoring embedded graphene nanoribbons. Patterned holes (mesopore dia.) in graphene nanoribbons are chemically generated, leading to a high density of the edge planes. These planes carry negatively charged surface groups (like -COOH and -OH) and therefore anchor the metal ions in a cordial fashion forming a string of metal ions along the edge planes. These strings of imbibed metal ions precipitate as tiny ZnO nanorings over lacey graphene nanoribbons. The thus obtained graphene nanoribbon (GNR) based hierarchical ZnO mesoporous structures are three dimensionally accessible to the electrolyte and demonstrate high performance in capacitive energy storage. The ZnO/GNR nanocomposite electrode in an asymmetric supercapacitor device with lacey reduced graphene oxide nanoribbons (LRGONRs) as a negative electrode exhibits a 2.0 V potential window in the aqueous electrolyte and an ultra-short time constant (0.08 s). The wide potential window consequently increased the energy density from 6.8 Wh kg-1 (ZnO/GNR symmetric) to 9.4 Wh kg-1 (ZnO/GNR||LRGONR asymmetric). The relaxation time constant obtained for the asymmetric supercapacitor device was three orders of magnitude less compared to the ZnO (symmetric, 33 s) supercapacitor device. The high cycling stability of ZnO/GNR||LRGONR up to 96.7% capacitance retention, after 5000 GCD cycles at 2 mA cm-2, paves the way to a high performance aqueous electrochemical supercapacitive energy storage.This article describes the synthesis and characterization of ZnO nanoring embedded graphene nanoribbons. Patterned holes (mesopore dia.) in graphene nanoribbons are chemically generated, leading to a high density of the edge planes. These planes carry negatively charged surface groups (like -COOH and -OH) and therefore anchor the metal ions in a cordial fashion forming a string of metal ions along the edge planes. These strings of imbibed metal ions precipitate as tiny Zn

  17. Ultrasonic synthesis, characterization and formation mechanism of aggregated nanorings of EuF3

    Institute of Scientific and Technical Information of China (English)

    WU Dapeng; WANG Xinjun; BAI Zhengyu; JIANG Kai

    2008-01-01

    The aggregated nanorings of EuF3 were synthesized via ultrasonic irritation in aqueous solution. The products were characterized by X-ray powder diffraction (XRD), scanning electron microscopy (SEM), and transmission electron microscopy (TEM). XRD pattern proved that the crystalline phase of the EuF3 rngs was hexagonal. The SEM and TEM images indicated that the as-prepared EuF3 nanocrys-tals had ring-like morphology and were aggregated by numerous small crystallites (about 10-15 nm in diameter); the outer diameter of the rings was in the range of 200-300 nm, while the inner diameter was in the range of 50-80 nm with a thickness of 30-40 nm. Moreover, the time-depend experiments were carried out to disclose the formation mechanism of the as-prepared ring-like nanostructures.

  18. Empty smectic liquid crystals of hard nanorings: Insights from a second-virial theory

    Science.gov (United States)

    Wensink, H. H.; Avendaño, C.

    2016-12-01

    Inspired by recent simulations on highly open liquid crystalline structures formed by rigid planar nanorings, we present a simple theoretical framework explaining the prevalence of smectic over nematic ordering in systems of ring-shaped objects. The key part of our study is a calculation of the excluded volume of such nonconvex particles in the limit of vanishing thickness to diameter ratio. Using a simple stability analysis we then show that dilute systems of ring-shaped particles have a strong propensity to order into smectic structures with an unusual antinematic order while solid disks of the same dimensions exhibit nematic order. Since our model rings have zero internal volume, these smectic structures are essentially empty, resembling the strongly porous structures found in simulation. We argue that the antinematic intralamellar order of the rings plays an essential role in stabilizing these smectic structures.

  19. 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.

  20. 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.

  1. 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.

  2. Single-crystalline MFe(2)O(4) nanotubes/nanorings synthesized by thermal transformation process for biological applications.

    Science.gov (United States)

    Fan, Hai-Ming; Yi, Jia-Bao; Yang, Yi; Kho, Kiang-Wei; Tan, Hui-Ru; Shen, Ze-Xiang; Ding, Jun; Sun, Xiao-Wei; Olivo, Malini Carolene; Feng, Yuan-Ping

    2009-09-22

    We report a general thermal transformation approach to synthesize single-crystalline magnetic transition metal oxides nanotubes/nanorings including magnetite Fe(3)O(4), maghematite gamma-Fe(2)O(3), and ferrites MFe(2)O(4) (M = Co, Mn, Ni, Cu) using hematite alpha-Fe(2)O(3) nanotubes/nanorings template. While the straightforward reduction or reduction-oxides process was employed to produce Fe(3)O(4) and gamma-Fe(2)O(3), the alpha-Fe(2)O(3)/M(OH)(2) core/shell nanostructure was used as precursor to prepare MFe(2)O(4) nanotubes via MFe(2)O(4-x) (0 MFe(2)O(4) nanocrystals with tunable size, shape, and composition have exhibited unique magnetic properties. Moreover, they have been demonstrated as a highly effective peroxidase mimic catalysts for laboratory immunoassays or as a universal nanocapsules hybridized with luminescent QDs for magnetic separation and optical probe of lung cancer cells, suggesting that these biocompatible magnetic nanotubes/nanorings have great potential in biomedicine and biomagnetic applications.

  3. 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.

  4. 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.

  5. 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.

  6. 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...

  7. 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.

  8. 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.

  9. Colloidal gold nanorings for improved photodynamic therapy through field-enhanced generation of reactive oxygen species

    Science.gov (United States)

    Hu, Yue; Yang, Yamin; Wang, Hongjun; Du, Henry

    2013-02-01

    Au nanostructures that exhibit strong localized surface plasmon resonance (SPR) have excellent potential for photo-medicine, among a host of other applications. Here, we report the synthesis and use of colloidal gold nanorings (GNRs) with potential for enhanced photodynamic therapy of cancer. The GNRs were fabricated via galvanic replacement reaction of sacrificial Co nanoparticles in gold salt solution with low molecular weight (Mw = 2,500) poly(vinylpyrrolidone) (PVP) as a stabilizing agent. The size and the opening of the GNRs were controlled by the size of the starting Co particles and the concentration of the gold salt. UV-Vis absorption measurements indicated the tunability of the SPR of the GNRs from 560 nm to 780 nm. MTT assay showed that GNRs were non-toxic and biocompatible when incubated with breast cancer cells as well as the healthy counterpart cells. GNRs conjugated with 5-aminolevulinic acid (5-ALA) photosensitizer precursor led to elevated formation of reactive oxygen species and improved efficacy of photodynamic therapy of breast cancer cells under light irradiation compared to 5-ALA alone. These results can be attributed to significantly enhance localized electromagnetic field of the GNRs.

  10. Vernier templating and synthesis of a 12-porphyrin nano-ring.

    Science.gov (United States)

    O'Sullivan, Melanie C; Sprafke, Johannes K; Kondratuk, Dmitry V; Rinfray, Corentin; Claridge, Timothy D W; Saywell, Alex; Blunt, Matthew O; O'Shea, James N; Beton, Peter H; Malfois, Marc; Anderson, Harry L

    2011-01-06

    Templates are widely used to arrange molecular components so they can be covalently linked into complex molecules that are not readily accessible by classical synthetic methods. Nature uses sophisticated templates such as the ribosome, whereas chemists use simple ions or small molecules. But as we tackle the synthesis of larger targets, we require larger templates-which themselves become synthetically challenging. Here we show that Vernier complexes can solve this problem: if the number of binding sites on the template, n(T), is not a multiple of the number of binding sites on the molecular building blocks, n(B), then small templates can direct the assembly of relatively large Vernier complexes where the number of binding sites in the product, n(P), is the lowest common multiple of n(B) and n(T) (refs 8, 9). We illustrate the value of this concept for the covalent synthesis of challenging targets by using a simple six-site template to direct the synthesis of a 12-porphyrin nano-ring with a diameter of 4.7 nm, thus establishing Vernier templating as a powerful new strategy for the synthesis of large monodisperse macromolecules.

  11. 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.``

  12. 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.

  13. 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.

  14. 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....

  15. 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....

  16. Energy levels and far-infrared optical absorption of impurity doped semiconductor nanorings: Intense laser and electric fields effects

    Science.gov (United States)

    Barseghyan, M. G.

    2016-11-01

    The effects of electron-impurity interaction on energy levels and far-infrared absorption in semiconductor nanoring under the action of intense laser and lateral electric fields have been investigated. Numerical calculations are performed using exact diagonalization technique. It is found that the electron-impurity interaction and external fields change the energy spectrum dramatically, and also have significant influence on the absorption spectrum. Strong dependence on laser field intensity and electric field of lowest energy levels, also supported by the Coulomb interaction with impurity, is clearly revealed.

  17. 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.

  18. 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.

  19. YBa{sub 2}Cu{sub 3}O{sub 7−δ} nanorings to probe fluxoid quantization in High Critical Temperature Superconductors

    Energy Technology Data Exchange (ETDEWEB)

    Arpaia, R. [Quantum Device Physics Laboratory, Department of Microtechnology and Nanoscience, Chalmers University of Technology, SE-41296 Göteborg (Sweden); CNR-SPIN, Dipartimento di Scienze Fisiche, Università degli Studi di Napoli Federico II, I-80126 Napoli (Italy); Charpentier, S. [Quantum Device Physics Laboratory, Department of Microtechnology and Nanoscience, Chalmers University of Technology, SE-41296 Göteborg (Sweden); Toskovic, R. [Quantum Device Physics Laboratory, Department of Microtechnology and Nanoscience, Chalmers University of Technology, SE-41296 Göteborg (Sweden); Department of Quantum Nanoscience, Kavli Institute of Nanoscience, Delft University of Technology, NL-2628 CJ Delft (Netherlands); Bauch, T. [Quantum Device Physics Laboratory, Department of Microtechnology and Nanoscience, Chalmers University of Technology, SE-41296 Göteborg (Sweden); Lombardi, F., E-mail: floriana.lombardi@chalmers.se [Quantum Device Physics Laboratory, Department of Microtechnology and Nanoscience, Chalmers University of Technology, SE-41296 Göteborg (Sweden)

    2014-11-15

    Highlights: • We fabricated YBCO nanorings, whose arms have cross sections down to 50 × 30 nm{sup 2}. • We measured the magnetoresistance R(B) close to the superconducting transition. • Large R(B) oscillations have been interpreted in terms of vortex dynamics. • The FFT peak of the R(B) oscillations can be associated to a h/2e periodicity. • The homogeneity in the rings favors a uniform vorticity of the order parameter. - Abstract: We have realized YBa{sub 2}Cu{sub 3}O{sub 7−δ} (YBCO) nanorings and measured the magnetoresistance R(B) close to the superconducting transition. The large oscillations that we have measured can be interpreted in terms of vortex dynamics triggering the nanowires to the resistive state. The Fast Fourier Transform spectrum of the magnetoresistance oscillations shows a single sharp peak for nanorings with narrower loop arm width: this peak can be univocally associated to a h/2e periodicity as predicted for optimally doped YBCO. Moreover it is a clear evidence of a uniform vorticity of the order parameter inside the rings, confirming a high degree of homogeneity of our nanostructures. This result gives a boost to further investigations of YBCO nanorings at different dopings within the superconducting dome, where in the underdoped regime a R(B) periodicity different from the conventional h/2e has been predicted.

  20. Generation of multiple excitons in Ag2S quantum dots: Single high-energy versus multiple-photon excitation

    KAUST Repository

    Sun, Jingya

    2014-02-20

    We explored biexciton generation via carrier multiplication (or multiple-exciton generation) by high-energy photons and by multiple-photon absorption in Ag2S quantum dots (QDs) using femtosecond broad-band transient absorption spectroscopy. Irrespective of the size of the QDs and how the multiple excitons are generated in the Ag2S QDs, two distinct characteristic time constants of 9.6-10.2 and 135-175 ps are obtained for the nonradiative Auger recombination of the multiple excitons, indicating the existence of two binding excitons, namely, tightly bound and weakly bound excitons. More importantly, the lifetimes of multiple excitons in Ag 2S QDs were about 1 and 2 orders of magnitude longer than those of comparable size PbS QDs and single-walled carbon nanotubes, respectively. This result is significant because it suggests that by utilizing an appropriate electron acceptor, there is a higher possibility to extract multiple electron-hole pairs in Ag2S QDs, which should improve the performance of QD-based solar cell devices. © 2014 American Chemical Society.

  1. 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...

  2. 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.

  3. 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.

  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. Optical response and excitons in gapped graphene

    DEFF Research Database (Denmark)

    Pedersen, Thomas Garm; Jauho, Antti-Pekka; Pedersen, K.

    2009-01-01

    Graphene can be rendered semiconducting via energy gaps introduced in a variety of ways, e.g., coupling to substrates, electrical biasing, or nanostructuring. To describe and compare different realizations of gapped graphene we propose a simple two-band model in which a "mass" term is responsible...... for the gap. The optical conductivity predicted for this model is obtained as a simple closed-form expression. In addition, analytical estimates for the binding energy of excitons are derived and the impact of excitons on the optical response is analyzed....

  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. 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.

  8. 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.

  9. Development and understanding of multifunctional gold nanorings for photodynamic therapy of cancer

    Science.gov (United States)

    Hu, Yue

    Gold nanostructures of various geometries and dimensions are being broadly explored in the fast expanding field of nanomedicine due to the unusual combination of biocompatibility, versatility of surface functionalization, and localized surface-plasmon resonance (LSPR). Examples of relevant applications include biomedical imaging, clinical diagnostics and therapeutics. Gold nanorings (Au NRs) are of particular interest because of their intricate structure and LSPR tunability over a wide wavelength range. A solution-based synthesis approach is yet to be developed, however, to allow exploration of Au NRs for basic and applied studies. This dissertation focuses on the fabrication, characterization, and evaluation of colloidal Au NRs for enhanced photodynamic therapy (PDT) of breast cancer cells. We have developed a novel synthesis strategy and associated pathways toward Au NRs by galvanic replacement reaction of Co nanoparticles (Co NPs) in HAuCl4 solution. We have shown that surface-chemistry mediated particle-particle interaction of the Co NPs that leads to their 1D chain-like assembly as sacrificial template is critically important for the growth of Au NRs. Otherwise, Au nanoshells or Au nanotubes may result. The Au NRs exhibit tunable LSPR wavelengths from visible to near-infrared (NIR) region via varying the aspect ratio, in agreement with our theoretical calculations using the finite-difference time domain (FDTD) method. A layer-by-layer (LbL) assembly method was used to load Al(III) phthalocyanine chloride tetrasulfonic acid (AlPcS4) photosensitizer (PS) onto the surface of Au NRs. We have revealed that the photosensitivity of AlPcS4 can be quenched unless desorbed from the surface of Au NRs in the cellular compartment. An eight-fold increase in PDT killing efficiency of human breast cancer cells (MDA-MB-231) has been achieved using LbL-assembled AlPcS4-Au NR complexes in comparison to AlPcS4 only or the mixture of AlPcS 4 and Au NRs. This strategy allows

  10. 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.

  11. 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...

  12. 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...

  13. 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...

  14. 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...

  15. 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.

  16. 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.

  17. Width dependent transition of quantized spin-wave modes in Ni{sub 80}Fe{sub 20} square nanorings

    Energy Technology Data Exchange (ETDEWEB)

    Banerjee, Chandrima; Saha, Susmita; Barman, Saswati; Barman, Anjan, E-mail: abarman@bose.res.in [Thematic Unit of Excellence on Nanodevice Technology, Department of Condensed Matter Physics and Material Sciences, S. N. Bose National Centre for Basic Sciences, Block JD, Sector III, Salt Lake, Kolkata 700098 (India); Rousseau, Olivier [CEMS-RIKEN, 2-1 Hirosawa, Wako, Saitama 351-0198 (Japan); Otani, YoshiChika [CEMS-RIKEN, 2-1 Hirosawa, Wako, Saitama 351-0198 (Japan); Institute for Solid State Physics, University of Tokyo, 5-1-5 Kashiwanoha, Kashiwa, Chiba 277-8581 (Japan)

    2014-10-28

    We investigated optically induced ultrafast magnetization dynamics in square shaped Ni{sub 80}Fe{sub 20} nanorings with varying ring width. Rich spin-wave spectra are observed whose frequencies showed a strong dependence on the ring width. Micromagnetic simulations showed different types of spin-wave modes, which are quantized upto very high quantization number. In the case of widest ring, the spin-wave mode spectrum shows quantized modes along the applied field direction, which is similar to the mode spectrum of an antidot array. As the ring width decreases, additional quantization in the azimuthal direction appears causing mixed modes. In the narrowest ring, the spin-waves exhibit quantization solely in azimuthal direction. The different quantization is attributed to the variation in the internal field distribution for different ring width as obtained from micromagnetic analysis and supported by magnetic force microscopy.

  18. 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.

  19. 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 b...

  20. 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, ...

  1. 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.

  2. 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.

  3. 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.

  4. 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.

  5. 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

  6. 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...

  7. Exciton transfer dynamics in a trimer system

    Institute of Scientific and Technical Information of China (English)

    Tan Qing-Shou; Xu Lan; Kuang Le-Man

    2013-01-01

    We study exciton transfer dynamics in a trimer system by investigating excitation transfer probability (ETP).We calculate ETP in the zero-temperature limit and theoretically predict the environment-assisted quantum critical effect,in which ETP exhibits a sudden change at the critical point of quantum phase transition for the trimer.In particular,we find that the steady-state ETP can be observed in the presence of the environment interaction.

  8. 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.

  9. 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.

  10. 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.

  11. 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.

  12. 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.

  13. 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.

  14. 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.

  15. 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...

  16. 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....

  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 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.

  19. 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.

  20. 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.

  1. 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...

  2. 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...

  3. 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...

  4. 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...

  5. 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...

  6. 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.

  7. 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.

  8. 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).

  9. 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...

  10. 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.

  11. 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.

  12. 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.

  13. 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.

  14. 铁磁性坡莫合金纳米环的制备与磁性研究%Preparation and Magnetic Properties of Ferromagnetic Permalloy Nanorings

    Institute of Scientific and Technical Information of China (English)

    曾帅; 郭振刚; 潘礼庆

    2013-01-01

    铁磁性纳米环是一种纳米尺寸的环状实体,由于具备高密度磁存储的能力,被认为是下一代高性能存储器——磁随机存储器(MRAM)的重要结构单元.利用聚苯乙烯微球模板法制备了单分散的坡莫合金Ni75Fe25(NiFe)纳米环,并用扫描电子显微镜(SEM)表征了纳米环的分布情况;用振动样品磁强计(VSM)测量了NiFe纳米环的磁化曲线,显示出两种磁状态,即涡旋态(Vortex state)和双畴态(Onion state),并利用OOMMF软件对NiFe纳米环的磁化翻转过程进行微磁模拟,观察到纳米环不同磁化状态下的自旋组态.%Ferromagnetic nanoring is a ring entity,which is considered to be the elementary unit for the next generation of high-performance memory,i.e.magnetic random access memory (MRAM).Permalloy Ni75Fe25 (NiFe) nanorings were fabricated by polystyrene nanosphere template,characterized by scanning electron microscopy (SEM).The magnetic hysteresis loops were measured by using vibrating sample magnetometer,which show that there are two magnetic states:vortex and onion state.And the magnetic properties of NiFe nanorings were studied by micromagnetic simulation with OOMMF.The spin configurations of different magnetic states were obtained by calculation.

  15. Length-dependent optical effects in single walled carbon nanotubes.

    Science.gov (United States)

    Rajan, Aruna; Strano, Michael S; Heller, Daniel A; Hertel, Tobias; Schulten, Klaus

    2008-05-15

    Recently, Heller et al. reported length-dependent effects on the relative photoluminescence (PL) quantum yield of single walled carbon nanotubes (SWNTs) [Heller et al J. Am. Chem. Soc. 2004, 126, 14567-14573]. We propose a simple model involving thermal diffusion of excitons along the nanotube axis and quenching at the ends, to explain the observed trend in their data. By fitting to our model, we extract a diffusion coefficient of 6 cm(2)/s for excitons in SWNTs. Assuming a mono exponential decay of exciton PL, we also predict that effective length-dependent PL lifetimes for these excitons lie in the range of 1-27 ps. Experimental observations are shown to be consistent with stochastic rather than wavepacket-like exciton migration, which is in agreement with ultrafast excitonic dephasing. Edge effects seem to limit the use of short SWNTs in imaging and optical sensing applications.

  16. 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

  17. 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.

  18. 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.

  19. 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.

  20. 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.

  1. 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.

  2. 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.

  3. 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.

  4. 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.

  5. 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.

  6. 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.

  7. 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.

  8. 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.

  9. 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.

  10. 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.

  11. 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.)

  12. Exciton-dominant Electroluminescence from a Diode of Monolayer MoS2

    Science.gov (United States)

    2014-05-14

    Auger recombination may lead to rapid exciton- exciton annihilation when extra or multiple excitations are present.16–21 At a low electron-hole pair ...sufficiently efficient, it will quickly deplete the population of electron-hole pairs . The annihilation of the electron-hole pairs comes to a stop when only a...of the exciton-exciton annihilation of bound exciton emission is observed under a high electron-hole pair injection rate at room temperature. At a high

  13. 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 ...

  14. 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.

  15. 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

  16. 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...

  17. 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.

  18. 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.

  19. 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.

  20. 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.

  1. 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...

  2. 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.

  3. 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...

  4. 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.

  5. Nano-rings with a handle – Synthesis of substituted cycloparaphenylenes

    Directory of Open Access Journals (Sweden)

    Anne-Florence Tran-Van

    2014-08-01

    Full Text Available The research of cycloparaphenylenes (CPPs, the smallest armchair carbon nanotube, has been a quest for the past decades which experienced a revival in 2008 when the first synthesis was achieved. Since then CPPs with various ring sizes have been realized. The incorporation of substituents and the synthesis of CPPs with building blocks different from phenyl rings bear challenges of their own. Such structures, however, are highly interesting, as they allow for an incorporation of CPPs as defined nano-objects for other applications. Therefore, this review provides a status report about the current efforts in synthesizing CPPs beyond the parent unsubstituted oligo-phenylene structure.

  6. 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.

  7. 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.

  8. Nanorings and rods interconnected by self-assembly mimicking an artificial network of neurons

    Science.gov (United States)

    Escárcega-Bobadilla, Martha V.; Zelada-Guillén, Gustavo A.; Pyrlin, Sergey V.; Wegrzyn, Marcin; Ramos, Marta M. D.; Giménez, Enrique; Stewart, Andrew; Maier, Gerhard; Kleij, Arjan W.

    2013-11-01

    Molecular electronics based on structures ordered as neural networks emerges as the next evolutionary milestone in the construction of nanodevices with unprecedented applications. However, the straightforward formation of geometrically defined and interconnected nanostructures is crucial for the production of electronic circuitry nanoequivalents. Here we report on the molecularly fine-tuned self-assembly of tetrakis-Schiff base compounds into nanosized rings interconnected by unusually large nanorods providing a set of connections that mimic a biological network of neurons. The networks are produced through self-assembly resulting from the molecular conformation and noncovalent intermolecular interactions. These features can be easily generated on flat surfaces and in a polymeric matrix by casting from solution under ambient conditions. The structures can be used to guide the position of electron-transporting agents such as carbon nanotubes on a surface or in a polymer matrix to create electrically conducting networks that can find direct use in constructing nanoelectronic circuits.

  9. 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).

  10. Influence of NaOH on the formation and morphology of Bi{sub 2}Te{sub 3} nanostructures in a solvothermal process: From hexagonal nanoplates to nanorings

    Energy Technology Data Exchange (ETDEWEB)

    Liang Yujie [School of Science, Minzu University of China, Beijing 100081 (China); Wang, Wenzhong, E-mail: wzhwang@aphy.iphy.ac.cn [School of Science, Minzu University of China, Beijing 100081 (China); School of Physical Electronics, University of Electronic Science and Technology of China, Chengdu 610054 (China); Zeng Baoqing [School of Physical Electronics, University of Electronic Science and Technology of China, Chengdu 610054 (China); Zhang Guling [School of Science, Minzu University of China, Beijing 100081 (China); He Qingyu [Institute of Electronic Information Material and Apparatus, Laboratory of Quantum Information Technology, School of Physics and Telecommunication Engineering, South China Normal University, Guangzhou 510006 (China); Fu Junli [School of Science, Minzu University of China, Beijing 100081 (China)

    2011-09-15

    Highlights: {yields} Bi{sub 2}Te{sub 3} nanoplates and nanorings were synthesized by a simple solvothermal process. {yields} NaOH is not necessary for Bi{sub 2}Te{sub 3} nanostructure growth in a solvothermal process. {yields} Hexagonal Bi{sub 2}Te{sub 3} nanoplates were achieved with NaOH concentrations of 5-7 M. {yields} Hexagonal Bi{sub 2}Te{sub 3} nanorings were fabricated with NaOH concentrations of 9-11 M. {yields} Bi{sub 2}Te{sub 3} nanorings were fabricated by dissolving the inner part of the nanoplates with NaOH. - Abstarct: Hexagonal bismuth telluride (Bi{sub 2}Te{sub 3}) nanoplates and nanorings were synthesized by a simple solvothermal process. The composition, morphology and size of the as-prepared products were investigated by X-ray diffraction and transmission electron microscopy in detail. The systemically experiments have been performed to investigate the effect of alkaline additive NaOH on composition and morphology of Bi{sub 2}Te{sub 3} nanostructures. The results indicate that alkaline additive NaOH is not necessary for the formation of Bi{sub 2}Te{sub 3} nanostructures in a solvothermal process. However, NaOH plays an important role in determining the morphology and size of Bi{sub 2}Te{sub 3} nanostructures. When the experiment was carried out with NaOH concentration ranging from 5 to 7 M, hexagonal Bi{sub 2}Te{sub 3} nanoplates with edge length of 140-280 nm were synthesized. When the experiment was carried out at higher NaOH concentration of 9-11 M, hexagonal Bi{sub 2}Te{sub 3} nanorings were fabricated by dissolving the inner part of the hexagonal nanoplates with NaOH for the first time. A possible formation mechanism has been proposed based on the experimental results and analysis. This work may open a new rational route for the synthesis of hexagonal Bi{sub 2}Te{sub 3} nanorings which may have some scientific and technological applications in various functional devices.

  11. 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.

  12. 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

  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. 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.

  15. 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.

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

    Science.gov (United States)

    Scully, Shawn Ryan

    Organic photovoltaics have attracted significant interest over the last decade due to their promise as clean low-cost alternatives to large-scale electric power generation such as coal-fired power, natural gas, and nuclear power. Many believe power conversion efficiency targets of 10-15% must be reached before commercialization is possible. Consequently, understanding the loss mechanisms which currently limit efficiencies to 4-5% is crucial to identify paths to reach higher efficiencies. In this work, we investigate the dominant loss mechanisms in some of the leading organic photovoltaic architectures. In the first class of architectures, which include planar heterojunctions and bulk heterojunctions with large domains, efficiencies are primarily limited by the distance photogenerated excitations (excitons) can be transported (termed the exciton diffusion length) to a heterojunction where the excitons may dissociate. We will discuss how to properly measure the exciton diffusion length focusing on the effects of optical interference and of energy transfer when using fullerenes as quenching layers and show how this explains the variety of diffusion lengths reported for the same material. After understanding that disorder and defects limit exciton diffusion lengths, we suggest some approaches to overcome this. We then extensively investigate the use of long-range resonant energy transfer to increase exciton harvesting. Using simulations and experiments as support, we discuss how energy transfer can be engineered into architectures to increase the distance excitons can be harvested. In an experimental model system, DOW Red/PTPTB, we will show how the distance excitons are harvested can be increased by almost an order of magnitude up to 27 nm from a heterojunction and give design rules and extensions of this concept for future architectures. After understanding exciton harvesting limitations we will look at other losses that are present in planar heterojunctions. One of

  17. 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.

  18. Exciton dephasing and biexciton binding in CdSe/ZnSe islands

    DEFF Research Database (Denmark)

    Wagner, Hans Peter; Tranitz, H.-P.; Preis, H;

    1999-01-01

    The dephasing of excitons and the formation of biexcitons in self-organized CdSe/ZnSe islands grown by molecular-beam epitaxy is investigated using spectrally resolved four-wave mixing. A distribution of exciton-exciton scattering efficiencies and dephasing times in the range of 0.5-10 ps...

  19. Enhanced energy transport in genetically engineered excitonic networks

    Science.gov (United States)

    Park, Heechul; Heldman, Nimrod; Rebentrost, Patrick; Abbondanza, Luigi; Iagatti, Alessandro; Alessi, Andrea; Patrizi, Barbara; Salvalaggio, Mario; Bussotti, Laura; Mohseni, Masoud; Caruso, Filippo; Johnsen, Hannah C.; Fusco, Roberto; Foggi, Paolo; Scudo, Petra F.; Lloyd, Seth; Belcher, Angela M.

    2016-02-01

    One of the challenges for achieving efficient exciton transport in solar energy conversion systems is precise structural control of the light-harvesting building blocks. Here, we create a tunable material consisting of a connected chromophore network on an ordered biological virus template. Using genetic engineering, we establish a link between the inter-chromophoric distances and emerging transport properties. The combination of spectroscopy measurements and dynamic modelling enables us to elucidate quantum coherent and classical incoherent energy transport at room temperature. Through genetic modifications, we obtain a significant enhancement of exciton diffusion length of about 68% in an intermediate quantum-classical regime.

  20. Environment-assisted quantum walks in excitonic energy transport

    Science.gov (United States)

    Mohseni, Masoud; Rebentrost, Patrick; Lloyd, Seth; Aspuru-Guzik, Alan

    2010-03-01

    Long-lived quantum coherence has recently been observed experimentally via ultrafast nonlinear spectroscopy in excitonic energy transfer within light-harvesting photosynthetic complexes, conjugated polymers, and marine alga even at room temperature. Here, we demonstrate that directed quantum walks lead to an enhancement of energy transfer efficiency in such systems. We introduce two complementary theoretical approaches, based on a Green's function method and energy transfer susceptibilities, to partition open quantum dynamics. We quantify the role of fundamental physical processes involved in energy transport. In particular, we examine the contributions of classical hopping, coherent excitonic Hamiltonian, and phonon-induced decoherence effects for pure dephasing, Markovian, and non-Markovian limits.

  1. 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.

  2. Coherent secondary emission from resonantly excited two-exciton states

    DEFF Research Database (Denmark)

    Birkedal, Dan

    2000-01-01

    The coherent interaction of light and the electronic states of semiconductors near the fundamental bandgap has been a very active topic of research since the advent of ultrafast lasers. While many of the ultrafast nonlinear properties of semiconductors have been well explained within mean field...... theories as e.g. the semiconductor Bloch equations, recent experimental and theoretical developments have demonstrated contributions to the third order nonlinear susceptibility from exciton-exciton correlations beyond the mean field approximation. Ultrafast transient four-wave mixing (TFWM)has been...

  3. Bimolecular Recombination Kinetics of an Exciton-Trion Gas

    Science.gov (United States)

    2015-07-01

    The second and third reactions are catalytic agents for the loss of excitons. This implies that the constants R and S will appear only in the exciton...change the electron density. 3 Note that Reaction 3 in Table 2 is catalytic as defined above, because it changes the electron and e−trion...from the PL laser, which is fixed. Table 2 Reactions that change νe Reaction Rate Constant 1. νe + νh → ϕ A 2. νe + τh → Ex P 3

  4. Realization of an all optical exciton-polariton router

    Energy Technology Data Exchange (ETDEWEB)

    Marsault, Félix; Nguyen, Hai Son; Tanese, Dimitrii; Lemaître, Aristide; Galopin, Elisabeth; Sagnes, Isabelle; Amo, Alberto [Laboratoire de Photonique et de Nanostructures, LPN/CNRS, Route de Nozay, 91460 Marcoussis (France); Bloch, Jacqueline, E-mail: jacqueline.bloch@lpn.cnrs.fr [Laboratoire de Photonique et de Nanostructures, LPN/CNRS, Route de Nozay, 91460 Marcoussis (France); Physics Department, Ecole Polytechnique, F-91128 Palaiseau Cedex (France)

    2015-11-16

    We report on the experimental realization of an all optical router for exciton-polaritons. This device is based on the design proposed by Flayac and Savenko [Appl. Phys. Lett. 103, 201105 (2013)], in which a zero-dimensional island is connected through tunnel barriers to two periodically modulated wires of different periods. Selective transmission of polaritons injected in the island, into either of the two wires, is achieved by tuning the energy of the island state across the band structure of the modulated wires. We demonstrate routing of ps polariton pulses using an optical control beam which controls the energy of the island quantum states, thanks to polariton-exciton interactions.

  5. Hybridized exciton-polariton resonances in core-shell nanoparticles

    CERN Document Server

    Gentile, Martin J

    2016-01-01

    The goal of nanophotonics is to control and manipulate light at length scales below the diffraction limit. Typically nanostructured metals are used for this purpose, light being confined by exploiting the surface plasmon-polaritons such structures support. Recently excitonic (molecular) materials have been identified as an alternative candidate material for nanophotonics. Here we use theoretical modelling to explore how hybridisation of surface exciton-polaritons can be achieved through appropriate nanostructuring. We focus on the extent to which the frequency of the hybridised modes can be shifted with respect to the underlying material resonances.

  6. Singlet exciton fission in polycrystalline pentacene: from photophysics toward devices.

    Science.gov (United States)

    Wilson, Mark W B; Rao, Akshay; Ehrler, Bruno; Friend, Richard H

    2013-06-18

    Singlet exciton fission is the process in conjugated organic molecules bywhich a photogenerated singlet exciton couples to a nearby chromophore in the ground state, creating a pair of triplet excitons. Researchers first reported this phenomenon in the 1960s, an event that sparked further studies in the following decade. These investigations used fluorescence spectroscopy to establish that exciton fission occurred in single crystals of several acenes. However, research interest has been recently rekindled by the possibility that singlet fission could be used as a carrier multiplication technique to enhance the efficiency of photovoltaic cells. The most successful architecture to-date involves sensitizing a red-absorbing photoactive layer with a blue-absorbing material that undergoes fission, thereby generating additional photocurrent from higher-energy photons. The quest for improved solar cells has spurred a drive to better understand the fission process, which has received timely aid from modern techniques for time-resolved spectroscopy, quantum chemistry, and small-molecule device fabrication. However, the consensus interpretation of the initial studies using ultrafast transient absorption spectroscopy was that exciton fission was suppressed in polycrystalline thin films of pentacene, a material that would be otherwise expected to be an ideal model system, as well as a viable candidate for fission-sensitized photovoltaic devices. In this Account, we review the results of our recent transient absorption and device-based studies of polycrystalline pentacene. We address the controversy surrounding the assignment of spectroscopic features in transient absorption data, and illustrate how a consistent interpretation is possible. This work underpins our conclusion that singlet fission in pentacene is extraordinarily rapid (∼80 fs) and is thus the dominant decay channel for the photoexcited singlet exciton. Further, we discuss our demonstration that triplet excitons

  7. Strong-field terahertz-optical mixing in excitons

    CERN Document Server

    Su, M Y; Sherwin, M S; Huntington, A S; Coldren, L A

    2002-01-01

    Driving a double-quantum-well excitonic intersubband resonance with a terahertz (THz) electric field of frequency \\omega_{THz} generated terahertz optical sidebands \\omega=\\omega_{THz}+\\omega_{NIR} on a weak NIR probe. At high THz intensities, the intersubband dipole energy which coupled two excitons was comparable to the THz photon energy. In this strong-field regime the sideband intensity displayed a non-monotonic dependence on the THz field strength. The oscillating refractive index which gives rise to the sidebands may be understood by the formation of Floquet states, which oscillate with the same periodicity as the driving THz field.

  8. Nongeneric dispersion of excitons in the bulk of WSe2

    Science.gov (United States)

    Schuster, R.; Wan, Y.; Knupfer, M.; Büchner, B.

    2016-08-01

    We combine electron energy-loss spectroscopy (EELS) and density functional theory (DFT) calculations to study the dispersion and effective mass of excitons in the bulk of WSe2. Our EELS data suggest substantial deviations from the generic quadratic momentum dependence along the Γ K direction. From the DFT-derived Kohn-Sham states we deduce the EELS response without the inclusion of particle-hole attraction to study the possible role of the single-particle band structure on the exciton behavior. Based on this analysis we argue in favor of a strongly momentum dependent particle-hole interaction in WSe2 and other group-VI-transition-metal dichalcogenides.

  9. Incomplete Exciton Harvesting from Fullerenes in Bulk Heterojunction Solar Cells

    KAUST Repository

    Burkhard, George F.

    2009-12-09

    We investigate the internal quantum efficiencies (IQEs) of high efficiency poly-3-hexylthiophene:[6,6]-phenyl-C61-butyric acid methyl ester (P3HT:PCBM) solar cells and find them to be lower at wavelengths where the PCBM absorbs. Because the exciton diffusion length in PCBM is too small, excitons generated in PCBM decay before reaching the donor-acceptor interface. This result has implications for most state of the art organic solar cells, since all of the most efficient devices use fullerenes as electron acceptors. © 2009 American Chemical Society.

  10. Binding Energy of Excitons in a Quantum Ring

    Institute of Scientific and Technical Information of China (English)

    XIE Wen-Fang

    2008-01-01

    The binding energy of excitons confined to a quantum ring under the influence of perpendicular homogeneous magnetic field is calculated as a function of the ring radius. Calculations are made by using the method of exact diagonalization within the effective-mass approximation. The feature of binding energy of the ground state as a function of the ring radius for several values of the magnetic field has been revealed. The interesting feature of our study is that, in a quantum ring, the geometric structure of excitons may reveal transition.

  11. Quantum Statistical Properties of the Exciton in a Leaky Quasi-Mode Cavity

    Institute of Scientific and Technical Information of China (English)

    YU Zhao-Xian; JIAO Zhi-Yong

    2002-01-01

    We have studied quantum statistical properties of the exciton in a leaky quasi-mode cavity. It is shown that when the exciton is initially in a squeezed coherent state whereas cavity initially in a vacuum state, there is energy exchange between the exciton and cavity. Both the exciton and cavity may exhibit sub-Poissonian distribution and exist quadrature squeezing. Calculation shows that correlation between the exciton and cavity is classical, which implies that there is not the violation of the Cauchy-Schwartz inequality.

  12. Spectral signatures of x((5)) processes in four-wave mixing of homogeneously broadened excitons

    DEFF Research Database (Denmark)

    Langbein, W.; Meier, T.; Koch, S.W.;

    2001-01-01

    The influence of fifth-order coherences on the spectrally resolved four-wave mixing response of predominantly homogeneously broadened quasi-two-dimensional excitons is studied. Fifth-order signatures are discussed as a function of spectral position and excitation polarization. An exciton-biexcito...... of one- and two-exciton resonances up to the fifth order in the optical field.......The influence of fifth-order coherences on the spectrally resolved four-wave mixing response of predominantly homogeneously broadened quasi-two-dimensional excitons is studied. Fifth-order signatures are discussed as a function of spectral position and excitation polarization. An exciton...

  13. Exciton-Phonon Scattering in CdSe/ZnSe Quantum Dots

    Institute of Scientific and Technical Information of China (English)

    张立功; 申德振; 范希武; 吕少哲

    2002-01-01

    A temperature-dependent photoluminescence measurement is performed in CdSe/ZnSe quantum dots with a ZnCdSe quantum well. We deduce the temperature dependence of the exciton linewidth and peak energy of the zero-dimensional exciton in the quantum dots and two-dimensional exciton in the CdSe wetting layer. The experimental data reveal a reduction of homogeneous broadening of the exciton line in the quantum dots in comparison with that in the two-dimensional wetting layer, which indicates the decrease of exciton and optical phonon coupling in the CdSe quantum dots.

  14. Transient demonstration of exciton behaviours in solid state cathodoluminescence under different driving voltage

    Institute of Scientific and Technical Information of China (English)

    Zhang Fu-Jun; Zhao Su-Ling; Xu Zheng; Huang Jin-Zhao; Xu Xu-Rong

    2007-01-01

    In the solid state cathodoluminescence (SSCL), organic materials were excited by hot electrons accelerated in silicon oxide (SiO2) layer under alternating current (AC). In this paper exciton behaviours were analysed by using transient spectra under different driving voltages. The threshold voltages of SSCL and exciton ionization were obtained from the transient spectra. The recombination radiation occurred when the driving voltage went beyond the threshold voltage of exciton ionization. Prom the transient spectrum of two kinds of luminescence (exciton emission and recombination radiation), it was demonstrated that recombination radiation should benefit from the exciton ionization.

  15. Dark-bright exciton spin-flip rates of quantum dots determined by a modified local density of optical states

    DEFF Research Database (Denmark)

    Lodahl, Peter; Johansen, Jeppe; Julsgaard, Brian;

    2009-01-01

    This work investigates the influence of dark excitons on the radiative dynamics of semiconductor quantum dots (QDs). Dark excitons have total angular momentum of 2 and contribute to the fine structure of the exciton ground state. As opposed to bright excitons that have total angular momentum 1...

  16. Hamiltonian multiplex interaction based on excitons effect in semiconductor QCs

    Directory of Open Access Journals (Sweden)

    Arezu Jahanshir

    2014-11-01

    Full Text Available The subject of modern technology has been the focus of extensive theoretical investigations in semiconducting nanostructures which we know as quantum dots (QCs. The possibility of monitoring and controlling the properties of QCs attracted considerable attention to these objects, as an important basic system in future technology. So, the quantum-mechanical effects play a significant role in the description of the formation mechanism QCs, determination of mass spectrum, binding energy and other characteristics. Based on QFT and by using oscillator representation method (ORM and operator product expansion technique developed in QFT, we study the properties of electron-hole QDs, determine mass spectrum and peruse spin-spin interactions in exciton system and its multiple pair systems. This method has applications to calculate the binding energy of exciton system in ground and excited states with semi-nuclear structure in semiconductor QCs or cold atomic few-body systems and develop the general calculation’s theory of few-body systems based on the Coulomb interaction between particles by forming excitonic pairs in semiconductor QCs. We investigate the binding energy of exciton bound states. It is shown that fermion particles have a very small mass, and after bonding together by dynamically force, constituent particles become massive, which is analogous to what happens in QCD.

  17. Excitons in van der Waals Heterostructures: A theoretical study

    DEFF Research Database (Denmark)

    Latini, Simone

    to experimental results. Ultimately this thesis puts forth a first-principles methodology that allows us to address scientific questions that are beyond the capability of existing state of the art techniques and enables 2D materials researcher to predict and design dielectric, electronic and excitonic properties...

  18. Excitonic Doppler-Rabi Oscillations in a Moving Organic Slab

    Institute of Scientific and Technical Information of China (English)

    2005-01-01

    It is theoretically shown that excitonic Doppler-Rabi oscillations can occur in an organic slab moving along the axis of a high-Q cavity. Due to the √N enhancement of the vacuum Rabi frequency, this effect can be more easily observed than that in a moving two-level atom.

  19. Excitonic insulator transition in the conjugated polymer polyacene

    NARCIS (Netherlands)

    Rice, MJ; Gartstein, YN

    2004-01-01

    According to molecular orbital theory, the symmetrically positioned one-dimensional (I-D) conduction and valence bands of polyacene touch at the X point. Clearly, the exciton binding energy of this semimetal exceeds the band gap so that polyacene should be a textbook case of a semimetal undergoing a

  20. Exploration of exciton delocalization in organic crystalline thin films

    Science.gov (United States)

    Hua, Kim; Manning, Lane; Rawat, Naveen; Ainsworth, Victoria; Furis, Madalina

    The electronic properties of organic semiconductors play a crucial role in designing new materials for specific applications. Our group recently found evidence for a rotation of molecular planes in phthalocyanines that is responsible for the disappearance of a delocalized exciton in these systems for T >150K.................()().......1 In this study, we attempt to tune the exciton delocalization of small organic molecules using strain effects and alloying different molecules in the same family. The exciton behavior is monitored using time- and polarization resolved photolumniscence (PL) spectroscopy as a function of temperature. Specifically, organic crystalline thin films of octabutoxy phthalocyanine (H2OBPc), octyloxy phthalocyanines and H-bonded semiconductors such as the quinacridone and indigo derivatives are deposited on flexible substrates (i.e. Kapton and PEN) using an in-house developed pen-writing method.........2 that results in crystalline films with macroscopic long range order. The room temperature PL studies show redshift and changes in polarization upon bending of the film. Crystalline thin films of alloyed H2OBPc and octabutoxy naphthalocyanine with ratios ranging from 1:1 to 100:1 fabricated on both sapphire and flexible substrates are also explored using the same PL spectroscopy to elucidate the behaviors of delocalized excitons. .1N. Rawat, et al., J Phys Chem Lett 6, 1834 (2015). 2R. L. Headrick, et al., Applied Physics Letters 92, 063302 (2008). NSF DMR-1056589, NSF DMR-1062966.

  1. 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

  2. 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

  3. Exciton transport in thin-film cyanine dye J-aggregates

    CERN Document Server

    Valleau, Stéphanie; Yung, Man-Hong; Aspuru-Guzik, Alán

    2012-01-01

    We present a theoretical model for the study of exciton dynamics in J-aggregated monolayers of fluorescent dyes. The excitonic evolution is described by a Monte-Carlo wave function approach which allows for a unified description of the quantum (ballistic) and classical (diffusive) propagation of an exciton on a lattice in different parameter regimes. The transition between the ballistic and diffusive regime is controlled by static and dynamic disorder. As an example, the model is applied to three cyanine dye J-aggregates: TC, TDBC, and U3. Each of the molecule-specific structure and excitation parameters are estimated using time-dependent density functional theory. The exciton diffusion coefficients are calculated and analyzed for different degrees of film disorder and are correlated to the physical properties and the structural arrangement of molecules in the aggregates. Further, exciton transport is anisotropic and dependent on the initial exciton energy. The upper-bound estimation of the exciton diffusion ...

  4. Coherent optical writing and reading of the exciton spin state in single quantum dots

    CERN Document Server

    Benny, Y; Kodriano, Y; Poem, E; Presman, R; Galushko, D; Petroff, P M; Gershoni, D

    2010-01-01

    We demonstrate a one to one correspondence between the polarization state of a light pulse tuned to excitonic resonances of single semiconductor quantum dots and the spin state of the exciton that it photogenerates. This is accomplished using two variably polarized and independently tuned picosecond laser pulses. The first "writes" the spin state of the resonantly excited exciton. The second is tuned to biexcitonic resonances, and its absorption is used to "read" the exciton spin state. The absorption of the second pulse depends on its polarization relative to the exciton spin direction. Changes in the exciton spin result in corresponding changes in the intensity of the photoluminescence from the biexciton lines which we monitor, obtaining thus a one to one mapping between any point on the Poincare sphere of the light polarization to a point on the Bloch sphere of the exciton spin.

  5. Electron energy loss spectroscopy of excitons in two-dimensional-semiconductors as a function of temperature

    KAUST Repository

    Tizei, Luiz H. G.

    2016-04-21

    We have explored the benefits of performing monochromated Electron Energy Loss Spectroscopy(EELS) in samples at cryogenic temperatures. As an example, we have observed the excitonic absorption peaks in single layer Transition Metal Dichalcogenides. These peaks appear separated by small energies due to spin orbit coupling. We have been able to distinguish the split for MoS2 below 300 K and for MoSe2 below 220 K. However, the distinction between peaks is only clear at 150 K. We have measured the change in absorption threshold between 150 K and 770 K for MoS2 and MoSe2. We discuss the effect of carbon and ice contamination in EELSspectra. The increased spectral resolution available made possible with modern monochromators in electron microscopes will require the development of stable sample holders which reaches temperatures far below that of liquid nitrogen.

  6. Exciton-polariton dynamics in quantum dot-cavity system

    Energy Technology Data Exchange (ETDEWEB)

    Neto, Antonio F.; Lima, William J.; Villas-Boas, Jose M. [Universidade Federal de Uberlandia (UFU), MG (Brazil). Inst. de Fisica

    2012-07-01

    Full text: One of the basic requirement for quantum information processing systems is the ability to completely control the state of a single qubit. This imply in know all sources of decoherence and elaborate ways to avoid them. In recent work, A. Laucht et al. [1] presented detailed theoretical and experimental investigations of electrically tunable single quantum dot (QD) - photonic crystal (PhC) nanocavity systems operating in the strong coupling regime of the light matter interaction. Unlike previous studies, where the exciton-cavity spectral detuning was varied by changing the lattice temperature, or by the adsorption of inert gases at low temperatures, they employ the quantum confined Stark-effect to electro-optically control the exciton-cavity detuning. The new built device enabled them to systematically probe the emission spectrum of the strongly coupled system as a function of external control parameters, as for example the incoherent excitation power density or the lattice temperature. Those studies reveal for the first time insights in dephasing mechanisms of 0D exciton polaritons [1]. In another study [2], using a similar device, they investigate the coupling between two different QDs with a single cavity mode. In both works, incoherent pumping was used, but for quantum information, coherent and controlled excitations are necessary. Here, we theoretically investigate the dynamics a single quantum dot inside a cavity under coherent pulse excitation and explore a wide range of parameters, as for example, the exciton-cavity detunings, the excitation power, the spontaneous decay, and pure dephasing. We use density matrix formalism in the Lindblad form, and we solve it numerically. Our results show that coherent excitation can be used to probe strong coupling between exciton and cavity mode by monitoring the exciton Rabi oscillation as function of the cavity detuning. This can give new insights for future experimental measurement focusing on quantum

  7. 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.

  8. Jointly Tuned Plasmonic–Excitonic Photovoltaics Using Nanoshells

    KAUST Repository

    Paz-Soldan, Daniel

    2013-04-10

    Recent advances in spectrally tuned, solution-processed plasmonic nanoparticles have provided unprecedented control over light\\'s propagation and absorption via engineering at the nanoscale. Simultaneous parallel progress in colloidal quantum dot photovoltaics offers the potential for low-cost, large-area solar power; however, these devices suffer from poor quantum efficiency in the more weakly absorbed infrared portion of the sun\\'s spectrum. Here, we report a plasmonic-excitonic solar cell that combines two classes of solution-processed infrared materials that we tune jointly. We show through experiment and theory that a plasmonic-excitonic design using gold nanoshells with optimized single particle scattering-to-absorption cross-section ratios leads to a strong enhancement in near-field absorption and a resultant 35% enhancement in photocurrent in the performance-limiting near-infrared spectral region. © 2013 American Chemical Society.

  9. Collective oscillations in spatially modulated exciton-polariton condensate arrays

    Science.gov (United States)

    Tikhomirov, Andrey A.; Kanakov, Oleg I.; Altshuler, Boris L.; Ivanchenko, Mikhail V.

    2015-02-01

    We study collective dynamics of interacting centers of exciton-polariton condensation in presence of spatial inhomogeneity, as modeled by diatomic active oscillator lattices. The mode formalism is developed and employed to derive existence and stability criteria of plane wave solutions. It is demonstrated that k0 = 0 wave number mode with the binary elementary cell on a diatomic lattice possesses superior existence and stability properties. Decreasing net on-site losses (balance of dissipation and pumping) or conservative nonlinearity favors multistability of modes, while increasing frequency mismatch between adjacent oscillators detriments it. On the other hand, spatial inhomogeneity may recover stability of modes at high nonlinearities. Entering the region where all single-mode solutions are unstable we discover subsequent transitions between localized quasiperiodic, chaotic and global chaotic dynamics in the mode space, as nonlinearity increases. Importantly, the last transition evokes the loss of synchronization. These effects may determine lasing dynamics of interacting exciton-polariton condensation centers.

  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. Exciton and Biexciton Binding Energies in Rectangular Quantum Dots

    Institute of Scientific and Technical Information of China (English)

    LIU Yong-Hui; KONG Xiao-Jun

    2005-01-01

    @@ In the effective mass approximation, using the variational technology and a method of expanding the wavefunctions of exciton in terms of the eigenfunctions of the noninteracting electron-hole system, we calculate the exciton and biexciton ground state binding energies for rectangular quantum dots (QDs). In the calculation, a three-dimensional Fourier expansion of Coulomb potential is used to remove the numerical difficulty with the 1/r singularity, and it considerably reduces the computational effort. Our results agree fairly well with the previous results. It is found that the binding energies are highly correlated to the size of QDs. The quantum confinement effect of spherical QDs about biexciton is obviously larger than that of rectangular QDs when the well width is narrower than 2.0aB.

  12. Multiple exciton collection in a sensitized photovoltaic system.

    Science.gov (United States)

    Sambur, Justin B; Novet, Thomas; Parkinson, B A

    2010-10-01

    Multiple exciton generation, the creation of two electron-hole pairs from one high-energy photon, is well established in bulk semiconductors, but assessments of the efficiency of this effect remain controversial in quantum-confined systems like semiconductor nanocrystals. We used a photoelectrochemical system composed of PbS nanocrystals chemically bound to TiO(2) single crystals to demonstrate the collection of photocurrents with quantum yields greater than one electron per photon. The strong electronic coupling and favorable energy level alignment between PbS nanocrystals and bulk TiO(2) facilitate extraction of multiple excitons more quickly than they recombine, as well as collection of hot electrons from higher quantum dot excited states. Our results have implications for increasing the efficiency of photovoltaic devices by avoiding losses resulting from the thermalization of photogenerated carriers.

  13. 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.

  14. 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.

  15. Quasiparticle Gaps and Exciton Coulomb Energies in Si Nanoshells

    Energy Technology Data Exchange (ETDEWEB)

    Frey, K. [University of Illinois, Chicago; Idrobo Tapia, Juan C [ORNL; Tiago, Murilo L [ORNL; Reboredo, Fernando A [ORNL; Ogut, Serdar [University of Illinois, Chicago

    2009-01-01

    Quasiparticle gaps and exciton Coulomb energies of H-passivated spherical Si nanoshells are computed using rst principles SCF and GW methods. We nd that the quasiparticle gap of a nanoshell depends on both its inner radius R1 (weakly) and outer radius R2 (strongly). These dependences on R1 and R2 are mostly consistent with electrostatics of a metallic shell. We also nd that the unscreened Coulomb energy ECoul in Si nanoshells has a somewhat unexpected size dependence at xed outer radius R2: ECoul decreases as the nanoshell becomes more conning, contrary to what one would expect from quantum connement eects. We show that this is a consequence of an increase in the average electron-hole distance, giving rise to reduced exciton Coulomb energies in spite of the reduction in the conning nanoshell volume.

  16. Interaction of excitons with optical phonons in layer crystals

    Science.gov (United States)

    Nitsovich, Bohdan M.; Zenkova, C. Y.; Kramar, N. K.

    2002-02-01

    The investigation is concerned with layer crystals of the GaSe, InSe, GaTe, MoS2-type and other inorganic semiconductors, whose phonon spectrum has a great number of peculiarities, among them the availability of low-energy optical phonons. In this case the dispersion of these phonons can be essential and vary in character. The mass operator of the exciton-phonon system and the light absorption coefficient for different dispersion laws of optical phonons have been calculated. The influence of the sign of the phonon 'effective mass' on the exciton absorption band of layer crystals, which causes the opposite in sign dynamics of the absorption maximum shift, and the change of the absorption curve asymmetry have been determined.

  17. Chemical potential and compressibility of quantum Hall bilayer excitons,.

    Energy Technology Data Exchange (ETDEWEB)

    Skinner, Brian

    2016-02-25

    I consider a system of two parallel quantum Hall layers with total filling factor 0 or 1. When the distance between the layers is small enough, electrons and holes in opposite layers can form inter-layer excitons, which have a finite effective mass and interact via a dipole-dipole potential. I present results for the chemical potential u of the resulting bosonic system as a function of the exciton concentration n and the interlayer separation d. I show that both u and the interlayer capacitance have an unusual nonmonotonic dependence on d, owing to the interplay between an increasing dipole moment and an increasing effective mass with increasing d. Finally, I discuss the transition between the superfluid and Wigner crystal phases, which is shown to occur at d x n-1/10. Results are derived first via simple intuitive arguments, and then verified with more careful analytic derivations and numeric calculations.

  18. Lindblad theory of dynamical decoherence of quantum-dot excitons

    OpenAIRE

    Eastham, P. R.; Spracklen, A O; Keeling, Jonathan Mark James

    2013-01-01

    We use the Bloch-Redfield-Wangsness theory to calculate the effects of acoustic phonons in coherent control experiments where quantum-dot excitons are driven by shaped laser pulses. This theory yields a generalized Lindblad equation for the density operator of the dot, with time-dependent damping and decoherence due to phonon transitions between the instantaneous dressed states. It captures similar physics to the form recently applied to Rabi oscillation experiments [Ramsay et al., Phys. Rev....

  19. One Dimensional Time-Dependent Tunnelling of Excitons

    Science.gov (United States)

    Kilcullen, Patrick; Salayka-Ladouceur, Logan; Malmgren, Kevin; Reid, Matthew; Shegelski, Mark R. A.

    2017-03-01

    We study the time-dependent tunnelling of excitons in one dimension using numerical integration based on the Crank-Nicholson method. A complete development of the time-dependent simulator is provided. External barriers studied include single and double delta barriers. We find that the appearance of transmission resonances depends strongly on the dielectric constant, relative effective masses, and initial spatial spread of the wavefunction. A discussion regarding applications to realistic systems is provided.

  20. Exciton-mediated photothermal cooling in GaAs membranes

    CERN Document Server

    Xuereb, André; Naesby, Andreas; Polzik, Eugene S; Hammerer, Klemens

    2012-01-01

    Cooling of the mechanical motion of a GaAs nano-membrane using the photothermal effect mediated by excitons was recently demonstrated by some of us [K. Usami, et al., Nature Phys. 8, 168 (2012)] and provides a clear example of the use of thermal forces to cool down mechanical motion. Here, we report on a single-free-parameter theoretical model to explain the results of this experiment which matches the experimental data remarkably well.

  1. Exciton lifetime measurements on single silicon quantum dots.

    Science.gov (United States)

    Sangghaleh, Fatemeh; Bruhn, Benjamin; Schmidt, Torsten; Linnros, Jan

    2013-06-01

    We measured the exciton lifetime of single silicon quantum dots, fabricated by electron beam lithography, reactive ion etching and oxidation. The observed photoluminescence decays are of mono-exponential character with a large variation (5-45 μs) from dot to dot, even for the same emission energy. We show that this lifetime variation may be the origin of the heavily debated non-exponential (stretched) decays typically observed for ensemble measurements.

  2. Exciton spin dynamics in ZnO epilayers

    Energy Technology Data Exchange (ETDEWEB)

    Lagarde, D.; Lombez, L.; Balocchi, A.; Renucci, P.; Carrere, H.; Amand, T.; Marie, X. [Laboratoire de Nanophysique, Magnetisme et Optoelectronique, INSA, 135 avenue de Rangueil, 31077 Toulouse Cedex 4 (France); Mei, Z.X.; Du, X.L.; Xue, Q.K. [Institute of Physics, Chinese Academy of Sciences and National Center for Nano-Science and Technology, Beijing 100080 (China)

    2007-07-01

    We used time-resolved optical orientation experiments to study the low temperature spin dynamics of a ZnO epilayer. The sample shows a circular polarisation of the donor-bound exciton of 11% with a decay time of 275 ps. A very narrow spectral dependence of the initial polarisation and a rapid decrease of the polarisation decay time with temperature are also observed. (copyright 2007 WILEY-VCH Verlag GmbH and Co. KGaA, Weinheim) (orig.)

  3. Electronic absorption of Frenkel excitons in topologically disordered systems

    Science.gov (United States)

    Schweizer, Kenneth S.

    1986-10-01

    A self-consistent effective medium theory of the electronic absorption spectra of tightly bound dipolar excitons in simple fluids is developed within the adiabatic picture. The theoretical approach is based on the isomorphism between the path-integral formulation of quantum theory and classical statistical mechanics and is an extension of previous work [D. Chandler, K. S. Schweizer, and P. G. Wolynes, Phys. Rev. Lett. 49, 1100 (1982)]. The consequences of fluid structural disorder on resonant excitation transfer and the statistical fluctuations of single molecule energy levels are simultaneously treated. Detailed numerical calculations are performed to establish the dependence of the absorption spectrum on fluid density, short range order, and the relative magnitude of the resonant transfer vs the single site disorder. The density dependence of the spectral features are found to be a sensitive function of fluid structure and the relative strength of the localizing vs the delocalizing interactions. By comparing the liquid state results with the corresponding crystalline solid behavior, the consequences of topological disorder on the exciton spectrum are identified. The relevance of the theoretical predictions to spectroscopic probes of exciton delocalization in molecular liquids and glasses is discussed.

  4. Excitons in conjugated polymers: Do we need a paradigma change?

    Energy Technology Data Exchange (ETDEWEB)

    Beenken, Wichard J.D. [Department of Theoretical Physics I, Ilmenau University of Thechnology (Germany)

    2009-12-15

    We have previously shown that both, polymer conformation and dynamics are crucial for the exciton transport in conjugated polymers. Thereby we found that the usual Foerster-type hopping transfer model - even if one applies the line-dipole approximation - falls short in one crucial aspect: the nature of the sites the excitons are transferred between is still unclear. We found that the simple model of spectroscopic units defined as segments of the polymer chains separated by structural defects breaking the {pi}-conjugation is only justified for chemical defects like hydrogenated double bonds, or extreme gauche (90 ) torsions between the monomers. Both defects are far too rare in a well-prepared conjugated polymer to explain the mean spectroscopic-unit length of typically 6-7 monomers. Meanwhile, also the concept of dynamical formation of the spectroscopic units, we had previously suggested, has also failed. Thus the question of a paradigma change concerning the exciton transport in conjugated polymers appears on the agenda. (Abstract Copyright [2009], Wiley Periodicals, Inc.)

  5. Photoluminescence of localized excitons in InGan quantum dots

    Energy Technology Data Exchange (ETDEWEB)

    Usov, S. O., E-mail: S.Usov@mail.ioffe.ru; Tsatsul' nikov, A. F.; Lundin, V. V.; Sakharov, A. V.; Zavarin, E. E.; Ledentsov, N. N. [Russian Academy of Sciences, Ioffe Physicotechnical Institute (Russian Federation)

    2008-02-15

    Photoluminescence spectra of samples with ultrathin InGaN layers embedded in AlGaN and GaN matrices are studied experimentally in the temperature range of 80 to 300 K. It is shown that the temperature dependences can be understood in the context of Eliseev's model and that, in the active region of the structures under study, the dispersion {sigma} of the exciton-localization energy depends on the average In content in InGaN-alloy layers. Furthermore, the Urbach energy E{sub U}, which characterizes the localization energy of excitons in the tails of the density of states, was determined from an analysis of the shape of the low-energy slope of the spectrum. It is shown that {sigma} and E{sub U}, quantities representing the scale of the exciton-localization effects, vary linearly with the photoluminescence-peak wavelength in the range from the ultraviolet to the green region of the spectrum.

  6. 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.

  7. Role of Strain on the Coherent Properties of GaAs Excitons and Biexcitons

    CERN Document Server

    Wilmer, Brian L; Ashley, Joseph M; Hall, Kimberley C; Bristow, Alan D

    2016-01-01

    Polarization-dependent two-dimensional Fourier-transform spectroscopy (2DFTS) is performed on excitons in strained bulk GaAs layers probing the coherent response for differing amounts of strain. Biaxial tensile strain lifts the degeneracy of heavy-hole (HH) and light-hole (LH) valence states, leading to an observed splitting of the associated excitons at low temperature. Increasing the strain increases the magnitude of the HH/LH exciton peak splitting, induces an asymmetry in the off-diagonal coherences, increases the difference in the HH and LH exciton homogenous linewidths, and increases the inhomogeneous broadening of both exciton species. All results arise from strain-induced variations in the local electronic environment, which is not uniform along the growth direction of the thin layers. For cross-linear polarized excitation, wherein excitonic signals give way to biexcitonic signals, the high-strain sample shows evidence of bound LH, HH, and mixed biexcitons.

  8. The mechanism of long-range exciton diffusion in a nematically organized porphyrin layer.

    Science.gov (United States)

    Huijser, Annemarie; Savenije, Tom J; Meskers, Stefan C J; Vermeulen, Martien J W; Siebbeles, Laurens D A

    2008-09-17

    The exciton diffusion length in a nematically organized meso-tetra(4-n-butylphenyl)porphyrin (TnBuPP) layer was found to exceed 40 nm at a temperature of 90 K and to be equal to 22 +/- 3 nm at 300 K. The exciton diffusion coefficient decreases from > or = 3.1 x 10(-6) m(2)/s at 90 K to (2.5 +/- 0.5) x 10(-7) m(2)/s at 300 K. This thermal deactivation is attributed to exciton motion via a band mechanism. The motion of an exciton is not limited by polaronic effects; that is, the deformation of the atomic lattice around the exciton. The absence of polaronic self-trapping implies that the exciton diffusion coefficient can be enhanced by improvement of structural order and rigidity of the material.

  9. Effect of Strong Orbital Magnetic Field on the Exciton Condensation in an Extended Falicov Kimball Model

    Science.gov (United States)

    Pradhan, S.; Taraphder, A.

    2016-10-01

    A spinless, extended Falicov-Kimball model in the presence of a perpendicular magnetic field is investigated employing a self-consistent mean-field theory in two dimensions. In the presence of the field the excitonic average Δ = is modified: the exciton responds in subtle different ways for different values of the magnetic flux. We examine the effects of Coulomb interaction and hybridization between the localized and itinerant electrons on the excitonic average, for rational values of the applied magnetic field. The excitonic average is found to get enhanced exponentially with the Coulomb interaction while it saturates at large hybridization. The orbital magnetic field suppresses the excitonic average in general, though a strong commensurability effect of the magnetic flux on the behaviour of the excitonic order parameter is observed.

  10. Role of strain on the coherent properties of GaAs excitons and biexcitons

    Science.gov (United States)

    Wilmer, Brian L.; Webber, Daniel; Ashley, Joseph M.; Hall, Kimberley C.; Bristow, Alan D.

    2016-08-01

    Polarization-dependent two-dimensional Fourier-transform spectroscopy (2DFTS) is performed on excitons in strained bulk GaAs layers, probing the coherent response for differing amounts of strain. Uniaxial tensile strain lifts the degeneracy of heavy-hole (HH) and light-hole (LH) valence states, leading to an observed splitting of the associated excitons at low temperature. Increasing the strain increases the magnitude of the HH/LH exciton peak splitting, induces an asymmetry in the off-diagonal interaction coherences, increases the difference in the HH and LH exciton homogenous linewidths, and increases the inhomogeneous broadening of both exciton species. All results arise from strain-induced variations in the local electronic environment, which is not uniform along the growth direction of the thin layers. For cross-linear polarized excitation, wherein excitonic signals give way to biexcitonic signals, the high-strain sample shows evidence of bound LH, HH, and mixed biexcitons.

  11. Theory for electric dipole superconductivity with an application for bilayer excitons.

    Science.gov (United States)

    Jiang, Qing-Dong; Bao, Zhi-qiang; Sun, Qing-Feng; Xie, X C

    2015-07-08

    Exciton superfluid is a macroscopic quantum phenomenon in which large quantities of excitons undergo the Bose-Einstein condensation. Recently, exciton superfluid has been widely studied in various bilayer systems. However, experimental measurements only provide indirect evidence for the existence of exciton superfluid. In this article, by viewing the exciton in a bilayer system as an electric dipole, we derive the London-type and Ginzburg-Landau-type equations for the electric dipole superconductors. By using these equations, we discover the Meissner-type effect and the electric dipole current Josephson effect. These effects can provide direct evidence for the formation of the exciton superfluid state in bilayer systems and pave new ways to drive an electric dipole current.

  12. Rapid determination of memantine in human plasma by using nanoring carboxyl-functionalized paramagnetic molecularly imprinted polymer d-μ-SPE and UFLC-MS/MS.

    Science.gov (United States)

    Qiu, Hai-Wen; Xia, Lei; Gong, Li-Min; Ruan, Lie-Min; Zhao, Yong-Gang

    2015-06-01

    A novel, simple, and sensitive method based on the use of dispersive micro-solid-phase extraction (d-μ-SPE) procedure combined with ultra-fast liquid chromatography-tandem quadrupole mass spectrometry (UFLC-MS/MS) for the determination of memantine (ME) was developed and validated over the linearity range 0.05-10.0 µg/L with 100 μL of human plasma using memantine-D6 (ME-D6) as the internal standard. The novel nanoring carboxyl-functionalized paramagnetic molecularly imprinted polymer (NR-CF-Mag-MIP) was synthesized by ultrasound-assisted suspension polymerization, using ME as a template molecule, methacrylic acid as a functional monomer, and divinylbenzene as a cross-linking agent. The NR-CF-Mag-MIP was used as the d-μ-SPE sorbent to extract ME from human plasma samples. The obtained results demonstrated the higher extraction capacity of NR-CF-Mag-MIP with recoveries between 97.6 and 101%. The limits of quantification (LOQs) for ME was 0.015 µg/L. Validation results on linearity, specificity, accuracy, precision, and stability, as well as on application to the analysis of samples taken up to 480 h after oral administration of 20 mg (two 10 mg capsules) of ME in healthy volunteers demonstrated the applicability to bioequivalence studies.

  13. Temperature dependence of excitonic transition in ZnSe/ZnCdSe quantum wells

    Institute of Scientific and Technical Information of China (English)

    GUO Zi-zheng; LIANG Xi-xia; BAN Shi-liang

    2005-01-01

    A theoretical calculation for the temperature dependence of the excitonic transition in ZnSe/ZnCdSe quantum wells is performed. The exciton binding energy is calculated with a variational technique by considering the temperature-dependence parameters. Our results show that the exciton binding energy reduces linearly with temperature increasing. We find that the strain due to lattice mismatch and differential thermal expansion decreases with the temperature increasing.

  14. Collective Behavior of a Spin-Aligned Gas of Interwell Excitons in Double Quantum Wells

    DEFF Research Database (Denmark)

    Larionov, A. V.; Bayer, M.; Hvam, Jørn Märcher;

    2005-01-01

    The kinetics of a spin-aligned gas of interwell excitons in GaAs/AlGaAs double quantum wells (n–i–n heterostructure) is studied. The temperature dependence of the spin relaxation time for excitons, in which a photoexcited electron and hole are spatially separated between two adjacent quantum wells...... is associated with indirect evidence of the coherence of the collective phase of interwell excitons at temperatures below the critical value....

  15. Spatial mapping of exciton lifetimes in single ZnO nanowires

    Directory of Open Access Journals (Sweden)

    J. S. Reparaz

    2013-07-01

    Full Text Available We investigate the spatial dependence of the exciton lifetimes in single ZnO nanowires. We have found that the free exciton and bound exciton lifetimes exhibit a maximum at the center of nanowires, while they decrease by 30% towards the tips. This dependence is explained by considering the cavity-like properties of the nanowires in combination with the Purcell effect. We show that the lifetime of the bound-excitons scales with the localization energy to the power of 3/2, which validates the model of Rashba and Gurgenishvili at the nanoscale.

  16. Exciton binding energy in GaAsBiN spherical quantum dot heterostructures

    Science.gov (United States)

    Das, Subhasis; Dhar, S.

    2017-03-01

    The ground state exciton binding energies (EBE) of heavy hole excitons in GaAs1-x-yBixNy - GaAs spherical quantum dots (QD) are calculated using a variational approach under 1s hydrogenic wavefunctions within the framework of effective mass approximation. Both the nitrogen and the bismuth content in the material are found to affect the binding energy, in particular for larger nitrogen content and lower dot radii. Calculations also show that the ground state exciton binding energies of heavy holes increase more at smaller dot sizes as compared to that for the light hole excitons.

  17. Singlet Exciton Lifetimes in Conjugated Polymer Films for Organic Solar Cells

    Directory of Open Access Journals (Sweden)

    Stoichko D. Dimitrov

    2016-01-01

    Full Text Available The lifetime of singlet excitons in conjugated polymer films is a key factor taken into account during organic solar cell device optimization. It determines the singlet exciton diffusion lengths in polymer films and has a direct impact on the photocurrent generation by organic solar cell devices. However, very little is known about the material properties controlling the lifetimes of singlet excitons, with most of our knowledge originating from studies of small organic molecules. Herein, we provide a brief summary of the nature of the excited states in conjugated polymer films and then present an analysis of the singlet exciton lifetimes of 16 semiconducting polymers. The exciton lifetimes of seven of the studied polymers were measured using ultrafast transient absorption spectroscopy and compared to the lifetimes of seven of the most common photoactive polymers found in the literature. A plot of the logarithm of the rate of exciton decay vs. the polymer optical bandgap reveals a medium correlation between lifetime and bandgap, thus suggesting that the Energy Gap Law may be valid for these systems. This therefore suggests that small bandgap polymers can suffer from short exciton lifetimes, which may limit their performance in organic solar cell devices. In addition, the impact of film crystallinity on the exciton lifetime was assessed for a small bandgap diketopyrrolopyrrole co-polymer. It is observed that the increase of polymer film crystallinity leads to reduction in exciton lifetime and optical bandgap again in agreement with the Energy Gap Law.

  18. Transport of dipolar excitons in (Al,Ga)N/GaN quantum wells

    Science.gov (United States)

    Fedichkin, F.; Andreakou, P.; Jouault, B.; Vladimirova, M.; Guillet, T.; Brimont, C.; Valvin, P.; Bretagnon, T.; Dussaigne, A.; Grandjean, N.; Lefebvre, P.

    2015-05-01

    We investigate the transport of dipolar indirect excitons along the growth plane of polar (Al,Ga)N/GaN quantum well structures by means of spatially and time-resolved photoluminescence spectroscopy. The transport in these strongly disordered quantum wells is activated by dipole-dipole repulsion. The latter induces an emission blue shift that increases linearly with exciton density, whereas the radiative recombination rate increases exponentially. Under continuous, localized excitation, we observe continuously decreasing emission energy, as excitons propagate away from the excitation spot. This corresponds to a steady-state gradient of exciton density, measured over several tens of micrometers. Time-resolved microphotoluminescence experiments provide information on the dynamics of recombination and transport of dipolar excitons. We account for the ensemble of experimental results by solving the nonlinear drift-diffusion equation. Quantitative analysis suggests that in such structures, exciton propagation on the scale of 10 to 20 μ m is mainly driven by diffusion, rather than by drift, due to the strong disorder and the presence of nonradiative defects. Secondary exciton creation, most probably by the intense higher-energy luminescence, guided along the sample plane, is shown to contribute to the exciton emission pattern on the scale up to 100 μ m . The exciton propagation length is strongly temperature dependent, the emission being quenched beyond a critical distance governed by nonradiative recombination.

  19. Effects of Electric and Magnetic Fields on Pure Dephasing of Exciton Qubits

    Institute of Scientific and Technical Information of China (English)

    LIU Yun-Fei; XIAO Jing-Lin

    2009-01-01

    In a two-dimensional quantum dot (QD) with parabolic confinement potential, we investigate pure dephasing due to deformation potential exciton-bulk longitudinal acoustic phonons (LAP) interaction for exciton qubits under the influence of external static electric and magnetic fields by adopting the full quantum-mechanical method of Kunihiro Kojima and Akihisa Tomita. The wave function is found and the dependence of the pure dephusing factor on the confinement length of the QD and time and temperature is discussed. We find the external electric and magnetic fields have important effects on pure dephasing of exciton qubits because exciton-LAP interaction increases, leading to more pure dephasing.

  20. Excitonic optical nonlinearities and transport in the layered compound semiconductor GaSe

    DEFF Research Database (Denmark)

    Mizeikis, V.; Vadim, Lyssenko; Østergaard, John Erland;

    1995-01-01

    Dephasing and transient grating experiments in the direct excitonic absorption region of GaSe at low temperatures show that a fast relaxation within the one-dimensionally disordered excitonic band results in band filling being the dominant mechanism of the optical nonlinearity. Correspondingly, we...... observe a blueshift of the nonlinear signal with excitation density. The temperature dependence of the exciton diffusion constant measured in directions parallel to the GaSe layer planes indicates that temperature-independent scattering (trapping) and scattering by acoustic phonons determine the exciton...

  1. Singlet Exciton Lifetimes in Conjugated Polymer Films for Organic Solar Cells

    KAUST Repository

    Dimitrov, Stoichko

    2016-01-13

    The lifetime of singlet excitons in conjugated polymer films is a key factor taken into account during organic solar cell device optimization. It determines the singlet exciton diffusion lengths in polymer films and has a direct impact on the photocurrent generation by organic solar cell devices. However, very little is known about the material properties controlling the lifetimes of singlet excitons, with most of our knowledge originating from studies of small organic molecules. Herein, we provide a brief summary of the nature of the excited states in conjugated polymer films and then present an analysis of the singlet exciton lifetimes of 16 semiconducting polymers. The exciton lifetimes of seven of the studied polymers were measured using ultrafast transient absorption spectroscopy and compared to the lifetimes of seven of the most common photoactive polymers found in the literature. A plot of the logarithm of the rate of exciton decay vs. the polymer optical bandgap reveals a medium correlation between lifetime and bandgap, thus suggesting that the Energy Gap Law may be valid for these systems. This therefore suggests that small bandgap polymers can suffer from short exciton lifetimes, which may limit their performance in organic solar cell devices. In addition, the impact of film crystallinity on the exciton lifetime was assessed for a small bandgap diketopyrrolopyrrole co-polymer. It is observed that the increase of polymer film crystallinity leads to reduction in exciton lifetime and optical bandgap again in agreement with the Energy Gap Law.

  2. On the binding energies of excitons in polar quantum well structures in a weak electric field

    Institute of Scientific and Technical Information of China (English)

    Wu Yun-Feng; Liang Xi-Xia; K. K. Bajaj

    2005-01-01

    The binding energies of excitons in quantum well structures subjected to an applied uniform electric field by taking into account the exciton longitudinal optical phonon interaction is calculated. The binding energies and corresponding Stark shifts for Ⅲ-Ⅴ and Ⅱ-Ⅵ compound semiconductor quantum well structures have been numerically computed.The results for GaAs/AlGaAs and ZnCdSe/ZnSe quantum wells are given and discussed. Theoretical results show that the exciton-phonon coupling reduces both the exciton binding energies and the Stark shifts by screening the Coulomb interaction. This effect is observable experimentally and cannot be neglected.

  3. Dephasing in the quasi-two-dimensional exciton-biexciton system

    DEFF Research Database (Denmark)

    Langbein, Wolfgang Werner; Hvam, Jørn Märcher

    2000-01-01

    The polarization decay in the exciton-biexciton system of a homogeneously broadened single quantum well is studied by transient four-wave mixing. All three decay rates in the exciton-biexciton three-level system are deduced. The relation between the rates unravels correlations between scattering...... processes of excitons and biexcitons. Density and temperature dependences show that the involved processes are mainly radiative decay and phonon scattering. The radiative decay rate of the biexcitons is found to be comparable to the one of the excitons, and the involved spontaneous photon emissions from...

  4. Exciton dynamics and non-linearities in two-dimensional hybrid organic perovskites

    Science.gov (United States)

    Abdel-Baki, K.; Boitier, F.; Diab, H.; Lanty, G.; Jemli, K.; Lédée, F.; Garrot, D.; Deleporte, E.; Lauret, J. S.

    2016-02-01

    Due to their high potentiality for photovoltaic applications or coherent light sources, a renewed interest in hybrid organic perovskites has emerged for few years. When they are arranged in two dimensions, these materials can be considered as hybrid quantum wells. One consequence of the unique structure of 2D hybrid organic perovskites is a huge exciton binding energy that can be tailored through chemical engineering. We present experimental investigations of the exciton non-linearities by means of femtosecond pump-probe spectroscopy. The exciton dynamics is fitted with a bi-exponential decay with a free exciton life-time of ˜100 ps. Moreover, an ultrafast intraband relaxation (energy.

  5. Anomalous Photoluminescence of Weakly Confined Excitons including Radiative Correction in Nano-to-Bulk Crossover Regime

    Science.gov (United States)

    Matsuda, Takuya; Yokoshi, Nobuhiko; Ishihara, Hajime

    2015-06-01

    We develop a theoretical formalism to calculate photoluminescence (PL) spectrum of weakly confined excitons incorporating the microscopic nonlocal optical response. The nonlocality is caused by the center-of-mass (c. m.) motion of exciton and becomes remarkable in nano-to-bulk crossover regime. The theory successfully explains the characteristics of recently observed peculiar PL spectra in high quality CuCl films [5], wherein the signals appear at the exciton states with the very large radiative corrections not only for the lowest level but also for the higher ones including non-dipole types of excitons.

  6. On the kinetics and thermodynamics of excitons at the surface of semiconductor nanocrystals: Are there surface excitons?

    Energy Technology Data Exchange (ETDEWEB)

    Kambhampati, Patanjali, E-mail: pat.kambhampati@mcgill.ca

    2015-01-13

    Highlights: • The surface of semiconductor nanocrystals is one of their defining features. • The kinetics of surface trapping can be monitored by pump/probe spectroscopy. • The thermodynamics of surface trapping is revealed by photoluminescence spectroscopy. • We produce the first microscopic picture of how excitons are coupled to the surface. • We discuss the possibility of surface excitons in nanocrystals. - Abstract: The surface of semiconductor nanocrystals is one of their defining features by virtue of their nanometer size. Yet the surface is presently among the most poorly understood aspects of nanocrystal science. This perspective provides an overview of spectroscopic work that has revealed the first insights into the nature of the surface, focusing upon CdSe nanocrystals. We focus on two aspects of surface processes in nanocrystals: the kinetics of surface trapping and the thermodynamics of core/surface equilibria. We describe femtosecond pump/probe spectroscopic experiments which reveal the signatures of carrier trapping at the surface. We also describe temperature dependent steady-state photoluminescence experiments which reveal new aspects of the surface. This work suggest that the surface emission is largely driven by homogeneous broadening via phonon progressions. The implications are that the surface electronic state bears similarity to the quantized excitonic core of the nanocrystal.

  7. Spectroscopy of Optical Excitations in Carbon Nanotubes

    Science.gov (United States)

    Ma, Yingzhong

    2006-03-01

    Understanding the optical spectra and electronic excited state dynamics of carbon naotubes is important both for fundamental research and a wide variety of potential applications. In this presentation, we will report the results of a systematic study on semiconducting single-walled carbon nanotubes (SWNTs) obtained by utilizing complementary femtosecond spectroscopic techniques, including fluorescence up-conversion, frequency-resolved transient absorption, and three-pulse photon echo peakshift (3PEPS) spectroscopy. Our efforts have focused on optically selective detection of the spectra and dynamics associated with structurally distinct semiconducting SWNT species. Using individual nanotube enriched micelle-dispersed SWNT preparations, in combination with resonant excitation and detection, has enabled us to independently access selected species, such as the (8,3), (6,5), (7,5), (11,0), (7,6) and (9,5) nanotubes. We will discuss the following topics: (1) the excitonic nature of the elementary excitation and its unambiguous identification from direct determination of the exciton binding energy for a selected semiconducting nanotube, the (8,3) tube; (2) the spectroscopic and dynamical signatures of exciton-exciton annihilation and its predominant role in governing ultrafast excited state relaxation; (3) the annihilation-concomitant exciton dissociation and the spectroscopic and dynamic features of the resulting electron-hole continuum; (4) timescales characterizing the ultrafast thermalization processes. In addition, we will demonstrate the power of 3PEPS spectroscopy to elucidate the spectral properties and dynamics of SWNTs. This work was supported by the NSF.

  8. Radiative recombination of localized excitons and mobility edge excitons in GaInNAs/GaAs quantum wells with strong carrier localization

    Energy Technology Data Exchange (ETDEWEB)

    Zhao, Q.X. [Physical Electronics and Photonics, Department of Physics, Chalmers University of Technology and Goeteborg University, SE-412 96 Goeteborg (Sweden)]. E-mail: zhao@fly.chalmers.se; Wang, S.M. [Photonics Laboratory, Department of Microtechnology and Nanoscience, Chalmers University of Technology, SE-412 96 Goeteborg (Sweden); Wei, Y.Q. [Photonics Laboratory, Department of Microtechnology and Nanoscience, Chalmers University of Technology, SE-412 96 Goeteborg (Sweden); Sadeghi, M. [Photonics Laboratory, Department of Microtechnology and Nanoscience, Chalmers University of Technology, SE-412 96 Goeteborg (Sweden); Larsson, A. [Photonics Laboratory, Department of Microtechnology and Nanoscience, Chalmers University of Technology, SE-412 96 Goeteborg (Sweden); Willander, M. [Physical Electronics and Photonics, Department of Physics, Chalmers University of Technology and Goeteborg University, SE-412 96 Goeteborg (Sweden)

    2005-06-20

    The radiative recombination in In{sub x}Ga{sub 1-x}N{sub 0.01}As{sub 0.99}/GaAs quantum well structures exhibiting strong carrier localization was investigated by optical spectroscopy. For In-concentration from 0 to 30%, the results indicate that the degree of carrier localization decreases with increasing In-concentration. At temperatures below 100 K, the mobility edge excitons as well as localized excitons are identified and their transitions energies strongly depend on the excitation intensity. At elevated temperatures the localized excitons become quenched. The temperature dependence of the photoluminescence emission energy shows different behaviors at different excitation intensities.

  9. 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

  10. PREFACE: International Conference on Optics of Excitons in Confined Systems

    Science.gov (United States)

    Viña, Luis; Tejedor, Carlos; Calleja, José M.

    2010-01-01

    The OECS11 (International Conference on Optics of Excitons in Confined Systems) was the eleventh of a very successful series of conferences that started in 1987 in Rome (Italy). Afterwards the conference was held at Naxos (Sicily, Italy, 1991), Montpellier (France, 1993), Cortona (Italy, 1995), Göttingen (Germany, 1997), Ascona (Switzerland, 1999), Montpellier (France, 2001), Lecce (Italy, 2003), Southampton (UK, 2005) and Patti (Sicily, Italy, 2007). It is addressed to scientists who lead fundamental and applied research on the optical properties of excitons in novel condensed-matter nanostructures. The 2009 meeting (7-11 September 2009) has brought together a large representation of the world leading actors in this domain, with the aim of stimulating the exchange of ideas, promoting international collaborations, and coordinating research on the newest exciton-related issues such as quantum information science and exciton quantum-collective phenomena. The meeting has included invited lectures, contributed oral presentations and posters, covering the following general topics: low-dimensional heterostructures: quantum wells, quantum wires and quantum dots polaritons quantum optics with excitons and polaritons many-body effects under coherent and incoherent excitation coherent optical spectroscopy quantum coherence and quantum-phase manipulation Bose-Einstein condensation and other collective phenomena excitons in novel materials The OECS 11 was held at the campus of the Universidad Autónoma de Madrid in Cantoblanco. The scientific program was composed of more than 200 contributions divided into 16 invited talks, 44 oral contributions and 3 poster sessions with a total of 150 presentations. The scientific level of the presentations was guaranteed by a selection process where each contribution was rated by three members of the Program Committee. The Conference has gathered 238 participants from 21 different countries, with the following distribution: Germany (43

  11. Exciton-polariton trapping and potential landscape engineering

    Science.gov (United States)

    Schneider, C.; Winkler, K.; Fraser, M. D.; Kamp, M.; Yamamoto, Y.; Ostrovskaya, E. A.; Höfling, S.

    2017-01-01

    Exciton-polaritons in semiconductor microcavities have become a model system for the studies of dynamical Bose-Einstein condensation, macroscopic coherence, many-body effects, nonclassical states of light and matter, and possibly quantum phase transitions in a solid state. These low-mass bosonic quasiparticles can condense at comparatively high temperatures up to 300 K, and preserve the fundamental properties of the condensate, such as coherence in space and time domain, even when they are out of equilibrium with the environment. Although the presence of a confining potential is not strictly necessary in order to observe Bose-Einstein condensation, engineering of the polariton confinement is a key to controlling, shaping, and directing the flow of polaritons. Prototype polariton-based optoelectronic devices rely on ultrafast photon-like velocities and strong nonlinearities exhibited by polaritons, as well as on their tailored confinement. Nanotechnology provides several pathways to achieving polariton confinement, and the specific features and advantages of different methods are discussed in this review. Being hybrid exciton-photon quasiparticles, polaritons can be trapped via their excitonic as well as photonic component, which leads to a wide choice of highly complementary trapping techniques. Here, we highlight the almost free choice of the confinement strengths and trapping geometries that provide powerful means for control and manipulation of the polariton systems both in the semi-classical and quantum regimes. Furthermore, the possibilities to observe effects of the polariton blockade, Mott insulator physics, and population of higher-order energy bands in sophisticated lattice potentials are discussed. Observation of such effects could lead to realization of novel polaritonic non-classical light sources and quantum simulators.

  12. Exciton and Hole-Transfer Dynamics in Polymer: Fullerene Blends

    Directory of Open Access Journals (Sweden)

    van Loosdrecht P. H. M.

    2013-03-01

    Full Text Available Ultrafast hole transfer dynamics from fullerene derivative to polymer in bulk heterojunction blends are studied with visible-pump - IR-probe spectroscopy. The hole transfer process is found to occur in 50/300 fs next to the interface, while a longer 15-ps time is attributed to exciton diffusion towards interface in PC71BM domains. High polaron generation efficiency in P3HT blends indicates excellent intercalation between the polymer and the fullerene even at highest PC71BM concentration thereby yielding a valuable information on the blend morphology.

  13. Soliton physics with semiconductor exciton-polaritons in confined systems

    Science.gov (United States)

    Sich, Maksym; Skryabin, Dmitry V.; Krizhanovskii, Dmitry N.

    2016-10-01

    In the past decade, there has been a significant progress in the study of non-linear polariton phenomena in semiconductor microcavities. One of the key features of non-linear systems is the emergence of solitons. The complexity and the inherently strong nonlinearity of the polariton system made it a perfect sandpit for observing solitonic effects in half-light half-matter environment. This review focuses on the theory and the latest experimental elucidating physics as well as potential applications of conservative and dissipative solitons in exciton-polariton systems. xml:lang="fr"

  14. Surface exciton-polaritons in ternary mixed crystals

    Institute of Scientific and Technical Information of China (English)

    2007-01-01

    The surface exciton-polaritons in ternary mixed crystals are investigated. The numerical calculations for several Ⅲ-Ⅴ and Ⅱ-Ⅵ compound systems are performed and the polariton frequencies as functions of the wave-vector and the compositions for ternary mixed crystals AlxGa1-xAs, CdxZn1-xSe and AlxGa1-xN as examples are given and discussed. The results show that the dependence of the energies of surface polaritons on the composition of ternary mixed crystals are slightly nonlinear different from the bulk modes.

  15. Effects of disorder on the optical properties of Frenkel excitons

    Science.gov (United States)

    Boukahil, Abdelkrim; Zettili, Nouredine

    2002-03-01

    The Coherent Potential Approximation (CPA) is used to study the effects of disorder on the absorption line shapes of Frenkel excitons in one, two, and three dimensions. A Gaussian distribution of transition frequencies with rms width σ was used. The average oscillator strength per state (AOSPS) introduced by Schreiber and Toyozawa is calculated for several values of the disorder parameter σ. The CPA results show that short tails on the high-energy side of the peaks are σ dependent, and long tails on the low-energy side of the peaks do not depend on the disorder parameter σ.

  16. Density of states of Frenkel excitons in weakly disordered systems

    Science.gov (United States)

    Boukahil, Abdelkrim; Zettili, Nouredine

    2002-04-01

    We present the calculation of the density of states of Frenkel excitons in weakly disordered one , two , and three-dimensional systems. A random distribution of transition frequencies with variance s2 characterizes the disorder. The Coherent Potential Approximation (CPA) calculations show that the density of states (DOS) is very sensitive to any variations in the disorder parameter s. Our calculations are in good agreement with previous work based on the Monte Carlo simulation. One of us (AB) acknowldges the support of the University of Wisconsin--Whitewater for this work through a university research grant.

  17. Effects of disorder on the optical properties of Frenkel excitons

    Science.gov (United States)

    Boukahil, Abdelkrim; Siemann, Robert

    2014-03-01

    The Coherent Potential Approximation (CPA) is used to study the effects of disorder on the absorption line shapes of Frenkel excitons in one-, two-, and three-dimensional systems. A Gaussian distribution of transition frequencies with rms width σ was used. Several values of the disorder parameter σ. The CPA results show that short tails on the high-energy side of the peaks are σ dependent, and long tails on the low-energy side of the peaks are independent of the disorder parameter σ.

  18. Tunable Magnetic Alignment between Trapped Exciton-Polariton Condensates

    Science.gov (United States)

    Ohadi, H.; del Valle-Inclan Redondo, Y.; Dreismann, A.; Rubo, Y. G.; Pinsker, F.; Tsintzos, S. I.; Hatzopoulos, Z.; Savvidis, P. G.; Baumberg, J. J.

    2016-03-01

    Tunable spin correlations are found to arise between two neighboring trapped exciton-polariton condensates which spin polarize spontaneously. We observe a crossover from an antiferromagnetic to a ferromagnetic pair state by reducing the coupling barrier in real time using control of the imprinted pattern of pump light. Fast optical switching of both condensates is then achieved by resonantly but weakly triggering only a single condensate. These effects can be explained as the competition between spin bifurcations and spin-preserving Josephson coupling between the two condensates, and open the way to polariton Bose-Hubbard ladders.

  19. Ultrafast exciton formation at the ZnO(1010) surface.

    Science.gov (United States)

    Deinert, J-C; Wegkamp, D; Meyer, M; Richter, C; Wolf, M; Stähler, J

    2014-08-01

    We study the ultrafast quasiparticle dynamics in and below the ZnO conduction band using femtosecond time-resolved two-photon photoelectron spectroscopy. Above band gap excitation causes hot electron relaxation by electron-phonon scattering down to the Fermi level E_{F} followed by ultrafast (200 fs) formation of a surface exciton (SX). Transient screening of the Coulomb interaction reduces the SX formation probability at high excitation densities near the Mott limit. Located just below the surface, the SX are stable with regard to hydrogen-induced work function modifications and thus the ideal prerequisite for resonant energy transfer applications.

  20. An Exciton Bound to a Neutral Donor in Quantum Dots

    Institute of Scientific and Technical Information of China (English)

    解文方

    2002-01-01

    The binding energies for an exciton (X) trapped in a two-dimensional quantum dot by a neutral donor have been calculated using the method of few-body physics for the heavy hole (σ= 0.196) and the light hole (σr = 0.707).We find that the (D0, X) complex confined in a quantum dot has in general a larger binding energy than those in a two-dimensional quantum well and a three-dimensional bulk semiconductor, and the binding energy increases with the decrease of the dot radius. At dot radius R →∞, we compare our calculated result with the previous results.

  1. 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.

  2. Quantum-well thickness dependence of spin polarization of excitons

    Directory of Open Access Journals (Sweden)

    M. Idrish Miah

    2011-07-01

    Full Text Available The optical orientation of exciton spins in semiconductor quantum wells (SQWs was investigated by observing the circular polarization of the photoluminescence (PL. The left/right circularly polarized PL in SQWs was measured. It was found that there is a difference between the two different polarization conditions, which is caused by spin-dependent phase-space filling. The PL polarization was estimated from the signals of the left and right circularly polarized PL and was found to depend on the well thickness of SQWs as well as on the sample temperature. The influence of an electric field on the PL polarization was studied.

  3. Exciton recombination dynamics in single ZnO tetrapods

    Energy Technology Data Exchange (ETDEWEB)

    Fernandes-Silva, Lígia C. [Departamento de Física de Materiales, Universidad Autónoma de Madrid, E-28049 Madrid (Spain); Martín, Maria D.; Meulen, Herko P. van der; Calleja, José M.; Viña, Luis [Departamento de Física de Materiales, Universidad Autónoma de Madrid, E-28049 Madrid, Spain and Instituto de Ciencia de Materiales Nicolás Cabrera, Universidad Autónoma de Madrid, E-28049 Madrid (Spain); Klopotowski, Lukasz [Polish Academy of Sciences, Institute of Physics, 02-668 Warsaw (Poland)

    2013-12-04

    We present the optical properties of individual ZnO tetrapods as a function of excitation power and temperature by time-integrated and time-resolved spectroscopy. At 10K, we identify the different excitonic transitions by both their characteristic energy and their excitation power dependence. When we increase the tetrapod temperature we observe that the emission intensity decrease and occur a red shift of the emission energies. Our time-resolved studies confirm the predominance of the radiative recombination at low temperatures (< 45 K). Increasing the temperature opens up the non-radiative channels, which are evidenced by a much faster decay time.

  4. Exciton recombination dynamics in single ZnO tetrapods

    Science.gov (United States)

    Fernandes-Silva, Lígia C.; Martín, Maria D.; van der Meulen, Herko P.; Klopotowski, Lukasz; Calleja, José M.; Viña, Luis

    2013-12-01

    We present the optical properties of individual ZnO tetrapods as a function of excitation power and temperature by time-integrated and time-resolved spectroscopy. At 10K, we identify the different excitonic transitions by both their characteristic energy and their excitation power dependence. When we increase the tetrapod temperature we observe that the emission intensity decrease and occur a red shift of the emission energies. Our time-resolved studies confirm the predominance of the radiative recombination at low temperatures (< 45 K). Increasing the temperature opens up the non-radiative channels, which are evidenced by a much faster decay time.

  5. Excitons and biexcitons in CuCl nanocrystallites

    Energy Technology Data Exchange (ETDEWEB)

    Hoenerlage, B. [Institut de Physique et Chimie des Materiaux, Strasbourg (France). Groupe d`Optique Nonlineaire et d`Optoelectronique; Levy, R. [Institut de Physique et Chimie des Materiaux, Strasbourg (France). Groupe d`Optique Nonlineaire et d`Optoelectronique; Grun, J.B. [Institut de Physique et Chimie des Materiaux, Strasbourg (France). Groupe d`Optique Nonlineaire et d`Optoelectronique

    1995-06-01

    Because of the important binding energies of excitons and biexcitons in CuCl, these elementary excitations can be treated in the weak confinement regime if excited in semiconductor nanocrystallites. Their optical properties and dynamics are similar to those of CuCl bulk material. Besides the well-known blue shift of resonances due to the confinement and their inhomogeneous broadening due to the size distribution of the nanocrystallites, the main difference between both systems results from surface effects and the lack of translational invariance in nanocrystallites. The latter affects the selection rules of optical transitions and the exchange interaction of the quasiparticules. (orig.).

  6. Ultrafast dynamics of confined and localised excitons and biexcitons in low-dimensional semiconductors

    DEFF Research Database (Denmark)

    Hvam, Jørn Märcher; Langbein, Wolfgang; Borri, Paola

    1999-01-01

    Coherent optical spectroscopy in the form of nonlinear transient four-wave mixing (TFWM) and linear resonant Rayleigh scattering (RRS) has been applied to investigate the exciton dynamics of low-dimensional semiconductor heterostructures. The dephasing times of excitons are determined from...

  7. Influence of exciton-phonon interaction on long energy transport in J-aggregates

    OpenAIRE

    Bartnik, E. A.; Bednarz, M.

    1998-01-01

    This paper presents a theoretical model intended to address the question of energy transfer in two-dimensional molecular assemblies such as Scheibe aggregates. A new phonon-exciton interaction is introduced to explain the exciton width in J aggregates. It is shown that the long range energy transport can occur for weakly interacting acceptors.

  8. Thermal effects in exciton harvesting in biased one-dimensional systems

    NARCIS (Netherlands)

    Vlaming, S. M.; Malyshev, V.A.; Knoester, J.

    2008-01-01

    The study of energy harvesting in chain-like structures is important due to its relevance to a variety of interesting physical systems. Harvesting is understood as the combination of exciton transport through intra-band exciton relaxation (via scattering on phonon modes) and subsequent quenching by

  9. Real-Time Tracking of Singlet Exciton Diffusion in Organic Semiconductors

    NARCIS (Netherlands)

    Kozlov, Oleg V.; de Haan, Foppe; Kerner, Ross A.; Rand, Barry P.; Cheyns, David; Pshenichnikov, Maxim S.

    2016-01-01

    Exciton diffusion in organic materials provides the operational basis for functioning of such devices as organic solar cells and light-emitting diodes. Here we track the exciton diffusion process in organic semiconductors in real time with a novel technique based on femtosecond photoinduced absorpti

  10. 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.

  11. Direct observation of free-exciton thermalization in quantum-well structures

    DEFF Research Database (Denmark)

    Umlauff, M.; Hoffmann, J.; Kalt, H.;

    1998-01-01

    We report on a direct observation of free-exciton thermalization in quantum-well structures. A narrow energy distribution of free 1s excitons is created in ZnSe-based quantum wells by emission of one LO phonon after optical excitation of the continuum stales with picosecond laser pulses. The subs...

  12. Particle-in-a-Box Model of Exciton Absorption and Electroabsorption in Conjugated Polymers

    DEFF Research Database (Denmark)

    Pedersen, Thomas Garm

    2001-01-01

    The recently proposed particle-in-a-box model of one-dimensional excitons in conjugated polymers is applied in calculations of optical absorption and electroabsorption spectra. It is demonstrated that for polymers of long conjugation length a superposition of single exciton resonances produces...

  13. Exciton states in a circular graphene quantum dot: Magnetic field induced intravalley to intervalley transition

    Science.gov (United States)

    Li, L. L.; Zarenia, M.; Xu, W.; Dong, H. M.; Peeters, F. M.

    2017-01-01

    The magnetic-field dependence of the energy spectrum, wave function, binding energy, and oscillator strength of exciton states confined in a circular graphene quantum dot (CGQD) is obtained within the configuration interaction method. We predict that (i) excitonic effects are very significant in the CGQD as a consequence of a combination of geometric confinement, magnetic confinement, and reduced screening; (ii) two types of excitons (intravalley and intervalley) are present in the CGQD because of the valley degree of freedom in graphene; (iii) the intravalley and intervalley exciton states display different magnetic-field dependencies due to the different electron-hole symmetries of the single-particle energy spectra; (iv) with increasing magnetic field, the exciton ground state in the CGQD undergoes an intravalley to intervalley transition accompanied by a change of angular momentum; (v) the exciton binding energy does not increase monotonically with the magnetic field due to the competition between geometric and magnetic confinements; and (vi) the optical transitions of the intervalley and intravalley excitons can be tuned by the magnetic field, and valley-dependent excitonic transitions can be realized in a CGQD.

  14. Direct Measurement of the Triplet Exciton Diffusion Length in Organic Semiconductors

    NARCIS (Netherlands)

    Mikhnenko, Oleksandr V.; Ruiter, Roald; Blom, Paul W. M.; Loi, Maria Antonietta

    2012-01-01

    We present a new method to measure the triplet exciton diffusion length in organic semiconductors. N,N'-di-[(1-naphthyl)-N,N'-diphenyl]-1,1'-biphenyl-4,4'-diamine (NPD) has been used as a model system. Triplet excitons are injected into a thin film of NPD by a phosphorescent thin film, which is opti

  15. Dynamics of the Exciton Screening in CuCl on a Subpicosecond Time Scale

    Science.gov (United States)

    Hulin, D.; Antonetti, A.; Chase, L. L.; Martin, J. L.; Migus, A.; Mysyrowicz, A.; Löwenau, J. P.; Schmitt-Rink, S.; Haug, H.

    1984-02-01

    The dynamics of exciton screening in CuCl, following optical injection of a high-density hot plasma, is studied with subpicosecond resolution. A delayed response for exciton bleaching of ~1 ps is attributed to thermal relaxation of the plasma. The results are compared to a theoretical treatment of the particle density- and temperature-dependent dielectric function.

  16. Excitonic-biexcitonic polariton interference in thin platelet of CuCl

    Science.gov (United States)

    Koinov, Z. G.

    1999-04-01

    The spectral position in Q-space of the transmission maxima of a 0.15 μm thick CuCl single crystal with parallel plates in Z 3-excitonic resonance region, measured by Mita and Nagasawa, has been interpreted as an indication for the mutual interference effect between two propagating excitonic-biexcitonic polariton modes.

  17. Coherent dynamics of interwell excitons in GaAs/AlxGa1-xAs superlattices

    DEFF Research Database (Denmark)

    Mizeikis, V.; Birkedal, Dan; Langbein, Wolfgang Werner;

    1997-01-01

    Coherent exciton dynamics in a GaAs/AlxGa1-xAs narrow-miniband superlattice is studied by spectrally resolved transient four-wave mixing. Coherent optical properties of the investigated structure are found to be strongly affected by the existence of two different heavy-hole excitonic states. One ...

  18. Exciton states and optical absorption in quantum wires under laser radiation

    Energy Technology Data Exchange (ETDEWEB)

    Gonzalez-Santander, C., E-mail: cglezsantander@fis.ucm.e [GISC, Departamento de Fisica de Materiales, Universidad Complutense, E-28040 Madrid (Spain); Dominguez-Adame, F. [GISC, Departamento de Fisica de Materiales, Universidad Complutense, E-28040 Madrid (Spain)

    2010-05-03

    We analyze the exciton states in a quantum wire under intense laser radiation. Electrons and holes are confined by the parabolic potential of the quantum wire. An exactly solvable model is introduced for calculating the exciton binding energy, replacing the actual Coulomb interaction between the electron and the hole by a projective operator.

  19. Dephasing and interaction of excitons CdSe/ZnSe islands

    DEFF Research Database (Denmark)

    Wagner, H. P.; Tranitz, H.-P.; Preis, H.;

    2000-01-01

    The dephasing of excitons in self-organized CdSe/ZnSe islands grown by molecular-beam epitaxy is investigated using spectrally resolved four-wave mixing. A distribution of dephasing times is observed, indicating the existence of localized excitons with different relaxation times at comparable...

  20. The Role of Excitons on Light Amplification in Lead Halide Perovskites.

    Science.gov (United States)

    Lü, Quan; Wei, Haohan; Sun, Wenzhao; Wang, Kaiyang; Gu, Zhiyuan; Li, Jiankai; Liu, Shuai; Xiao, Shumin; Song, Qinghai

    2016-12-01

    The role of excitons on the amplifications of lead halide perovskites has been explored. Unlike the photoluminescence, the intensity of amplified spontaneous emission is partially suppressed at low temperature. The detailed analysis and experiments show that the inhibition is attributed to the existence of exciton and a quantitative model has been built to explain the experimental observations.

  1. Thermalization of Hot Free Excitons in ZnSe-Based Quantum Wells

    DEFF Research Database (Denmark)

    Hoffmann, J.; Umlauff, M.; Kalt, H.;

    1997-01-01

    Thermalization of hot-exciton populations in ZnSe quantum wells occurs on a time scale of 100 ps. Strong exciton-phonon coupling in II-VI semiconductors leads to a direct access to the thermalization dynamics via time-resolved spectroscopy of phonon-assisted luminescence. The experimental spectra...

  2. Coherent spin dynamics of an interwell excitonic gas in GaAs/AlGaAs coupled quantum wells

    DEFF Research Database (Denmark)

    Larionov, A. V.; Bisti, V. E.; Bayer, M.;

    2006-01-01

    The spin dynamics of an interwell exciton gas has been investigated in n-i-n GaAs/AlGaAs coupled quantum wells. The time evolution kinetics of the interwell exciton photoluminescence has been measured under resonant excitation of the 1s heavy-hole intrawell exciton, using a pulsed tunable laser...

  3. Simple Screened Hydrogen Model of Excitons in Two-Dimensional Materials

    DEFF Research Database (Denmark)

    Olsen, Thomas; Latini, Simone; Rasmussen, Filip Anselm;

    2016-01-01

    We present a generalized hydrogen model for the binding energies (EB) and radii of excitons in two-dimensional (2D) materials that sheds light on the fundamental differences between excitons in two and three dimensions. In contrast to the well-known hydrogen model of three-dimensional (3D) excitons...... the recently observed linear scaling of exciton binding energies with band gap. It is also shown that the model accurately reproduces the nonhydrogenic Rydberg series in WS2 and can account for screening from the environment....... that only depends on the excitonic mass and the 2D polarizability α. The model is shown to produce accurate results for 51 transition metal dichalcogenides. Remarkably, over a wide range of polarizabilities the binding energy becomes independent of the mass and we obtain E2DB≈3/(4πα), which explains...

  4. Rayleigh surface wave interaction with the 2D exciton Bose-Einstein condensate

    Energy Technology Data Exchange (ETDEWEB)

    Boev, M. V.; Kovalev, V. M., E-mail: vadimkovalev@isp.nsc.ru [Russian Academy of Sciences, Institute of Semiconductor Physics, Siberian Branch (Russian Federation)

    2015-06-15

    We describe the interaction of a Rayleigh surface acoustic wave (SAW) traveling on the semiconductor substrate with the excitonic gas in a double quantum well located on the substrate surface. We study the SAW attenuation and its velocity renormalization due to the coupling to excitons. Both the deformation potential and piezoelectric mechanisms of the SAW-exciton interaction are considered. We focus on the frequency and excitonic density dependences of the SAW absorption coefficient and velocity renormalization at temperatures both above and well below the critical temperature of Bose-Einstein condensation of the excitonic gas. We demonstrate that the SAW attenuation and velocity renormalization are strongly different below and above the critical temperature.

  5. Suppression of space broadening of exciton polariton beams by Bloch oscillation effects

    CERN Document Server

    Duan, Xudong; Zhang, Yongyou

    2015-01-01

    We theoretically study the transport of exciton polaritons under different applied photon potentials. The relation between the photon potentials and the thickness of the cavity layer is calculated by the finite element simulation. The theoretical analysis and numerical calculation indicate that the cavity photon potential is proportional to the thickness of the cavity layer with the coefficient being about $1.8$ meV/nm. Further, the periodic and linear photon potentials are considered to control the transport of the exciton polaritons in weak- and strong-field pump situations. In both situations the periodic potential cannot by itself effectively suppress the scatterings of the disorder potentials of the cavity photons and excitons and the nonlinear exciton-exciton interaction. When the linear potential is added to the cavity photons, the polariton transport exhibits the Bloch oscillation behavior. Importantly, the polariton Bloch oscillation can strongly suppress the space broadening due to the disorder pote...

  6. 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.

  7. Low-Energy Excitation Spectra in the Excitonic Phase of Cobalt Oxides

    Science.gov (United States)

    Yamaguchi, Tomoki; Sugimoto, Koudai; Ohta, Yukinori

    2017-04-01

    We study the excitonic phase and low-energy excitation spectra of perovskite cobalt oxides. Constructing the five-orbital Hubbard model defined on the three-dimensional cubic lattice for the 3d bands of Pr0.5Ca0.5CoO3, we calculate the excitonic susceptibility in the normal state in the random-phase approximation (RPA) to show the presence of the instability toward excitonic condensation. On the basis of the excitonic ground state with a magnetic multipole obtained in the mean-field approximation, we calculate the dynamical susceptibility of the excitonic phase in the RPA and find that there appear a gapless collective excitation in the spin-transverse mode (Goldstone mode) and a gapful collective excitation in the spin-longitudinal mode (Higgs mode). The experimental relevance of our results is discussed.

  8. Nanophotonic interactions between organic excitons and plasmonic metasurfaces (Conference Presentation)

    Science.gov (United States)

    O'Carroll, Deirdre M.

    2016-09-01

    Thin-film organic semiconductor materials are emerging as energy-efficient, versatile alternatives to inorganic semiconductors for display and solid-state lighting applications. Additionally, thin-film organic laser and photovoltaic technologies, while not yet competitive with inorganic semiconductor-based analogues, can exhibit small device embodied energies (due to comparatively low temperature and low energy-use fabrication processes) which is of interest for reducing overall device cost. To improve energy conversion efficiency in thin-film organic optoelectronics, light management using nanophotonic structures is necessary. Here, our recent work on improving light trapping and light extraction in organic semiconductor thin films using nanostructured silver plasmonic metasurfaces will be presented [1,2]. Numerous optical phenomena, such as absorption induced scattering, out-of-plane waveguiding and morphology-dependent surface plasmon outcoupling, are identified due to exciton-plasmon coupling between the organic semiconductor and the metasurface. Interactions between localized and propagating surface plasmon polaritons and the excitonic transitions of a variety of organic conjugated polymer materials will be discussed and ways in which these interactions may be optimized for particular optoelectronic applications will be presented. [1] C. E. Petoukhoff, D. M. O'Carroll, Absorption-Induced Scattering and Surface Plasmon Out-Coupling from Absorber-Coated Plasmonic Metasurfaces. Nat. Commun. 6, 7899-1-13 (2015). [2] Z. Shen, D. M. O'Carroll, Nanoporous Silver Thin Films: Multifunctional Platforms for Influencing Chain Morphology and Optical Properties of Conjugated Polymers. Adv. Funct. Mater. 25, 3302-3313 (2015).

  9. 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.

  10. Quantum process tomography quantifies coherence transfer dynamics in vibrational exciton.

    Science.gov (United States)

    Chuntonov, Lev; Ma, Jianqiang

    2013-10-31

    Quantum coherence has been a subject of great interest in many scientific disciplines. However, detailed characterization of the quantum coherence in molecular systems, especially its transfer and relaxation mechanisms, still remains a major challenge. The difficulties arise in part because the spectroscopic signatures of the coherence transfer are typically overwhelmed by other excitation-relaxation processes. We use quantum process tomography (QPT) via two-dimensional infrared spectroscopy to quantify the rate of the elusive coherence transfer between two vibrational exciton states. QPT retrieves the dynamics of the dissipative quantum system directly from the experimental observables. It thus serves as an experimental alternative to theoretical models of the system-bath interaction and can be used to validate these theories. Our results for coupled carbonyl groups of a diketone molecule in chloroform, used as a benchmark system, reveal the nonsecular nature of the interaction between the exciton and the Markovian bath and open the door for the systematic studies of the dissipative quantum systems dynamics in detail.

  11. Boosting the performance of red PHOLEDs by exciton harvesting

    Science.gov (United States)

    Chang, Y.-L.; Wang, Z. B.; Helander, M. G.; Qiu, J.; Lu, Z. H.

    2012-09-01

    Significant development has been made on phosphorescent organic light emitting diodes (PHOLEDs) over the past decade, which eventually resulted in the commercialization of widely distributed active-matrix organic light emitting diode displays for mobile phones. However, higher efficiency PHOLEDs are still needed to further reduce the cost and lower the power consumption for general lighting and LED backlight applications. In particular, red PHOLEDs currently have in general the lowest efficiencies among the three primary colors, due most likely to the energy-gap law. Therefore, a number of groups have of made use of various device configurations, including insertion of a carrier blocking or exciton confining layer, doping the transport layers, as well as employing multiple emissive zone structures to improve the device efficiency. However, these approaches are rather inconvenient for commercial applications. In this work, we have developed a simpler way to boost the performance of red PHOLEDs by incorporating an exciton harvesting green emitter, which transfers a large portion of the energy to the co-deposited red emitter. A high external quantum efficiency (EQE) of 20.6% was achieved, which is among the best performances for red PHOLEDs.

  12. 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.

  13. Efficient Multiple Exciton Generation Observed in Colloidal PbSe Quantum Dots with Temporally and Spectrally Resolved Intraband Excitation

    KAUST Repository

    Ji, Minbiao

    2009-03-11

    We have spectrally resolved the intraband transient absorption of photogenerated excitons to quantify the exciton population dynamics in colloidal PbSe quantum dots (QDs). These measurements demonstrate that the spectral distribution, as well as the amplitude, of the transient spectrum depends on the number of excitons excited in a QD. To accurately quantify the average number of excitons per QD, the transient spectrum must be spectrally integrated. With spectral integration, we observe efficient multiple exciton generation In colloidal PbSe QDs. © 2009 American Chemical Society.

  14. Collective State of Interwell Excitons in GaAs/AlGaAs Double Quantum Wells under Pulse Resonance Excitation

    DEFF Research Database (Denmark)

    Larionov, A. V.; Timofeev, V. B.; Hvam, Jørn Märcher

    2002-01-01

    The time evolution and kinetics of photoluminescence (PL) spectra of interwell excitons in double GaAs/AlGaAs quantum wells (n–i–n structures) have been investigated under the pulse resonance excitation of intrawell 1sHH excitons using a pulsed tunable laser. It is found that the collective exciton......, and a significant increase in the radiative decay rate of the condensed phase. The collective exciton phase arises at temperatures T properties of the collective phase of interwell excitons and experimental manifestations of this coherence...

  15. Excitonic pairing and insulating transition in two-dimensional semi-Dirac semimetals

    Science.gov (United States)

    Wang, Jing-Rong; Liu, Guo-Zhu; Zhang, Chang-Jin

    2017-02-01

    A sufficiently strong long-range Coulomb interaction can induce excitonic pairing in gapless Dirac semimetals, which generates a finite gap and drives the semimetal-insulator quantum phase transition. This phenomenon is in close analogy to dynamical chiral symmetry breaking in high-energy physics. In most realistic Dirac semimetals, including suspended graphene, the Coulomb interaction is too weak to open an excitonic gap. The Coulomb interaction plays a more important role at low energies in a two-dimensional semi-Dirac semimetal, in which the fermion spectrum is linear in one component of momenta and quadratic in the other, than a Dirac semimetal, and indeed leads to breakdown of Fermi liquid theory. We study dynamical excitonic gap generation in a two-dimensional semi-Dirac semimetal by solving the Dyson-Schwinger equation, and show that a moderately strong Coulomb interaction suffices to induce excitonic pairing. Additional short-range four-fermion coupling tends to promote excitonic pairing. Among the available semi-Dirac semimetals, we find that the TiO2/VO2 nanostructure provides a promising candidate for the realization of an excitonic insulator. We also apply the renormalization group method to analyze the strong coupling between the massless semi-Dirac fermions and the quantum critical fluctuation of the excitonic order parameter at the semimetal-insulator quantum critical point, and reveal non-Fermi liquid behaviors of semi-Dirac fermions.

  16. Exciton dynamics and non-linearities in two-dimensional hybrid organic perovskites

    Energy Technology Data Exchange (ETDEWEB)

    Abdel-Baki, K.; Boitier, F.; Diab, H.; Lanty, G.; Jemli, K.; Lédée, F.; Deleporte, E.; Lauret, J. S., E-mail: jean-sebastien.lauret@lac.u-psud.fr [Laboratoire Aimé Cotton, CNRS, Univ. Paris-Sud, ENS Cachan, Université Paris-Saclay, 91405 Orsay Cedex (France); Garrot, D. [GEMAC, CNRS, UVSQ, Université Paris-Saclay, 45 avenue des États Unis 78035 Versailles Cedex (France)

    2016-02-14

    Due to their high potentiality for photovoltaic applications or coherent light sources, a renewed interest in hybrid organic perovskites has emerged for few years. When they are arranged in two dimensions, these materials can be considered as hybrid quantum wells. One consequence of the unique structure of 2D hybrid organic perovskites is a huge exciton binding energy that can be tailored through chemical engineering. We present experimental investigations of the exciton non-linearities by means of femtosecond pump-probe spectroscopy. The exciton dynamics is fitted with a bi-exponential decay with a free exciton life-time of ∼100 ps. Moreover, an ultrafast intraband relaxation (<150 fs) is also reported. Finally, the transient modification of the excitonic line is analyzed through the moment analysis and described in terms of reduction of the oscillator strength and linewidth broadening. We show that excitonic non-linearities in 2D hybrid organic perovskites share some behaviours of inorganic semiconductors despite their high exciton binding energy.

  17. Calculation of Excitonic Transitions in ZnO/MgZnO Quantum-Well Heterostructures

    Institute of Scientific and Technical Information of China (English)

    徐天宁; 吴惠桢; 邱东江; 陈乃波

    2003-01-01

    We calculate the excitonic transition energies and exciton binding energies in ZnO/MgxZn1-xO quantum-well heterostructures with Mg composition x varied from 0.08 to 0.36. The effect of the exciton-phonon interaction on the exciton binding energies is taken into account in the model. For the ZnO/Mg0.12Zn0.88O quantum-well structure, we compare the calculated result with the available experimental data at 5 K, and a good agreement is achieved. The excitonic transition energies at room temperature in ZnO/MgxZn1-xO quantum-well heterostructures are also calculated. The results show that when the well width exceeds 50 A, the quantum size effect is neglectable and the excitonic transition energies in ZnO/MgxZn1-xO (with x varied from 0.08 to 0.36)quantum-well heterostructures are close to the value of bulk ZnO. The maximum exciton binding energy as large as 121.1 meV is obtained for the well width of 12.5 A in the ZnO/Mg0.36Zn0.64O quantum-well heterostructures.

  18. Excitons into one-axis crystals of zinc phosphide (Zn3P2

    Directory of Open Access Journals (Sweden)

    D.M. Stepanchikov

    2009-01-01

    Full Text Available Theoretical study of excitons spectra is offered in this report as for Zn3P2 crystals. Spectra are got in the zero approach of the theory of perturbations with consideration of both the anisotropy of the dispersion law and the selection rules. The existence of two exciton series was found, which corresponds to two valence bands (hh, lh and the conductivity band (c. It is noteworthy that anisotropy of the dispersion law plus the existence of crystalline packets (layers normal to the main optical axis, both will permit the consideration of two-dimensional excitons too. The high temperature displaying of these 2D-exciton effects is not eliminated even into bulk crystals. The calculated values of the binding energies as well as the oscillator's strength for the optical transitions are given for a volume (3D and for two-dimensional (2D excitons. The model of energy exciton transitions and four-level scheme of stimulated exciton radiation for receiving laser effect are offered.

  19. Intrinsic homogeneous linewidth and broadening mechanisms of excitons in monolayer transition metal dichalcogenides

    KAUST Repository

    Moody, Galan

    2015-09-18

    The band-edge optical response of transition metal dichalcogenides, an emerging class of atomically thin semiconductors, is dominated by tightly bound excitons localized at the corners of the Brillouin zone (valley excitons). A fundamental yet unknown property of valley excitons in these materials is the intrinsic homogeneous linewidth, which reflects irreversible quantum dissipation arising from system (exciton) and bath (vacuum and other quasiparticles) interactions and determines the timescale during which excitons can be coherently manipulated. Here we use optical two-dimensional Fourier transform spectroscopy to measure the exciton homogeneous linewidth in monolayer tungsten diselenide (WSe2). The homogeneous linewidth is found to be nearly two orders of magnitude narrower than the inhomogeneous width at low temperatures. We evaluate quantitatively the role of exciton–exciton and exciton–phonon interactions and population relaxation as linewidth broadening mechanisms. The key insights reported here—strong many-body effects and intrinsically rapid radiative recombination—are expected to be ubiquitous in atomically thin semiconductors.

  20. Evolution from the plasmon to exciton state in ligand-protected atomically precise gold nanoparticles

    Science.gov (United States)

    Zhou, Meng; Zeng, Chenjie; Chen, Yuxiang; Zhao, Shuo; Sfeir, Matthew Y.; Zhu, Manzhou; Jin, Rongchao

    2016-10-01

    The evolution from the metallic (or plasmonic) to molecular state in metal nanoparticles constitutes a central question in nanoscience research because of its importance in revealing the origin of metallic bonding and offering fundamental insights into the birth of surface plasmon resonance. Previous research has not been able to probe the transition due to the unavailability of atomically precise nanoparticles in the 1-3 nm size regime. Herein, we investigate the transition by performing ultrafast spectroscopic studies on atomically precise thiolate-protected Au25, Au38, Au144, Au333, Au~520 and Au~940 nanoparticles. Our results clearly map out three distinct states: metallic (size larger than Au333, that is, larger than 2.3 nm), transition regime (between Au333 and Au144, that is, 2.3-1.7 nm) and non-metallic or excitonic state (smaller than Au144, that is, smaller than 1.7 nm). The transition also impacts the catalytic properties as demonstrated in both carbon monoxide oxidation and electrocatalytic oxidation of alcohol.

  1. Symmetry and size effects on energy and entanglement of an exciton in coupled quantum dots

    Institute of Scientific and Technical Information of China (English)

    Shen Man; Bai Yan-Kui; An Xing-Tao; Liu Jian-Jun

    2013-01-01

    We study theoretically the essential properties of an exciton in vertically coupled Gaussian quantum dots in the presence of an extemal magnetic field.The ground state energy of a heavy-hole exciton is split into four energy levels due to the Zeeman effect.For the symmetrical system,the entanglement entropy of the exciton state can reach a value of 1.However,for a system with broken symmetry,it is close to zero.Our results are in good agreement with previous studies.

  2. Numerical simulation of exciton dynamics in cuprous oxide at ultra low temperatures

    Energy Technology Data Exchange (ETDEWEB)

    Som, Sunipa

    2015-06-29

    This thesis is a theoretical investigation of the relaxation behaviour of excitons in Cuprous Oxide at ultra low temperatures when the excitons are confined within a potential trap and also in a homogeneous system. Under the action of deformation potential phonon scattering only, Bose Einstein Condensation (BEC) occurs for all temperatures in the investigated range. In the case of Auger decay, we do not find at any temperature a BEC due to the heating of the exciton gas. In the case of elastic and phonon-scattering together BEC occurs in this case of 0.1 K.

  3. 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%.

  4. Polarised two-photon excitation of quantum well excitons for manipulation of optically pumped terahertz lasers

    Energy Technology Data Exchange (ETDEWEB)

    Slavcheva, G., E-mail: gsk23@bath.ac.uk [Blackett Laboratory, Imperial College London, Prince Consort Road, London SW7 2AZ (United Kingdom); Kavokin, A.V., E-mail: A.Kavokin@soton.ac.uk [School of Physics and Astronomy, University of Southampton, Highfield, Southampton SO17 1BJ (United Kingdom); Spin Optics Laboratory, St. Petersburg State University, 1, Ulyanovskaya 198504 (Russian Federation)

    2014-11-15

    Optical pumping of excited exciton states in a semiconductor quantum well embedded in a microcavity is a tool for realisation of ultra-compact terahertz (THz) lasers based on stimulated optical transition between excited (2p) and ground (1s) exciton state. We show that the probability of two-photon absorption by a 2p-exciton is strongly dependent on the polarisation of both pumping photons. Five-fold variation of the threshold power for terahertz lasing by switching from circular to co-linear pumping is predicted. We identify photon polarisation configurations for achieving maximum THz photon generation quantum efficiency.

  5. Scattering and Recombination of Two Triplet Excitons in polymer light-emitting diodes

    CERN Document Server

    Meng, Y; Liu, X J; Wang, Y D; An, Z

    2010-01-01

    The scattering and recombination processes between two triplet excitons in conjugated polymers are investigated by using a nonadiabatic evolution method, based on an extended Su-Schrieffer-Heeger model including interchain interactions. Due to the interchain coupling, the electron and/or hole in the two triplet excitons can exchange. The results show that the recombination induces the formation of singlet excitons, excited polarons and biexcitons. Moreover, we also find the yields of these products, which can contribute to the emission, increase with the interchain coupling strength, in good agreement with results from experiments.

  6. Particle-in-a-bos model of one-dimensional excitons in conjugated polymers

    DEFF Research Database (Denmark)

    Pedersen, T.G.; Johansen, P.M.; Pedersen, H.C.

    2000-01-01

    A simple two-particle model of excitons in conjugated polymers is proposed as an alternative to usual highly computationally demanding quantum chemical methods. In the two-particle model, the exciton is described as an electron-hole pair interacting via Coulomb forces and confined to the polymer...... of these cases an approximate solution for the general case is obtained. As an application of the model the influence of a static electric field on the electron-hole overlap integral and exciton energy is considered....

  7. Dynamic Control of Plasmon-Exciton Coupling in Au Nanodisk–J-Aggregate Hybrid Nanostructure Arrays

    KAUST Repository

    Zheng, Yue Bing

    2009-01-01

    We report the dynamic control of plasmon-exciton coupling in Au nanodisk arrays adsorbed with J-aggregate molecules by incident angle of light. The angle-resolved spectra of an array of bare Au nanodisks exhibit continuous shifting of localized surface plasmon resonances. This characteristic enables the production of real-time, controllable spectral overlaps between molecular and plasmonic resonances, and the efficient measurement of plasmon-exciton coupling as a function of wavelength with one or fewer nanodisk arrays. Experimental observations of varying plasmon-exciton coupling match with coupled dipole approximation calculations.

  8. PHONON-EXCITON MECHANISM IN YBa2Cu3O7-δ SYSTEM

    Institute of Scientific and Technical Information of China (English)

    Li Zhenji; Li Fengyue

    2006-01-01

    In this paper, based on the phonon-exciton mechanism, the superconductivity of yttrium barium copper oxide (YBCO) system is explained. The transition temperature (Tc) 's formula is derived by the extended BCS-Eliashberg theory, i.e. phonon-exciton mechanism and McMillan's energy gap function, and the Tc's expressions isreduced by using the Einstein spectrum. Last, the calculating method of element metal effective phonon spectrum is used to the high Tc cuprate YBCO system by using a crystal average atom approximation model. The theoretical analysis and calculational results show that the superconductivity of high Tc YBCO system maybe described by phonon-exciton model.

  9. Resonant Rayleigh scattering of exciton-polaritons in multiple quantum wells

    DEFF Research Database (Denmark)

    Malpuech, Guillaume; Kavokin, Alexey; Langbein, Wolfgang Werner;

    2000-01-01

    A theoretical concept of resonant Rayleigh scattering (RRS) of exciton-polaritons in multiple quantum wells (QWs) is presented. The optical coupling between excitons in different QWs can strongly affect the RRS dynamics, giving rise to characteristic temporal oscillations on a picosecond scale....... Bragg and anti-Bragg arranged QW structures with the same excitonic parameters are predicted to have drastically different RRS spectra. Experimental data on the RRS from multiple QWs show the predicted strong temporal oscillations at small scattering angles, which are well explained by the presented...

  10. Rabi Oscillation of Exciton Dressed by Phonons In a Quantum Dot

    Institute of Scientific and Technical Information of China (English)

    李惠生; 朱卡的

    2003-01-01

    The effect of strong exciton-phonon interaction on the excitonic Rabi oscillations in a coherently driven quantum dot in a high-Q single mode cavity is investigated theoretically. We show that the Rabi oscillation of exciton dressed by phonons can persists with the Rabi frequency ge-λ/2 at absolute zero temperature, where g is the single-photon Rabi frequency and λ is the Huang-Rhys factor. The results also present that such coherent oscillations can be modified by manipulating the Rabi frequency of the driving field.

  11. Role of Exciton Screening in the 7/3 Fractional Quantum Hall Effect

    Science.gov (United States)

    Balram, Ajit C.; Wu, Ying-Hai; Sreejith, G. J.; Wójs, Arkadiusz; Jain, Jainendra K.

    2013-05-01

    The excitations of the 7/3 fractional Hall state, one of the most prominent states in the second Landau level, are not understood. We study the effect of screening by composite fermion excitons and find that it causes a strong renormalization at 7/3, thanks to a relatively small exciton gap and a relatively large residual interaction between composite fermions. The excitations of the 7/3 state are to be viewed as composite fermions dressed by a large exciton cloud. Their wide extent has implications for experiments as well as for analysis of finite system exact diagonalization studies.

  12. Synthesis of titanium dioxide and zinc oxide nanowires for excitonic solar cells

    Science.gov (United States)

    Boercker, Janice Elaine

    Dye-sensitized, quantum-dot sensitized, quantum-dot, and hybrid organic/inorganic solar cells are promising excitonic photovoltaic devices for the generation of low cost, carbon free energy. Wide-band gap semiconductor nanowire photoanodes have the potential to increase the efficiencies of these excitonic solar cells. Controlling and tailoring the dimensions of the nanowires (i.e. nanowire height, diameter, and planar number density) for each solar cell type is important for efficiency improvement. Obtaining such control will require a detailed and fundamental understanding of the nanowire growth process. Towards this end, the synthesis of TiO2 and ZnO nanowire films in aqueous solutions was studied. Anatase TiO2 nanowire films were grown on flexible titanium foil substrates using a three step hydrothermal synthesis. First, the top surface of the titanium foil was transformed to Na2Ti2O 4(OH)2 nanotubes through hydrothermal oxidation in NaOH. Next, the Na2Ti2O4(OH)2 nanotubes were converted to H2Ti2O4(OH)2 nanotubes by ion exchange. Finally, the H2Ti2O 4(OH)2 nanotubes were converted to polycrystalline anatase nanowires through a topotactic transformation. The film morphology evolution, crystal structure transformations, and growth mechanism were examined in detail. Dye-sensitized solar cells (DSSCs) were assembled from these TiO 2 nanowire films. Transient photocurrent and photovoltage spectroscopies were used to measure the electron transport and recombination rates in these solar cells. Compared to TiO2 nanoparticle DSSCs the electron collection efficiency in the TiO2 nanowire DSSCs was increased due to decreased electron recombination. However, the electron transport in the nanowire DSSCs was similar to that of TiO2 nanoparticle DSSCs. The synthesis of ZnO nanowires from aqueous solutions of methenamine (HMT) and zinc nitrate hexahydrate on substrates was studied in detail. A ZnO nanowire growth mechanism was proposed which predicts that the precursor is a zinc

  13. Nonradiative recombination of excitons in semimagnetic quantum dots

    Energy Technology Data Exchange (ETDEWEB)

    Chernenko, A. V., E-mail: chernen@issp.ac.ru [Russian Academy of Sciences, Institute of Solid State Physics (Russian Federation)

    2015-12-15

    The mechanisms of the nonradiative recombination of excitons in neutral and charged quantum dots based on II–VI semimagnetic semiconductors are investigated. It is shown that, along with the dipole–dipole and direct-exchange mechanisms, there is one more mechanism referred to as the indirect-exchange mechanism and related to sp–d mixing. The selection rules for nonradiative recombination by exchange mechanisms are subsequently derived. The dependence of the efficiency of all recombination mechanisms on the quantum-dot size is studied. The experimentally observed growth in the intracenter photoluminescence intensity with decreasing size of dots and nanocrystals is accounted for. Methods for experimental determination of the contributions of different mechanisms to nonradiative recombination are discussed.

  14. Light-hole exciton in a nanowire quantum dot

    Science.gov (United States)

    Jeannin, Mathieu; Artioli, Alberto; Rueda-Fonseca, Pamela; Bellet-Amalric, Edith; Kheng, Kuntheak; André, Régis; Tatarenko, Serge; Cibert, Joël; Ferrand, David; Nogues, Gilles

    2017-01-01

    Quantum dots inserted inside semiconductor nanowires are extremely promising candidates as building blocks for solid-state-based quantum computation and communication. They provide very high crystalline and optical properties and offer a convenient geometry for electrical contacting. Having a complete determination and full control of their emission properties is one of the key goals of nanoscience researchers. Here we use strain as a tool to create in a single magnetic nanowire quantum dot a light-hole exciton, an optically active quasiparticle formed from a single electron bound to a single light hole. In this frame, we provide a general description of the mixing within the hole quadruplet induced by strain or confinement. A multi-instrumental combination of cathodoluminescence, polarization-resolved Fourier imaging, and magneto-optical spectroscopy, allows us to fully characterize the hole ground state, including its valence band mixing with heavy-hole states.

  15. Dynamic Stark effect in strongly coupled microcavity exciton polaritons.

    Science.gov (United States)

    Hayat, Alex; Lange, Christoph; Rozema, Lee A; Darabi, Ardavan; van Driel, Henry M; Steinberg, Aephraim M; Nelsen, Bryan; Snoke, David W; Pfeiffer, Loren N; West, Kenneth W

    2012-07-20

    We present experimental observations of a nonresonant dynamic Stark shift in strongly coupled microcavity quantum well exciton polaritons--a system which provides a rich variety of solid-state collective phenomena. The Stark effect is demonstrated in a GaAs/AlGaAs system at 10 K by femtosecond pump-probe measurements, with the blueshift approaching the meV scale for a pump fluence of 2  mJ cm(-2) and 50 meV red detuning, in good agreement with theory. The energy level structure of the strongly coupled polariton Rabi doublet remains unaffected by the blueshift. The demonstrated effect should allow generation of ultrafast density-independent potentials and imprinting well-defined phase profiles on polariton condensates, providing a powerful tool for manipulation of these condensates, similar to dipole potentials in cold-atom systems.

  16. Hyperbolic spin vortices and textures in exciton-polariton condensates

    Science.gov (United States)

    Manni, F.; Léger, Y.; Rubo, Y. G.; André, R.; Deveaud, B.

    2013-10-01

    From cosmology to the microscopic scales of the quantum world, the study of topological excitations is essential for the understanding of phase conformation and phase transitions. Quantum fluids are convenient systems to investigate topological entities because well-established techniques are available for their preparation, control and measurement. Across a phase transition, a system dramatically changes its properties because of the spontaneous breaking of certain continuous symmetries, leading to generation of topological defects. In particular, attention is given to entities that involve both spin and phase topologies. Exciton-polariton condensates are quantum fluids combining coherence and spin properties that, thanks to their light-matter nature, bring the advantage of direct optical access to the condensate order parameter. Here we report on the spontaneous occurrence of hyperbolic spin vortices in polariton condensates, by directly imaging both their phase and spin structure, and observe the associated spatial polarization patterns, spin textures that arise in the condensate.

  17. Free exciton emission and vibrations in pentacene monolayers

    Science.gov (United States)

    He, Rui

    2011-03-01

    Pentacene is a benchmark organic semiconductor material because of its potential applications in electronic and optoelectronic devices. Recently we demonstrated that optical and vibrational characterizations of pentacene films can be carried out down to the sub-monolayer limit. These milestones were achieved in highly uniform pentacene films that were grown on a compliant polymeric substrate. Films with thickness ranging from sub- monolayer to tens of monolayers were studied at low temperatures. The intensity of the free exciton (FE) luminescence band increases quadratically with the number of layers N when N is small. This quadratic dependence is explained as arising from the linear dependence of the intensity of absorption and the probability of emission on the number of layers N. Large enhancements of Raman scattering intensities at the FE resonance enable the first observations of low-lying lattice modes in the monolayers. The measured low- lying modes (in the 20 to 100 cm-1 range) display characteristic changes when going from a single monolayer to two layers. The Raman intensities by high frequency intra-molecular vibrations display resonance enhancement double-peaks when incident or scattered photon energies overlap the FE optical emission. The double resonances are about the same strength which suggests that Franck-Condon overlap integrals for the respective vibronic transitions have the same magnitude. The interference between scattering amplitudes in the Raman resonance reveals quantum coherence of the symmetry-split states (Davydov doublet) of the lowest intrinsic singlet exciton. These results demonstrate novel venues for ultra-thin film characterization and studies of fundamental physics in organic semiconductor structures. In collaboration with Nancy G. Tassi (Dupont), Graciela B. Blanchet (Nanoterra, Cambridge, MA), and Aron Pinczuk (Columbia University).

  18. Plasmon-exciton interaction and screening of exciton in ZnO-based thin film on bulk Pt as analyzed by spectroscopic ellipsometry

    Science.gov (United States)

    Darma, Yudi; Dimas Satrya, Christoforus; Marlina, Resti; Kurniawan, Robi; Herng, Tun Seng; Ding, Jun; Rusydi, Andrivo

    2017-01-01

    We study plasmon-exciton interaction in ZnO-based thin film on bulk Pt by using high resolution spectroscopic ellipsometry. ZnO films on quartz are used as reference. This study shows the strong electronic interactions between ZnO film and Pt by considering the significant suppression of exciton in ZnO film, in comparison to ZnO film on quartz. We found that plasmon in Pt are responsible to provide transferred electron for electronic blocking of exciton in ZnO film induce by spontaneous recombination from Pt. In the case of Cu doped ZnO film, we confirm screening effects on exciton and a localized interband transition for both systems (ZnO film on Pt and ZnO film on quartz). In Cu-doped ZnO film, electronic blocking of exciton by Pt plasmon is more pronounce rather than screening effect by interband transition. Our results show the importance of plasmon from substrate and doping to modify the optical properties of wide bandgap semiconductor.

  19. Exciton-plasmon Coupling and Electromagnetically Induced Transparency in Monolayer Semiconductors Hybridized with Ag Nanoparticles

    CERN Document Server

    Weijie, Zhao; Bo, Liu; Ivan, Verzhbitskiy; Shisheng, Li; Francesco, Giustiniano; Daichi, Kozawa; Ping, Loh Kian; Kazunari, Matsuda; Koichi, Okamoto; Rupert, Oulton F; Goki, Eda

    2016-01-01

    Hybrid systems of excitons strongly coupled to localized surface plasmons supported by metallic nanoparticles define a new approach to control light-matter interactions. Here, we report exciton-plasmon coupling in two-dimensional (2D) semiconductors, such as MoS2 and WS2, hybridized with silver nanoparticles. Prominent photoluminescence enhancement in monolayer MoS2 was observed with localized surface plasmon resonance (LSPR) tuned to the exciton resonance. By tuning the excitation energy, the contributions from near field enhancement and radiative emission rate enhancement via Purcell effect were resolved. Strong coherent dipole-dipole coupling between excitons and LSPR in resonant condition manifests as an electromagnetically induced transparency window in the extinction spectra of the localized surface plasmon. In this strong coupling regime a new quasi-particle, known as a plexciton, is expected to exhibit distinct properties, which exist in neither of the original particles. Our results demonstrate that ...

  20. Influence of intra-pigment vibrations on dynamics of photosynthetic exciton

    Energy Technology Data Exchange (ETDEWEB)

    Sato, Yoshihiro, E-mail: sato.yoshihiro77@nihon-u.ac.jp, E-mail: ysato.colby@gmail.com; Doolittle, Brian [Department of Physics and Astronomy, Colby College, Waterville, Maine 04901 (United States)

    2014-11-14

    We have numerically investigated the effect of an underdamped intra-pigment vibrational mode on an exciton's quantum coherence and energy transfer efficiency. Our model describes a bacteriochlorophyll a pigment-protein dimer under the conditions at which photosynthetic energy transfer occurs. The dimer is modeled using a theoretical treatment of a vibronic exciton, and its dynamics are numerically analyzed using a non-Markovian and non-perturbative method. We examined the system's response to various values of the Huang-Rhys factor, site energy difference, reorganization energy, and reorganization energy difference. We found that the inclusion of the intra-pigment vibronic mode allows for long-lived oscillatory quantum coherences to occur. This excitonic coherence is robust against static site-energy disorder. The vibrational mode also promotes exciton transfer along the site-energy landscape thus improving the overall energy transfer efficiency.

  1. Microscopic origins of the surface exciton photoluminescence in ZnO nanostructures

    Science.gov (United States)

    Biswas, Mahua; Jung, Yun Suk; Kim, Hong Koo; Kumar, Kumarappan; Hughes, Gregory J.; Newcomb, S.; Henry, Martin O.; McGlynn, Enda

    2012-02-01

    Photoluminescence (PL) studies of the surface exciton peak in ZnO nanostructures at ~3.367 eV are reported to elucidate the nature and origin of the emission and its relationship to nanostructure morphology. Localised voltage application in high vacuum and different gas atmospheres show a consistent PL variation (and recovery), allowing an association of the PL to a bound excitonic transition at the ZnO surface modified by an adsorbate. Studies of samples treated by plasma and of samples exposed to UV light under high vacuum conditions show no consistent effects on the surface exciton peak indicating no involvement of oxygen species. X-ray photoelectron spectroscopy data indicate involvement of adsorbed OH species. The relationship of the surface exciton peak to the nanostructure morphology is discussed in light of x-ray diffraction, scanning and transmission electron microscopy data.

  2. Nanosecond pump and probe observation of bimolecular exciton effects in rubrene single crystals

    Energy Technology Data Exchange (ETDEWEB)

    Ward, Kebra A.; Richman, Brittany R.; Biaggio, Ivan [Department of Physics, Lehigh University, Bethlehem, Pennsylvania 18015 (United States)

    2015-06-01

    Transient grating pump and probe experiments are used to investigate excitonic processes on the nanosecond time scale in rubrene single crystals. We find that bimolecular interactions cause a photoinduced excited state density on the order of 0.5 × 10{sup 20 }cm{sup −3}—corresponding to an average distance of ∼3 nm between individual states—to decrease by a factor of 2 after 2 ns, following a typical power-law decay. We assign the observed power-law decays to high-density interactions between excited states. Because of the high efficiency singlet exciton fission observed in rubrene, these bimolecular interactions are likely those between triplet excitons or between coherent quantum superpositions of a singlet and a pair of triplet-excitons.

  3. 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.

  4. Observation of forbidden exciton transitions mediated by Coulomb interactions in photoexcited semiconductor quantum wells.

    Science.gov (United States)

    Rice, W D; Kono, J; Zybell, S; Winnerl, S; Bhattacharyya, J; Schneider, H; Helm, M; Ewers, B; Chernikov, A; Koch, M; Chatterjee, S; Khitrova, G; Gibbs, H M; Schneebeli, L; Breddermann, B; Kira, M; Koch, S W

    2013-03-29

    We use terahertz pulses to induce resonant transitions between the eigenstates of optically generated exciton populations in a high-quality semiconductor quantum well sample. Monitoring the excitonic photoluminescence, we observe transient quenching of the 1s exciton emission, which we attribute to the terahertz-induced 1s-to-2p excitation. Simultaneously, a pronounced enhancement of the 2s exciton emission is observed, despite the 1s-to-2s transition being dipole forbidden. A microscopic many-body theory explains the experimental observations as a Coulomb-scattering mixing of the 2s and 2p states, yielding an effective terahertz transition between the 1s and 2s populations.

  5. Exciton Localization in Extended {\\pi}-electron Systems: Comparison of Linear and Cyclic Structures

    CERN Document Server

    Thiessen, Alexander; Jester, Stefan-S; Aggarwal, A Vikas; Idelson, Alissa; Bange, Sebastian; Vogelsang, Jan; Höger, Sigurd; Lupton, John M

    2015-01-01

    We employ five {\\pi}-conjugated model materials of different molecular shape --- oligomers and cyclic structures --- to investigate the extent of exciton self-trapping and torsional motion of the molecular framework following optical excitation. Our studies combine steady-state and transient fluorescence spectroscopy in the ensemble with measurements of polarization anisotropy on single molecules, supported by Monte Carlo simulations. The dimer exhibits a significant spectral red-shift within $\\sim$ 100 ps after photoexcitation which is attributed to torsional relaxation. This relaxation mechanism is inhibited in the structurally rigid macrocyclic analogue. However, both systems show a high degree of exciton localization but with very different consequences: while in the macrocycle the exciton localizes randomly on different parts of the ring, scrambling polarization memory, in the dimer, localization leads to a deterministic exciton position with luminescence characteristics of a dipole. Monte Carlo simulati...

  6. Impact of the Crystallite Orientation Distribution on Exciton Transport in Donor-Acceptor Conjugated Polymers.

    Science.gov (United States)

    Ayzner, Alexander L; Mei, Jianguo; Appleton, Anthony; DeLongchamp, Dean; Nardes, Alexandre; Benight, Stephanie; Kopidakis, Nikos; Toney, Michael F; Bao, Zhenan

    2015-12-30

    Conjugated polymers are widely used materials in organic photovoltaic devices. Owing to their extended electronic wave functions, they often form semicrystalline thin films. In this work, we aim to understand whether distribution of crystallographic orientations affects exciton diffusion using a low-band-gap polymer backbone motif that is representative of the donor/acceptor copolymer class. Using the fact that the polymer side chain can tune the dominant crystallographic orientation in the thin film, we have measured the quenching of polymer photoluminescence, and thus the extent of exciton dissociation, as a function of crystal orientation with respect to a quenching substrate. We find that the crystallite orientation distribution has little effect on the average exciton diffusion length. We suggest several possibilities for the lack of correlation between crystallographic texture and exciton transport in semicrystalline conjugated polymer films.

  7. Impact of the Crystallite Orientation Distribution on Exciton Transport in Donor–Acceptor Conjugated Polymers

    KAUST Repository

    Ayzner, Alexander L.

    2015-12-30

    © 2015 American Chemical Society. Conjugated polymers are widely used materials in organic photovoltaic devices. Owing to their extended electronic wave functions, they often form semicrystalline thin films. In this work, we aim to understand whether distribution of crystallographic orientations affects exciton diffusion using a low-band-gap polymer backbone motif that is representative of the donor/acceptor copolymer class. Using the fact that the polymer side chain can tune the dominant crystallographic orientation in the thin film, we have measured the quenching of polymer photoluminescence, and thus the extent of exciton dissociation, as a function of crystal orientation with respect to a quenching substrate. We find that the crystallite orientation distribution has little effect on the average exciton diffusion length. We suggest several possibilities for the lack of correlation between crystallographic texture and exciton transport in semicrystalline conjugated polymer films.

  8. Long-range coherence of interacting Bose gas of dipolar excitons

    Energy Technology Data Exchange (ETDEWEB)

    Timofeev, V B; Gorbunov, A V; Larionov, A V [Institute of Solid State Physics, Russian Academy of Sciences, 142432 Chernogolovka (Russian Federation)

    2007-07-25

    Experiments connected with dipolar exciton Bose condensation in lateral traps are reviewed. Observations of long-range coherence of condensate in ring electrostatic traps in Schottky-diode heterostructures with double and single quantum wells are presented and discussed.

  9. Dipolar excitons indirect in real and momentum space in a GaAs/AlAs heterostructure

    Energy Technology Data Exchange (ETDEWEB)

    Gorbunov, A. V., E-mail: gorbunov@issp.ac.ru; Timofeev, V. B. [Russian Academy of Sciences, Institute of Solid State Physics (Russian Federation)

    2015-01-15

    For a Schottky-diode structure containing two narrow GaAs (3.5 nm) and AlAs (5 nm) heterolayers, the photoluminescence properties of long-living dipolar excitons, indirect in both real and momentum space, are studied in perpendicular magnetic fields in the Faraday configuration of measurements. With an external perpendicular electric field, the lifetimes of such excitons can be extended to ∼1 μs. Nevertheless the exciton spin subsystem remains nonequilibrium: the exciton spin-relaxation time is even longer. The degree of circular polarization of the photoluminescence attains 80% in a field of 6 T. With an electric field, it is possible to control the degree and sign of the circular polarization.

  10. Strong Photocurrent from Two-Dimensional Excitons in Solution-Processed Stacked Perovskite Semiconductor Sheets.

    Science.gov (United States)

    Ahmad, Shahab; Kanaujia, Pawan K; Beeson, Harry J; Abate, Antonio; Deschler, Felix; Credgington, Dan; Steiner, Ullrich; Prakash, G Vijaya; Baumberg, Jeremy J

    2015-11-18

    Room-temperature photocurrent measurements in two-dimensional (2D) inorganic-organic perovskite devices reveal that excitons strongly contribute to the photocurrents despite possessing binding energies over 10 times larger than the thermal energies. The p-type (C6H9C2H4NH3)2PbI4 liberates photocarriers at metallic Schottky aluminum contacts, but incorporating electron- and hole-transport layers enhances the extracted photocurrents by 100-fold. A further 10-fold gain is found when TiO2 nanoparticles are directly integrated into the perovskite layers, although the 2D exciton semiconducting layers are not significantly disrupted. These results show that strong excitonic materials may be useful as photovoltaic materials despite high exciton binding energies and suggest mechanisms to better understand the photovoltaic properties of the related three-dimensional perovskites.

  11. Photon echo in exciton-plasmon nanomaterials: a signature of strong coupling

    CERN Document Server

    Blake, Adam

    2016-01-01

    The results of rigorous numerical simulations of photon echoes in exciton-plasmon systems are presented. Using a self-consistent model based on coupled Maxwell-Bloch equations we investigate femtosecond time dynamics of ensembles of interacting molecules and molecular aggregates optically coupled to surface-plasmon supporting materials. It is shown that observed photon echoes under two pulse pump-probe sequence are highly dependent on various material parameters such as molecular concentration and periodicity. Simulations of photon echoes in exciton-plasmon materials reveal a unique signature of the strong exciton-plasmon coupling, namely a double-peak structure in spectra of recorded echo signals. This phenomenon is shown to be related to hybrid states (upper and lower polaritons) in exciton-plasmon systems under strong coupling conditions. It is also demonstrated that the double-peak echo is highly sensitive to mild deviations of the coupling from the resonance between molecules and plasmons making it a gre...

  12. Effect of thermal annealing on exciton diffusion in a diketopyrrolopyrrole derivative.

    Science.gov (United States)

    Mikhnenko, Oleksandr V; Lin, Jason; Shu, Ying; Anthony, John E; Blom, Paul W M; Nguyen, Thuc-Quyen; Loi, Maria Antonietta

    2012-11-07

    We show that the method we have developed for measuring the singlet exciton diffusion length in blends with [6,6]-phenyl-C(61)-butyric acid methyl ester (PCBM) can be applied not only to polymeric materials, but also to small molecule organic semiconductors. Small organic molecules have a large potential for molecular re-organization upon thermal annealing. Here we show that the exciton diffusion length is decreased upon annealing from 9 to 3 nm in a thin film of a diketopyrrolopyrrole derivative. Such a variation is attributed to exciton delocalization effects in the crystalline domains that are formed during the annealing process as well as to the exciton quenching at grain boundaries.

  13. Phonon induced pure dephasing process of excitonic state in colloidal semiconductor quantum dots

    Science.gov (United States)

    Huang, Tongyun; Han, Peng; Wang, Xinke; Feng, Shengfei; Sun, Wenfeng; Ye, Jiasheng; Zhang, Yan

    2016-04-01

    We present a theoretical study on the pure dephasing process of colloidal semiconductor quantum dots induced by lattice vibrations using continuum model calculations. By solving the time dependent Liouville-von Neumann equation, we present the ultrafast Rabi oscillations between excitonic state and virtual state via exciton-phonon interaction and obtain the pure dephasing time from the fast decayed envelope of the Rabi oscillations. The interaction between exciton and longitudinal optical phonon vibration is found to dominate the pure dephasing process and the dephasing time increases nonlinearly with the reduction of exciton-phonon coupling strength. We further find that the pure dephasing time of large quantum dots is more sensitive to temperature than small quantum dots.

  14. External pumping of hybrid nanostructures in microcavity with Frenkel and Wannier-Mott excitons

    Science.gov (United States)

    Dubovskiy, O. A.; Agranovich, V. M.

    2016-09-01

    The exciton-exciton interaction in hybrid nanostructures with resonating Frenkel and Wannier-Mott excitons was investigated in many publications. In microcavity the hybrid nanostructures can be exposed to different types of optical pumping, the most common one being pumping through one of the microcavity side. However, not investigated and thus never been discussed the hybrid excitons generation by pumping of confined quantum wells from the side of empty microcavity without nanostructures in a wave guided configuration. Here, we consider the hybrid excitations in cavity with organic and inorganic quantum wells and with different types of pumping from external source. The frequency dependence for intensity of excitations in hybrid structure is also investigated. The results may be used for search of most effective fluorescence and relaxation processes. The same approach may be used when both quantum wells are organic or inorganic.

  15. Quantum theory of exciton-photon coupling in photonic crystal slabs with embedded quantum wells

    CERN Document Server

    Gerace, D

    2007-01-01

    A theoretical description of radiation-matter coupling for semiconductor-based photonic crystal slabs is presented, in which quantum wells are embedded within the waveguide core layer. A full quantum theory is developed, by quantizing both the electromagnetic field with a spatial modulation of the refractive index and the exciton center of mass field in a periodic piecewise constant potential. The second-quantized hamiltonian of the interacting system is diagonalized with a generalized Hopfield method, thus yielding the complex dispersion of mixed exciton-photon modes including losses. The occurrence of both weak and strong coupling regimes is studied, and it is concluded that the new eigenstates of the system are described by quasi-particles called photonic crystal polaritons, which can occur in two situations: (i) below the light line, when a resonance between exciton and non-radiative photon levels occurs (guided polaritons), (ii) above the light line, provided the exciton-photon coupling is larger than th...

  16. 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.

  17. 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

  18. 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.

  19. Observation of Superfluorescence from a Spontaneous Coherence of Excitons in ZnTe Crystal: Evidence for Bose-Einstein Condensation of Excitons?

    CERN Document Server

    Dai, D C

    2011-01-01

    Superfluorescence (SF) is the emission from a dense coherent system in population inversion, formed from an initially incoherent ensemble. This is characterised by an induction time (t_D) for the spontaneous development of the macroscopic quantum coherence. Here we report detailed observation of SF on ultrafast timescale from a quantum ensemble of coherent excitons in highly excited intrinsic bulk ZnTe single crystal at 5 K, showing a characteristic t_D from 40 ps to 10 ps, quantum noise and fluctuations, and quantum beating and ringing. From this clear observation of SF from a spontaneous coherence of excitons we infer that this is indicative of the formation of BEC of excitons on an ultrafast timescale.

  20. High-quality elliptical iron glycolate nanosheets: selective synthesis and chemical conversion into FexOy nanorings, porous nanosheets, and nanochains with enhanced visible-light photocatalytic activity

    Science.gov (United States)

    Tong, Guoxiu; Liu, Yun; Wu, Tong; Ye, Yucheng; Tong, Chaoli

    2015-10-01

    This paper describes an original and facile polyol-mediated solvothermal synthesis of elliptical iron glycolate nanosheets (IGNSs) combined with precursor thermal conversion into γ-Fe2O3 and α-Fe2O3/γ-Fe2O3 porous nanosheets (PNSs), α-Fe2O3 nanochains (NCs), and elliptical Fe3O4 nanorings (NRs). The IGNSs were produced via the oxidation-reduction and co-precipitation reactions in the presence of iron(iii) salts, ethylene glycol, polyethylene glycol, and ethylenediamine. Control over Fe3+ concentration, temperature, and time can considerably modulate the size and phase of the products. The IGNSs can be transformed to γ-Fe2O3 and α-Fe2O3/γ-Fe2O3 PNSs, α-Fe2O3 NCs, and elliptical Fe3O4 NRs by heat treatment under various annealing temperatures and ambiences. The PNSs and NCs exhibited high soft magnetic properties and coercivity, respectively. Visible-light photocatalytic activity toward RhB in the presence of H2O2 by PNSs and NCs was phase-, SBET, size-, porosity-, and local structure-dependent, following the order: α-Fe2O3 NCs > α-Fe2O3/γ-Fe2O3 PNSs > γ-Fe2O3 PNSs > IGNSs. In particular, α-Fe2O3/γ-Fe2O3 PNSs possessed significantly enhanced photocatalytic activity with good recyclability and could be conveniently separated by an applied magnetic field because of high magnetization. We believe that the as-prepared α-Fe2O3/γ-Fe2O3 PNSs have potential practical use in waste water treatment and microwave absorption.This paper describes an original and facile polyol-mediated solvothermal synthesis of elliptical iron glycolate nanosheets (IGNSs) combined with precursor thermal conversion into γ-Fe2O3 and α-Fe2O3/γ-Fe2O3 porous nanosheets (PNSs), α-Fe2O3 nanochains (NCs), and elliptical Fe3O4 nanorings (NRs). The IGNSs were produced via the oxidation-reduction and co-precipitation reactions in the presence of iron(iii) salts, ethylene glycol, polyethylene glycol, and ethylenediamine. Control over Fe3+ concentration, temperature, and time can

  1. 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.

  2. Effects of distance dependence of exciton hopping on the Davydov soliton

    OpenAIRE

    Bartnik, E. A.; Tuszynski, J. A.; Sept, D.

    1995-01-01

    The Davydov model of energy transfer in molecular chains is reconsidered assuming the distance dependence of the exciton hopping term. New equations of motion for phonons and excitons are derived within the coherent state approximation. Solving these nonlinear equations result in the existence of Davydov-like solitons. In the case of a dilatational soliton, the amplitude and width is decreased as a results of the mechanism introduced here and above a critical coupling strength our equations d...

  3. Effect of the Electron-LO-Phonon Coupling on an Exciton Quantum Dot

    Institute of Scientific and Technical Information of China (English)

    XIE Wen-Fang; ZHU Wu

    2002-01-01

    The influence of the electron-LO-phonon coupling on energy spectrum of the low-lying states ofan exciton inparabolic quantum dots is investigated as a function of dot size. Calculations are made by using the method of few-bodyphysics within the effective-mass approximation. A considerable decrease of the energy in the stronger confinement rangeis found for the low-lying states of an exciton in quantum dots, which results from the confinement of electron-phononcoupling.

  4. Nature of the narrow optical band in H*-aggregates: Dozy-chaos-exciton coupling

    Science.gov (United States)

    Egorov, Vladimir V.

    2014-07-01

    Dozy chaos emerges as a combined effect of the collective chaotic motion of electrons and nuclei, and their chaotic electromagnetic interactions in the transient state of molecules experiencing quantum transitions. Following earlier discussions of the well-known Brönsted relations for proton-transfer reactions; the temperature-dependent electron transfer in Langmuir-Blodgett films; the shape of the optical bands of polymethine dye monomers, their dimers, and J-aggregates, this paper reports one more application of the dozy-chaos theory of molecular quantum transitions. The qualitative and quantitative explanations for shape of a narrow and blue-shifted optical absorption band in H*-aggregates is given on the basis of the dozy-chaos theory by taking into account the dozy-chaos-exciton coupling effect. It is emphasized that in the H*-aggregate chromophore (dimer of cyclic bis-thiacarbocyanines) there is a competition between two Frenkel exciton transitions through the chaotic reorganization motion of nuclear environment. As a result, the highly organized quantum transition to the upper exciton state becomes an exciton-induced source of dozy chaos for the low organized transition to the lower exciton state. This manifests itself in appearing the narrow peak and broad wing in the optical spectrum pattern of H*-aggregates. A similar enhancement in the H*-effect caused by the strengthening of the exciton coupling in H*-dimers, which could be achieved by synthesizing tertiary and quarternary thiacarbocyanine monomers, is predicted.

  5. 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.

  6. A Comparison Between Magnetic Field Effects in Excitonic and Exciplex Organic Light-Emitting Diodes

    Science.gov (United States)

    Sahin Tiras, Kevser; Wang, Yifei; Harmon, Nicholas J.; Wohlgenannt, Markus; Flatte, Michael E.

    In flat-panel displays and lighting applications, organic light emitting diodes (OLEDs) have been widely used because of their efficient light emission, low-cost manufacturing and flexibility. The electrons and holes injected from the anode and cathode, respectively, form a tightly bound exciton as they meet at a molecule in organic layer. Excitons occur as spin singlets or triplets and the ratio between singlet and triplet excitons formed is 1:3 based on spin degeneracy. The internal quantum efficiency (IQE) of fluorescent-based OLEDs is limited 25% because only singlet excitons contribute the light emission. To overcome this limitation, thermally activated delayed fluorescent (TADF) materials have been introduced in the field of OLEDs. The exchange splitting between the singlet and triplet states of two-component exciplex systems is comparable to the thermal energy in TADF materials, whereas it is usually much larger in excitons. Reverse intersystem crossing occurs from triplet to singlet exciplex state, and this improves the IQE. An applied small magnetic field can change the spin dynamics of recombination in TADF blends. In this study, magnetic field effects on both excitonic and exciplex OLEDs will be presented and comparison similarities and differences will be made.

  7. Strain Gradient Modulated Exciton Evolution and Emission in ZnO Fibers

    Science.gov (United States)

    Wei, Bin; Ji, Yuan; Gauvin, Raynald; Zhang, Ze; Zou, Jin; Han, Xiaodong

    2017-01-01

    One-dimensional semiconductor can undergo large deformation including stretching and bending. This homogeneous strain and strain gradient are an easy and effective way to tune the light emission properties and the performance of piezo-phototronic devices. Here, we report that with large strain gradients from 2.1–3.5% μm−1, free-exciton emission was intensified, and the free-exciton interaction (FXI) emission became a prominent FXI-band at the tensile side of the ZnO fiber. These led to an asymmetric variation in energy and intensity along the cross-section as well as a redshift of the total near-band-edge (NBE) emission. This evolution of the exciton emission was directly demonstrated using spatially resolved CL spectrometry combined with an in situ tensile-bending approach at liquid nitrogen temperature for individual fibers and nanowires. A distinctive mechanism of the evolution of exciton emission is proposed: the enhancement of the free-exciton-related emission is attributed to the aggregated free excitons and their interaction in the narrow bandgap in the presence of high bandgap gradients and a transverse piezoelectric field. These results might facilitate new approaches for energy conversion and sensing applications via strained nanowires and fibers. PMID:28084427

  8. Strain Gradient Modulated Exciton Evolution and Emission in ZnO Fibers

    Science.gov (United States)

    Wei, Bin; Ji, Yuan; Gauvin, Raynald; Zhang, Ze; Zou, Jin; Han, Xiaodong

    2017-01-01

    One-dimensional semiconductor can undergo large deformation including stretching and bending. This homogeneous strain and strain gradient are an easy and effective way to tune the light emission properties and the performance of piezo-phototronic devices. Here, we report that with large strain gradients from 2.1–3.5% μm‑1, free-exciton emission was intensified, and the free-exciton interaction (FXI) emission became a prominent FXI-band at the tensile side of the ZnO fiber. These led to an asymmetric variation in energy and intensity along the cross-section as well as a redshift of the total near-band-edge (NBE) emission. This evolution of the exciton emission was directly demonstrated using spatially resolved CL spectrometry combined with an in situ tensile-bending approach at liquid nitrogen temperature for individual fibers and nanowires. A distinctive mechanism of the evolution of exciton emission is proposed: the enhancement of the free-exciton-related emission is attributed to the aggregated free excitons and their interaction in the narrow bandgap in the presence of high bandgap gradients and a transverse piezoelectric field. These results might facilitate new approaches for energy conversion and sensing applications via strained nanowires and fibers.

  9. Selectively tunable optical Stark effect of anisotropic excitons in atomically thin ReS2

    Science.gov (United States)

    Sim, Sangwan; Lee, Doeon; Noh, Minji; Cha, Soonyoung; Soh, Chan Ho; Sung, Ji Ho; Jo, Moon-Ho; Choi, Hyunyong

    2016-11-01

    The optical Stark effect is a coherent light-matter interaction describing the modification of quantum states by non-resonant light illumination in atoms, solids and nanostructures. Researchers have strived to utilize this effect to control exciton states, aiming to realize ultra-high-speed optical switches and modulators. However, most studies have focused on the optical Stark effect of only the lowest exciton state due to lack of energy selectivity, resulting in low degree-of-freedom devices. Here, by applying a linearly polarized laser pulse to few-layer ReS2, where reduced symmetry leads to strong in-plane anisotropy of excitons, we control the optical Stark shift of two energetically separated exciton states. Especially, we selectively tune the Stark effect of an individual state with varying light polarization. This is possible because each state has a completely distinct dependence on light polarization due to different excitonic transition dipole moments. Our finding provides a methodology for energy-selective control of exciton states.

  10. Energy harvesting of non-emissive triplet excitons in tetracene by emissive PbS nanocrystals

    Science.gov (United States)

    Thompson, Nicholas J.; Wilson, Mark W. B.; Congreve, Daniel N.; Brown, Patrick R.; Scherer, Jennifer M.; Bischof, Thomas S.; Wu, Mengfei; Geva, Nadav; Welborn, Matthew; Voorhis, Troy Van; Bulović, Vladimir; Bawendi, Moungi G.; Baldo, Marc A.

    2014-11-01

    Triplet excitons are ubiquitous in organic optoelectronics, but they are often an undesirable energy sink because they are spin-forbidden from emitting light and their high binding energy hinders the generation of free electron-hole pairs. Harvesting their energy is consequently an important technological challenge. Here, we demonstrate direct excitonic energy transfer from ‘dark’ triplets in the organic semiconductor tetracene to colloidal PbS nanocrystals, thereby successfully harnessing molecular triplet excitons in the near infrared. Steady-state excitation spectra, supported by transient photoluminescence studies, demonstrate that the transfer efficiency is at least (90 ± 13)%. The mechanism is a Dexter hopping process consisting of the simultaneous exchange of two electrons. Triplet exciton transfer to nanocrystals is expected to be broadly applicable in solar and near-infrared light-emitting applications, where effective molecular phosphors are lacking at present. In particular, this route to ‘brighten’ low-energy molecular triplet excitons may permit singlet exciton fission sensitization of conventional silicon solar cells.

  11. Effects of magnetic fields on free excitons in CuInSe{sub 2}

    Energy Technology Data Exchange (ETDEWEB)

    Martin, R.W. [Department of Physics, Strathclyde University, Glasgow (United Kingdom); Babinski, A. [Institute of Experimental Physics, University of Warsaw (Poland); Mudryi, A.V. [Scientific-Practical Material Research Centre, National Academy of Science of Belarus, Minsk (Belarus); Yakushev, M.V.

    2009-05-15

    The effects of magnetic fields up to 20 T were studied in CuInSe{sub 2} single crystals using photoluminescence (PL) at 4.2 K. Diamagnetic shifts of the free A and B excitons measured in the PL spectra in CuInSe{sub 2} at 4.2 K under the magnetic fields were used to estimate the reduced masses (0.095m{sub 0} for the A and 0.098m{sub 0} for the B exciton), binding energies (7.0 meV for the A and 7.2 meV for the B exciton) and Bohr radii (7.6 nm for the A and 7.3 nm for the B exciton) of the free-excitons in CuInSe{sub 2} assuming that both excitons are isotropic and hydrogen-like. (copyright 2009 WILEY-VCH Verlag GmbH and Co. KGaA, Weinheim) (orig.)

  12. 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.

  13. Single-mode tunable laser emission in the single-exciton regime from colloidal nanocrystals.

    Science.gov (United States)

    Grivas, Christos; Li, Chunyong; Andreakou, Peristera; Wang, Pengfei; Ding, Ming; Brambilla, Gilberto; Manna, Liberato; Lagoudakis, Pavlos

    2013-01-01

    Whispering-gallery-mode resonators have been extensively used in conjunction with different materials for the development of a variety of photonic devices. Among the latter, hybrid structures, consisting of dielectric microspheres and colloidal core/shell semiconductor nanocrystals as gain media, have attracted interest for the development of microlasers and studies of cavity quantum electrodynamic effects. Here we demonstrate single-exciton, single-mode, spectrally tuned lasing from ensembles of optical antenna-designed, colloidal core/shell CdSe/CdS quantum rods deposited on silica microspheres. We obtain single-exciton emission by capitalizing on the band structure of the specific core/shell architecture that strongly localizes holes in the core, and the two-dimensional quantum confinement of electrons across the elongated shell. This creates a type-II conduction band alignment driven by coulombic repulsion that eliminates non-radiative multi-exciton Auger recombination processes, thereby inducing a large exciton-bi-exciton energy shift. Their ultra-low thresholds and single-mode, single-exciton emission make these hybrid lasers appealing for various applications, including quantum information processing.

  14. Nature of the narrow optical band in H*-aggregates: Dozy-chaos–exciton coupling

    Directory of Open Access Journals (Sweden)

    Vladimir V. Egorov

    2014-07-01

    Full Text Available Dozy chaos emerges as a combined effect of the collective chaotic motion of electrons and nuclei, and their chaotic electromagnetic interactions in the transient state of molecules experiencing quantum transitions. Following earlier discussions of the well-known Brönsted relations for proton-transfer reactions; the temperature-dependent electron transfer in Langmuir–Blodgett films; the shape of the optical bands of polymethine dye monomers, their dimers, and J-aggregates, this paper reports one more application of the dozy-chaos theory of molecular quantum transitions. The qualitative and quantitative explanations for shape of a narrow and blue-shifted optical absorption band in H*-aggregates is given on the basis of the dozy-chaos theory by taking into account the dozy-chaos–exciton coupling effect. It is emphasized that in the H*-aggregate chromophore (dimer of cyclic bis-thiacarbocyanines there is a competition between two Frenkel exciton transitions through the chaotic reorganization motion of nuclear environment. As a result, the highly organized quantum transition to the upper exciton state becomes an exciton-induced source of dozy chaos for the low organized transition to the lower exciton state. This manifests itself in appearing the narrow peak and broad wing in the optical spectrum pattern of H*-aggregates. A similar enhancement in the H*-effect caused by the strengthening of the exciton coupling in H*-dimers, which could be achieved by synthesizing tertiary and quarternary thiacarbocyanine monomers, is predicted.

  15. 纳米化和酸洗对赤泥吸附Cd2+动力学的影响%Kinetics of Cd2 + adsorption on red mud affected by nanorization and acidification

    Institute of Scientific and Technical Information of China (English)

    梁振飞; 王立群; 陈世宝; 韦东普; 马义兵

    2013-01-01

    为揭示赤泥类钝化剂对Cd2+的吸附规律和动力学特性,研究了纳米化和酸洗处理,以及不同Cd2+添加质量浓度对赤泥类钝化剂吸附Cd2+动力学的影响.结果表明:准二级动力学方程和指数(Ⅱ)型方程可用于描述赤泥对Cd2+的吸附动力学特征.溶液中Cd2+的质量浓度从50 mg/L增加到100 mg/L,其平衡吸附量相应增加1倍,平衡时间也相应延长.纳米化赤泥、酸洗赤泥、酸洗纳米化赤泥的准二级动力学方程拟合参数K值(反应速率常数)与原状赤泥的比值分别为2.34、0.15、0.63,而指数(Ⅱ)型方程拟合参数-B(吸附量达到平衡吸附量36.8%时所需的时间)与原状赤泥的比值分别为0.53、2.09、0.85.赤泥类钝化剂既作用于Cd2+的吸附离子交换反应,又作用于表面络合反应,吸附速率受膜扩散和颗粒间扩散的联合控制.纳米化增大了赤泥的比表面积,提高了赤泥的吸附性能;酸洗处理也增大了赤泥的比表面积,但同时降低了赤泥的pH值,从而降低了赤泥的吸附性能.%This paper aims to report our investigation findings of the kinetic characteristics of Cd2+ adsorption for the red mud by way of nanorizing and acidifying process at different initial concentrations of Cd2+. For this purpose, we have applied three kinetics equations, that is, pseudo second-order kinetics equation, exponential equation Ⅱ and parabolic diffusion equation. The results of our investigation indicate that the pseudo second-order adsorption equation and exponential equation Ⅱ are fit best for describing the adsorption process. The reason is that, when the concentration increased to 100 mg Cd2+ /L from 50 mg Cd2 + /L, the adsorptive capacity in balance would also increase twice as much as it was before, correspondingly, if the equilibrium time can be made to prolong as it is needed. The pH of the solution would increase gradually before getting stable in the adsorption process. As to the pseudo

  16. Collective state of interwall excitons on GaAs/AlGaAs double quantum wells under pulse resonant excitation

    CERN Document Server

    Larionov, A V; Hvam, J; Soerensen, K

    2002-01-01

    The time evolution and kinetics of the photoluminescence (PL) spectra of the interwall excitons under the pulse resonant excitation of the interwall excitons are studied in the GaAs/AlGaAs binary quantum well. It is established, that the collective exciton phase originates with the time delay relative to the exciting pulse (several nanoseconds), which is conditioned by the density and temperature relaxation to the equilibrium values.The origination of the collective phase of the interwall excitons is accompanied by the strong narrowing of the corresponding photoluminescence line, the superlinear growth of its intensity and large time of change in the degree of the circular polarization.The collective exciton phase originates at the temperatures < 6 K and the interwall excitons densities 3 x 10 sup 1 sup 0 cm sup - sup 2

  17. Transition from bound to free excitons observed in deep- ultraviolet photoluminescence of AlN grown by MOCVD

    Science.gov (United States)

    Wang, Weiying; Jin, Peng; Tang, Ning; Liu, Yali; Fu, Lei; Xu, Fujun; Qin, Zhixin; Ge, Weikun; Shen, Bo

    2016-07-01

    The transition from bound exciton to free exciton and exciton-phonon interaction in an AlN epilayer have been investigated by time resolved deep ultraviolet photoluminescence spectroscopy. Based on the analysis of the energy position (S-shaped dependence with temperature), integrated intensity as well as decay time, the main X peak located at 6.06 eV at 7.7 K is assigned to originate from radiative recombination of excitons bound to some unintentionally doped Si or O impurities. While the other two peaks on the lower energy side should be from the bound exciton’s phonon replicas. The corresponding small Huang-Rhys factor indicates weak interaction between phonon and bound excitons, in comparison to the case of free exciton, for which our experimental results are in good agreement with the theoretical calculation of the Huang-Rhys factors.

  18. Stability of singlet and triplet trions in carbon nanotubes

    DEFF Research Database (Denmark)

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

    2009-01-01

    We investigate singlet and triplet trion states in semiconducting carbon nanotubes using a one-dimensional model. It is concluded that singlet trion states in bind up to 13.5% stronger than exciton states, and that they lower the optical transition energy with up to 50% of the tight binding band ...

  19. EXCITON ENERGY OF THE InAs/GaAs SELF-ASSEMBLED QUANTUM DOT IN A SEMICONDUCTOR MICROCAVITY

    Institute of Scientific and Technical Information of China (English)

    PAN LIU-XIAN; LI SHU-SHEN; XIA JlAN-BAI

    2001-01-01

    We report on the theoretical study of the interaction of the quantum dot(QD)exciton with the photon waveguide models in a semiconductor microcavity. The lnAs/GaAs self-assembled QD exciton energies are calculated in a microcavity. The calculated results reveal that the electromagnetic field reduces the exciton energies in a semiconductor microcavity. The effect of the electromagnetic field decreases as the radius of the QD increases. Our calculated results are useful for designing and fabricating photoelectron devices.

  20. Effect of exciton oscillator strength on upconversion photoluminescence in GaAs/AlAs multiple quantum wells

    Energy Technology Data Exchange (ETDEWEB)

    Kojima, Osamu, E-mail: kojima@phoenix.kobe-u.ac.jp; Okumura, Shouhei; Kita, Takashi [Department of Electrical and Electronic Engineering, Graduate School of Engineering, Kobe University, 1-1 Rokkodai, Nada, Kobe 657-8501 (Japan); Akahane, Kouichi [National Institute of Information and Communications Technology, 4-2-1 Nukui-kitamachi, Koganei, Tokyo 184-8795 (Japan)

    2014-11-03

    We report upconversion photoluminescence (UCPL) in GaAs/AlAs multiple quantum wells. UCPL from the AlAs barrier is caused by the resonant excitation of the excitons in the GaAs well. When the quantum well has sufficient miniband width, UCPL is hardly observed because of the small exciton oscillator strength. The excitation-energy and excitation-density dependences of UCPL intensity show the exciton resonant profile and a linear increase, respectively. These results demonstrate that the observed UCPL caused by the saturated two-step excitation process requires a large number of excitons.

  1. Collective behavior of interwell excitons laterally confined in GaAs/AlGaAs double quantum wells

    Energy Technology Data Exchange (ETDEWEB)

    Timofeev, V.B.; Gorbunov, A.V. [Institute of Solid State Physics, Russian Academy of Sciences, Chernogolovka 142432 (Russian Federation)

    2005-02-01

    The luminescence of interwell excitons laterally confined by long range potential fluctuations and with the use of inhomogeneous electric field in n-i-n GaAs/AlGaAs heterostructures double quantum wells has been investigated under variation of excitation power and temperature. Above mobility threshold very narrow interwell exciton line has been observed and its intensity decrease is linearly dependent on temperature growth. The observed phenomena, which were critical to exciton density and temperature, are attributed to the Bose-condensation in laterally confined quasi-two dimensional system of interwell excitons. (copyright 2005 WILEY-VCH Verlag GmbH and Co. KGaA, Weinheim) (orig.)

  2. 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.

  3. Directional Control of Plasmon-Exciton interaction with Plexcitonic Crystals

    Science.gov (United States)

    Balci, Sinan; Karademir, Ertugrul; Kocabas, Coskun; Aydinli, Atilla

    2015-03-01

    Plexcitons are strongly coupled plasmon excitons modes. In this work, we developed a platform, consisting of one and two dimensional corrugated surface patterns coated with a thin metal film and a dye solution. This system shows a controlled coupling action based on the excitation direction of SPP modes. Our scheme is based on the control of wavelengths of the forbidden SPP modes. Three kinds of patterns have been tested; a one dimensional uniform, a triangular, and a square lattice type crystals. For all three cases, lowest wavelength of the band gap is observed in Γ to M direction. For triangular and square lattice cases, band gap center oscillates between two finite values for every 60° and 90°s, respectively. We utilized this behavior to control SPP and J-aggregate coupling. We observe directional dependence of Rabi splitting energy varying between 0 meV and 60 meV . Square lattice gives the ability to tune a larger band gap, whereas triangular lattice gives higher number of symmetry points. Simulations show that, an 80 nm deep triangular lattice with 280 nm periodicity can result in omnidirectional decoupling of plexcitons. TUBITAK, Grants 110T790, 110T589, and 112T091.

  4. Measuring Exciton Migration in Conjugated Polymer Films with Ultrafast Time Resolved Stimulated Emission Depletion Microscopy

    Science.gov (United States)

    Penwell, Samuel

    Conjugated polymers are highly tunable organic semiconductors, which can be solution processed to form thin films, making them prime candidates for organic photovoltaic devices. One of the most important parameters in a conjugated polymer solar cell is the exciton diffusion length, which depends on intermolecular couplings, and is typically on the order of 10 nm. This mean exciton migration can vary dramatically between films and within a single film due to heterogeneities in morphology on length scales of 10's to 100's nm. To study the variability of exciton diffusion and morphology within individual conjugated polymer films, we are adapting stimulated emission depletion (STED) microscopy. STED is typically used in biology with sparse well-engineered fluorescent labels or on NV-centers in diamond. I will, however, describe how we have demonstrated the extension of STED to conjugated polymer films and nanoparticles of MEH-PPV and CN-PPV, despite the presence of two photon absorption, by taking care to first understand the material's photophysical properties. We then further adapt this approach, by introducing a second ultrafast STED pulse at a variable delay. Excitons that migrate away from the initial subdiffraction excitation volume during the ps-ns time delay, are preferentially quenched by the second STED pulse, while those that remain in the initial volume survive. The resulting effect of the second STED pulse is modulated by the degree of migration over the ultrafast time delay, thus providing a new method to study exciton migration. Since this technique utilizes subdiffraction optical excitation and detection volumes with ultrafast time resolution, it provides a means of spatially and temporally resolving measurements of exciton migration on the native length and time scales. In this way, we will obtain a spatiotemporal map of exciton distributions and migration that will help to correlate the energetic landscape to film morphology at the nanoscale.

  5. Exciton spectrum of surface-corrugated quantum wells: the adiabatic self-consistent approach

    Energy Technology Data Exchange (ETDEWEB)

    Atenco A, N.; Perez R, F. [lnstituto de Fisica, Universidad Autonoma de Puebla, A.P. J-48, 72570 Puebla (Mexico); Makarov, N.M. [lnstituto de Ciencias, Universidad Autonoma de Puebla, Priv. 17 Norte No 3417, Col. San Miguel Hueyotlipan, 72050 Puebla (Mexico)

    2005-07-01

    A theory for calculating the relaxation frequency {nu} and the shift {delta} {omega} of exciton resonances in quantum wells with finite potential barriers and adiabatic surface disorder is developed. The adiabaticity implies that the correlation length R{sub C} for the well width fluctuations is much larger than the exciton radius a{sub 0} (R{sub C} >> a{sub 0}). Our theory is based on the self-consistent Green's function method, and therefore takes into account the inherent action of the exciton scattering on itself. The self-consistent approach is shown to describe quantitatively the sharp exciton resonance. It also gives the qualitatively correct resonance picture for the transition to the classical limit, as well as within the domain of the classical limit itself. We present and analyze results for h h-exciton in a GaAs quantum well with Al{sub 0.3} Ga{sub 0.7}As barriers. It is established that the self-consistency and finite height of potential barriers significantly influence on the line-shape of exciton resonances, and make the values of {nu} and {delta} {omega} be quite realistic. In particular, the relaxation frequency {nu} for the ground-state resonance has a broad, almost symmetric maximum near the resonance frequency {omega}{sub 0}, while the surface-induced resonance shift {delta} {omega} vanishes near {omega}{sub 0}, and has different signs on the sides of the exciton resonance. (Author) 43 refs., 4 figs.

  6. Stability and signatures of biexcitons in carbon nanotubes

    DEFF Research Database (Denmark)

    Pedersen, Thomas Garm; Pedersen, Kjeld; Cornean, Horia Decebal;

    2005-01-01

    The linear optical properties of semiconducting carbon nanotubes are dominated by quasi-one-dimensional excitons formed by single electron-hole pairs. Hence, the nonlinear response at high pump levels most likely leads to the formation of exciton complexes involving several electron-hole pairs....... Such complexes would threfore play an important role in e.g. lasing applications. We demonstrate here that the biexciton complex is surprisingly stable for nanotubes in a wide diameter range. Theoretical predictions for the signature of such states in pump-probe spectroscopy are presented....

  7. Ultrafast and Nonlinear Optical Spectroscopy of Carbon Nanotubes

    Science.gov (United States)

    Kono, Junichiro

    2011-03-01

    Single-walled carbon nanotubes (SWNTs) provide a variety of unique opportunities for studying the dynamics and interactions of one-dimensional (1-D) electrons and phonons. We have carried out a series of ultrafast and nonlinear optical experiments on SWNTs, revealing novel properties of high- density 1-D excitons as well as coherent lattice vibrations. We have shown that there exists an upper limit on the density of 1-D excitons in SWNTs, which results in photoluminescence saturation. Using a model based on diffusion-limited exciton- exciton annihilation, we provided realistic estimates for the exciton densities in the saturation regime. We also predicted and demonstrated that there is an optimum temperature at which the exciton density can be maximized, due to the existence of a dark exciton state. Using ultrashort pulses, we have also investigated the dynamics of coherent phonons (CPs) in SWNTs, including both the low frequency radial breathing mode and high frequency G-mode phonons. Pulse shaping techniques allowed us to generate and detect CPs in SWNTs in a chirality-selective manner, which provided insight into the chirality dependence of light absorption, phonon generation, and phonon-induced band- structure modulations. Finally, we observed novel large- amplitude CPs through near-band-edge excitations as well as strongly polarization-dependent CP signals in highly-aligned SWNTs. This work was performed in collaboration with Y. Murakami, A. Srivastava, T. A. Searles, L. G. Booshehri, E. H. Hároz, D. T. Morris, J.-H. Kim, K.-J. Yee, Y.-S. Lim, G. D. Sanders, C. J. Stanton, and R. Saito.

  8. Strain-tuning of the excitonic fine structure splitting in semiconductor quantum dots

    Energy Technology Data Exchange (ETDEWEB)

    Plumhof, Johannes D.; Ding, Fei; Herklotz, Andreas; Doerr, Kathrin; Rastelli, Armando; Schmidt, Oliver G. [IFW Dresden, Helmholtzstr. 20, D-01069 Dresden (Germany); Krapek, Vlastimil; Klenovsky, Petr [Institute of Condensed Matter Physics, Masaryk University, Kotlarska 2, 61137 Brno (Czech Republic); Joens, Klaus D.; Hafenbrak, Robert; Michler, Peter [Institut fuer Halbleiteroptik und Funktionelle Grenzflaechen, University of Stuttgart, Allmandring 3, 70569 Stuttgart (Germany)

    2011-07-01

    For the creation of polarization entangled photon pairs from semiconductor quantum dots (QDs) it is important to decrease the fine structure splitting (FSS) of the neutral exciton to energies comparable to the emission linewidth. We employ a piezoelectric actuator (PMN-PT) to manipulate the excitonic emission of GaAs/AlGaAs as well as InGaAs/GaAs QDs embedded in {approx}200 nm thick (Al)GaAs membranes. By attaching the membranes on the PMN-PT we can apply anisotropic strain to the nanostructures. Polarization resolved {mu}-photoluminescence spectroscopy is used to estimate the excitonic FSS as well as the orientation of the linear polarization of the emitted light. The strain makes it possible to manipulate the FSS in a range of 70 {mu} eV. We also observe rotations of up to 70 of the linear polarization of the light emitted by neutral excitons. These effects can be explained as an strain-induced anticrossing of the bright excitonic states.

  9. Excitonic fine structure of elongated InAs/InP quantum dots

    Science.gov (United States)

    Zieliński, M.

    2013-10-01

    The bright exciton splitting in nanosystems and its origins are of primary importance for quantum-dot-based entangled-photon-pair generation. In this paper, I investigate excitonic energies and fine structure for million-atom InAs/InP quantum dots using many-body theory in conjunction with the empirical tight-binding method. Whereas the phenomenological theories relate the fine-structure splitting to quantum-dot-shape asymmetry, using an atomistic approach I demonstrate that for certain elongated quantum-dot shapes the bright exciton splitting can be significantly reduced. I demonstrate that strain effects play an essential role as the main contribution to the bright exciton splitting in InAs/InP quantum dots and observe highly reduced fine-structure splitting for high-symmetry quantum dots without wetting layer. I report the “intrinsic” fine-structure splitting, due to the underlying crystal lattice, to be generally significantly larger than the values predicted by the empirical pseudopotential calculations. Finally, I study excitonic properties of alloyed InAsP quantum dots and demonstrate that alloying effects can significantly reduce fine-structure splitting even in significantly elongated quantum dots.

  10. Nanoscale interfaces in hybrid materials for exciton fission and fusion (Conference Presentation)

    Science.gov (United States)

    Bardeen, Christopher J.

    2016-09-01

    The ability to downconvert (1 photon to 2 photons) and upconvert (2 photons to 1 photon) energy can have applications in many fields, including solar energy. Singlet fission provides a way to convert one photon into a pair of triplet excitons. It occurs efficiently in organic semiconductors, but the question remains how to extract the triplet excitons in a useful form. In this talk, we will describe efforts to transform triplet excitons into other forms through energy transfer into inorganic semiconductors like silicon. Heterogeneous solid-liquid approaches to use spin-orbit coupling to enhance the triplet excitons' oscillator strength so they can emit photons will also be described. The solid-solid and solid-liquid interface appears to be critical for these schemes to succeed. Upconversion occurs via the reverse process, where a pair of triplet excitons fuse into a high-energy singlet state. A new approach to triplet state sensitization involves absorption of low energy photons by the semiconductor nanocrystals followed by energy transfer to the molecular triplet states. These states can then undergo triplet-triplet annihilation to create high energy singlet states that emit upconverted light in the visible and ultraviolet regions. By using conjugated organic ligands to form an energy cascade, the upconversion can be enhanced by up to three orders of magnitude. The mechanism of the nanocrystal-to-triplet energy transfer is investigated using time-resolved spectroscopy. Again, the role of organic ligand-inorganic surface interactions is important for determining the ultimate efficiency.

  11. Measuring Exciton Diffusion in Conjugated Polymer Films with Super-resolution Microscopy

    Science.gov (United States)

    Penwell, Samuel; Ginsberg, Lucas; Noriega Manez, Rodrigo; Ginsberg, Naomi

    2015-03-01

    Conjugated polymers are highly tunable organic semiconductors, which can be solution processed to form thin films, making them prime candidates for organic photovoltaic devices. One of the most important parameters in a conjugated polymer solar cell is the exciton diffusion length, which depends on intermolecular couplings, and is typically on the order of 10 nm. This mean exciton migration can vary dramatically between films and within a single film due to heterogeneities in morphology on length scales of 10's to 100's nm. To study the variability of exciton diffusion and morphology within individual conjugated polymer films, we are adapting stimulated emission depletion microscopy. STED is typically used in biology with well-engineered fluorescent labels or on NV-centers in diamond. I will, however, describe how we have demonstrated STED in conjugated polymer films of MEH-PPV and CN-PPV by taking care to first understand the film's photophysical properties. This new approach provides a way to study exciton diffusion by utilizing subdiffraction optical excitation volumes. In this way, we will obtain a spatiotemporal map of exciton distributions that will help to correlate the energetic landscape to film morphology at the nanoscale. This research is supported in part by the Department of Energy Office of Science Graduate Fellowship Program (DOE SCGF), made possible in part by the American Recovery and Reinvestment Act of 2009, administered by ORISE-ORAU under Contract No. DE-AC05-06.

  12. The effective excitonic g factors of Mn-doped InAs nanowires

    Science.gov (United States)

    Xiong, Wen

    2017-04-01

    Based on the derived eight-band k · p Hamiltonian, the electronic structures of Mn-doped InAs nanowires in the magnetic field are calculated. We find the lowest optical transition will be split to four individual transitions when the magnetic field is applied along z axis, and two of them are σ polarized light. Furthermore, the Zeeman splitting energy at the Γ point of two σ polarized light will increase nonlinearly as the increase of the magnetic field. Additionally, an effective excitonic g factor at the Γ point is defined, and the effective excitonic g factors will decrease greatly with the increase of the radius of nanowires and the decrease of the concentration of manganese ions, while the effective excitonic g factors decrease slightly when the magnetic field increases. Interestingly, the effective excitonic g factors can experience a substantial decrease when the temperature increases from 10 K to 100 K and is almost not affected when the temperature varies from 100 K to 300 K. Therefore, we can infer that large effective excitonic g factors can be obtained when small radius of nanowires, high concentration of manganese ions and low temperature are satisfied.

  13. Supersonic exciton gratings: coherent inter-polariton scattering in semiconductor microcavities

    DEFF Research Database (Denmark)

    Birkedal, Dan; Vadim, Lyssenko; Hvam, Jørn Märcher

    2002-01-01

    We report on a coherent nonlinear phenomenon in a semiconductor microcavity (SMC), which has no parallel for QW excitons. When two different polariton modes of the SMC are impulsively excited they undergo normal mode oscillations (NMOs) with coherent energy exchange between the exciton and the ca......We report on a coherent nonlinear phenomenon in a semiconductor microcavity (SMC), which has no parallel for QW excitons. When two different polariton modes of the SMC are impulsively excited they undergo normal mode oscillations (NMOs) with coherent energy exchange between the exciton...... and the cavity mode. In our experiment the two polaritons are excited with slightly different angles resulting in a travelling wave exciton grating. When a test polariton mode is excited it will scatter in the travelling grating producing amplitude modulation sidebands. This phenomenon produces a transient four......-wave mixing (TFWM) signal, which is shifted in frequency from that of the test beam by the NMO frequency, in our case, in the THz range corresponding to a grating velocity = 1 /spl times/ 10/sup 7/ m/s, which is four orders of magnitude larger than the sound velocity. The sample under investigation is a Ga...

  14. Giant bandgap renormalization and excitonic effects in a monolayer transition metal dichalcogenide semiconductor.

    Science.gov (United States)

    Ugeda, Miguel M; Bradley, Aaron J; Shi, Su-Fei; da Jornada, Felipe H; Zhang, Yi; Qiu, Diana Y; Ruan, Wei; Mo, Sung-Kwan; Hussain, Zahid; Shen, Zhi-Xun; Wang, Feng; Louie, Steven G; Crommie, Michael F

    2014-12-01

    Two-dimensional (2D) transition metal dichalcogenides (TMDs) are emerging as a new platform for exploring 2D semiconductor physics. Reduced screening in two dimensions results in markedly enhanced electron-electron interactions, which have been predicted to generate giant bandgap renormalization and excitonic effects. Here we present a rigorous experimental observation of extraordinarily large exciton binding energy in a 2D semiconducting TMD. We determine the single-particle electronic bandgap of single-layer MoSe2 by means of scanning tunnelling spectroscopy (STS), as well as the two-particle exciton transition energy using photoluminescence (PL) spectroscopy. These yield an exciton binding energy of 0.55 eV for monolayer MoSe2 on graphene—orders of magnitude larger than what is seen in conventional 3D semiconductors and significantly higher than what we see for MoSe2 monolayers in more highly screening environments. This finding is corroborated by our ab initio GW and Bethe-Salpeter equation calculations which include electron correlation effects. The renormalized bandgap and large exciton binding observed here will have a profound impact on electronic and optoelectronic device technologies based on single-layer semiconducting TMDs.

  15. Dynamical Process of Dissociation of Excitons in Polymer Chains with Impurities

    Institute of Scientific and Technical Information of China (English)

    ZHAO Hong-Xia; ZHAO Hui; CHEN Yu-Guang

    2011-01-01

    @@ Within an extended Su-Schrieffer-Heeger model including impurity interactions,the dynamical process of exciton dissociation in the presence of an external electric field is investigated by using a non-adiabatic evolution method Under the action of impurities,the stability as well as the effective mass of the exciton is reduced.Our results show that the field required to dissociate the excitons depends sensitively on the strength of the impurity potential.As the impurity potential strength increases,the dissociation field decreases effectively.The theoretical results are expected to provide useful predictions concerning which polymers with properly impurity-assisted interactions are likely to be more suitable for use in organic solar cells.%Within an extended Su-Schrieffer-Heeger model including impurity interactions, the dynamical process ofexciton dissociation in the presence of an external electric field is investigated by using a non-adiabatic evolution method. Under the action of impurities, the stability as well as the effective mass of the exciton is reduced. Our results show that the field required to dissociate the excitons depends sensitively on the strength of the impurity potential. As the impurity potential strength increases, the dissociation field decreases effectively. The theoretical results are expected to provide useful predictions concerning which polymers with properly impurity-assisted interactions are likely to be more suitable for use in organic solar cells.

  16. Exciton dynamics in a site-controlled quantum dot coupled to a photonic crystal cavity

    Energy Technology Data Exchange (ETDEWEB)

    Jarlov, C., E-mail: clement.jarlov@epfl.ch; Lyasota, A.; Ferrier, L.; Gallo, P.; Dwir, B.; Rudra, A.; Kapon, E. [Laboratory of Physics of Nanostructures, Ecole Polytechnique Fédérale de Lausanne (EPFL), CH-1015 Lausanne (Switzerland)

    2015-11-09

    Exciton and cavity mode (CM) dynamics in site-controlled pyramidal quantum dots (QDs), integrated with linear photonic crystal membrane cavities, are investigated for a range of temperatures and photo-excitation power levels. The absence of spurious multi-excitonic effects, normally observed in similar structures based on self-assembled QDs, permits the observation of effects intrinsic to two-level systems embedded in a solid state matrix and interacting with optical cavity modes. The coupled exciton and CM dynamics follow the same trend, indicating that the CM is fed only by the exciton transition. The Purcell reduction of the QD and CM decay times is reproduced well by a theoretical model that includes exciton linewidth broadening and temperature dependent non-radiative processes, from which we extract a Purcell factor of 17 ± 5. For excitation powers above QD saturation, we show the influence of quantum wire barrier states at short delay time, and demonstrate the absence of multiexcitonic background emission.

  17. Ultrafast exciton migration in an HJ-aggregate: Potential surfaces and quantum dynamics

    Science.gov (United States)

    Binder, Robert; Polkehn, Matthias; Ma, Tianji; Burghardt, Irene

    2017-01-01

    Quantum dynamical and electronic structure calculations are combined to investigate the mechanism of exciton migration in an oligothiophene HJ aggregate, i.e., a combination of oligomer chains (J-type aggregates) and stacked aggregates of such chains (H-type aggregates). To this end, a Frenkel exciton model is parametrized by a recently introduced procedure [Binder et al., J. Chem. Phys. 141, 014101 (2014)] which uses oligomer excited-state calculations to perform an exact, point-wise mapping of coupled potential energy surfaces to an effective Frenkel model. Based upon this parametrization, the Multi-Layer Multi-Configuration Time-Dependent Hartree (ML-MCTDH) method is employed to investigate ultrafast dynamics of exciton transfer in a small, asymmetric HJ aggregate model composed of 30 sites and 30 active modes. For a partially delocalized initial condition, it is shown that a torsional defect confines the trapped initial exciton, and planarization induces an ultrafast resonant transition between an HJ-aggregated segment and a covalently bound "dangling chain" end. This model is a minimal realization of experimentally investigated mixed systems exhibiting ultrafast exciton transfer between aggregated, highly planarized chains and neighboring disordered segments.

  18. 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.

  19. 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.

  20. Electronic, bonding, and optical properties of 1d [CuCN]n (n = 1-10) chains, 2d [CuCN]n (n = 2-10) nanorings, and 3d [Cun (CN)n ]m (n = 4, m = 2, 3; n = 10, m = 2) tubes studied by DFT/TD-DFT methods.

    Science.gov (United States)

    Tsipis, Athanassios C; Stalikas, Alexandros V

    2015-06-30

    The electronic, bonding, and photophysical properties of one-dimensional [CuCN](n) (n = 1-10) chains, 2-D [CuCN](n) (n = 2-10) nanorings, and 3-D [Cu(n)(CN)(n)](m) (n = 4, m = 2, 3; n = 10, m = 2) tubes are investigated by means of a multitude of computational methodologies using density functional theory (DFT) and time-dependent-density-functional theory (TD-DFT) methods. The calculations revealed that the 2-D [CuCN](n) (n = 2-10) nanorings are more stable than the respective 1-D [CuCN](n) (n = 2-10) linear chains. The 2-D [CuCN](n) (n = 2-10) nanorings are predicted to form 3-D [Cun (CN)(n)](m) (n = 4, m = 2, 3; n = 10, m = 2) tubes supported by weak stacking interactions, which are clearly visualized as broad regions in real space by the 3D plots of the reduced density gradient. The bonding mechanism in the 1-D [CuCN](n) (n = 1-10) chains, 2-D [CuCN](n) (n = 2-10) nanorings, and 3-D [Cu(n)(CN)(n)](m) (n = 4, m = 2, 3; n = 10, m = 2) tubes are easily recognized by a multitude of electronic structure calculation approaches. Particular emphasis was given on the photophysical properties (absorption and emission spectra) of the [CuCN](n) chains, nanorings, and tubes which were simulated by TD-DFT calculations. The absorption and emission bands in the simulated TD-DFT absorption and emission spectra have thoroughly been analyzed and assignments of the contributing principal electronic transitions associated to individual excitations have been made.

  1. Controlling excitons. Concepts for phosphorescent organic LEDs at high brightness

    Energy Technology Data Exchange (ETDEWEB)

    Reineke, Sebastian

    2009-11-15

    This work focusses on the high brightness performance of phosphorescent organic light-emitting diodes (OLEDs). The use of phosphorescent emitter molecules in OLEDs is essential to realize internal electron-photon conversion efficiencies of 100 %. However, due to their molecular nature, the excited triplet states have orders of magnitude longer time constants compared to their fluorescent counterparts which, in turn, strongly increases the probability of bimolecular annihilation. As a consequence, the efficiencies of phosphorescent OLEDs decline at high brightness - an effect known as efficiency roll-off, for which it has been shown to be dominated by triplet-triplet annihilation (TTA). In this work, TTA of the archetype phosphorescent emitter Ir(ppy){sub 3} is investigated in time-resolved photoluminescence experiments. For the widely used mixed system CBP:Ir(ppy){sub 3}, host-guest TTA - an additional unwanted TTA channel - is experimentally observed at high excitation levels. By using matrix materials with higher triplet energies, this effect is efficiently suppressed, however further studies show that the efficiency roll-off of Ir(ppy)3 is much more pronounced than predicted by a model based on Foerster-type energy transfer, which marks the intrinsic limit for TTA. These results suggest that the emitter molecules show a strong tendency to form aggregates in the mixed film as the origin for enhanced TTA. Transmission electron microscopy images of Ir(ppy){sub 3} doped mixed films give direct proof of emitter aggregates. Based on these results, two concepts are developed that improve the high brightness performance of OLEDs. In a first approach, thin intrinsic matrix interlayers are incorporated in the emission layer leading to a one-dimensional exciton confinement that suppresses exciton migration and, consequently, TTA. The second concept reduces the efficiency roll-off by using an emitter molecule with slightly different chemical structure, i.e. Ir(ppy){sub 2

  2. Exciton mechanisms and modeling of the ionoluminescence in silica

    Science.gov (United States)

    Bachiller-Perea, D.; Jiménez-Rey, D.; Muñoz-Martín, A.; Agulló-López, F.

    2016-03-01

    A theoretical model is presented in order to discuss detailed kinetic data describing the evolution of the two main ionoluminescence bands at 650 nm (1.9 eV) and 460 nm (2.7 eV) in silica as a function of the irradiation fluence at room temperature. The model is based on the generation of self-trapped excitons (STEs), their hopping migration through the silica network and their recombination at non-bridging oxygen hole and Type II oxygen-deficient centers to produce the red and blue emission bands, respectively. For heavy ions, which have a high electronic stopping power, the two emission yields experience a fast initial growth with fluence up to a maximum value and then decrease at a fairly comparable rate. The fluence for such a maximum strongly increases on decreasing ion mass and stopping power and, finally, for H and He it is not observed for any of the investigated energy and fluence range. This kinetic behavior is explained in terms of the strong structural distortions (compaction) induced by the heavy-ion irradiations. In particular, it is proposed that these strong structural distortions cause a significant decrease in the STE migration length and, consequently, in the recombination rates at the two active recombination centers. The model offers a good quantitative accordance with detailed infrared spectroscopy reporting on the changes in the frequency ω 4 of a first-order vibrational mode in the SiO2 network as a function of irradiation fluence.

  3. Metastable states in magnetic nanorings

    DEFF Research Database (Denmark)

    Castaño, F. J.; Ross, C. A.; Frandsen, Cathrine;

    2003-01-01

    Magnetization states and hysteresis behavior of small ferromagnetic rings, of diameters 180-520 nm, have been investigated using magnetic force microscopy. In addition to the expected bi-domain ("onion") and flux-closed ("vortex") magnetization states, a metastable state has been found...

  4. Stimulated emission of free excitons in Cd{sub 1-x}Mn{sub x}Te under nonresonant two-photon excitation

    Energy Technology Data Exchange (ETDEWEB)

    Jang, J.I. [Department of Physics and Astronomy, Northwestern University, 2145 Sheridan Road, Evanston, IL 60208 (United States)], E-mail: joon-jang@northwestern.edu; Mani, S.; Ketterson, J.B. [Department of Physics and Astronomy, Northwestern University, 2145 Sheridan Road, Evanston, IL 60208 (United States); Park, H.Y. [Department of Semiconductor Applications, Ulsan College, San 29 Mugeo Dong, Ulsan 680-749 (Korea, Republic of)], E-mail: hypark@mail.uc.ac.kr

    2008-08-25

    We report on free excitons coexisting with exciton magnetic polarons (EMPs) in bulk semimagnetic semiconductors of Cd{sub 1-x}Mn{sub x}Te for 0.04{<=}x{<=}0.36 at 2 K under nonresonant two-photon excitation. This two-photon excitation not only generates free excitons but also more efficiently creates EMPs compared with ordinary one-photon excitation. Stimulated emission from free excitons is demonstrated under strong two-photon excitation.

  5. Exciton fine structure splitting in InP quantum dots in GaInP.

    Science.gov (United States)

    Ellström, C; Seifert, W; Pryor, C; Samuelson, L; Pistol, M-E

    2007-07-25

    We have investigated the electronic structure of excitons in InP quantum dots in GaInP. The exciton is theoretically expected to have four states. Two of the states are allowed to optically decay to the ground (vacuum) state in the dipole approximation. We see these two lines in photoluminescence (PL) experiments and find that the splitting between the lines (the fine structure splitting) is 150(± 30) µeV. The lines were perpendicularly polarized. We verified that the lines arise from neutral excitons by using correlation spectroscopy. The theoretical calculations show that the polarization of the emission lines are along and perpendicular to the major axis of elongated dots. The fine structure splitting depends on the degree of elongation of the dots and is close to zero for dots of cylindrical symmetry, despite the influence of the piezoelectric polarization, which is included in the calculation.

  6. Van der Waals Interactions among Alkali Rydberg Atoms with Excitonic States

    CERN Document Server

    Zoubi, Hashem

    2015-01-01

    We investigate the influence of the appearance of excitonic states on van der Waals interactions among two Rydberg atoms. The atoms are assumed to be in different Rydberg states, e.g., in the $|ns\\rangle$ and $|np\\rangle$ states. The resonant dipole-dipole interactions yield symmetric and antisymmetric excitons, with energy splitting that give rise to new resonances as the atoms approach each other. Only far from these resonances the van der Waals coefficients, $C_6^{sp}$, can be defined. We calculate the $C_6$ coefficients for alkali atoms and present the results for lithium by applying perturbation theory. At short interatomic distances of several $\\mu m$, we show that the widely used simple model of two-level systems for excitons in Rydberg atoms breaks down, and the correct representation implies multi-level atoms. Even though, at larger distances one can keep the two-level systems but in including van der Waals interactions among the atoms.

  7. Splitting between bright and dark excitons in transition metal dichalcogenide monolayers

    Science.gov (United States)

    Echeverry, J. P.; Urbaszek, B.; Amand, T.; Marie, X.; Gerber, I. C.

    2016-03-01

    The optical properties of transition metal dichalcogenide monolayers such as the two-dimensional semiconductors MoS2 and WSe2 are dominated by excitons, Coulomb bound electron-hole pairs. The light emission yield depends on whether the electron-hole transitions are optically allowed (bright) or forbidden (dark). By solving the Bethe-Salpeter equation on top of G W wave functions in density functional theory calculations, we determine the sign and amplitude of the splitting between bright and dark exciton states. We evaluate the influence of the spin-orbit coupling on the optical spectra and clearly demonstrate the strong impact of the intra-valley Coulomb exchange term on the dark-bright exciton fine structure splitting.

  8. Probing ultrafast energy transfer between excitons and plasmons in the ultrastrong coupling regime

    Science.gov (United States)

    Balci, Sinan; Kocabas, Coskun; Küçüköz, Betül; Karatay, Ahmet; Akhüseyin, Elif; Gul Yaglioglu, H.; Elmali, Ayhan

    2014-08-01

    We investigate ultrafast energy transfer between excitons and plasmons in ensembles of core-shell type nanoparticles consisting of metal core covered with a concentric thin J-aggregate (JA) shell. The high electric field localization by the Ag nanoprisms and the high oscillator strength of the JAs allow us to probe this interaction in the ultrastrong plasmon-exciton coupling regime. Linear and nonlinear optical properties of the coupled system have been measured using transient absorption spectroscopy revealing that the hybrid system shows half-plasmonic and half-excitonic properties. The tunability of the nanoprism plasmon resonance provides a flexible platform to study the dynamics of the hybrid state in a broad range of wavelengths.

  9. Poly-(3-hexylthiophene) Aggregate Formation in Binary Solvent Mixtures: An Excitonic Coupling Analysis

    Science.gov (United States)

    Boucher, David; Johnson, Calynn

    2014-03-01

    We have studied the aggregation behavior of P3HT [Mn ~ 28.2 kDa, regioregularity >96 %, PDI ~ 1.3] in 96 solvent mixtures is studied using UV-Vis absorption spectroscopy. We used Hansen solubility parameters (HSPs) and Spano excitonic coupling analyses to identify correlations between the properties of the solvent mixtures and the extent of structural order of the aggregates. It is clear that the identity of the poor solvent used to drive aggregation has a significant impact on the excitonic coupling behavior and, hence, the structural order of the P3HT aggregates. However, solubility parameter theory does not account nor provide a predictive theory for the observed trends. Instead, qualitative arguments based on the nature of the interactions between the solvents and the polythiophene and hexyl side chain motifs are used to rationalize the kinetics of formation and the observed excitonic coupling characteristics of the P3HT aggregates.

  10. Femtosecond study of exciton dynamics in polyfluorene statistical copolymers in solutions and thin films

    Science.gov (United States)

    Zhang, Jin Z.; Kreger, Melissa A.; Klaerner, Gerrit; Kreyenschmidt, M.; Miller, Robert D.; Scott, J. Campbell

    1997-12-01

    The formation and decay dynamics of photogenerated excitons in polyfluorene statistical co-polymers in solutions and in thin films have been studied using femtosecond transient absorption spectroscopy. In solution photoexcitation of the polymer generates primarily intrachain singlet excitons which are initially hot and then relax quickly (polaron pairs in films at low intensities. At high intensities, the possibility cannot be ruled out completely, especially in relation to the fast decay. If bound polaron pairs are formed as indicated by the fast decay, they must be generated as a result of interaction between excitons on different chains since they are absent at low power, an they must be created and then decay within about 1 ps.

  11. Excitonic luminescence of SiGe/Si quantum wells δ-doped with boron

    Energy Technology Data Exchange (ETDEWEB)

    Bagaev, V. S.; Nikolaev, S. N.; Onishchenko, E. E.; Pruchkina, A. A. [P.N. Lebedev Physical Institute, Russian Academy of Sciences, Moscow (Russian Federation); Krivobok, V. S., E-mail: krivobok@lebedev.ru [P.N. Lebedev Physical Institute, Russian Academy of Sciences, Moscow (Russian Federation); Moscow Institute of Physics and Technology (State University), Dolgoprudny, Moscow Region (Russian Federation); Novikov, A. V. [Institute for Physics of Microstructures Russian Academy of Sciences, Nizhny Novgorod (Russian Federation); Lobachevsky State University of Nizhni Novgorod, Nizhny Novgorod (Russian Federation)

    2015-05-14

    Low-temperature photoluminescence of undoped and moderately δ-doped Si{sub 1−x}Ge{sub x}/Si (x < 0.1) quantum wells has been studied. The influence of boron δ-layer on the excitonic luminescence and the luminescence caused by a dense electron plasma was demonstrated. The conditions under which the luminescence spectra of quantum wells are dominated by impurity-bound excitons (BE) have been established. Some unusual properties of these BE are explained in terms of type II band-offset in Si{sub 1−x}Ge{sub x}/Si (x < 0.1) quantum wells, which favors a spatial separation of electrons and holes. It is shown that the temperature dependence of an excitonic emission in the quantum wells allows to calculate the BE-related density of states and, thus, can be used for contactless estimation of the impurity concentration in quantum wells.

  12. 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.

  13. Suppression of population transport and control of exciton distributions by entangled photons.

    Science.gov (United States)

    Schlawin, Frank; Dorfman, Konstantin E; Fingerhut, Benjamin P; Mukamel, Shaul

    2013-01-01

    Entangled photons provide an important tool for secure quantum communication, computing and lithography. Low intensity requirements for multi-photon processes make them idealy suited for minimizing damage in imaging applications. Here we show how their unique temporal and spectral features may be used in nonlinear spectroscopy to reveal properties of multiexcitons in chromophore aggregates. Simulations demostrate that they provide unique control tools for two-exciton states in the bacterial reaction centre of Blastochloris viridis. Population transport in the intermediate single-exciton manifold may be suppressed by the absorption of photon pairs with short entanglement time, thus allowing the manipulation of the distribution of two-exciton states. The quantum nature of the light is essential for achieving this degree of control, which cannot be reproduced by stochastic or chirped light. Classical light is fundamentally limited by the frequency-time uncertainty, whereas entangled photons have independent temporal and spectral characteristics not subjected to this uncertainty.

  14. Optical spectrum of MoS2: many-body effects and diversity of exciton states.

    Science.gov (United States)

    Qiu, Diana Y; da Jornada, Felipe H; Louie, Steven G

    2013-11-22

    We present first-principles calculations of the optical response of monolayer molybdenum disulfide employing the GW-Bethe-Salpeter equation (GW-BSE) approach including self-energy, excitonic, and electron-phonon effects. We show that monolayer MoS2 possesses a large and diverse number of strongly bound excitonic states with novel k-space characteristics that were not previously seen experimentally or theoretically. The absorption spectrum is shown to be dominated by excitonic states with a binding energy close to 1 eV and by strong electron-phonon broadening in the visible to ultraviolet range. Our results explain recent experimental measurements and resolve inconsistencies between previous GW-BSE calculations.

  15. Fluctuating exciton localisation in giant pi-conjugated spoked-wheel macrocycles

    CERN Document Server

    Aggarwal, Vikas; Idelson, Alissa; Kalle, Daniel; Wuersch, Dominik; Stang, Thomas; Steiner, Florian; Jester, Stefan-S; Vogelsang, Jan; Hoeger, Sigurd; Lupton, John M

    2015-01-01

    Conjugated polymers offer potential for many diverse applications but we still lack a fundamental microscopic understanding of their electronic structure. Elementary photoexcitations - excitons - span only a few nanometres of a molecule, which itself can extend over microns, and how their behaviour is affected by molecular dimensions is not fully understood. For example, where is the exciton formed within a conjugated segment, is it always situated on the same repeat units? Here, we introduce structurally-rigid molecular spoked wheels, 6 nanometres in diameter, as a model of extended pi-conjugation. Single-molecule fluorescence reveals random exciton localisation, leading to temporally-varying emission polarisation. Initially, this random localisation arises after every photon absorption event because of temperature independent spontaneous symmetry breaking. These fast fluctuations are slowed to millisecond timescales following prolonged illumination. Intramolecular heterogeneity is revealed in cryogenic spec...

  16. Exciton-photon coupling in a ZnSe based microcavity fabricated using epitaxial liftoff

    CERN Document Server

    Curran, A; Morrod, J K; Prior, K A; Warburton, R J

    2007-01-01

    We report the observation of strong exciton-photon coupling in a ZnSe based microcavity fabricated using epitaxial liftoff. Molecular beam epitaxial grown ZnSe/Zn$_{0.9}$Cd$_{0.1}$Se quantum wells with a one wavelength optical length at the exciton emission were transferred to a SiO$_2$/Ta$_2$O$_5$ mirror with a reflectance of 96% to form finesse matched microcavities. Analysis of our angle resolved transmission spectra reveals key features of the strong coupling regime: anticrossing with a normal mode splitting of $23.6 meV$ at $20 K$; composite evolution of the lower and upper polaritons; and narrowing of the lower polariton linewidth near resonance. The heavy hole exciton oscillator strength per quantum well is also deduced to be $1.78 \\times 10^{13} cm^{-2}$.

  17. Relaxation dynamics and exciton energy transfer in the low-temperature phase of MEH-PPV

    Energy Technology Data Exchange (ETDEWEB)

    Consani, Cristina; Koch, Federico [Institut für Physikalische und Theoretische Chemie, Universität Würzburg, Am Hubland, 97074 Würzburg (Germany); Panzer, Fabian; Unger, Thomas; Köhler, Anna [Lehrstuhl Experimentalphysik II, Universität Bayreuth, Universitätsstraße 30, 95440 Bayreuth (Germany); Brixner, Tobias, E-mail: brixner@phys-chemie.uni-wuerzburg.de [Institut für Physikalische und Theoretische Chemie, Universität Würzburg, Am Hubland, 97074 Würzburg (Germany); Center for Nanosystems Chemistry (CNC), Universität Würzburg, Am Hubland, 97074 Würzburg (Germany)

    2015-06-07

    Understanding the effects of aggregation on exciton relaxation and energy transfer is relevant to control photoinduced function in organic electronics and photovoltaics. Here, we explore the photoinduced dynamics in the low-temperature aggregated phase of a conjugated polymer by transient absorption and coherent electronic two-dimensional (2D) spectroscopy. Coherent 2D spectroscopy allows observing couplings among photoexcited states and discriminating band shifts from homogeneous broadening, additionally accessing the ultrafast dynamics at various excitation energies simultaneously with high spectral resolution. By combining the results of the two techniques, we differentiate between an initial exciton relaxation, which is not characterized by significant exciton mobility, and energy transport between different chromophores in the aggregate.

  18. Exciton quenching at PEDOT:PSS anode in polymer blue-light-emitting diodes

    Energy Technology Data Exchange (ETDEWEB)

    Abbaszadeh, D.; Wetzelaer, G. A. H. [Molecular Electronics, Zernike Institute for Advanced Materials, University of Groningen, Nijenborgh 4, 9747 AG, Groningen (Netherlands); Dutch Polymer Institute, P.O. Box 902, 5600 AX, Eindhoven (Netherlands); Nicolai, H. T. [TNO/Holst Centre, High Tech Campus 31, 5605 KN, Eindhoven (Netherlands); Blom, P. W. M., E-mail: blom@mpip-mainz.mpg.de [Max Planck Institute for Polymer Research, Ackermannweg 10, 55128 Mainz (Germany); Department of Physics, Faculty of Science, King Abdulaziz University, Jeddah (Saudi Arabia)

    2014-12-14

    The quenching of excitons at the poly(3,4-ethylenedioxythiophene):poly(styrenesulfonic acid) (PEDOT:PSS) anode in blue polyalkoxyspirobifluorene-arylamine polymer light-emitting diodes is investigated. Due to the combination of a higher electron mobility and the presence of electron traps, the recombination zone shifts from the cathode to the anode with increasing voltage. The exciton quenching at the anode at higher voltages leads to an efficiency roll-off. The voltage dependence of the luminous efficiency is reproduced by a drift-diffusion model under the condition that quenching of excitons at the PEDOT:PSS anode and metallic cathode is of equal strength. Experimentally, the efficiency roll-off at high voltages due to anode quenching is eliminated by the use of an electron-blocking layer between the anode and the light-emitting polymer.

  19. Coherent Exciton and Biexciton Nonlinearities in Semiconductor Nanostructures: Effects of Disorder

    DEFF Research Database (Denmark)

    Langbein, Wolfgang; Borri, Paola; Hvam, Jørn Märcher

    1999-01-01

    The coherent response of excitons in semiconductor nanostructures measured in four-wave mixing (FWM) depends strongly on the inhomogenous broadening of the exciton transition. We investigate InAs/Al0.3Ga0.7As single quantum wells (SQW) and AlxGa1-xAs mixed crystals. Additional to the usual phase......-exciton-states. Here, the third-order polarization at X-XX is not at the same resonance as the first-order polarization at 0-X. Consequently, the rephasing of the microscopic third-order polarization to the macroscopic FWM photon echo is blurred by the non-perfect correlation of X and XX energies, leading to a fast...

  20. Decay of the resonance fluorescence following pulsed excitation of a weakly disordered excitonic system

    Science.gov (United States)

    Boukahil, A.; Huber, D. L.

    1993-12-01

    A study is made of the decay of the resonance fluorescence following pulsed excitation of a weakly disordered system whose optical excitations are Frenkel excitons. The disorder is characterized by a Gaussian distribution of optical transition frequencies with no correlation between different sites. The duration of the resonant pulse is taken to be short in comparison with the reciprocal of the optical linewidth, and the wavelength of the light is assumed to be large in comparison with either the size of the array or the exciton mean free path associated with the disorder. In the limit where σ, the standard deviation of the Gaussian distribution, is much less than the exciton bandwidth, the integrated intensity of the fluorescence decays non-exponentially and is characterized by universal functions of σ xt, where x= 4/3, 2, and 4 in one, two, and three dimensions, respectively. Analytic approximations to the scaling functions in two and three dimensions are presented.

  1. Excitonic spectra and energy band structure of ZnAl2Se4 crystals

    Science.gov (United States)

    Syrbu, N. N.; Zalamai, V. V.; Tiron, A. V.; Tiginyanu, I. M.

    2015-11-01

    Absorption, reflection and wavelength modulated reflection spectra were investigated in ZnAl2Se4 crystals. The energy positions of ground and excited states for three excitonic series (A, B and C) were determined. The main parameters of excitons and more precise values of energy intervals V1(Γ7)-C1(Γ6), V2(Γ6)-C1(Γ6), and V3(Γ7)-C1(Γ6) were estimated. Values of splitting due to crystal field and spin-orbital interaction were calculated. Effective masses of electrons (mC1∗) and holes (mV1∗, mV2∗, mV3∗) were estimated. Reflection spectra contours in excitonic region were calculated using dispersion equations. Optical functions for E > Eg from measured reflection spectra were assigned on the base of Kramers-Kronig relations.

  2. An exciton-polariton laser based on biologically produced fluorescent protein

    Science.gov (United States)

    Dietrich, Christof P.; Steude, Anja; Tropf, Laura; Schubert, Marcel; Kronenberg, Nils M.; Ostermann, Kai; Höfling, Sven; Gather, Malte C.

    2016-01-01

    Under adequate conditions, cavity polaritons form a macroscopic coherent quantum state, known as polariton condensate. Compared to Wannier-Mott excitons in inorganic semiconductors, the localized Frenkel excitons in organic emitter materials show weaker interaction with each other but stronger coupling to light, which recently enabled the first realization of a polariton condensate at room temperature. However, this required ultrafast optical pumping, which limits the applications of organic polariton condensates. We demonstrate room temperature polariton condensates of cavity polaritons in simple laminated microcavities filled with biologically produced enhanced green fluorescent protein (eGFP). The unique molecular structure of eGFP prevents exciton annihilation even at high excitation densities, thus facilitating polariton condensation under conventional nanosecond pumping. Condensation is clearly evidenced by a distinct threshold, an interaction-induced blueshift of the condensate, long-range coherence, and the presence of a second threshold at higher excitation density that is associated with the onset of photon lasing. PMID:27551686

  3. Strong coupling of two interacting excitons confined in a nanocavity-quantum dot system

    Energy Technology Data Exchange (ETDEWEB)

    Cardenas, Paulo C; RodrIguez, Boris A [Instituto de Fisica, Universidad de Antioquia, AA 1226 MedellIn (Colombia); Quesada, Nicolas [McLennan Physical Laboratories, University of Toronto, 60 St George Street, Toronto, ON, M5S 1A7 (Canada); Vinck-Posada, Herbert, E-mail: pcardenas@fisica.udea.edu.co [Departamento de Fisica, Universidad Nacional de Colombia, Ciudad Universitaria, Bogota (Colombia)

    2011-07-06

    We present a study of the strong coupling between radiation and matter, considering a system of two quantum dots, which are in mutual interaction and interact with a single mode of light confined in a semiconductor nanocavity. We take into account dissipative mechanisms such as the escape of the cavity photons, decay of the quantum dot excitons by spontaneous emission, and independent exciton pumping. It is shown that the mutual interaction between the dots can be measured off-resonance only if the strong coupling condition is reached. Using the quantum regression theorem, a reasonable definition of the dynamical coupling regimes is introduced in terms of the complex Rabi frequency. Finally, the emission spectrum for relevant conditions is presented and compared with the above definition, demonstrating that the interaction between the excitons does not affect the strong coupling.

  4. 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.

  5. Quantum-Confinement Effects on Binding Energies and Optical Properties of Excitons in Quantum Dots

    Institute of Scientific and Technical Information of China (English)

    潘晖

    2004-01-01

    Quantum-confinement effects on the binding energy and the linear optical susceptibility of excitons in quantum dots are studied. It is found that the binding energy and the linear optical susceptibility are sensitive to the barrier height and the dot size. For an infinite barrier, the binding energy of excitons decreases monotonically with the increasing dot radius, and the absorption intensity has almost the same amplitude with the increasing photon energy. For a finite barrier, the binding energy has a maximum value with the increasing dot radius, and the absorption intensity damps rapidly with the increasing photon energy. The effective mass ratio is also found to have an influence on the binding energy. The results could be confirmed by future experiments on excitons in quantum dots.

  6. Two's Company, Three's a Crowd: Exciton Localization in Cofacially Arrayed Polyfluorenes.

    Science.gov (United States)

    Talipov, Marat R; Ivanov, Maxim V; Reid, Scott A; Rathore, Rajendra

    2016-08-01

    Understanding the mechanisms of long-range energy transfer through polychromophoric assemblies is critically important in photovoltaics and biochemical systems. Using a set of cofacially arrayed polyfluorenes (Fn), we investigate the mechanism of (singlet) exciton delocalization in π-stacked polychromophoric assemblies. Calculations reveal that effective stabilization of an excimeric state requires an ideal sandwich-like arrangement; yet surprisingly, emission spectroscopy indicates that exciton delocalization is limited to only two fluorene units for all n. Herein, we show that delocalization is determined by the interplay between the energetic gain from delocalization, which quickly saturates beyond two units in larger Fn, and an energetic penalty associated with structural reorganization, which increases linearly with n. With these insights, we propose a hopping mechanism for exciton transfer, based upon the presence of multiple excimeric tautomers of similar energy in larger polyfluorenes (n ≥ 4) together with the anticipated low thermal barrier of their interconversion.

  7. An exciton-polariton laser based on biologically produced fluorescent protein.

    Science.gov (United States)

    Dietrich, Christof P; Steude, Anja; Tropf, Laura; Schubert, Marcel; Kronenberg, Nils M; Ostermann, Kai; Höfling, Sven; Gather, Malte C

    2016-08-01

    Under adequate conditions, cavity polaritons form a macroscopic coherent quantum state, known as polariton condensate. Compared to Wannier-Mott excitons in inorganic semiconductors, the localized Frenkel excitons in organic emitter materials show weaker interaction with each other but stronger coupling to light, which recently enabled the first realization of a polariton condensate at room temperature. However, this required ultrafast optical pumping, which limits the applications of organic polariton condensates. We demonstrate room temperature polariton condensates of cavity polaritons in simple laminated microcavities filled with biologically produced enhanced green fluorescent protein (eGFP). The unique molecular structure of eGFP prevents exciton annihilation even at high excitation densities, thus facilitating polariton condensation under conventional nanosecond pumping. Condensation is clearly evidenced by a distinct threshold, an interaction-induced blueshift of the condensate, long-range coherence, and the presence of a second threshold at higher excitation density that is associated with the onset of photon lasing.

  8. Excitons and Cooper pairs two composite bosons in many-body physics

    CERN Document Server

    Combescot, Monique

    2015-01-01

    This book bridges a gap between two major communities of Condensed Matter Physics, Semiconductors and Superconductors, that have thrived independently. Through an original perspective that their key particles, excitons and Cooper pairs, are composite bosons, the authors raise fundamental questions of current interest: how does the Pauli exclusion principle wield its power on the fermionic components of bosonic particles at a microscopic level and how this affects the macroscopic physics? What can we learn from Wannier and Frenkel excitons and from Cooper pairs that helps us understand "bosonic condensation" of composite bosons and its difference from Bose-Einstein condensation of elementary bosons? The authors start from solid mathematical and physical foundation to derive excitons and Cooper pairs. They further introduce Shiva diagrams as a graphic support to grasp the many-body physics induced by fermion exchange - a novel mechanism not visualized by standard Feynman diagrams. Advanced undergraduate or grad...

  9. 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.

  10. Real-time observation of ultrafast Rabi oscillations between excitons and plasmons in metal/molecular aggregate hybrid nanostructures

    Directory of Open Access Journals (Sweden)

    Cerullo G.

    2013-03-01

    Full Text Available We demonstrate ultrafast coherent manipulation of the normal mode splitting in metal/molecular-aggregate nanostructures by real-time observation of Rabi oscillations between excitons and surface-plasmon-polaritons. Oscillations in exciton density on a 10-fs timescale control the Rabi splitting.

  11. Phase Diagram of the Bose Condensation of Interwell Excitons in GaAs/AlGaAs Double Quantum Wells

    DEFF Research Database (Denmark)

    Dremin, A. A.; Timofeev, V. B.; Larionov, A. V.

    2002-01-01

    The luminescence of interwell excitons in GaAs/AlGaAs double quantum wells (n–i–n heterostructures) with large-scale fluctuations of random potential in the heteroboundary planes was studied at low temperatures down to 0.5 K. The properties of excitons whose photoexcited electron and hole...

  12. An experimental study on the molecular organization and exciton diffusion in a bilayer of a porphyrin and poly(3-hexylthiophene)

    NARCIS (Netherlands)

    Huijser, A.; Savenije, T.J.; Shalav, A.; Siebbeles, L.D.A.

    2008-01-01

    The exciton root-mean-square displacement (ΛD) in regioregular poly(3-hexylthiophene) (P3HT) deposited onto meso-tetrakis (n-methyl-4-pyridyl) porphyrin tetrachloride (H2TMPyP) has been determined from the photovoltaic response of a device based on these materials in a bilayer configuration. Exciton

  13. Nature of the narrow optical band in H*-aggregates: Dozy-chaos–exciton coupling

    Energy Technology Data Exchange (ETDEWEB)

    Egorov, Vladimir V., E-mail: egorov@photonics.ru [Photochemistry Center, Russian Academy of Sciences, Moscow, 119421 (Russian Federation)

    2014-07-15

    Dozy chaos emerges as a combined effect of the collective chaotic motion of electrons and nuclei, and their chaotic electromagnetic interactions in the transient state of molecules experiencing quantum transitions. Following earlier discussions of the well-known Brönsted relations for proton-transfer reactions; the temperature-dependent electron transfer in Langmuir–Blodgett films; the shape of the optical bands of polymethine dye monomers, their dimers, and J-aggregates, this paper reports one more application of the dozy-chaos theory of molecular quantum transitions. The qualitative and quantitative explanations for shape of a narrow and blue-shifted optical absorption band in H{sup *}-aggregates is given on the basis of the dozy-chaos theory by taking into account the dozy-chaos–exciton coupling effect. It is emphasized that in the H{sup *}-aggregate chromophore (dimer of cyclic bis-thiacarbocyanines) there is a competition between two Frenkel exciton transitions through the chaotic reorganization motion of nuclear environment. As a result, the highly organized quantum transition to the upper exciton state becomes an exciton-induced source of dozy chaos for the low organized transition to the lower exciton state. This manifests itself in appearing the narrow peak and broad wing in the optical spectrum pattern of H{sup *}-aggregates. A similar enhancement in the H{sup *}-effect caused by the strengthening of the exciton coupling in H{sup *}-dimers, which could be achieved by synthesizing tertiary and quarternary thiacarbocyanine monomers, is predicted.

  14. 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.

  15. Pure Optical Dephasing Dynamics in Semiconducting Single-Walled Carbon Nanotubes

    Energy Technology Data Exchange (ETDEWEB)

    Graham, Matt [University of California, Berkeley; Fleming, Graham [University of California, Berkeley; Ma, Yingzhong [ORNL; Green, Alexander A. [Northwestern University, Evanston; Hersam, Mark C. [Northwestern University, Evanston

    2011-01-01

    We report a detailed study of ultrafast exciton dephasing processes in semiconducting single-walled carbon nanotubes (SWNTs) employing a sample highly enriched in a single tube species, the (6,5) tube. Systematic measurements of femtosecond pump-probe, two-pulse photon echo and three-pulse photon echo peak shift over a broad range of excitation intensities and lattice temperature (from 4.4 to 292 K) enable us to quantify the timescales of pure optical dephasing (T 2 ), along with exciton-exciton and exciton-phonon scattering, environmental effects as well as spectral diffusion. While the exciton dephasing time (T2 ) increases from 205 fs at room temperature to 320 fs at 70 K, we found that further decrease of the lattice temperature leads to a shortening of the T2 times. This complex temperature dependence was found to arise from an enhanced relaxation of exciton population at lattice temperatures below 80 K. By quantitatively accounting the contribution from the population relaxation, the corresponding pure optical dephasing times increase monotonically from 225 fs at room temperature to 508 fs at 4.4 K. We further found that below 180 K, the inverse of the pure dephasing time (1/T 2 ) scales linearly with temperature with a slope of 6.7 0.6 eV/K, which suggests dephasing arising from one-phonon scattering (i.e. acoustic phonons). In view ofthe large dynamic disorder of the surrounding environment, the origin of the long room temperature pure dephasing time is proposed to result from reduced strength of exciton-phonon coupling by motional narrowing over nuclear fluctuations. This consideration further suggests the occurrence of remarkable initial exciton delocalization, and makes nanotubes ideal to study many-body effects in spatially confined systems.

  16. Coherence of Bose-Einstein condensates of dipolar excitons in GaAs/AlGaAs heterostructures

    Science.gov (United States)

    Gorbunov, A. V.; Timofeev, V. B.

    2016-05-01

    Experiments relating to studies of the coherence of Bose condensates of dipolar excitons in GaAs/AlGaAs heterostructures with a wide, single quantum well and a Schottky gate are analyzed. Dipolar excitons were excited by light in an annular trap formed along the perimeter of a window in a metal gate with an applied electric voltage. A dual-beam interference technique involving interference combination of the amplitudes of the luminescence light field, together with subsequent analysis of first order correlators, is used to study the temporal (longitudinal) and spatial (transverse) coherence of the exciton condensates. It is found that the transverse coherence length of an exciton condensate is considerably longer than its thermal De Broglie wavelength. Experimental studies of the luminescence intensity correlator also confirm the coherence of the exciton Bose condensate.

  17. Intensity dependent absorption bleaching of high subband excitons in GaAs/AlGaAs multiple quantum wells

    CERN Document Server

    Shin, S H; Lee, E H; Chae, K M; Park, S H; Kim, U

    1998-01-01

    We have investigated the influence of carrier generation on the absorption bleaching of the n=2 and n=3 excitons in GaAs/AlGaAs multiple quantum wells (MQWs). With the excitation near the resonance of the n=1 exciton absorption, the long range coulomb screening and collision broadening had significant effects on the exciton bleaching. At low excitation intensity, the absorption bleaching of the n=2 exciton in 75 A-thick MQWs and that of the n=3 exciton in 150 A-thick MQWs were due to linewidth broadening by the collision broadening effect only. At high excitation intensity, however, the reduction of oscillator strength due to the long range coulomb screening contributed dominantly to absorption bleaching.

  18. Plexciton Dynamics: Exciton-Plasmon Coupling in a J-Aggregate-Au Nanoshell Complex Provides a Mechanism for Nonlinearity

    Energy Technology Data Exchange (ETDEWEB)

    Fofang, Nche T. [Rice Univ., Houston, TX (United States); Grady, Nathaniel K. [Rice Univ., Houston, TX (United States); Fan, Zhiyuan [Ohio Univ., Athens, OH (United States); Govorov, Alexander [Ohio Univ., Athens, OH (United States); Halas, Naomi J. [Rice Univ., Houston, TX (United States)

    2011-03-18

    Coherently coupled plasmons and excitons give rise to new optical excitations- plexcitons - due to the strong coupling of these two oscillator systems. Time-resolved studies of J-aggregate-Au nanoshell complexes when the nanoshell plasmon and J-aggregate exciton energies are degenerate probe the dynamical behavior of this coupled system. Transient absorption of the interacting plasmon-exciton system is observed, in dramatic contrast to the photoinduced transmission of the pristine J-aggregate. An additional, transient Fano-shaped modulation within the Fano dip is also observable. The behavior of the J-aggregate-Au nanoshell complex is described by a combined one-exciton and two-exciton state model coupled to the nanoshell plasmon.

  19. 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.

  20. Three-dimensional localization of excitons in the InAs/GaAs wetting layer - magnetospectroscopic study

    Energy Technology Data Exchange (ETDEWEB)

    Babinski, A.; Golnik, A.; Kossacki, P.; Gaj, J.A. [Institute of Experimental Physics, University of Warsaw (Poland); Borysiuk, J. [Institute of Experimental Physics, University of Warsaw (Poland); Institute of Electronic Materials Technology, Warszawa (Poland); Kret, S. [Institute of Physics, Polish Academy of Sciences, Warszawa (Poland); Raymond, S.; Wasilewski, Z.R. [Institute for Microstructural Sciences, NRC, Ottawa, Ontario (Canada); Potemski, M. [High Magnetic Field Laboratory, CNRS BP-166, Grenoble (France)

    2009-04-15

    Magnetospectroscopic studies of individual excitonic states confined in potential fluctuations in the InAs/GaAs wetting layer (WL) are presented. A neutral exciton and a trion emission have been identified. They split in magnetic field in two components of orthogonal circular polarizations. The respective Zeeman splitting changes linearly with magnetic field up to 10 T. A significant scatter of the effective excitonic g{sup *}-factor is observed, reflecting the distribution of sizes and compositions of potential fluctuations in the WL. The distribution affects also diamagnetic shift of the excitonic emission. The observed properties of the excitons are consistent with a picture of shallow quantum dots formed in the WL due to In composition fluctuations. (copyright 2009 WILEY-VCH Verlag GmbH and Co. KGaA, Weinheim) (orig.)

  1. Tailoring the exciton fine structure of cadmium selenide nanocrystals with shape anisotropy and magnetic field.

    Science.gov (United States)

    Sinito, Chiara; Fernée, Mark J; Goupalov, Serguei V; Mulvaney, Paul; Tamarat, Philippe; Lounis, Brahim

    2014-11-25

    We use nominally spheroidal CdSe nanocrystals with a zinc blende crystal structure to study how shape perturbations lift the energy degeneracies of the band-edge exciton. Nanocrystals with a low degree of symmetry exhibit splitting of both upper and lower bright state degeneracies due to valence band mixing combined with the isotropic exchange interaction, allowing active control of the level splitting with a magnetic field. Asymmetry-induced splitting of the bright states is used to reveal the entire 8-state band-edge fine structure, enabling complete comparison with band-edge exciton models.

  2. Singlet Exciton Migration in a Conjugated Polymer by Picosecond Time-Resolved Photoluminescence

    Institute of Scientific and Technical Information of China (English)

    马国宏; 钱士雄; 雷洪; 汪河洲; 王荣秋; 李永舫

    2001-01-01

    The transient photoluminescence (PL) of DO-PPV (poly-(2,5-dioctyloxy-1,4-phenylene vinylene)) solution in chloroform was investigated by picosecond time-resolved PL spectroscopy. An ultrafast rise of PL and the following single exponential decay with a time constant of about 400ps were assigned to the formation of the intrachain exciton and its decay process, respectively. The redshift of the PL emission spectrum with time was caused by the subsequent exciton migration among the different conjugated segments in the DO-PPV polymer.

  3. Characteristics of exciton photoluminescence kinetics in low-dimensional silicon structures

    CERN Document Server

    Sachenko, A V; Manojlov, E G; Svechnikov, S V

    2001-01-01

    The time-resolved visible photoluminescence of porous nanocrystalline silicon films obtained by laser ablation have been measured within the temperature range 90-300 K. A study has been made of the interrelationship between photoluminescence characteristics (intensity, emission spectra, relaxation times, their temperature dependencies and structural and dielectric properties (size and shapes of Si nanocrystals, oxide phase of nanocrystal coating, porosity). A photoluminescence model is proposed that describes photon absorption and emission occurring in quantum-size Si nanocrystals while coupled subsystems of electron-hole pairs and excitons take part in the recombination. Possible excitonic Auger recombination mechanism in low-dimensional silicon structures is considered

  4. Plasmonic-exciton coupling in synthesized metal/semiconductor hybrid nanocomposites

    Energy Technology Data Exchange (ETDEWEB)

    Gadalla, A.; Hamad, D. A. [Physics Department, Assiut University, Assiut (Egypt); Mohamed, M. B. [National Institute of Laser Enhanced science (NIELS), Cairo University, Cairo (Egypt)

    2015-12-31

    A new method has been developed to grow plasmonic semiconductor nanocomposites of Au/CdSe and Ag/CdSe. Their chemical composition and crystal structure are determined by X-ray diffraction. The collective optical properties of the prepared semiconductor nanohybrid have been measured using spectrophotometer techniques and compared to those of the individual components. The electron transfer processes from CdSe to the gold are faster than that of the silver. Au/CdSe has a strong plasmonic-excitonic coupling, but Ag/CdSe has a weak plasmonic-excitonic coupling.

  5. Controlling the polarization eigenstate of a quantum dot exciton with light

    CERN Document Server

    Belhadj, Thomas; Amand, Thierry; Renucci, Pierre; Krebs, Olivier; Lemaitre, Aristide; Voisin, Paul; Marie, Xavier; Urbaszek, Bernhard

    2009-01-01

    We demonstrate optical control of the polarization eigenstates of a neutral quantum dot exciton without any external fields. By varying the excitation power of a circularly polarized laser in micro-photoluminescence experiments on individual InGaAs quantum dots we control the magnitude and direction of an effective internal magnetic field created via optical pumping of nuclear spins. The adjustable nuclear magnetic field allows us to tune the linear and circular polarization degree of the neutral exciton emission. The quantum dot can thus act as a tunable light polarization converter.

  6. Type II InAs/GaAsSb quantum dots: Highly tunable exciton geometry and topology

    Energy Technology Data Exchange (ETDEWEB)

    Llorens, J. M.; Wewior, L.; Cardozo de Oliveira, E. R.; Alén, B., E-mail: benito.alen@csic.es [IMM-Instituto de Microelectrónica de Madrid (CNM-CSIC), Isaac Newton 8, PTM, E-28760 Tres Cantos, Madrid (Spain); Ulloa, J. M.; Utrilla, A. D.; Guzmán, A.; Hierro, A. [Institute for Systems based on Optoelectronics and Microtechnology (ISOM), Universidad Politécnica de Madrid, Ciudad Universitaria s/n, 28040 Madrid (Spain)

    2015-11-02

    External control over the electron and hole wavefunctions geometry and topology is investigated in a p-i-n diode embedding a dot-in-a-well InAs/GaAsSb quantum structure with type II band alignment. We find highly tunable exciton dipole moments and largely decoupled exciton recombination and ionization dynamics. We also predicted a bias regime where the hole wavefunction topology changes continuously from quantum dot-like to quantum ring-like as a function of the external bias. All these properties have great potential in advanced electro-optical applications and in the investigation of fundamental spin-orbit phenomena.

  7. Synthesis of cadmium chalcogenide based quantum dots for enhanced multiple exciton generation

    OpenAIRE

    2014-01-01

    Quantum dots (QDs) have the potential to produce more than one exciton per incident photon, if the photon energy is greater than twice the band gap energy. This process of multiple exciton generation (MEG) has the potential to lead to a step change in the efficiency of solar panels, by utilising energy commonly wasted as heat in conventional solar cells. A wide range of CdSe/CdTe and CdTe/CdSe quantum dots with and without a CdS shell were synthesised with varying core sizes and shell thickne...

  8. Tuning surface plasmon-exciton coupling via thickness dependent plasmon damping

    Science.gov (United States)

    Balci, Sinan; Kocabas, Coskun; Ates, Simge; Karademir, Ertugrul; Salihoglu, Omer; Aydinli, Atilla

    2012-12-01

    In this paper, we report experimental and theoretical investigations on tuning of the surface plasmon-exciton coupling by controlling the plasmonic mode damping, which is defined by the plasmonic layer thickness. The results reveal the formation of plasmon-exciton hybrid state characterized by a tunable Rabi splitting with energies ranging from 0 to 150 meV. Polarization-dependent spectroscopic reflection measurements were employed to probe the dispersion of the coupled system. The transfer matrix method and analytical calculations were used to model the self-assembled J-aggregate/metal multilayer structures in excellent agreement with experimental observations.

  9. Ground state of excitons in quantum-dot quantum-well nanoparticles:stochastic variational method

    Institute of Scientific and Technical Information of China (English)

    Zhang Heng; Shi Jun-Jie

    2004-01-01

    Within the framework of effective mass approximation, the ground state of excitons confined in spherical core-shell quantum-dot quantum-well (QDQW) nanoparticles is solved by using the stochastic variational method, in which the finite band offset and the heavy (light) hole exciton states are considered. The calculated lse-lsh transition energies for the chosen CdS/HgS/CdS QDQW samples are in good agreement with the experimental measurements. Moreover,some previous theoretical results are improved.

  10. Excitons in solids with non-empirical hybrid time-dependent density-functional theory

    Science.gov (United States)

    Ullrich, Carsten; Yang, Zeng-Hui; Sottile, Francesco

    2015-03-01

    The Bethe-Salpeter equation (BSE) accurately describes the optical properties of solids, but is computationally expensive. Time-dependent density-functional theory (TDDFT) is more efficient, but standard functionals do not produce excitons in extended systems. We present a new, non-empirical hybrid TDDFT approach whose computational cost is much less than BSE, while the accuracy for both bound excitons and the continuum spectra is comparable to that of the BSE. Good performance is observed for both small-gap semiconductors and large-gap insulators. Work supported by NSF Grant DMR-1408904.

  11. Excitons in solids with time-dependent density-functional theory: the bootstrap kernel and beyond

    Science.gov (United States)

    Byun, Young-Moo; Yang, Zeng-Hui; Ullrich, Carsten

    Time-dependent density-functional theory (TDDFT) is an efficient method to describe the optical properties of solids. Lately, a series of bootstrap-type exchange-correlation (xc) kernels have been reported to produce accurate excitons in solids, but different bootstrap-type kernels exist in the literature, with mixed results. In this presentation, we reveal the origin of the confusion and show a new empirical TDDFT xc kernel to compute excitonic properties of semiconductors and insulators efficiently and accurately. Our method can be used for high-throughput screening calculations and large unit cell calculations. Work supported by NSF Grant DMR-1408904.

  12. Ionization of Water Clusters is Mediated by Exciton Energy Transfer from Argon Clusters

    Energy Technology Data Exchange (ETDEWEB)

    Golan, Amir; Ahmed, Musahid

    2012-01-25

    The exciton energy deposited in an argon cluster, (Arn ,< n=20>) using VUV radiation is transferred to softly ionize doped water clusters, ((H2O)n, n=1-9) leading to the formation of non-fragmented clusters. Following the initial excitation, electronic energy is channeled to ionize the doped water cluster while evaporating the Ar shell, allowing identification of fragmented and complete water cluster ions. Examination of the photoionization efficiency curve shows that cluster evaporation from excitons located above 12.6 eV are not enough to cool the energized water cluster ion, and leads to their dissociation to (H2O)n-2H+ (protonated) clusters.

  13. Auger recombination of dark excitons in WS2 and WSe2 monolayers

    Science.gov (United States)

    Danovich, Mark; Zólyomi, Viktor; Fal'ko, Vladimir I.; Aleiner, Igor L.

    2016-09-01

    We propose a novel phonon assisted Auger process unique to the electronic band structure of monolayer transition metal dichalcogenides (TMDCs), which dominates the radiative recombination of ground state excitons in tungsten based TMDCs. Using experimental and density functional theory computed values for the exciton energies, spin-orbit splittings, optical matrix element, and the Auger matrix elements, we find that the Auger process begins to dominate at carrier densities as low as {10}9-10 {{cm}}-2, thus providing a plausible explanation for the low quantum efficiencies reported for these materials.

  14. Exciton Localization in Extended π-Electron Systems: Comparison of Linear and Cyclic Structures.

    Science.gov (United States)

    Thiessen, Alexander; Würsch, Dominik; Jester, Stefan-S; Aggarwal, A Vikas; Idelson, Alissa; Bange, Sebastian; Vogelsang, Jan; Höger, Sigurd; Lupton, John M

    2015-07-30

    We employ five π-conjugated model materials of different molecular shape-oligomers and cyclic structures-to investigate the extent of exciton self-trapping and torsional motion of the molecular framework following optical excitation. Our studies combine steady state and transient fluorescence spectroscopy in the ensemble with measurements of polarization anisotropy on single molecules, supported by Monte Carlo simulations. The dimer exhibits a significant spectral red shift within ∼100 ps after photoexcitation which is attributed to torsional relaxation. This relaxation mechanism is inhibited in the structurally rigid macrocyclic analogue. However, both systems show a high degree of exciton localization but with very different consequences: while, in the macrocycle, the exciton localizes randomly on different parts of the ring, scrambling polarization memory, in the dimer, localization leads to a deterministic exciton position with luminescence characteristics of a dipole. Monte Carlo simulations allow us to quantify the structural difference between the emitting and absorbing units of the π-conjugated system in terms of disorder parameters.

  15. Red, green, and blue lasing enabled by single-exciton gain in colloidal quantum dot films

    Science.gov (United States)

    Nurmikko, Arto V.; Dang, Cuong

    2016-06-21

    The methods and materials described herein contemplate the use films of colloidal quantum dots as a gain medium in a vertical-cavity surface-emitting laser. The present disclosure demonstrates a laser with single-exciton gain in the red, green, and blue wavelengths. Leveraging this nanocomposite gain, the results realize a significant step toward full-color single-material lasers.

  16. Microscopic origins of the surface exciton photoluminescence peak in ZnO nanostructures

    Science.gov (United States)

    Biswas, Mahua; Jung, Yun Suk; Kim, Hong Koo; Kumar, Kumarappan; Hughes, Gregory J.; Newcomb, S.; Henry, Martin O.; McGlynn, Enda

    2011-06-01

    We report photoluminescence (PL) studies of the surface exciton peak in ZnO nanostructures at ~3.367 eV aimed at elucidation of the nature and origin of the emission and its relationship to the nanostructure morphology. PL spectra in conjunction with localized voltage application in high vacuum and different gas atmospheres show a consistent variation (and recovery), allowing an association of the PL to a bound excitonic transition at the ZnO surface, which is modified by an adsorbate. PL studies of samples treated by plasma and of samples exposed to UV light under high vacuum conditions, both well-known processes for desorption of surface adsorbed oxygen, show no consistent effects on the surface exciton peak indicating the lack of involvement of oxygen species. X-ray photoelectron spectroscopy data strongly suggest involvement of adsorbed OH species. X-ray diffraction, scanning, and transmission electron microscopy data are presented also, and the relationship of the surface exciton peak to the nanostructure morphology is discussed.

  17. Scaling Relations and Optimization of Excitonic Energy Transfer Rates between One-Dimensional Molecular Aggregates

    NARCIS (Netherlands)

    Chuang, Chern; Knoester, Jasper; Cao, Jianshu

    2014-01-01

    We theoretically study the distance, chain length, and temperature dependence of the electronic couplings as well as the excitonic energy transfer rates between one-dimensional (1D) chromophore aggregates. In addition to the well-known geometry dependent factor that leads to the deviation from Forst

  18. Tunable excitonic transitions in strained GaAs ultra-thin quantum disk

    Science.gov (United States)

    El-Yadri, M.; Aghoutane, N.; Feddi, E.; Dujardin, F.

    2017-02-01

    Simultaneous influences of hydrostatic pressure and temperature combined to the size effect on the behaviour of the exciton in 2D AlAs / GaAs / AlAs ultra thin quantum disk are investigated. Our approach is performed in the framework of effective mass theory and adiabatic approximation by using a variational method with a robust trial wave function and by taking into account the dependence of the size, the dielectric constant and the effective masses on the pressure and temperature. Variations of the excitonic binding energy, photoluminescence energy and oscillator strength are determined according to hydrostatic pressure and temperature for different confinement regimes. The results of our numerical calculations show that the applied pressure favours the electron-hole attraction while the temperature tends to decrease the exciton binding energy. Another interesting result is the possibility of transforming a thin quantum disk into a large-gap material by strain effect. The opposing effects caused by temperature and pressure reveal a big practical interest and offer an alternative way to the tuning of the excitonic transition in optoelectronic devices.

  19. Properties of Excitons Bound to Neutral Donors in GaAs Quantum-Well Wires

    Institute of Scientific and Technical Information of China (English)

    LIU Jian-Jun; WANG Xue-Feng

    2005-01-01

    @@ In the effective mass approximation, the binding energy of an exciton bound to a neutral donor (D0, X) is calcu-lated variationally for rectangular GaAs quantum-well wires (QWWs) by using a three-parameter wavefunction.

  20. Excitons in C-60 studied by temperature-dependent optical second-harmonic generation

    NARCIS (Netherlands)

    Janner, A.M; Eder, R; Koopmans, B; Jonkman, H.T.; Sawatzky, G.A

    1995-01-01

    The electric-dipole-forbidden T-1(1g) excitonic state of solid C-60 at hw=1.81 eV can be probed with a second-harmonic generation (SHG) experiment. We show that the SHG line shape depends strongly on the degree of rotational order. We observe a splitting into two peaks below the rotational ordering