Near-Band-Edge Optical Responses of CH3NH3PbCl3 Single Crystals: Photon Recycling of Excitonic Luminescence

Science.gov (United States)

Yamada, Takumi; Aharen, Tomoko; Kanemitsu, Yoshihiko

2018-02-01

The determination of the band gap and exciton energies of lead halide perovskites is very important from the viewpoint of fundamental physics and photonic device applications. By using photoluminescence excitation (PLE) spectra, we reveal the optical properties of CH3NH3PbCl3 single crystals in the near-band-edge energy regime. The one-photon PLE spectrum exhibits the 1 s exciton peak at 3.11 eV. On the contrary, the two-photon PLE spectrum exhibits no peak structure. This indicates photon recycling of excitonic luminescence. By analyzing the spatial distribution of the excitons and photon recycling, we obtain 3.15 eV for the band gap energy and 41 meV for the exciton binding energy.

Density-dependent squeezing of excitons in highly excited semiconductors

International Nuclear Information System (INIS)

Nguyen Hong Quang.

1995-07-01

The time evolution from coherent states to squeezed states of high density excitons is studied theoretically based on the boson formalism and within the Random Phase Approximation. Both the mutual interaction between excitons and the anharmonic exciton-photon interaction due to phase-space filling of excitons are taken into account. It is shown that the exciton squeezing depends strongly on the exciton density in semiconductors and becomes smaller with increasing the latter. (author). 16 refs, 2 figs

Pronounced enhancement of exciton Rabi oscillation for a two-photon transition based on quantum dot coupling control

International Nuclear Information System (INIS)

Luo Jian; Lu Di; Du Chaoling; Liu Youwen; Shi Daning; Lai Wei; Guo Chunlei; Gong Shangqing

2012-01-01

We theoretically investigate how to control the Rabi oscillation of excitons of the coupling quantum dots by manipulating static electric fields. Our results show that, for a single-photon process, when direct excitons change into indirect excitons with a bias applied on the sample, the Rabi oscillation rarely alters. However, for the two-photon process, a pronounced enhancement of Rabi oscillation is observed, which can be utilized as the logic gate in quantum information. (paper)

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

International Nuclear Information System (INIS)

Ye, Jinwu; Sun, Fadi; Yu, Yi-Xiang; Liu, Wuming

2013-01-01

The photoluminescence (PL) measurements on photons and the transport measurements on excitons are the two types of independent and complementary detection tools to search for possible exciton superfluids in electron–hole semi-conductor bilayer systems. In fact, it was believed that the transport measurements can provide more direct evidences on superfluids than the spectroscopic measurements. It is important to establish the relations between the two kinds of measurements. In this paper, using quantum Heisenberg–Langevin equations, we establish such a connection by calculating various exciton correlation functions in the putative exciton superfluids. These correlation functions include both normal and anomalous greater, lesser, advanced, retarded, and time-ordered exciton Green functions and also various two exciton correlation functions. We also evaluate the corresponding normal and anomalous spectral weights and the Keldysh distribution functions. We stress the violations of the fluctuation and dissipation theorem among these various exciton correlation functions in the non-equilibrium exciton superfluids. We also explore the input–output relations between various exciton correlation functions and those of emitted photons such as the angle resolved photon power spectrum, phase sensitive two mode squeezing spectrum and two photon correlations. Applications to possible superfluids in the exciton–polariton systems are also mentioned. For a comparison, using conventional imaginary time formalism, we also calculate all the exciton correlation functions in an equilibrium dissipative exciton superfluid in the electron–electron coupled semi-conductor bilayers at the quantum Hall regime at the total filling factor ν T =1. We stress the analogies and also important differences between the correlations functions in the two exciton superfluid systems. - Highlights: ► Establish the relations between photoluminescence and transport measurements. ► Stress the

Optical nutation in the exciton range of spectrum

International Nuclear Information System (INIS)

Khadzhi, P. I.; Vasiliev, V. V.

2013-01-01

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

Slow light enhanced singlet exciton fission solar cells with a 126% yield of electrons per photon

International Nuclear Information System (INIS)

Thompson, Nicholas J.; Congreve, Daniel N.; Baldo, Marc A.; Goldberg, David; Menon, Vinod M.

2013-01-01

Singlet exciton fission generates two triplet excitons per absorbed photon. It promises to increase the power extracted from sunlight without increasing the number of photovoltaic junctions in a solar cell. We demonstrate solar cells with an external quantum efficiency of 126% by enhancing absorption in thin films of the singlet exciton fission material pentacene. The device structure exploits the long photon dwell time at the band edge of a distributed Bragg reflector to achieve enhancement over a broad range of angles. Measuring the reflected light from the solar cell establishes a lower bound of 137% for the internal quantum efficiency

Slow light enhanced singlet exciton fission solar cells with a 126% yield of electrons per photon

Energy Technology Data Exchange (ETDEWEB)

Thompson, Nicholas J.; Congreve, Daniel N.; Baldo, Marc A., E-mail: vmenon@qc.cuny.edu, E-mail: baldo@mit.edu [Energy Frontier Research Center for Excitonics, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139 (United States); Goldberg, David; Menon, Vinod M., E-mail: vmenon@qc.cuny.edu, E-mail: baldo@mit.edu [Department of Physics, Queens College and Graduate Center, The City University of New York, Flushing, New York 11367 (United States)

2013-12-23

Singlet exciton fission generates two triplet excitons per absorbed photon. It promises to increase the power extracted from sunlight without increasing the number of photovoltaic junctions in a solar cell. We demonstrate solar cells with an external quantum efficiency of 126% by enhancing absorption in thin films of the singlet exciton fission material pentacene. The device structure exploits the long photon dwell time at the band edge of a distributed Bragg reflector to achieve enhancement over a broad range of angles. Measuring the reflected light from the solar cell establishes a lower bound of 137% for the internal quantum efficiency.

Strong excitonic interactions in the oxygen K-edge of perovskite oxides.

Science.gov (United States)

Tomita, Kota; Miyata, Tomohiro; Olovsson, Weine; Mizoguchi, Teruyasu

2017-07-01

Excitonic interactions of the oxygen K-edge electron energy-loss near-edge structure (ELNES) of perovskite oxides, CaTiO 3 , SrTiO 3 , and BaTiO 3 , together with reference oxides, MgO, CaO, SrO, BaO, and TiO 2 , were investigated using a first-principles Bethe-Salpeter equation calculation. Although the transition energy of oxygen K-edge is high, strong excitonic interactions were present in the oxygen K-edge ELNES of the perovskite oxides, whereas the excitonic interactions were negligible in the oxygen K-edge ELNES of the reference compounds. Detailed investigation of the electronic structure suggests that the strong excitonic interaction in the oxygen K-edge ELNES of the perovskite oxides is caused by the directionally confined, low-dimensional electronic structure at the Ti-O-Ti bonds. Copyright © 2016 Elsevier B.V. All rights reserved.

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

KAUST Repository

Sun, Jingya; Yu, Weili; Usman, Anwar; Isimjan, Tayirjan T.; Del Gobbo, Silvano; Alarousu, Erkki; Takanabe, Kazuhiro; Mohammed, Omar F.

2014-01-01

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.

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.

Plasmonic, excitonic and exciton-plasmonic photoinduced nanocomposites

Science.gov (United States)

Bityurin, N.; Ermolaev, N.; Smirnov, A. A.; Afanasiev, A.; Agareva, N.; Koryukina, T.; Bredikhin, V.; Kamensky, V.; Pikulin, A.; Sapogova, N.

2016-03-01

UV irradiation of materials consisting of a polymer matrix that possesses precursors of different kinds can result in creation of nanoparticles within the irradiated domains. Such photoinduced nanocomposites are promising for photonic applications due to the strong alteration of their optical properties compared to initial non-irradiated materials. We report our results on the synthesis and investigation of plasmonic, excitonic and exciton-plasmonic photoinduced nanocomposites. Plasmonic nanocomposites contain metal nanoparticles of noble metals with a pronounced plasmon resonance. Excitonic nanocomposites possess semiconductor nanoclusters (quantum dots). We consider the CdS-Au pair because the luminescent band of CdS nanoparticles enters the plasmon resonance band of gold nanoparticles. The obtaining of such particles within the same composite materials is promising for the creation of media with exciton-plasmon resonance. We demonstrate that it is possible to choose appropriate precursor species to obtain the initially transparent poly(methyl methacrylate) (PMMA) films containing both types of these molecules either separately or together. Proper irradiation of these materials by a light-emitting diode operating at the wavelength of 365 nm provides material alteration demonstrating light-induced optical absorption and photoluminescent properties typical for the corresponding nanoparticles. Thus, an exciton-plasmonic photoinduced nanocomposite is obtained. It is important that here we use the precursors that are different from those usually employed.

Excitons in atomically thin 2D semiconductors and their applications

Science.gov (United States)

Xiao, Jun; Zhao, Mervin; Wang, Yuan; Zhang, Xiang

2017-06-01

The research on emerging layered two-dimensional (2D) semiconductors, such as molybdenum disulfide (MoS2), reveals unique optical properties generating significant interest. Experimentally, these materials were observed to host extremely strong light-matter interactions as a result of the enhanced excitonic effect in two dimensions. Thus, understanding and manipulating the excitons are crucial to unlocking the potential of 2D materials for future photonic and optoelectronic devices. In this review, we unravel the physical origin of the strong excitonic effect and unique optical selection rules in 2D semiconductors. In addition, control of these excitons by optical, electrical, as well as mechanical means is examined. Finally, the resultant devices such as excitonic light emitting diodes, lasers, optical modulators, and coupling in an optical cavity are overviewed, demonstrating how excitons can shape future 2D optoelectronics.

Probing different regimes of strong field light-matter interaction with semiconductor quantum dots and few cavity photons

Science.gov (United States)

Hargart, F.; Roy-Choudhury, K.; John, T.; Portalupi, S. L.; Schneider, C.; Höfling, S.; Kamp, M.; Hughes, S.; Michler, P.

2016-12-01

In this work we present an extensive experimental and theoretical investigation of different regimes of strong field light-matter interaction for cavity-driven quantum dot (QD) cavity systems. The electric field enhancement inside a high-Q micropillar cavity facilitates exceptionally strong interaction with few cavity photons, enabling the simultaneous investigation for a wide range of QD-laser detuning. In case of a resonant drive, the formation of dressed states and a Mollow triplet sideband splitting of up to 45 μeV is measured for a mean cavity photon number ≤slant 1. In the asymptotic limit of the linear AC Stark effect we systematically investigate the power and detuning dependence of more than 400 QDs. Some QD-cavity systems exhibit an unexpected anomalous Stark shift, which can be explained by an extended dressed 4-level QD model. We provide a detailed analysis of the QD-cavity systems properties enabling this novel effect. The experimental results are successfully reproduced using a polaron master equation approach for the QD-cavity system, which includes the driving laser field, exciton-cavity and exciton-phonon interactions.

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

Science.gov (United States)

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

2017-06-01

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

Strong Exciton–Photon Coupling and Lasing Behavior in All-Inorganic CsPbBr3 Micro/Nanowire Fabry-Pérot Cavity

KAUST Repository

Du, Wenna; Zhang, Shuai; Shi, Jia; Chen, Jie; Wu, Zhiyong; Mi, Yang; Liu, Zhixiong; Li, Yuanzheng; Sui, Xinyu; Wang, Rui; Qiu, Xiaohui; Wu, Tao; Xiao, Yunfeng; Zhang, Qing; Liu, Xinfeng

2018-01-01

for their optical application, however, is rarely studied. In this work, we demonstrated the strong coupling of exciton-photon and polariton lasing in high quality CsPbBr micro/nanowires synthesized by a CVD method. By exploring spatial resolved PL spectra of CsPbBr

Confined exciton spectroscopy

International Nuclear Information System (INIS)

Torres, Clivia M.S.

1998-01-01

Full text: In this work, the exciton is considered as a sensor of the electronic and optical properties of materials such as semiconductors, which have size compared to the exciton De Broglie wavelength, approximately 20 nm, depending on the semiconductor. Examples of electron-phonon, electron-electron, photon-electron, exciton-polariton, phonon-plasmon, are presented, under different confinement conditions such as quantum wells, superlattices

Strong Exciton–Photon Coupling and Lasing Behavior in All-Inorganic CsPbBr3 Micro/Nanowire Fabry-Pérot Cavity

KAUST Repository

Du, Wenna

2018-03-14

All-inorganic perovskite micro/nanowire materials hold great promises as nanoscale coherent light source due to their superior optical and electronic properties. The coupling strength between exciton and photon in this system is important for their optical application, however, is rarely studied. In this work, we demonstrated the strong coupling of exciton-photon and polariton lasing in high quality CsPbBr micro/nanowires synthesized by a CVD method. By exploring spatial resolved PL spectra of CsPbBr cavity, we observed mode volume dependent coupling strength with a vacuum Rabi splitting up to 656 meV, as well as significant increase in group index. Moreover, low threshold polariton lasing was achieved at room temperature within strong coupling regime; the polariton characteristic is confirmed by comparing lasing spectra with waveguided output spectra and the dramatically reduced lasing threshold. Our present results provide new avenues to achieve high coupling strengths potentially enabling application of exciting phenomena such as Bose-Einstein condensation of polaritons, efficient light-emitting diodes, and lasers.

Bright triplet excitons in caesium lead halide perovskites

Science.gov (United States)

Becker, Michael A.; Vaxenburg, Roman; Nedelcu, Georgian; Sercel, Peter C.; Shabaev, Andrew; Mehl, Michael J.; Michopoulos, John G.; Lambrakos, Samuel G.; Bernstein, Noam; Lyons, John L.; Stöferle, Thilo; Mahrt, Rainer F.; Kovalenko, Maksym V.; Norris, David J.; Rainò, Gabriele; Efros, Alexander L.

2018-01-01

Nanostructured semiconductors emit light from electronic states known as excitons. For organic materials, Hund’s rules state that the lowest-energy exciton is a poorly emitting triplet state. For inorganic semiconductors, similar rules predict an analogue of this triplet state known as the ‘dark exciton’. Because dark excitons release photons slowly, hindering emission from inorganic nanostructures, materials that disobey these rules have been sought. However, despite considerable experimental and theoretical efforts, no inorganic semiconductors have been identified in which the lowest exciton is bright. Here we show that the lowest exciton in caesium lead halide perovskites (CsPbX3, with X = Cl, Br or I) involves a highly emissive triplet state. We first use an effective-mass model and group theory to demonstrate the possibility of such a state existing, which can occur when the strong spin-orbit coupling in the conduction band of a perovskite is combined with the Rashba effect. We then apply our model to CsPbX3 nanocrystals, and measure size- and composition-dependent fluorescence at the single-nanocrystal level. The bright triplet character of the lowest exciton explains the anomalous photon-emission rates of these materials, which emit about 20 and 1,000 times faster than any other semiconductor nanocrystal at room and cryogenic temperatures, respectively. The existence of this bright triplet exciton is further confirmed by analysis of the fine structure in low-temperature fluorescence spectra. For semiconductor nanocrystals, which are already used in lighting, lasers and displays, these excitons could lead to materials with brighter emission. More generally, our results provide criteria for identifying other semiconductors that exhibit bright excitons, with potential implications for optoelectronic devices.

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.

Exciton-plasmon coupling interactions: from principle to applications

Science.gov (United States)

Cao, En; Lin, Weihua; Sun, Mengtao; Liang, Wenjie; Song, Yuzhi

2018-01-01

The interaction of exciton-plasmon coupling and the conversion of exciton-plasmon-photon have been widely investigated experimentally and theoretically. In this review, we introduce the exciton-plasmon interaction from basic principle to applications. There are two kinds of exciton-plasmon coupling, which demonstrate different optical properties. The strong exciton-plasmon coupling results in two new mixed states of light and matter separated energetically by a Rabi splitting that exhibits a characteristic anticrossing behavior of the exciton-LSP energy tuning. Compared to strong coupling, such as surface-enhanced Raman scattering, surface plasmon (SP)-enhanced absorption, enhanced fluorescence, or fluorescence quenching, there is no perturbation between wave functions; the interaction here is called the weak coupling. SP resonance (SPR) arises from the collective oscillation induced by the electromagnetic field of light and can be used for investigating the interaction between light and matter beyond the diffraction limit. The study on the interaction between SPR and exaction has drawn wide attention since its discovery not only due to its contribution in deepening and broadening the understanding of SPR but also its contribution to its application in light-emitting diodes, solar cells, low threshold laser, biomedical detection, quantum information processing, and so on.

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

NARCIS (Netherlands)

Dusanowski, L.; Syperek, M.; Marynski, A.; Li, L.H.; Misiewicz, J.; Höfling, S.; Kamp, M.; Fiore, A.; Sek, G.

2015-01-01

We demonstrate a non-classical photon emitter at near infrared wavelength based on a single (In,Ga)As/GaAs epitaxially grown columnar quantum dot. Charged exciton complexes have been identified in magneto-photoluminescence. Photon auto-correlation histograms from the recombination of a trion

Time-resolved photon echoes from donor-bound excitons in ZnO epitaxial layers

Science.gov (United States)

Poltavtsev, S. V.; Kosarev, A. N.; Akimov, I. A.; Yakovlev, D. R.; Sadofev, S.; Puls, J.; Hoffmann, S. P.; Albert, M.; Meier, C.; Meier, T.; Bayer, M.

2017-07-01

The coherent optical response from 140 nm and 65 nm thick ZnO epitaxial layers is studied using four-wave-mixing spectroscopy with picosecond temporal resolution. Resonant excitation of neutral donor-bound excitons results in two-pulse and three-pulse photon echoes. For the donor-bound A exciton (D0XA ) at temperature of 1.8 K we evaluate optical coherence times T2=33 -50 ps corresponding to homogeneous line widths of 13 -19 μ eV , about two orders of magnitude smaller as compared with the inhomogeneous broadening of the optical transitions. The coherent dynamics is determined mainly by the population decay with time T1=30 -40 ps, while pure dephasing is negligible. Temperature increase leads to a significant shortening of T2 due to interaction with acoustic phonons. In contrast, the loss of coherence of the donor-bound B exciton (D0XB ) is significantly faster (T2=3.6 ps ) and governed by pure dephasing processes.

Plasmon-exciton polaritons in two-dimensional semiconductor/metal interfaces

Science.gov (United States)

Gonçalves, P. A. D.; Bertelsen, L. P.; Xiao, Sanshui; Mortensen, N. Asger

2018-01-01

The realization and control of polaritons is of paramount importance in the prospect of novel photonic devices. Here, we investigate the emergence of plasmon-exciton polaritons in hybrid structures consisting of a two-dimensional transition-metal dichalcogenide (TMDC) deposited onto a metal substrate or coating a metallic thin film. We determine the polaritonic spectrum and show that, in the former case, the addition of a top dielectric layer and, in the latter case, the thickness of the metal film can be used to tune and promote plasmon-exciton interactions well within the strong-coupling regime. Our results demonstrate that Rabi splittings exceeding 100 meV can readily be achieved in planar dielectric/TMDC/metal structures under ambient conditions. We thus believe that this Rapid Communication provides a simple and intuitive picture to tailor strong coupling in plexcitonics with potential applications for engineering compact photonic devices with tunable optical properties.

Disturbing the coherent dynamics of an excitonic polarization with strong terahertz fields

Science.gov (United States)

Drexler, M. J.; Woscholski, R.; Lippert, S.; Stolz, W.; Rahimi-Iman, A.; Koch, M.

2014-11-01

We present a paper based on combining four-wave mixing and strong fields in the terahertz frequency range to monitor the time evolution of a disturbed excitonic polarization in a multiple quantum well system. Our findings not only confirm a lower field-dependent ionization threshold for higher excitonic states, but furthermore provide experimental evidence for intraexcitonic Rabi flopping in the time domain. These measurements correspond to the picture of a reversible and irreversible transfer as previously predicted by a microscopic theory.

Magneto-exciton dephasing in a single quantum dot

Science.gov (United States)

Rodriguez, F. J.; Reyes, A.; Olaya-Castro, A.; Quiroga, L.

2001-03-01

Ultrafast spectroscopy experiments on single quantum dot (SQD) in magnetic fields provide a variety of unexpected results, one of them being the recently reported entanglement of exciton states. In order to explore the entanglement robustness, dephasing mechanisms must be considered. By calculating the non-linear time resolved optical spectrum of a SQD, we present a theoretical study on the exciton-exciton scattering contribution to the magneto-exciton dephasing time. Our results show that the time evolution of \\chi^(3) presents, under non-steady-state condition, a beating between the bound biexciton and the first unbound biexciton state in the strong confinement regime. The contribution coming from both left and right polarized emitted photons allows us to predict the creation of exciton entanglement, in agreement with recent experimental results. Previous theoretical works have only addressed the stationary optical response. By contrast, our results based on a full time dependent calculation show new features specially for the fast dephasing case.

The Exciton-Polariton Dispersion Law under the Action of Strong Pumping in the Region of the M-Band of Luminescence

Science.gov (United States)

Khadzhi, P. I.; Nad'kin, L. Yu.; Markov, D. A.

2018-04-01

The double-pulse interaction with excitons and biexcitons in semiconductors is studied theoretically. It is shown that the dispersion law of carrier wave has three branches under the action of a powerful pumping in the region of the M-band of luminescence. Values of parameters at which the dispersion law branches can intersect due to the degeneration of the exciton level energy have been found. The effect of a significant change in the force of coupling between the exciton and photon of a weak pulse with a change in the pumping intensity is predicted.

Fluorescence Spectroscopy, Exciton Dynamics and Photochemistry of Single Allophycocyanin Trimers

International Nuclear Information System (INIS)

Ying, Liming; Xie, Xiaoliang

1998-01-01

We report a study of the spectroscopy and exciton dynamics of the allophycocyanin trimer (APC), a light harvesting protein complex from cyanobacteria, by room-temperature single-molecule measurements of fluorescence spectra, lifetimes, intensity trajectories and polarization modulation. Emission spectra of individual APC trimers are found to be homogeneous on the time scale of seconds. In contrast, their emission lifetimes are found to be widely distributed, because of generation of exciton traps during the course of measurements. The intensity trajectories and polarization modulation experiments indicate reversible ixciton trap formation within the three quasi-independent pairs of strong interacting a84 and B84 chromophores in APC, as well a photobleaching of individual chromophores. Comparison experiments under continuous wave and pulsed excitation reveal a two-photon mechanism for generating exciton traps and/or photobleaching, which involves exciton-exciton annihilation. These single-molecule experiments provide new insights into exciton dynamics and photochemistry of light-harvesting complexes

Particularities of surface plasmon-exciton strong coupling with large Rabi splitting

International Nuclear Information System (INIS)

Symonds, C; Bonnand, C; Plenet, J C; Brehier, A; Parashkov, R; Lauret, J S; Deleporte, E; Bellessa, J

2008-01-01

This paper presents some of the particularities of the strong coupling regime occurring between surface plasmon (SP) modes and excitons. Two different active materials were deposited on a silver film: a cyanine dye J-aggregate, and a two-dimensional layered perovskite-type semiconductor. The dispersion relations, which are deduced from angular resolved reflectometry spectra, present an anticrossing characteristic of the strong coupling regime. The wavevector is a good parameter to determine the Rabi splitting. Due to the large interaction energies (several hundreds of milli-electron-volts), the calculations at constant angle can induce an overestimation of the Rabi splitting of more than a factor of two. Another property of polaritons based on SP is their nonradiative character. In order to observe the polaritonic emission, it is thus necessary to use particular extraction setups, such as gratings or prisms. Otherwise only the incoherent emission can be detected, very similar to the bare exciton emission

New nonlinear optical effect: self-reflection phenomenon due to exciton-biexciton-light interaction in semiconductors

Science.gov (United States)

Khadzhi, P. I.; Lyakhomskaya, K. D.; Nadkin, L. Y.; Markov, D. A.

2002-05-01

The characteristic peculiarities of the self-reflection of a strong electromagnetic wave in a system of coherent excitons and biexcitons due to the exciton-photon interaction and optical exciton-biexciton conversion in semiconductors were investigated as one of the manifestations of nonlinear optical Stark-effect. It was found that a monotonously decreasing standing wave with an exponential decreasing spatial tail is formed in the semiconductor. Under the action of the field of a strong pulse, an optically homogeneous medium is converted, into the medium with distributed feedback. The appearance of the spatially separated narrow pears of the reflective index, extinction and reflection coefficients is predicted.

Theory of two-photon absorption by exciton states in cubic semiconductors with degenerate valence bands

International Nuclear Information System (INIS)

Nguyen Ai Viet; Nguyen Toan Thang.

1987-06-01

The coefficient of the absorption of two polarized photons is calculated for direct band gap semiconductors with degenerate valence bands. Wannier-Mott exciton states are included in both the intermediate and final states. Numerical calculations are performed for ZnSe and are compared with Sondergeld's experimental and theoretical results. (author). 11 refs, 2 tabs

Robust tunable excitonic features in monolayer transition metal dichalcogenide quantum dots

Science.gov (United States)

Fouladi-Oskouei, J.; Shojaei, S.; Liu, Z.

2018-04-01

The effects of quantum confinement on excitons in parabolic quantum dots of monolayer transition metal dichalcogenides (TMDC QDs) are investigated within a massive Dirac fermion model. A giant spin-valley coupling of the TMDC QDs is obtained, larger than that of monolayer TMDC sheets and consistent with recent experimental measurements. The exciton transition energy and the binding energy are calculated, and it is found that the strong quantum confinement results in extremely high exciton binding energies. The enormously large exciton binding energy in TMDC QDs (({{E}{{B2D}}}∼ 500 meV)different kinds of TMDC QDs) ensures that the many body interactions play a significant role in the investigation of the optical properties of these novel nanostructures. The estimated oscillator strength and radiative lifetime of excitons are strongly size-dependent and indicate a giant oscillator strength enhancement and ultrafast radiative annihilation of excitons, varying from a few tens of femtoseconds to a few picoseconds. We found that the spin-dependent band gap, spin-valley coupling, binding energy and excitonic effects can be tuned by quantum confinements, leading to tunable quantum dots in monolayer TMDCs. This finding offers new functionality in engineering the interaction of a 2D material with light and creates promise for the quantum manipulation of spin and valley degrees of freedom in TMDC nanostructures, enabling versatile novel 2D quantum photonic and optoelectronic nanodevices.

Measurement of Exciton Binding Energy of Monolayer WS2

Science.gov (United States)

Chen, Xi; Zhu, Bairen; Cui, Xiaodong

Excitonic effects are prominent in monolayer crystal of transition metal dichalcogenides (TMDCs) because of spatial confinement and reduced Coulomb screening. Here we use linear differential transmission spectroscopy and two-photon photoluminescence excitation spectroscopy (TP-PLE) to measure the exciton binding energy of monolayer WS2. Peaks for excitonic absorptions of the direct gap located at K valley of the Brillouin zone and transitions from multiple points near Γ point of the Brillouin zone, as well as trion side band are shown in the linear absorption spectra of WS2. But there is no gap between distinct excitons and the continuum of the interband transitions. Strong electron-phonon scattering, overlap of excitons around Γ point and the transfer of the oscillator strength from interband continuum to exciton states make it difficult to resolve the electronic interband transition edge even down to 10K. The gap between excited states of the band-edge exciton and the single-particle band is probed by TP-PLE measurements. And the energy difference between 1s exciton and the single-particle gap gives the exciton binding energy of monolayer WS2 to be about 0.71eV. The work is supported by Area of excellency (AoE/P-04/08), CRF of Hong Kong Research Grant Council (HKU9/CRF/13G) and SRT on New Materials of The University of Hong Kong.

Detuning-Controlled Internal Oscillations in an Exciton-Polariton Condensate

Science.gov (United States)

Voronova, N. S.; Elistratov, A. A.; Lozovik, Yu. E.

2015-10-01

We theoretically analyze exciton-photon oscillatory dynamics within a homogenous polariton gas in the presence of energy detuning between the cavity and quantum well modes. Whereas pure Rabi oscillations consist of the particle exchange between the photon and exciton states in the polariton system without any oscillations of the phases of the two subcondensates, we demonstrate that any nonzero detuning results in oscillations of the relative phase of the photon and exciton macroscopic wave functions. Different initial conditions reveal a variety of behaviors of the relative phase between the two condensates, and a crossover from Rabi-like to Josephson-like oscillations is predicted.

Quantum confinement effect and exciton binding energy of layered perovskite nanoplatelets

Directory of Open Access Journals (Sweden)

Qiang Wang

2018-02-01

Full Text Available We report the preparation of monolayer (n = 1, few-layer (n = 2–5 and 3D (n = ∞ organic lead bromide perovskite nanoplatelets (NPLs by tuning the molar ratio of methylammonium bromide (MABr and hexadecammonium bromide (HABr. The absorption spectrum of the monolayer (HA2PbBr4 perovskite NPLs shows about 138 nm blue shift from that of 3D MAPbBr3 perovskites, which is attributed to strong quantum confinement effect. We further investigate the two-photon photoluminescence (PL of the NPLs and measure the exciton binding energy of monolayer perovskite NPLs using linear absorption and two-photon PL excitation spectroscopy. The exciton binding energy of monolayer perovskite NPLs is about 218 meV, which is far larger than tens of meV in 3D lead halide perovskites.

Manipulating light with strongly modulated photonic crystals

International Nuclear Information System (INIS)

Notomi, Masaya

2010-01-01

Recently, strongly modulated photonic crystals, fabricated by the state-of-the-art semiconductor nanofabrication process, have realized various novel optical properties. This paper describes the way in which they differ from other optical media, and clarifies what they can do. In particular, three important issues are considered: light confinement, frequency dispersion and spatial dispersion. First, I describe the latest status and impact of ultra-strong light confinement in a wavelength-cubic volume achieved in photonic crystals. Second, the extreme reduction in the speed of light is reported, which was achieved as a result of frequency dispersion management. Third, strange negative refraction in photonic crystals is introduced, which results from their unique spatial dispersion, and it is clarified how this leads to perfect imaging. The last two sections are devoted to applications of these novel properties. First, I report the fact that strong light confinement and huge light-matter interaction enhancement make strongly modulated photonic crystals promising for on-chip all-optical processing, and present several examples including all-optical switches/memories and optical logics. As a second application, it is shown that the strong light confinement and slow light in strongly modulated photonic crystals enable the adiabatic tuning of light, which leads to various novel ways of controlling light, such as adiabatic frequency conversion, efficient optomechanics systems, photon memories and photons pinning.

Semiconductor quantum optics with tailored photonic nanostructures

Energy Technology Data Exchange (ETDEWEB)

Laucht, Arne

2011-06-15

This thesis describes detailed investigations of the effects of photonic nanostructures on the light emission properties of self-assembled InGaAs quantum dots. Nanoscale optical cavities and waveguides are employed to enhance the interaction between light and matter, i.e. photons and excitons, up to the point where optical non-linearities appear at the quantum (single photon) level. Such non-linearities are an essential component for the realization of hardware for photon based quantum computing since they can be used for the creation and detection of non-classical states of light and may open the way to new genres of quantum optoelectronic devices such as optical modulators and optical transistors. For single semiconductor quantum dots in photonic crystal nanocavities we investigate the coupling between excitonic transitions and the highly localized mode of the optical cavity. We explore the non-resonant coupling mechanisms which allow excitons to couple to the cavity mode, even when they are not spectrally in resonance. This effect is not observed for atomic cavity quantum electrodynamics experiments and its origin is traced to phonon-assisted scattering for small detunings ({delta}E<{proportional_to}5 meV) and a multi-exciton-based, Auger-like process for larger detunings ({delta}E >{proportional_to}5 meV). For quantum dots in high-Q cavities we observe the coherent coupling between exciton and cavity mode in the strong coupling regime of light-matter interaction, probe the influence of pure dephasing on the coherent interaction at high excitation levels and high lattice temperatures, and examine the coupling of two spatially separated quantum dots via the exchange of real and virtual photons mediated by the cavity mode. Furthermore, we study the spontaneous emission properties of quantum dots in photonic crystal waveguide structures, estimate the fraction of all photons emitted into the propagating waveguide mode, and demonstrate the on-chip generation of

Anisotropic exchange interaction induced by a single photon in semiconductor microcavities

Science.gov (United States)

Chiappe, G.; Fernández-Rossier, J.; Louis, E.; Anda, E. V.

2005-12-01

We investigate coupling of localized spins in a semiconductor quantum dot embedded in a microcavity. The lowest cavity mode and the quantum dot exciton are coupled and close in energy, forming a polariton. The fermions forming the exciton interact with localized spins via exchange. Exact diagonalization of a Hamiltonian in which photons, spins, and excitons are treated quantum mechanically shows that a single polariton induces a sizable indirect anisotropic exchange interaction between spins. At sufficiently low temperatures strong ferromagnetic correlations show up without an appreciable increase in exciton population. In the case of a (Cd,Mn)Te quantum dot, Mn-Mn ferromagnetic coupling is still significant at 1 K : spin-spin correlation around 3 for exciton occupation smaller than 0.3. We find that the interaction mediated by photon-polaritons is 10 times stronger than the one induced by a classical field for equal Rabi splitting.

Exciton Binding Energy of Monolayer WS2

Science.gov (United States)

Zhu, Bairen; Chen, Xi; Cui, Xiaodong

2015-03-01

The optical properties of monolayer transition metal dichalcogenides (TMDC) feature prominent excitonic natures. Here we report an experimental approach to measuring the exciton binding energy of monolayer WS2 with linear differential transmission spectroscopy and two-photon photoluminescence excitation spectroscopy (TP-PLE). TP-PLE measurements show the exciton binding energy of 0.71 +/- 0.01 eV around K valley in the Brillouin zone.

A study of the cavity polariton under strong excitation:dynamics and nonlinearities in II-VI micro-cavities

International Nuclear Information System (INIS)

Muller, Markus

2000-01-01

This work contains an experimental study of the photoluminescence dynamics of cavity polaritons in strong coupling micro-cavities based on II-VI semiconductor compounds. The small exciton size and the strong exciton binding energy in these materials allowed us to study the strong coupling regime between photon and exciton up to high excitation densities, exploring the linear and non-linear emission regimes. Our main experimental techniques are picosecond time-resolved and angular photoluminescence spectroscopy. In the linear regime and for a negative photon-exciton detuning, we observe a suppression of the polariton relaxation by the emission of acoustic phonons leading to a non-equilibrium polariton distribution on the lower branch. This 'bottleneck' effect, which has already been described for polaritons in bulk semiconductors, results from the pronounced photon like character of the polaritons near k(parallel) = 0 in this configuration. At high excitation densities, non-linear relaxation processes, namely final state stimulation of the relaxation and polariton-polariton scattering, bypass this bottleneck giving rise to a very rapid relaxation down to the bottom of the band. We show that this dramatic change in the relaxation dynamics is finally responsible of the super-linear increase of the polariton emission from these states. (author) [fr

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

Semiconductor quantum optics with tailored photonic nanostructures

International Nuclear Information System (INIS)

Laucht, Arne

2011-01-01

This thesis describes detailed investigations of the effects of photonic nanostructures on the light emission properties of self-assembled InGaAs quantum dots. Nanoscale optical cavities and waveguides are employed to enhance the interaction between light and matter, i.e. photons and excitons, up to the point where optical non-linearities appear at the quantum (single photon) level. Such non-linearities are an essential component for the realization of hardware for photon based quantum computing since they can be used for the creation and detection of non-classical states of light and may open the way to new genres of quantum optoelectronic devices such as optical modulators and optical transistors. For single semiconductor quantum dots in photonic crystal nanocavities we investigate the coupling between excitonic transitions and the highly localized mode of the optical cavity. We explore the non-resonant coupling mechanisms which allow excitons to couple to the cavity mode, even when they are not spectrally in resonance. This effect is not observed for atomic cavity quantum electrodynamics experiments and its origin is traced to phonon-assisted scattering for small detunings (ΔE ∝5 meV). For quantum dots in high-Q cavities we observe the coherent coupling between exciton and cavity mode in the strong coupling regime of light-matter interaction, probe the influence of pure dephasing on the coherent interaction at high excitation levels and high lattice temperatures, and examine the coupling of two spatially separated quantum dots via the exchange of real and virtual photons mediated by the cavity mode. Furthermore, we study the spontaneous emission properties of quantum dots in photonic crystal waveguide structures, estimate the fraction of all photons emitted into the propagating waveguide mode, and demonstrate the on-chip generation of single photon emission into the waveguide. The results obtained during the course of this thesis contribute significantly to

Harnessing no-photon exciton generation chemistry to engineer semiconductor nanostructures.

Science.gov (United States)

Beke, David; Károlyházy, Gyula; Czigány, Zsolt; Bortel, Gábor; Kamarás, Katalin; Gali, Adam

2017-09-06

Production of semiconductor nanostructures with high yield and tight control of shape and size distribution is an immediate quest in diverse areas of science and technology. Electroless wet chemical etching or stain etching can produce semiconductor nanoparticles with high yield but is limited to a few materials because of the lack of understanding the physical-chemical processes behind. Here we report a no-photon exciton generation chemistry (NPEGEC) process, playing a key role in stain etching of semiconductors. We demonstrate NPEGEC on silicon carbide polymorphs as model materials. Specifically, size control of cubic silicon carbide nanoparticles of diameter below ten nanometers was achieved by engineering hexagonal inclusions in microcrystalline cubic silicon carbide. Our finding provides a recipe to engineer patterned semiconductor nanostructures for a broad class of materials.

Communication: Strong excitonic and vibronic effects determine the optical properties of Li₂O₂

DEFF Research Database (Denmark)

García Lastra, Juan Maria; Bass, J. D.; Thygesen, Kristian Sommer

2011-01-01

The band structure and optical absorption spectrum of lithium peroxide (Li2O2) is calculated from first-principles using the G0W0 approximation and the Bethe-Salpeter equation, respectively. A strongly localized (Frenkel type) exciton corresponding to the π*→σ* transition on the O2 −2 peroxide ion...

Ultrafast Mid-Infrared Intra-Excitonic Response of Individualized Single-Walled Carbon Nanotubes

International Nuclear Information System (INIS)

Wang, Jigang; Graham, Matt W.; Ma, Yingzhong; Fleming, Graham R.; Kaindl, Robert A.

2009-01-01

The quasi-1D confinement and reduced screening of photoexcited charges in single-walled carbon nanotubes (SWNTs) entails strongly-enhanced Coulomb interactions and exciton binding energies. Such amplified electron-hole (e-h) correlations have important implications for both fundamental physics and optoelectronic applications of nanotubes. The availability of 'individualized' SWNT ensembles with bright and structured luminescence has rendered specific tube chiralities experimentally accessible. In these samples, evidence for excitonic behavior was found in absorption-luminescence maps, two-photon excited luminescence, or ultrafast carrier dynamics. Here, we report ultrafast mid-infrared (mid-IR) studies of individualized SWNTs, evidencing strong photoinduced absorption around 200 meV in semiconducting tubes of (6,5) and (7,5) chiralities. This manifests the observation of quasi-1D intra-excitonic transitions between different relative-momentum states, in agreement with the binding energy and calculated oscillator strength. Our measurements further reveal a saturation of the photoinduced absorption with increasing phase-space filling of the correlated e-h pairs. The transient mid-IR response represents a new tool, unhindered by restrictions of momentum or interband dipole moment, to investigate the density and dynamics of SWNT excitons.

Exciton absorption spectrum of thin Ag sub 2 ZnI sub 4

CERN Document Server

Yunakova, O N; Kovalenko, E N

2002-01-01

In Ag sub 2 ZnI sub 4 compound thin films one investigated into the electron spectrum of absorption within 3-6 eV photon energy range. The boundary of interband absorption is determined to correspond to the direct permitted transitions with E sub g = 3.7 eV forbidden gap width. A strong exciton band at E = 3.625 eV (80 K) GAMMA half width temperature run of which within 80-390 K range is governed by exciton-phonon interaction typical for quasi-single-dimensional excitons, is adjacent to the absorption boundary. At T <= 390 K one observes a bend in E(T) and GAMMA(T) dependences associated with generation of the Frenkel defects and followed by transfer of Ag ions to the interstices and vacancies of the compound crystalline lattice

Strongly Enhanced Free-Exciton Luminescence in Microcrystalline CsPbBr3 Films

Science.gov (United States)

Kondo, Shin-ichi; Kakuchi, Mitsugu; Masaki, Atsushi; Saito, Tadaaki

2003-07-01

The luminescence properties of CsPbBr3 films prepared via the amorphous phase by crystallization are dominated by free-exciton emission, and only a weak trace of emission due to trapped excitons was observed, in contrast to the case of bulk CsPbBr3 crystals. In particular, the films in the microcrystalline state show by more than an order of magnitude stronger free-exciton emission than in the polycrystalline state. The enhanced free-exciton emission is suggestive of excitonic superradiance.

Energy and Information Transfer Via Coherent Exciton Wave Packets

Science.gov (United States)

Zang, Xiaoning

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

Positronium-photon and photon-positronium quantum transitions in strong magnetic fields

International Nuclear Information System (INIS)

Leinson, L.B.; Oraevskii, V.N.; Radio-Wave Propagation, Academy of Sciences of the USSR)

1985-01-01

The wave functions and energy levels of bound electron-positron pairs in a strong magnetic field H>>α 2 H 0 , where H 0 = m 2 0 c 3 /eh = 4.4 x 10 13 G and α = e 2 /hc, are found in the nonrelativistic approximation. The probabilities of one-photon annihilation of positronium and of the inverse transition from a resonance photon to a positronium atom are calculated. It is shown that in a sufficiently strong magnetic field H∼H 0 , when the probability of one-photon annihilation is considerably greater than the probability of two-photon annihilation of positronium, the lifetime of the decay photon with respect to the inverse transformation to a positronium atom is so small that the decay photon cannot propagate freely in the magnetic field. Therefore, the lifetime of the positronium atom in the case H∼H 0 is determined by the two-photon decay. The possibility of the decay γ→γ 1 +γ 2 via intermediate positronium states in a magnetic field with curved field lines is discussed

Accessing the dark exciton spin in deterministic quantum-dot microlenses

Science.gov (United States)

Heindel, Tobias; Thoma, Alexander; Schwartz, Ido; Schmidgall, Emma R.; Gantz, Liron; Cogan, Dan; Strauß, Max; Schnauber, Peter; Gschrey, Manuel; Schulze, Jan-Hindrik; Strittmatter, Andre; Rodt, Sven; Gershoni, David; Reitzenstein, Stephan

2017-12-01

The dark exciton state in semiconductor quantum dots (QDs) constitutes a long-lived solid-state qubit which has the potential to play an important role in implementations of solid-state-based quantum information architectures. In this work, we exploit deterministically fabricated QD microlenses which promise enhanced photon extraction, to optically prepare and read out the dark exciton spin and observe its coherent precession. The optical access to the dark exciton is provided via spin-blockaded metastable biexciton states acting as heralding states, which are identified by deploying polarization-sensitive spectroscopy as well as time-resolved photon cross-correlation experiments. Our experiments reveal a spin-precession period of the dark exciton of (0.82 ± 0.01) ns corresponding to a fine-structure splitting of (5.0 ± 0.7) μeV between its eigenstates |↑ ⇑ ±↓ ⇓ ⟩. By exploiting microlenses deterministically fabricated above pre-selected QDs, our work demonstrates the possibility to scale up implementations of quantum information processing schemes using the QD-confined dark exciton spin qubit, such as the generation of photonic cluster states or the realization of a solid-state-based quantum memory.

Strongly bound excitons in monolayer PtS2 and PtSe2

KAUST Repository

Sajjad, M.

2018-01-22

Based on first-principles calculations, the structural, electronic, and optical properties of monolayers PtS2 and PtSe2 are investigated. The bond stiffnesses and elastic moduli are determined by means of the spring constants and strain-energy relations, respectively. Dynamic stability is confirmed by calculating the phonon spectra, which shows excellent agreement with experimental reports for the frequencies of the Raman-active modes. The Heyd-Scuseria-Ernzerhof functional results in electronic bandgaps of 2.66 eV for monolayer PtS2 and 1.74 eV for monolayer PtSe2. G0W0 calculations combined with the Bethe-Salpeter equation are used to predict the optical spectra and exciton binding energies (0.78 eV for monolayer PtS2 and 0.60 eV for monolayer PtSe2). It turns out that the excitons are strongly bound and therefore very stable against external perturbations.

Exciton-relaxation dynamics in lead halides

International Nuclear Information System (INIS)

Iwanaga, Masanobu; Hayashi, Tetsusuke

2003-01-01

We survey recent comprehensive studies of exciton relaxation in the crystals of lead halides. The luminescence and electron-spin-resonance studies have revealed that excitons in lead bromide spontaneously dissociate and both electrons and holes get self-trapped individually. Similar relaxation has been also clarified in lead chloride. The electron-hole separation is ascribed to repulsive correlation via acoustic phonons. Besides, on the basis of the temperature profiles of self-trapped states, we discuss the origin of luminescence components which are mainly induced under one-photon excitation into the exciton band in lead fluoride, lead chloride, and lead bromide

Strong spin-photon coupling in silicon

Science.gov (United States)

Samkharadze, N.; Zheng, G.; Kalhor, N.; Brousse, D.; Sammak, A.; Mendes, U. C.; Blais, A.; Scappucci, G.; Vandersypen, L. M. K.

2018-03-01

Long coherence times of single spins in silicon quantum dots make these systems highly attractive for quantum computation, but how to scale up spin qubit systems remains an open question. As a first step to address this issue, we demonstrate the strong coupling of a single electron spin and a single microwave photon. The electron spin is trapped in a silicon double quantum dot, and the microwave photon is stored in an on-chip high-impedance superconducting resonator. The electric field component of the cavity photon couples directly to the charge dipole of the electron in the double dot, and indirectly to the electron spin, through a strong local magnetic field gradient from a nearby micromagnet. Our results provide a route to realizing large networks of quantum dot–based spin qubit registers.

Plasmon-exciton polaritons in two-dimensional semiconductor/metal interfaces

DEFF Research Database (Denmark)

Gonçalves, P. A. D.; Bertelsen, L. P.; Xiao, Sanshui

2018-01-01

The realization and control of polaritons is of paramount importance in the prospect of novel photonic devices. Here, we investigate the emergence of plasmon-exciton polaritons in hybrid structures consisting of a two-dimensional transition-metal dichalcogenide (TMDC) deposited onto a metal......-coupling regime. Our results demonstrate that Rabi splittings exceeding 100 meV can readily be achieved in planar dielectric/TMDC/metal structures under ambient conditions. We thus believe that this Rapid Communication provides a simple and intuitive picture to tailor strong coupling in plexcitonics...

Theoretical investigation of the hyper-Raman scattering in hexagonal semiconductors under two-photon excitation near resonance with the An=2 exciton level

Science.gov (United States)

Semenova, L. E.

2018-04-01

The hyper-Raman scattering of light by LO-phonons under two-photon excitation near resonance with the An=2 exciton level in the wurtzite semiconductors A2B6 was theoretically investigated, taking into account the influence of the complex structure of the top valence band.

Plasmon-exciton-polariton lasing

NARCIS (Netherlands)

Ramezani, M.; Halpin, A.; Fernández-Dominguez, A.I.; Feist, J.; Rodriguez, S.R.K.; Gómez-Rivas, J.; Garcia-Vidal, F.J.

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

Excitonic condensation in systems of strongly correlated electrons

Czech Academy of Sciences Publication Activity Database

Kuneš, Jan

2015-01-01

Roč. 27, č. 33 (2015), s. 333201 ISSN 0953-8984 Institutional support: RVO:68378271 Keywords : electronic correlations * exciton * Bose-Einstein condensation Subject RIV: BM - Solid Matter Physics ; Magnetism Impact factor: 2.209, year: 2015

Energy transfer of excitons between quantum wells separated by a wide barrier

International Nuclear Information System (INIS)

Lyo, S. K.

2000-01-01

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 (Δ) at low temperatures (T). Several important intrinsic energy-transfer mechanisms have been examined, including dipolar coupling, real and virtual photon-exchange coupling, and over-barrier ionization of the excitons via exciton-exciton Auger processes. The transfer rate is calculated as a function of T and the center-to-center distance d between the wells. The rates depend sensitively on T for plane-wave excitons. For localized excitons, the rates depend on T only through the T dependence of the exciton localization radius. For Stokes energy transfer, the dominant energy transfer occurs through a photon-exchange interaction, which enables the excitons from the higher-energy wells to decay into free electrons and holes in the lower-energy wells. The rate has a slow dependence on d, yielding reasonable agreement with recent data from GaAs/Al x Ga 1-x As quantum wells. The dipolar rate is about an order of magnitude smaller for large d (e.g., d=175Aa) with a stronger range dependence proportional to d -4 . However, the latter can be comparable to the radiative rate for small d (e.g., d≤80Aa). For anti-Stokes transfer through exchange-type (e.g., dipolar and photon-exchange) interactions, we show that thermal activation proportional to exp(-Δ/k B T) is essential for the transfer, contradicting a recent nonactivated result based on the Fo''rster-Dexter's spectral-overlap theory. Phonon-assisted transfer yields a negligibly small rate. On the other hand, energy transfer through over-barrier ionization of excitons via Auger processes yields a significantly larger nonactivated rate which is independent of d. The result is compared with recent data

Nearly Blinking-Free, High-Purity Single-Photon Emission by Colloidal InP/ZnSe Quantum Dots.

Science.gov (United States)

Chandrasekaran, Vigneshwaran; Tessier, Mickaël D; Dupont, Dorian; Geiregat, Pieter; Hens, Zeger; Brainis, Edouard

2017-10-11

Colloidal core/shell InP/ZnSe quantum dots (QDs), recently produced using an improved synthesis method, have a great potential in life-science applications as well as in integrated quantum photonics and quantum information processing as single-photon emitters. Single-particle spectroscopy of 10 nm QDs with 3.2 nm cores reveals strong photon antibunching attributed to fast (70 ps) Auger recombination of multiple excitons. The QDs exhibit very good photostability under strong optical excitation. We demonstrate that the antibunching is preserved when the QDs are excited above the saturation intensity of the fundamental-exciton transition. This result paves the way toward their usage as high-purity on-demand single-photon emitters at room temperature. Unconventionally, despite the strong Auger blockade mechanism, InP/ZnSe QDs also display very little luminescence intermittency ("blinking"), with a simple on/off blinking pattern. The analysis of single-particle luminescence statistics places these InP/ZnSe QDs in the class of nearly blinking-free QDs, with emission stability comparable to state-of-the-art thick-shell and alloyed-interface CdSe/CdS, but with improved single-photon purity.

Observation of surface excitons in rare gas solids

International Nuclear Information System (INIS)

Saile, V.; Skibowski, M.; Steinmann, W.; Guertler, P.; Koch, E.E.; Kozevnikov, A.

1976-04-01

Evidence is obtained for the excitation of surface excitons in solid Ar, Kr and Xe in optical transmission and reflection experiments using synchrotron radiation. They are located at photon energies ranging from 0.6 eV for Ar to 0.1 eV for Xe below the corresponding bulk excitons excited from the valence bands. Their halfwidths (20-50 MeV) is less than half the values found for the bulk excitons. Some are split by an amount considerably smaller than the spin orbit splitting of the valence bands. (orig.) [de

Strong room-temperature ultraviolet to red excitons from inorganic organic-layered perovskites, (MX4 (M=Pb, Sn, Hg; X=I-, Br-)

Science.gov (United States)

Ahmad, Shahab; Prakash, G. Vijaya

2014-01-01

Many varieties of layered inorganic-organic (IO) perovskite of type (MX4 (where R: organic moiety, M: divalent metal, and X: halogen) were successfully fabricated and characterized. X-ray diffraction data suggest that these inorganic and organic structures are alternatively stacked up along c-axis, where inorganic mono layers are of extended corner-shared MX6 octahedra and organic spacers are the bi-layers of organic entities. These layered perovskites show unusual room-temperature exciton absorption and photoluminescence due to the quantum and dielectric confinement-induced enhancement in the exciton binding energies. A wide spectral range of optical exciton tunability (350 to 600 nm) was observed experimentally from systematic compositional variation in (i) divalent metal ions (M=Pb, Sn, Hg), (ii) halides (X=I and Br-), and (iii) organic moieties (R). Specific photoluminescence features are due to the structure of the extended MX42- network and the eventual electronic band structure. The compositionally dependent photoluminescence of these IO hybrids could be useful in various photonic and optoelectronic devices.

Strong WW scattering at photon linear colliders

International Nuclear Information System (INIS)

Berger, M.S.

1994-06-01

We investigate the possibility of observing strong interactions of longitudinally polarized weak vector bosons in the process γγ → ZZ at a photon linear collider. We make use of polarization of the photon beams and cuts on the decay products of the Z bosons to enhance the signal relative to the background of transversely polarized ZZ pairs. We find that the background overwhelms the signal unless there are strong resonant effects, as for instance from a technicolor analogue of the hadronic f 2 (1270) meson

Excitonic bistabilities, instabilities and chaos in laser-pumped semiconductor

International Nuclear Information System (INIS)

Nguyen Ba An; Nguyen Trung Dan; Hoang Xuan Nguyen

1992-07-01

The Hurwitz criteria are used for a stability analysis of the steady state excitonic optical bistability curves in a semiconductor pumped by an external laser resonant with the exciton level. Besides the middle branch of the bistability curves which is unstable in the sense of the linear stability theory, we have found other domains of instability in the upper and lower branches of the steady state curves. Numerical results show that a possible route to chaos in the photon-exciton system is period-doubling self-oscillation process. The influence of the presence of free carriers that coexist with the excitons is also discussed. (author). 16 refs, 6 figs

Frenkel-Charge-Transfer exciton intermixing theory for molecular crystals with two isolated Frenkel exciton states.

Science.gov (United States)

Bondarev, Igor; Popescu, Adrian

We develop an analytical theory for the intra-intermolecular exciton intermixing in periodic 1D chains of planar organic molecules with two isolated low-lying Frenkel exciton states, typical of copper phthalocyanine (CuPc) and other transition metal phthalocyanine molecules. We formulate the Hamiltonian and use the exact Bogoliubov diagonalization procedure to derive the eigen energy spectrum for the two lowest intramolecular Frenkel excitons coupled to the intermolecular charge transfer (CT) exciton state. By comparing our theoretical spectrum with available experimental CuPc absorption data, we obtain the parameters of the Frenkel-CT exciton intermixing in CuPc thin films. The two Frenkel exciton states here are spaced apart by 0.26 eV, and the charge transfer exciton state is 50 meV above the lowest Frenkel exciton. Both Frenkel excitons are strongly mixed with the CT exciton, showing the coupling constant 0.17 eV in agreement with earlier electron transport experiments. Our results can be used for the proper interpretation of the physical properties of crystalline phthalocyanines. DOE-DE-SC0007117 (I.B.), UNC-GA ROI Grant (A.P.).

Exciton-polaritons in cuprous oxide: Theory and comparison with experiment

Science.gov (United States)

Schweiner, Frank; Ertl, Jan; Main, Jörg; Wunner, Günter; Uihlein, Christoph

2017-12-01

The observation of giant Rydberg excitons in cuprous oxide (Cu2O ) up to a principal quantum number of n =25 by T. Kazimierczuk et al. [Nature (London) 514, 343 (2014), 10.1038/nature13832] inevitably raises the question whether these quasiparticles must be described within a multipolariton framework since excitons and photons are always coupled in the solid. In this paper we present the theory of exciton-polaritons in Cu2O . To this end we extend the Hamiltonian which includes the complete valence-band structure, the exchange interaction, and the central-cell corrections effects, and which has been recently deduced by F. Schweiner et al. [Phys. Rev. B 95, 195201 (2017), 10.1103/PhysRevB.95.195201], for finite values of the exciton momentum ℏ K . We derive formulas to calculate not only dipole but also quadrupole oscillator strengths when using the complete basis of F. Schweiner et al., which has recently been proven as a powerful tool to calculate exciton spectra. Very complex polariton spectra for the three orientations of K along the axes [001 ] , [110 ] , and [111 ] of high symmetry are obtained and a strong mixing of exciton states is reported. The main focus is on the 1 S ortho-exciton-polariton, for which pronounced polariton effects have been measured in experiments. We set up a 5 ×5 matrix model, which accounts for both the polariton effect and the K -dependent splitting, and which allows treating the anisotropic polariton dispersion for any direction of K . We especially discuss the dispersions for K being oriented in the planes perpendicular to [1 1 ¯0 ] and [111 ] , for which experimental transmission spectra have been measured. Furthermore, we compare our results with experimental values of the K -dependent splitting, the group velocity, and the oscillator strengths of this exciton-polariton. The results are in good agreement. This proves the validity of the 5 ×5 matrix model as a useful theoretical model for further investigations on the 1 S

Synthesis of zinc oxide microrods and nano-fibers with dominant exciton emission at room temperature

Energy Technology Data Exchange (ETDEWEB)

Ramos-Brito, F., E-mail: fro_brito@yahoo.com.m [Laboratorio de Materiales Optoelectronicos del Centro de Ciencias de Sinaloa, Ave. de las Americas 2771 Col. Villa Universidad 80010, Culiacan, Sinaloa (Mexico); Alejo-Armenta, C. [Laboratorio de Materiales Optoelectronicos del Centro de Ciencias de Sinaloa, Ave. de las Americas 2771 Col. Villa Universidad 80010, Culiacan, Sinaloa (Mexico); Garcia-Hipolito, M. [Departamento de Materiales Metalicos y Ceramicos, Instituto de Investigaciones en Materiales, Universidad Nacional Autonoma de Mexico, AP 70-360, Coyoacan 04510, DF (Mexico); Camarillo, E.; Hernandez A, J. [Instituto de Fisica, Universidad Nacional Autonoma de Mexico, AP 20-364, Alvaro Obregon 01000, DF (Mexico); Falcony, C. [Departamento de Fisica, CINVESTAV-IPN, AP 14-740, 07000, DF (Mexico); Murrieta S, H. [Instituto de Fisica, Universidad Nacional Autonoma de Mexico, AP 20-364, Alvaro Obregon 01000, DF (Mexico)

2011-05-15

Employing a simple chemical synthesis method, hexagonal-shaped zinc oxide microrods and zinc oxide nano-fibers were deposited on pyrex-glass and aluminum substrates, respectively. Both kinds of deposits showed zincite crystalline phase with lattice parameters: a=3.2498 A and c=5.2066 A. Microrods showed very uniform wide and large sizes of around 1 and 10 {mu}m, respectively. Both deposits were homogeneous over all substrate surfaces. Microrods and nano-fibers resulted with good optical quality and with preferential crystalline growth in [1 0 1 0]and [0 0 0 1]directions. The principal optical characteristics for both microrods and nano-fibers were: a) room-temperature photo and cathodo-luminescent spectra with strong exciton emission centered around 390 nm and with FWHMs around 125 and 160 meV, respectively, b) poor photo and cathode-luminescent emissions in the visible region of the electromagnetic spectrum, c) energy band gap of 3.32 eV, d) good emission efficiency supported by the not-required high energy densities to obtain strong exciton emission and e) good ZnO stoichiometry endorsed by photoluminescent results. These characteristics make of these microrods and nano-fibers good for potential photonic applications. - Research highlights: {yields} Microrods and nano-fibers resulted with good optical quality and with preferential crystalline growth in [1 0 1 0]and [0 0 0 1]directions. {yields} Microrods and nano-fibers resulted with good emission efficiency supported by the not-required high energy densities to obtain strong exciton emission. {yields} The wet chemical method is appropriated for deposition of microrods and nano-fibers with the desired optical properties for its possible application in photonics.

Synthesis of zinc oxide microrods and nano-fibers with dominant exciton emission at room temperature

International Nuclear Information System (INIS)

Ramos-Brito, F.; Alejo-Armenta, C.; Garcia-Hipolito, M.; Camarillo, E.; Hernandez A, J.; Falcony, C.; Murrieta S, H.

2011-01-01

Employing a simple chemical synthesis method, hexagonal-shaped zinc oxide microrods and zinc oxide nano-fibers were deposited on pyrex-glass and aluminum substrates, respectively. Both kinds of deposits showed zincite crystalline phase with lattice parameters: a=3.2498 A and c=5.2066 A. Microrods showed very uniform wide and large sizes of around 1 and 10 μm, respectively. Both deposits were homogeneous over all substrate surfaces. Microrods and nano-fibers resulted with good optical quality and with preferential crystalline growth in [1 0 1 0] and [0 0 0 1] directions. The principal optical characteristics for both microrods and nano-fibers were: a) room-temperature photo and cathodo-luminescent spectra with strong exciton emission centered around 390 nm and with FWHMs around 125 and 160 meV, respectively, b) poor photo and cathode-luminescent emissions in the visible region of the electromagnetic spectrum, c) energy band gap of 3.32 eV, d) good emission efficiency supported by the not-required high energy densities to obtain strong exciton emission and e) good ZnO stoichiometry endorsed by photoluminescent results. These characteristics make of these microrods and nano-fibers good for potential photonic applications. - Research highlights: → Microrods and nano-fibers resulted with good optical quality and with preferential crystalline growth in [1 0 1 0] and [0 0 0 1] directions. → Microrods and nano-fibers resulted with good emission efficiency supported by the not-required high energy densities to obtain strong exciton emission. → The wet chemical method is appropriated for deposition of microrods and nano-fibers with the desired optical properties for its possible application in photonics.

Microscopic description of exciton polaritons in direct two-band semiconductors

Science.gov (United States)

Nguyen, Van Trong; Mahler, Günter

1999-07-01

Based on a quantum electrodynamical formulation, a microscopic description of exciton polaritons in a two-band semiconductor is presented. We show that the interband exchange Coulomb interaction, responsible for the coupling of the exciton with the longitudinal part of the induced field, should be treated on equal footing together with the coupling to the transverse part of the induced field (the photon field). The constitutive relation is established to connect the current density with the total electric field of polaritons. The classical Maxwell equations are derived from the quantum representation of photons to get a closed system of equations. The temporal evolution for an initial excited exciton state is studied in detail and an anisotropic polariton vacuum Rabi splitting is shown to occur. A number of up-to-now unresolved discrepancies in the literature are clarified.

Controlling the exciton energy of a nanowire quantum dot by strain fields

Energy Technology Data Exchange (ETDEWEB)

Chen, Yan; Zhang, Jiaxiang; Ding, Fei, E-mail: f.ding@ifw-dresden.de [Institute for Integrative Nanosciences, IFW Dresden, Helmholtz Strasse 20, 01069 Dresden (Germany); Zadeh, Iman Esmaeil; Jöns, Klaus D.; Fognini, Andreas; Zwiller, Val [Kavli Institute of Nanoscience, Delft University of Technology, 2600 GA Delft (Netherlands); Reimer, Michael E. [Institute for Quantum Computing and Department of Electrical and Computer Engineering, University of Waterloo, Waterloo, N2L 3G1 (Canada); Dalacu, Dan; Poole, Philip J. [National Research Council, Ottawa, Ontario K1A 0R6 (Canada); Schmidt, Oliver G. [Institute for Integrative Nanosciences, IFW Dresden, Helmholtz Strasse 20, 01069 Dresden (Germany); Material Systems for Nanoelectronics, Chemnitz University of Technology, Reichenhainer Strasse 70, 09107 Chemnitz (Germany)

2016-05-02

We present an experimental route to engineer the exciton energies of single quantum dots in nanowires. By integrating the nanowires onto a piezoelectric crystal, we controllably apply strain fields to the nanowire quantum dots. Consequently, the exciton energy of a single quantum dot in the nanowire is shifted by several meVs without degrading its optical intensity and single-photon purity. Second-order autocorrelation measurements are performed at different strain fields on the same nanowire quantum dot. The suppressed multi-photon events at zero time delay clearly verify that the quantum nature of single-photon emission is well preserved under external strain fields. The work presented here could facilitate on-chip optical quantum information processing with the nanowire based single photon emitters.

Dynamics of Charged Excitons and Biexcitons in CsPbBr3 Perovskite Nanocrystals Revealed by Femtosecond Transient-Absorption and Single-Dot Luminescence Spectroscopy.

Science.gov (United States)

Yarita, Naoki; Tahara, Hirokazu; Ihara, Toshiyuki; Kawawaki, Tokuhisa; Sato, Ryota; Saruyama, Masaki; Teranishi, Toshiharu; Kanemitsu, Yoshihiko

2017-04-06

Metal-halide perovskite nanocrystals (NCs) are promising photonic materials for use in solar cells, light-emitting diodes, and lasers. The optoelectronic properties of these devices are determined by the excitons and exciton complexes confined in their NCs. In this study, we determined the relaxation dynamics of charged excitons and biexcitons in CsPbBr 3 NCs using femtosecond transient-absorption (TA), time-resolved photoluminescence (PL), and single-dot second-order photon correlation spectroscopy. Decay times of ∼40 and ∼200 ps were obtained from the TA and PL decay curves for biexcitons and charged excitons, respectively, in NCs with an average edge length of 7.7 nm. The existence of charged excitons even under weak photoexcitation was confirmed by the second-order photon correlation measurements. We found that charged excitons play a dominant role in luminescence processes of CsPbBr 3 NCs. Combining different spectroscopic techniques enabled us to clarify the dynamical behaviors of excitons, charged excitons, and biexcitons.

Quantum-dot excitons in nanostructured environments

DEFF Research Database (Denmark)

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

2010-01-01

determined the oscillator strength, quantum efficiency and spin-flip rates of QD excitons as well as their dependencies on emission wavelength and QD size. Enhancement and inhibition of QD spontaneous emission in photonic crystal membranes (PCMs) is observed. Efficient coupling to PCM waveguides...

Quantum-dot excitons in nanostructured environments

DEFF Research Database (Denmark)

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

2011-01-01

determined the oscillator strength, quantum efficiency and spin-flip rates of QD excitons as well as their dependencies on emission wavelength and QD size. Enhancement and inhibition of QD spontaneous emission in photonic crystal membranes (PCMs) is observed. Efficient coupling to PCM waveguides...

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.

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.

Cosmogenic photons strongly constrain UHECR source models

Directory of Open Access Journals (Sweden)

van Vliet Arjen

2017-01-01

Full Text Available With the newest version of our Monte Carlo code for ultra-high-energy cosmic ray (UHECR propagation, CRPropa 3, the flux of neutrinos and photons due to interactions of UHECRs with extragalactic background light can be predicted. Together with the recently updated data for the isotropic diffuse gamma-ray background (IGRB by Fermi LAT, it is now possible to severely constrain UHECR source models. The evolution of the UHECR sources especially plays an important role in the determination of the expected secondary photon spectrum. Pure proton UHECR models are already strongly constrained, primarily by the highest energy bins of Fermi LAT’s IGRB, as long as their number density is not strongly peaked at recent times.

Multiphonon resonant Raman scattering in the semimagnetic semiconductor Cd1-xMnxTe: Froehlich and deformation potential exciton-phonon interaction

International Nuclear Information System (INIS)

Riera, R; Rosas, R; Marin, J L; Bergues, J M; Campoy, G

2003-01-01

A theory describing multiphonon resonant Raman scattering (MPRRS) processes in wide-gap diluted magnetic semiconductors is presented, with Cd 1-x Mn x Te as an example. The incident radiation frequency ω l is taken above the fundamental absorption region. The photoexcited electron and hole make real transitions through the LO phonon, when one considers Froehlich (F) and deformation potential (DP) interactions. The strong exchange interaction, typical of these materials, leads to a large spin splitting of the exciton states in the magnetic field. Neglecting Landau quantization, this Zeeman splitting gives rise to the formation of eight bands (two conduction and six valence ones) and ten different exciton states according to the polarization of the incident light. Explicit expressions for the MPRRS intensity of second and third order, the indirect creation and annihilation probabilities, the exciton lifetime, and the probabilities of transition between different exciton states and different types of exciton as a function of ω l and the external magnetic field are presented. The selection rules for all hot exciton transitions via exciton-photon interaction and F and DP exciton-phonon interactions are investigated. The exciton energies, as a function of B, the Mn concentration x, and the temperature T, are compared to a theoretical expression. Graphics for creation and annihilation probabilities, lifetime, and Raman intensity of second and third order are discussed

Charge separation in excitonic and bipolar solar cells - A detailed balance approach

International Nuclear Information System (INIS)

Kirchartz, Thomas; Rau, Uwe

2008-01-01

A generalized solar cell model for excitonic and classical, bipolar solar cells is developed that describes the combined transport and interaction of electrons, holes and excitons. Both, conventional inorganic solar cells as well as organic solar cells, where excitons play a dominant role for energy transport, turn out to be special cases of this model. Due to the inclusion of photon recycling effects, the approach is compatible with the principle of detailed balance and the Shockley-Queisser limit. We show how varying the interaction between excitons and charge carriers as well as varying the respective mobilities of the different species changes the operation mode of the solar cell path between excitonic and bipolar

Shear viscosities of photons in strongly coupled plasmas

Directory of Open Access Journals (Sweden)

Di-Lun Yang

2016-09-01

Full Text Available We investigate the shear viscosity of thermalized photons in the quark gluon plasma (QGP at weak coupling and N=4 super Yang–Mills plasma (SYMP at both strong and weak couplings. We find that the shear viscosity due to the photon–parton scattering up to the leading order of electromagnetic coupling is suppressed when the coupling of the QGP/SYMP is increased, which stems from the blue-shift of the thermal-photon spectrum at strong coupling. In addition, the shear viscosity rapidly increases near the deconfinement transition in a phenomenological model analogous to the QGP.

Recent advances in organic one-dimensional composite materials: design, construction, and photonic elements for information processing.

Science.gov (United States)

Yan, Yongli; Zhang, Chuang; Yao, Jiannian; Zhao, Yong Sheng

2013-07-19

Many recent activities in the use of one-dimensional nanostructures as photonic elements for optical information processing are explained by huge advantages that photonic circuits possess over traditional silicon-based electronic ones in bandwidth, heat dissipation, and resistance to electromagnetic wave interference. Organic materials are a promising candidate to support these optical-related applications, as they combine the properties of plastics with broad spectral tunability, high optical cross-section, easy fabrication, as well as low cost. Their outstanding compatibility allows organic composite structures which are made of two or more kinds of materials combined together, showing great superiority to single-component materials due to the introduced interactions among multiple constituents, such as energy transfer, electron transfer, exciton coupling, etc. The easy processability of organic 1D crystalline heterostructures enables a fine topological control of both composition and geometry, which offsets the intrinsic deficiencies of individual material. At the same time, the strong exciton-photon coupling and exciton-exciton interaction impart the excellent confinement of photons in organic microstructures, thus light can be manipulated according to our intention to realize specific functions. These collective properties indicate a potential utility of organic heterogeneous material for miniaturized photonic circuitry. Herein, focus is given on recent advances of 1D organic crystalline heterostructures, with special emphasis on the novel design, controllable construction, diverse performance, as well as wide applications in isolated photonic elements for integration. It is proposed that the highly coupled, hybrid optical networks would be an important material basis towards the creation of on-chip optical information processing. Copyright © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Plasmon exciton-polariton lasing

NARCIS (Netherlands)

Ramezani, M.; Halpin, H.A.; Feist, J.; Fernández-Dominguez, A.; Rodriguez, S.R.K.; Garcia-Vidal, F.J.; Gomez-Rivas, J.

2017-01-01

Strong light-matter interaction leads to the appearance of new states, i.e. exciton-polaritons, with photophysical properties rather distinct from their constituents. Recent developments in fabrication techniques allow us to make metallic structures with strong electric field confinement in

Self-trapped excitonic green emission from layered semiconductors

International Nuclear Information System (INIS)

Miah, M. Idrish

2009-01-01

Crystals of layered semiconductor are grown by Bridgman technique and are studied them under two-photon excitation by a Q-switched 20-ns pulse laser. The photoluminescence (PL) emission spectra of the crystals are measured at various pumping powers and temperatures. The PL spectra appear broad and structureless emissions with their peaks in the green spectral region. The characteristic emissions are from self-trapped excitons of the crystals. An analysis of the spectra measured at various pumping powers shows a quadratic dependence of the PL peak intensity on the power, confirming a biphotonic process of the two-photon pumping. The temperature dependence shows an enhancement of the nonlinear response at low temperatures. The activation energy is estimated and found to be 2.4 meV. The roles of the bound excitons in the observed PL are discussed briefly.

Self-trapped excitonic green emission from layered semiconductors

Energy Technology Data Exchange (ETDEWEB)

Miah, M. Idrish, E-mail: m.miah@griffith.edu.au [Nanoscale Science and Technology Centre, Griffith University, Nathan, Brisbane, QLD 4111 (Australia); School of Biomolecular and Physical Sciences, Griffith University, Nathan, Brisbane, QLD 4111 (Australia); Department of Physics, University of Chittagong, Chittagong 4331 (Bangladesh)

2009-08-15

Crystals of layered semiconductor are grown by Bridgman technique and are studied them under two-photon excitation by a Q-switched 20-ns pulse laser. The photoluminescence (PL) emission spectra of the crystals are measured at various pumping powers and temperatures. The PL spectra appear broad and structureless emissions with their peaks in the green spectral region. The characteristic emissions are from self-trapped excitons of the crystals. An analysis of the spectra measured at various pumping powers shows a quadratic dependence of the PL peak intensity on the power, confirming a biphotonic process of the two-photon pumping. The temperature dependence shows an enhancement of the nonlinear response at low temperatures. The activation energy is estimated and found to be 2.4 meV. The roles of the bound excitons in the observed PL are discussed briefly.

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...

Quantum condensation from a tailored exciton population in a microcavity

International Nuclear Information System (INIS)

Eastham, P. R.; Phillips, R. T.

2009-01-01

An experiment is proposed on the coherent quantum dynamics of a semiconductor microcavity containing quantum dots. Modeling the experiment using a generalized Dicke model, we show that a tailored excitation pulse can create an energy-dependent population of excitons, which subsequently evolves to a quantum condensate of excitons and photons. The population is created by a generalization of adiabatic rapid passage and then condenses due to a dynamical analog of the BCS instability.

Self-localization of excitons in a periodically modulated molecular medium

International Nuclear Information System (INIS)

Zabolotskii, A. A.

2006-01-01

Electromagnetic field propagation is analyzed in a one-dimensional Bragg grating consisting of periodically arranged linear molecules making up a resonant medium. Dye J-aggregates and conjugated polymers are considered as examples of the medium. Both adiabatic and nonadiabatic dynamics of the acoustic waves generated by electromagnetic field in the system are examined. The effects of exciton-phonon and exciton-phonon-photon interactions on the band structure and formation of self-localized excitations are examined on various time scales. A new mechanism for controlling bandgap parameters in a bistable regime is described. Some effects of electromagnetic-field nonuniformity on generation of phonons in molecules and exciton self-localization are investigated

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...

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.

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...

Effect of interface disorder on quantum well excitons and microcavity polaritons

International Nuclear Information System (INIS)

Savona, Vincenzo

2007-01-01

The theory of the linear optical response of excitons in quantum wells and polaritons in planar semiconductor microcavities is reviewed, in the light of the existing experiments. For quantum well excitons, it is shown that disorder mainly affects the exciton centre-of-mass motion and is modelled by an effective Schroedinger equation in two dimensions. For polaritons, a unified model accounting for quantum well roughness and fluctuations of the microcavity thickness is developed. Numerical results confirm that polaritons are mostly affected by disorder acting on the photon component, thus confirming existing studies on the influence of exciton disorder. The polariton localization length is estimated to be in the few-micrometres range, depending on the amplitude of disorder, in agreement with recent experimental findings

Multiple exciton generation in chiral carbon nanotubes: Density functional theory based computation

Science.gov (United States)

Kryjevski, Andrei; Mihaylov, Deyan; Kilina, Svetlana; Kilin, Dmitri

2017-10-01

We use a Boltzmann transport equation (BE) to study time evolution of a photo-excited state in a nanoparticle including phonon-mediated exciton relaxation and the multiple exciton generation (MEG) processes, such as exciton-to-biexciton multiplication and biexciton-to-exciton recombination. BE collision integrals are computed using Kadanoff-Baym-Keldysh many-body perturbation theory based on density functional theory simulations, including exciton effects. We compute internal quantum efficiency (QE), which is the number of excitons generated from an absorbed photon in the course of the relaxation. We apply this approach to chiral single-wall carbon nanotubes (SWCNTs), such as (6,2) and (6,5). We predict efficient MEG in the (6,2) and (6,5) SWCNTs within the solar spectrum range starting at the 2Eg energy threshold and with QE reaching ˜1.6 at about 3Eg, where Eg is the electronic gap.

Interlayer excitons in a bulk van der Waals semiconductor

DEFF Research Database (Denmark)

Arora, Ashish; Drueppel, Matthias; Schmidt, Robert

2017-01-01

Bound electron-hole pairs called excitons govern the electronic and optical response of many organic and inorganic semiconductors. Excitons with spatially displaced wave functions of electrons and holes (interlayer excitons) are important for Bose-Einstein condensation, superfluidity......, dissipationless current flow, and the light-induced exciton spin Hall effect. Here we report on the discovery of interlayer excitons in a bulk van der Waals semiconductor. They form due to strong localization and spin-valley coupling of charge carriers. By combining high-field magneto-reflectance experiments...

Nonlinear spectroscopy of excitons and biexcitons in ZnS

International Nuclear Information System (INIS)

Pavlov, L.I.; Paskov, P.P.; Lalov, I.J.

1989-01-01

Four- photon spectroscopy on exciton and biexciton states in ZnS is reported at T = 10 K. The Nd:YAG laser is used as a fundamental source in the experimental setup. Second harmonic radiation ω 2 pumps the dye laser of ω 1 tunable frequency. The ZnS single crystal is placed in an optical cryostat for resonant spectroscopy at low temperature. Four-photon mixing ω 3 = 2ω 1 -ω 2 signal is separated by MDR-23 monochromator and is registered by a laser photometer. The hexagonal ZnS crystal is experimentally investigated when the waves ω 1 and ω 2 propagate colinear with the optical axis. The crystal is cut along the (1120) plane. The photon 2ℎω 1 energy scans over the range 3.895-3.940 eV. The dispersion of I 3 (ω 3 ) upon 2ℎω 1 is obtained. Three resonances are registered E M = 3.8964, E B 1 = 3.9010 and E B 2 = 3.9311 eV. The recorded low temperature resonance in dispersion of nonlinearity χ (3) are identified with B 1 s and B 2 s excitons as well as with biexciton in ZnS which is observed for the first time in this crystal. An experimental dependence of the signal I 3 (ω 3 ) intensity upon the pump I 1 (ω 1 ) is obtained. The E M resonance is saturated with the I 1 (ω 1 ) enhancement while the E B 1 resonance increases. Authors explain such a behaviour by the fact that the recombination probability of the biexcitons to excitons increases with the pump level growth. Estimations for the exciton density and the bounding energy are given. (author)

Excitonic Effects in Methylammonium Lead Halide Perovskites

Energy Technology Data Exchange (ETDEWEB)

Beard, Matthew C [National Renewable Energy Laboratory (NREL), Golden, CO (United States); Chen, Xihan [National Renewable Energy Laboratory (NREL), Golden, CO (United States); Lu, Haipeng [National Renewable Energy Laboratory (NREL), Golden, CO (United States); Yang, Ye [National Renewable Energy Laboratory (NREL), Golden, CO (United States)

2018-05-01

The exciton binding energy in methylammonium lead iodide (MAPbI3) is about 10 meV, around 1/3 of the available thermal energy (kBT ~ 26 meV) at room temperature. Thus, exciton populations are not stable at room temperature at moderate photoexcited carrier densities. However, excitonic resonances dominate the absorption onset. Furthermore, these resonances determine the transient absorbance and transient reflectance spectra. The exciton binding energy is a reflection of the Coulomb interaction energy between photoexcited electrons and holes. As such, it serves as a marker for the strength of electron/hole interactions and impacts a variety of phenomena, such as, absorption, radiative recombination, and Auger recombination. In this Perspective, we discuss the role of excitons and excitonic resonances in the optical properties of lead-halide perovskite semiconductors. Finally, we discuss how the strong light-matter interactions induce an optical stark effect splitting the doubly spin degenerate ground exciton states and are easily observed at room temperature.

Microscopic theory of photon-correlation spectroscopy in strong-coupling semiconductors

Energy Technology Data Exchange (ETDEWEB)

Schneebeli, Lukas

2009-11-27

While many quantum-optical phenomena are already well established in the atomic systems, like the photon antibunching, squeezing, Bose-Einstein condensation, teleportation, the quantum-optical investigations in semiconductors are still at their beginning. The fascinating results observed in the atomic systems inspire physicists to demonstrate similar quantum-optical effects also in the semiconductor systems. In contrast to quantum optics with dilute atomic gases, the semiconductors exhibit a complicated many-body problem which is dominated by the Coulomb interaction between the electrons and holes and by coupling with the semiconductor environment. This makes the experimental observation of similar quantum-optical effects in semiconductors demanding. However, there are already experiments which have verified nonclassical effects in semiconductors. In particular, experiments have demonstrated that semiconductor quantum dots (QDs) can exhibit the single-photon emission and generation of polarization-entangled photon pairs. In fact, both atom and QD systems, embedded within a microcavity, have become versatile platforms where one can perform systematic quantum-optics investigations as well as development work toward quantum-information applications. Another interesting field is the strong-coupling regime in which the light-matter coupling exceeds both the decoherence rate of the atom or QD and the cavity resulting in a reversible dynamics between light and matter excitations. In the strong-coupling regime, the Jaynes-Cummings ladder is predicted and shows a photon-number dependent splitting of the new dressed strong-coupling states which are the polariton states of the coupled light-matter system. Although the semiclassical effect of the vacuum Rabi splitting has already been observed in QDs, the verification of the quantum-mechanical Jaynes-Cummings splitting is still missing mainly due to the dephasing. Clearly, the observation of the Jaynes-Cummings ladder in QDs

Interlayer excitons in a bulk van der Waals semiconductor.

Science.gov (United States)

Arora, Ashish; Drüppel, Matthias; Schmidt, Robert; Deilmann, Thorsten; Schneider, Robert; Molas, Maciej R; Marauhn, Philipp; Michaelis de Vasconcellos, Steffen; Potemski, Marek; Rohlfing, Michael; Bratschitsch, Rudolf

2017-09-21

Bound electron-hole pairs called excitons govern the electronic and optical response of many organic and inorganic semiconductors. Excitons with spatially displaced wave functions of electrons and holes (interlayer excitons) are important for Bose-Einstein condensation, superfluidity, dissipationless current flow, and the light-induced exciton spin Hall effect. Here we report on the discovery of interlayer excitons in a bulk van der Waals semiconductor. They form due to strong localization and spin-valley coupling of charge carriers. By combining high-field magneto-reflectance experiments and ab initio calculations for 2H-MoTe 2 , we explain their salient features: the positive sign of the g-factor and the large diamagnetic shift. Our investigations solve the long-standing puzzle of positive g-factors in transition metal dichalcogenides, and pave the way for studying collective phenomena in these materials at elevated temperatures.Excitons, quasi-particles of bound electron-hole pairs, are at the core of the optoelectronic properties of layered transition metal dichalcogenides. Here, the authors unveil the presence of interlayer excitons in bulk van der Waals semiconductors, arising from strong localization and spin-valley coupling of charge carriers.

Chromophore-Dependent Intramolecular Exciton-Vibrational Coupling in the FMO Complex: Quantification and Importance for Exciton Dynamics.

Science.gov (United States)

Padula, Daniele; Lee, Myeong H; Claridge, Kirsten; Troisi, Alessandro

2017-11-02

In this paper, we adopt an approach suitable for monitoring the time evolution of the intramolecular contribution to the spectral density of a set of identical chromophores embedded in their respective environments. We apply the proposed method to the Fenna-Matthews-Olson (FMO) complex, with the objective to quantify the differences among site-dependent spectral densities and the impact of such differences on the exciton dynamics of the system. Our approach takes advantage of the vertical gradient approximation to reduce the computational demands of the normal modes analysis. We show that the region of the spectral density that is believed to strongly influence the exciton dynamics changes significantly in the timescale of tens of nanoseconds. We then studied the impact of the intramolecular vibrations on the exciton dynamics by considering a model of FMO in a vibronic basis and neglecting the interaction with the environment to isolate the role of the intramolecular exciton-vibration coupling. In agreement with the assumptions in the literature, we demonstrate that high frequency modes at energy much larger than the excitonic energy splitting have negligible influence on exciton dynamics despite the large exciton-vibration coupling. We also find that the impact of including the site-dependent spectral densities on exciton dynamics is not very significant, indicating that it may be acceptable to apply the same spectral density on all sites. However, care needs to be taken for the description of the exciton-vibrational coupling in the low frequency part of intramolecular modes because exciton dynamics is more susceptible to low frequency modes despite their small Huang-Rhys factors.

Dark excitons in transition metal dichalcogenides

Science.gov (United States)

Malic, Ermin; Selig, Malte; Feierabend, Maja; Brem, Samuel; Christiansen, Dominik; Wendler, Florian; Knorr, Andreas; Berghäuser, Gunnar

2018-01-01

Monolayer transition metal dichalcogenides (TMDs) exhibit a remarkably strong Coulomb interaction that manifests in tightly bound excitons. Due to the complex electronic band structure exhibiting several spin-split valleys in the conduction and valence band, dark excitonic states can be formed. They are inaccessibly by light due to the required spin-flip and/or momentum transfer. The relative position of these dark states with respect to the optically accessible bright excitons has a crucial impact on the emission efficiency of these materials and thus on their technological potential. Based on the solution of the Wannier equation, we present the excitonic landscape of the most studied TMD materials including the spectral position of momentum- and spin-forbidden excitonic states. We show that the knowledge of the electronic dispersion does not allow to conclude about the nature of the material's band gap since excitonic effects can give rise to significant changes. Furthermore, we reveal that an exponentially reduced photoluminescence yield does not necessarily reflect a transition from a direct to a nondirect gap material, but can be ascribed in most cases to a change of the relative spectral distance between bright and dark excitonic states.

Self-assembly as a design tool for the integration of photonic structures into excitonic solar cells

KAUST Repository

Guldin, S.

2011-09-20

One way to successfully enhance light harvesting of excitonic solar cells is the integration of optical elements that increase the photon path length in the light absorbing layer. Device architectures which incorporate structural order in form of one- or three-dimensional refractive index lattices can lead to the localization of light in specific parts of the spectrum, while retaining the cell\\'s transparency in others. Herein, we present two routes for the integration of photonic crystals (PCs) into dye-sensitized solar cells (DSCs). In both cases, the self-assembly of soft matter plays a key role in the fabrication process of the TiO2 electrode. One approach relies on a combination of colloidal self-assembly and the self-assembly of block copolymers, resulting in a double layer dye-sensitized solar cell with increased light absorption from the 3D PC element. An alternative route is based on the fact that the refractive index of the mesoporous layer can be finely tuned by the interplay between block copolymer self-assembly and hydrolytic TiO2 sol-gel chemistry. Alternating deposition of high and low refractive index layers enables the integration of a 1D PC into a DSC.

Harmonic Quantum Coherence of Multiple Excitons in PbS/CdS Core-Shell Nanocrystals

Science.gov (United States)

Tahara, Hirokazu; Sakamoto, Masanori; Teranishi, Toshiharu; Kanemitsu, Yoshihiko

2017-12-01

The generation and recombination dynamics of multiple excitons in nanocrystals (NCs) have attracted much attention from the viewpoints of fundamental physics and device applications. However, the quantum coherence of multiple exciton states in NCs still remains unclear due to a lack of experimental support. Here, we report the first observation of harmonic dipole oscillations in PbS/CdS core-shell NCs using a phase-locked interference detection method for transient absorption. From the ultrafast coherent dynamics and excitation-photon-fluence dependence of the oscillations, we found that multiple excitons cause the harmonic dipole oscillations with ω , 2 ω , and 3 ω oscillations, even though the excitation pulse energy is set to the exciton resonance frequency, ω . This observation is closely related to the quantum coherence of multiple exciton states in NCs, providing important insights into multiple exciton generation mechanisms.

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...

Hyperspectral Probing of Exciton dynamics and Multiplication in PbSe Nanocrystals

OpenAIRE

Bawendi M.G.; Strasfeld D.; Roitblat A.; Sachs H.; Gdor I.; Ruhman S.

2013-01-01

Height time hyperspectral near IR probing providing broad-band coverage is employed on PbSe nanocrystals, uncovering spectral evolution following high energy photo-excitation due to hot exciton relaxation and recombination. Separation of single, double and triple exciton state contributions to these spectra is demonstrated, and the mechanisms underlying the course of spectral evolution are investigated. In addition no sign of MEG was detected in this sample up to a photon energy 3.7 times tha...

Exciton fission in monolayer transition metal dichalcogenide semiconductors.

Science.gov (United States)

Steinhoff, A; Florian, M; Rösner, M; Schönhoff, G; Wehling, T O; Jahnke, F

2017-10-27

When electron-hole pairs are excited in a semiconductor, it is a priori not clear if they form a plasma of unbound fermionic particles or a gas of composite bosons called excitons. Usually, the exciton phase is associated with low temperatures. In atomically thin transition metal dichalcogenide semiconductors, excitons are particularly important even at room temperature due to strong Coulomb interaction and a large exciton density of states. Using state-of-the-art many-body theory, we show that the thermodynamic fission-fusion balance of excitons and electron-hole plasma can be efficiently tuned via the dielectric environment as well as charge carrier doping. We propose the observation of these effects by studying exciton satellites in photoemission and tunneling spectroscopy, which present direct solid-state counterparts of high-energy collider experiments on the induced fission of composite particles.

Room-Temperature Single-Photon Emission from Micrometer-Long Air-Suspended Carbon Nanotubes

Science.gov (United States)

Ishii, A.; Uda, T.; Kato, Y. K.

2017-11-01

Statistics of photons emitted by mobile excitons in individual carbon nanotubes are investigated. Photoluminescence spectroscopy is used to identify the chiralities and suspended lengths of air-suspended nanotubes, and photon-correlation measurements are performed at room temperature on telecommunication-wavelength nanotube emission with a Hanbury-Brown-Twiss setup. We obtain zero-delay second-order correlation g(2 )(0 ) less than 0.5, indicating single-photon generation. Excitation power dependence of the photon antibunching characteristics is examined for nanotubes with various chiralities and suspended lengths, where we find that the minimum value of g(2 )(0 ) is obtained at the lowest power. The influence of exciton diffusion and end quenching is studied by Monte Carlo simulations, and we derive an analytical expression for the minimum value of g(2 )(0 ). Our results indicate that mobile excitons in micrometer-long nanotubes can in principle produce high-purity single photons, leading to new design strategies for quantum photon sources.

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....

Hyperspectral Probing of Exciton dynamics and Multiplication in PbSe Nanocrystals

Science.gov (United States)

Gdor, I.; Sachs, H.; Roitblat, A.; Strasfeld, D.; Bawendi, M. G.; Ruhman, S.

2013-03-01

Height time hyperspectral near IR probing providing broad-band coverage is employed on PbSe nanocrystals, uncovering spectral evolution following high energy photo-excitation due to hot exciton relaxation and recombination. Separation of single, double and triple exciton state contributions to these spectra is demonstrated, and the mechanisms underlying the course of spectral evolution are investigated. In addition no sign of MEG was detected in this sample up to a photon energy 3.7 times that of the band gap.

Hyperspectral Probing of Exciton dynamics and Multiplication in PbSe Nanocrystals

Directory of Open Access Journals (Sweden)

Bawendi M.G.

2013-03-01

Full Text Available Height time hyperspectral near IR probing providing broad-band coverage is employed on PbSe nanocrystals, uncovering spectral evolution following high energy photo-excitation due to hot exciton relaxation and recombination. Separation of single, double and triple exciton state contributions to these spectra is demonstrated, and the mechanisms underlying the course of spectral evolution are investigated. In addition no sign of MEG was detected in this sample up to a photon energy 3.7 times that of the band gap.

Excitonic effects and related properties in semiconductor nanostructures: roles of size and dimensionality

Science.gov (United States)

Wu, Shudong; Cheng, Liwen; Wang, Qiang

2017-08-01

The size- and dimensionality-dependence of excitonic effects and related properties in semiconductor nanostructures are theoretically studied in detail within the effective-mass approximation. When nanostructure sizes become smaller than the bulk exciton Bohr radius, excitonic effects are significantly enhanced with reducing size or dimensionality. This is as a result of quantum confinement in more directions leading to larger exciton binding energies and normalized exciton oscillator strengths. These excitonic effects originate from electron-hole Coulombic interactions, which strongly enhance the oscillator strength between the electron and hole. It is also established that the universal scaling of exciton binding energy versus the inverse of the exciton Bohr radius follows a linear scaling law. Herein, we propose a stretched exponential law for the size scaling of optical gap, which is in good agreement with the calculated data. Due to differences in the confinement dimensionality, the radiative lifetime of low-dimensional excitons becomes shorter than that of bulk excitons. The size dependence of the exciton radiative lifetimes is in good agreement with available experimental data. This strongly enhanced electron-hole exchange interaction is expected in low-dimensional structures due to enriched excitonic effects. The main difference in nanostructures compared to the bulk can be interpreted in terms of the enhanced excitonic effects induced by exciton localization. The enhanced excitonic effects are expected to be of importance in developing stable and high-efficiency nanoscale excitonic optoelectronic devices.

Bistable Topological Insulator with Exciton-Polaritons

Science.gov (United States)

Kartashov, Yaroslav V.; Skryabin, Dmitry V.

2017-12-01

The functionality of many nonlinear and quantum optical devices relies on the effect of optical bistability. Using microcavity exciton-polaritons in a honeycomb arrangement of microcavity pillars, we report the resonance response and bistability of topological edge states. A balance between the pump, loss, and nonlinearity ensures a broad range of dynamical stability and controls the distribution of power between counterpropagating states on the opposite edges of the honeycomb lattice stripe. Tuning energy and polarization of the pump photons, while keeping their momentum constant, we demonstrate control of the propagation direction of the dominant edge state. Our results facilitate the development of practical applications of topological photonics.

Magneto-exciton transitions in laterally coupled quantum dots

Science.gov (United States)

Barticevic, Zdenka; Pacheco, Monica; Duque, Carlos A.; Oliveira, Luiz E.

2008-03-01

We present a study of the electronic and optical properties of laterally coupled quantum dots. The excitonic spectra of this system under the effects of an external magnetic field applied perpendicular to the plane of the dots is obtained, with the potential of every individual dot taken as the superposition of a quantum well potential along the axial direction with a lateral parabolic confinement potential, and the coupled two- dot system then modeled by a superposition of the potentials of each dot, with their minima at different positions and truncated at the intersection plane. The wave functions and eigenvalues are obtained in the effective-mass approximation by using an extended variational approach in which the magneto- exciton states are simultaneously obtained [1]. The allowed magneto-exciton transitions are investigated by using circularly polarized radiation in the plane perpendicular to the magnetic field. We present results on the excitonic absorption coefficient as a function of the photon energy for different geometric quantum-dot confinement and magnetic-field values. Reference: [1] Z. Barticevic, M. Pacheco, C. A. Duque and L. E. Oliveira, Phys. Rev. B 68, 073312 (2003).

Femtosecond dynamics of excitons in π-conjugated oligomers: the role of intrachain two-exciton states in the formation of interchain species

Science.gov (United States)

Klimov, Victor I.; McBranch, Duncan W.; Barashkov, Nikolay N.; Ferraris, John P.

1997-10-01

We report femtosecond transient absorption results for solutions and thin films of a substituted oligomer of poly(para-phenylene vinylene) performed over wide spectral and pump-intensity ranges. Solutions and films exhibit a photoinduced absorption (PA) band with dynamics matching those of the stimulated emission, demonstrating unambiguously that these features originate from intrachain singlet excitons. Thin films exhibit an additional short-wavelength PA band with pump-independent dynamics, indicating the formation of non-emissive interchain excitons. Correlations in the dynamics of the two PA features, as well as the intensity-dependence, provide strong evidence that the formation of interchain excitons is mediated by intrachain two-exciton states.

Theoretical treatment of the processes involving the dipole transitions to the lowest exciton states in hexagonal semiconductors

Science.gov (United States)

Semenova, L. E.

2018-04-01

The treatment of the two-photon transitions to the An=1 exciton level and the resonant Raman scattering of light by LO-phonons is given for the hexagonal semiconductors A2B6, taking into account the influence of the complex top valence band and anisotropy of the exciton effective mass.

Numerical modeling of exciton-polariton Bose-Einstein condensate in a microcavity

Science.gov (United States)

Voronych, Oksana; Buraczewski, Adam; Matuszewski, Michał; Stobińska, Magdalena

2017-06-01

A novel, optimized numerical method of modeling of an exciton-polariton superfluid in a semiconductor microcavity was proposed. Exciton-polaritons are spin-carrying quasiparticles formed from photons strongly coupled to excitons. They possess unique properties, interesting from the point of view of fundamental research as well as numerous potential applications. However, their numerical modeling is challenging due to the structure of nonlinear differential equations describing their evolution. In this paper, we propose to solve the equations with a modified Runge-Kutta method of 4th order, further optimized for efficient computations. The algorithms were implemented in form of C++ programs fitted for parallel environments and utilizing vector instructions. The programs form the EPCGP suite which has been used for theoretical investigation of exciton-polaritons. Catalogue identifier: AFBQ_v1_0 Program summary URL:http://cpc.cs.qub.ac.uk/summaries/AFBQ_v1_0.html Program obtainable from: CPC Program Library, Queen's University, Belfast, N. Ireland Licensing provisions: BSD-3 No. of lines in distributed program, including test data, etc.: 2157 No. of bytes in distributed program, including test data, etc.: 498994 Distribution format: tar.gz Programming language: C++ with OpenMP extensions (main numerical program), Python (helper scripts). Computer: Modern PC (tested on AMD and Intel processors), HP BL2x220. Operating system: Unix/Linux and Windows. Has the code been vectorized or parallelized?: Yes (OpenMP) RAM: 200 MB for single run Classification: 7, 7.7. Nature of problem: An exciton-polariton superfluid is a novel, interesting physical system allowing investigation of high temperature Bose-Einstein condensation of exciton-polaritons-quasiparticles carrying spin. They have brought a lot of attention due to their unique properties and potential applications in polariton-based optoelectronic integrated circuits. This is an out-of-equilibrium quantum system confined

Theoretical and computational studies of excitons in conjugated polymers

Science.gov (United States)

Barford, William; Bursill, Robert J.; Smith, Richard W.

2002-09-01

We present a theoretical and computational analysis of excitons in conjugated polymers. We use a tight-binding model of π-conjugated electrons, with 1/r interactions for large r. In both the weak-coupling limit (defined by W>>U) and the strong-coupling limit (defined by Wparticle models. We compare these to density matrix renormalization group (DMRG) calculations, and find good agreement in the extreme limits. We use these analytical results to interpret the DMRG calculations in the intermediate-coupling regime (defined by W~U), most applicable to conjugated polymers. We make the following conclusions. (1) In the weak-coupling limit the bound states are Mott-Wannier excitons, i.e., conduction-band electrons bound to valence-band holes. Singlet and triplet excitons whose relative wave functions are odd under a reflection of the relative coordinate are degenerate. Thus, the 2 1A+g and 1 3A-g states are degenerate in this limit. (2) In the strong-coupling limit the bound states are Mott-Hubbard excitons, i.e., particles in the upper Hubbard band bound to holes in the lower Hubbard band. These bound states occur in doublets of even and odd parity excitons. Triplet excitons are magnons bound to the singlet excitons, and hence are degenerate with their singlet counterparts. (3) In the intermediate-coupling regime Mott-Wannier excitons are the more appropriate description for large dimerization, while for the undimerized chain Mott-Hubbard excitons are the correct description. For dimerizations relevant to polyacetylene and polydiacetylene both Mott-Hubbard and Mott-Wannier excitons are present. (4) For all coupling strengths an infinite number of bound states exist for 1/r interactions for an infinite polymer. As a result of the discreteness of the lattice and the restrictions on the exciton wave functions in one dimension, the progression of states does not follow the Rydberg series. In practice, excitons whose particle-hole separation exceeds the length of the polymer

Higher-order amplitude squeezing of photons propagating through a semiconductor

International Nuclear Information System (INIS)

Nguyen Ba An.

1996-12-01

Photon amplitude K th power squeezing is studied when the coherent photon propagates through a semiconductor containing the exciton. If the exciton is prepared initially in a coherent state, the photon may become amplitude K th power squeezed. It is shown that, in the short-time limit, the photon squeezing in the P direction does not appear at all while that in the X direction is possible for all the amplitude power K. In the latter case, the amount of squeezing is larger for higher power K. Dependences on all the system parameters as well as on the output light detection moment are investigated in detail. (author). 14 refs, 8 figs

New method for control over exciton states in quantum wells

International Nuclear Information System (INIS)

Maslov, A Yu; Proshina, O V

2010-01-01

The theoretical study of the exciton states in the quantum well is performed with regard to the distinctions of the dielectric properties of quantum well and barrier materials. The strong exciton-phonon interaction is shown to be possible in materials with high ionicity. This leads to the essential modification of the exciton states. The relationship between the exciton binding energy, along with oscillator strength and the barrier material dielectric properties is found. This suggests the feasibility of the exciton spectrum parameter control by the choice of the barrier material. It is shown that such exciton spectrum engineering also is possible in the quantum wells based on the materials with low ionicity. The reason is the dielectric confinement effect in the quantum wells.

A study of polaritonic transparency in couplers made from excitonic materials

Energy Technology Data Exchange (ETDEWEB)

Singh, Mahi R.; Racknor, Chris [Department of Physics and Astronomy, Western University, London, Ontario N6A 3K7 (Canada)

2015-03-14

We have studied light matter interaction in quantum dot and exciton-polaritonic coupler hybrid systems. The coupler is made by embedding two slabs of an excitonic material (CdS) into a host excitonic material (ZnO). An ensemble of non-interacting quantum dots is doped in the coupler. The bound exciton polariton states are calculated in the coupler using the transfer matrix method in the presence of the coupling between the external light (photons) and excitons. These bound exciton-polaritons interact with the excitons present in the quantum dots and the coupler is acting as a reservoir. The Schrödinger equation method has been used to calculate the absorption coefficient in quantum dots. It is found that when the distance between two slabs (CdS) is greater than decay length of evanescent waves the absorption spectrum has two peaks and one minimum. The minimum corresponds to a transparent state in the system. However, when the distance between the slabs is smaller than the decay length of evanescent waves, the absorption spectra has three peaks and two transparent states. In other words, one transparent state can be switched to two transparent states when the distance between the two layers is modified. This could be achieved by applying stress and strain fields. It is also found that transparent states can be switched on and off by applying an external control laser field.

Mixed fermion-photon condensate in strongly coupled quantum electrodynamics

International Nuclear Information System (INIS)

Gusynin, V.P.; Kushnir, V.A.

1989-01-01

The existence of a new mixed fermion-photon condensate breaking chiral symmetry in strongly coupled phase of quantum electrodynamics is shown. An analytical expression for the renormalized condensate is obtained. 20 refs.; 2 figs

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.

Light exiting from real photonic band gap crystals is diffuse and strongly directional

NARCIS (Netherlands)

Koenderink, A.F.; Vos, Willem L.

2003-01-01

Any photonic crystal is in practice periodic with some inevitable fabricational imperfections. We have measured angle-resolved transmission of photons that are multiply scattered by this disorder in strongly photonic crystals. Peculiar non-Lambertian distributions occur as a function of frequency:

Observation of squeezed states with strong photon-number oscillations

International Nuclear Information System (INIS)

Mehmet, Moritz; Vahlbruch, Henning; Lastzka, Nico; Danzmann, Karsten; Schnabel, Roman

2010-01-01

Squeezed states of light constitute an important nonclassical resource in the field of high-precision measurements, for example, gravitational wave detection, as well as in the field of quantum information, for example, for teleportation, quantum cryptography, and distribution of entanglement in quantum computation networks. Strong squeezing in combination with high purity, high bandwidth, and high spatial mode quality is desirable in order to achieve significantly improved performances contrasting any classical protocols. Here we report on the observation of 11.5 dB of squeezing, together with relatively high state purity corresponding to a vacuum contribution of less than 5%, and a squeezing bandwidth of about 170 MHz. The analysis of our squeezed states reveals a significant production of higher-order pairs of quantum-correlated photons and the existence of strong photon-number oscillations.

How exciton-vibrational coherences control charge separation in the photosystem II reaction center.

Science.gov (United States)

Novoderezhkin, Vladimir I; Romero, Elisabet; van Grondelle, Rienk

2015-12-14

In photosynthesis absorbed sun light produces collective excitations (excitons) that form a coherent superposition of electronic and vibrational states of the individual pigments. Two-dimensional (2D) electronic spectroscopy allows a visualization of how these coherences are involved in the primary processes of energy and charge transfer. Based on quantitative modeling we identify the exciton-vibrational coherences observed in 2D photon echo of the photosystem II reaction center (PSII-RC). We find that the vibrations resonant with the exciton splittings can modify the delocalization of the exciton states and produce additional states, thus promoting directed energy transfer and allowing a switch between the two charge separation pathways. We conclude that the coincidence of the frequencies of the most intense vibrations with the splittings within the manifold of exciton and charge-transfer states in the PSII-RC is not occurring by chance, but reflects a fundamental principle of how energy conversion in photosynthesis was optimized.

Surface Plasmon Polariton-Assisted Long-Range Exciton Transport in Monolayer Semiconductor Lateral Heterostructure

Science.gov (United States)

Shi, Jinwei; Lin, Meng-Hsien; Chen, Yi-Tong; Estakhri, Nasim Mohammadi; Tseng, Guo-Wei; Wang, Yanrong; Chen, Hung-Ying; Chen, Chun-An; Shih, Chih-Kang; Alã¹, Andrea; Li, Xiaoqin; Lee, Yi-Hsien; Gwo, Shangjr

Recently, two-dimensional (2D) semiconductor heterostructures, i.e., atomically thin lateral heterostructures (LHSs) based on transition metal dichalcogenides (TMDs) have been demonstrated. In an optically excited LHS, exciton transport is typically limited to a rather short spatial range ( 1 micron). Furthermore, additional losses may occur at the lateral interfacial regions. Here, to overcome these challenges, we experimentally implement a planar metal-oxide-semiconductor (MOS) structure by placing a monolayer of WS2/MoS2 LHS on top of an Al2O3 capped Ag single-crystalline plate. We found that the exciton transport range can be extended to tens of microns. The process of long-range exciton transport in the MOS structure is confirmed to be mediated by an exciton-surface plasmon polariton-exciton conversion mechanism, which allows a cascaded energy transfer process. Thus, the planar MOS structure provides a platform seamlessly combining 2D light-emitting materials with plasmonic planar waveguides, offering great potential for developing integrated photonic/plasmonic functionalities.

Fine structure of the exciton electroabsorption in semiconductor superlattices

Energy Technology Data Exchange (ETDEWEB)

Monozon, B.S., E-mail: borismonozon@mail.ru [Physics Department, Marine Technical University, 3 Lotsmanskaya Str., 190008 St.Petersburg (Russian Federation); Schmelcher, P. [Zentrum für Optische Quantentechnologien, The Hamburg Centre for Ultrafast Imaging, Universität Hamburg, Luruper Chaussee 149, 22761 Hamburg (Germany)

2017-02-15

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.

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

Nonlinearity of the refractive index due to an excitonic molecule resonance state in CdS

International Nuclear Information System (INIS)

Baumert, R.; Broser, I.; Buschick, K.

1986-01-01

The authors report the observation of an intensity-dependent refractive-index nonlinearity in CdS due to a resonance state where an excitonic molecule is created by induced absorption of light. The refractive index n as a function of the incident laser photon energy E is measured directly by light refraction in thin crystal prisms. A renormalized dielectric function describes the measured n(E) spectra well. This strong refractive-index nonlinearity is well suited to produce an optical bistability and to further strengthen the evidence of CdS to be an important material for laser-induced dynamic gratings

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 two......-dimensional (2D) excitons is still lacking. Here we provide a critical assessment of a widely used 2D hydrogenic exciton model, which assumes a dielectric function of the form epsilon(q) = 1 + 2 pi alpha q, and we develop a quasi-2D model with a much broader applicability. Within the quasi-2D picture, electrons...... exciton binding energies in both isolated and supported 2D materials. For isolated 2D materials, the quasi-2D treatment yields results almost identical to those of the strict 2D model, and both are in good agreement with ab initio many-body calculations. On the other hand, for more complex structures...

Exciton management in organic photovoltaic multidonor energy cascades.

Science.gov (United States)

Griffith, Olga L; Forrest, Stephen R

2014-05-14

Multilayer donor regions in organic photovoltaics show improved power conversion efficiency when arranged in decreasing exciton energy order from the anode to the acceptor interface. These so-called "energy cascades" drive exciton transfer from the anode to the dissociating interface while reducing exciton quenching and allowing improved overlap with the solar spectrum. Here we investigate the relative importance of exciton transfer and blocking in a donor cascade employing diphenyltetracene (D1), rubrene (D2), and tetraphenyldibenzoperiflanthene (D3) whose optical gaps monotonically decrease from D1 to D3. In this structure, D1 blocks excitons from quenching at the anode, D2 accepts transfer of excitons from D1 and blocks excitons at the interface between D2 and D3, and D3 contributes the most to the photocurrent due to its strong absorption at visible wavelengths, while also determining the open circuit voltage. We observe singlet exciton Förster transfer from D1 to D2 to D3 consistent with cascade operation. The power conversion efficiency of the optimized cascade OPV with a C60 acceptor layer is 7.1 ± 0.4%, which is significantly higher than bilayer devices made with only the individual donors. We develop a quantitative model to identify the dominant exciton processes that govern the photocurrent generation in multilayer organic structures.

The confinement effect in spherical inhomogeneous quantum dots and stability of excitons

Directory of Open Access Journals (Sweden)

F. Benhaddou

2017-06-01

Full Text Available We investigate in this work the quantum confinement effect of exciton in spherical inhomogeneous quantum dots IQDs. The spherical core is enveloped by two shells. The inner shell is a semiconductor characterized by a small band-gap. The core and the outer shell are the same semiconductor characterized by a large band-gap. So there is a significant gap-offset creating a deep potential well where the excitons are localized and strongly confined. We have adopted the Ritz variational method to calculate numerically the excitonic ground state energy and its binding energy in the strong, moderate and low confinement regimes. The results show that the Ritz variational method is in good agreement with the perturbation method in strong confinement. There is a double confinement effect and dual control. The calculation checks the effective Rydberg R* at the asymptotic limit of bulk semiconductor when the thickness takes very large values. The excitonic binding energy increases, Thus giving the excitons a high stability even at ambient temperature. These nanosystems are promising in several applications: lighting, detection, biological labeling and quantum computing.

Organic-Inorganic Composites of Semiconductor Nanocrystals for Efficient Excitonics.

Science.gov (United States)

Guzelturk, Burak; Demir, Hilmi Volkan

2015-06-18

Nanocomposites of colloidal semiconductor nanocrystals integrated into conjugated polymers are the key to soft-material hybrid optoelectronics, combining advantages of both plastics and particles. Synergic combination of the favorable properties in the hybrids of colloidal nanocrystals and conjugated polymers offers enhanced performance and new functionalities in light-generation and light-harvesting applications, where controlling and mastering the excitonic interactions at the nanoscale are essential. In this Perspective, we highlight and critically consider the excitonic interactions in the organic-inorganic nanocomposites to achieve highly efficient exciton transfer through rational design of the nanocomposites. The use of strong excitonic interactions in optoelectronic devices can trigger efficiency breakthroughs in hybrid optoelectronics.

Strong Exciton-photon Coupling in Semiconductor Microcavities

DEFF Research Database (Denmark)

Jensen, Jacob Riis; Borri, Paola; Hvam, Jørn Märcher

1999-01-01

The basic building block of vertical cavity surface emitting lasers (VCSELs) and high efficiency diodes, is a quantum well embedded in a semiconductor microcavity. The high finesse that may be achieved in such a cavity is utilised to get a low threshold current in the VCSELs and a high directiona......The basic building block of vertical cavity surface emitting lasers (VCSELs) and high efficiency diodes, is a quantum well embedded in a semiconductor microcavity. The high finesse that may be achieved in such a cavity is utilised to get a low threshold current in the VCSELs and a high......-optical switches based on semiconductor microcavities....

On the equivalence of two approaches in the exciton-polariton theory

International Nuclear Information System (INIS)

Ha Vinh Tan; Nguyen Toan Thang

1983-02-01

The polariton effect in the optical processes involving photons with energies near that of an exciton is investigated by the Bogolubov diagonalization and the Green function approaches in a simple model of the direct band gap semiconductor with the electrical dipole allowed transition. To take into account the non-resonant terms of the interaction Hamiltonian of the photon-exciton system the Green function approach derived by Nguyen Van Hieu is presented with the use of Green's function matrix technique analogous to that suggested by Nambu in the theory of superconductivity. It is shown that with the suitable choice of the phase factors the renormalization constants are equal to the diagonalization coefficients. The disperson of polaritons and the matrix elements of processes with the participation of polaritons are identically calculated by both methods. However the Green function approach has an advantage in including the damping effect of polaritons. (author)

Two-photon excitation spectroscopy of carotenoid-containing and carotenoid-depleted LH2 complexes from purple bacteria.

Science.gov (United States)

Stepanenko, Ilya; Kompanetz, Viktor; Makhneva, Zoya; Chekalin, Sergey; Moskalenko, Andrei; Razjivin, Andrei

2009-08-27

We applied two-photon fluorescence excitation spectroscopy to LH2 complex from purple bacteria Allochromatium minutissimum and Rhodobacter sphaeroides . Bacteriochlorophyll fluorescence was measured under two-photon excitation of the samples within the 1200-1500 nm region. Spectra were obtained for both carotenoid-containing and -depleted complexes of each bacterium to allow their direct comparison. The depletion of carotenoids did not alter the two-photon excitation spectra of either bacteria. The spectra featured a wide excitation band around 1350 nm (2x675 nm, 14,800 cm(-1)) which strongly resembled two-photon fluorescence excitation spectra of similar complexes published by other authors. We consider obtained experimental data to be evidence of direct two-photon excitation of bacteriochlorophyll excitonic states in this spectral region.

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.

Coherent quantum dynamics of excitons in monolayer transition metal dichalcogenides

KAUST Repository

Moody, Galan; Hao, Kai; Dass, Chandriker Kavir; Singh, Akshay; Xu, Lixiang; Tran, Kha; Chen, Chang-Hsiao; Li, Ming-yang; Li, Lain-Jong; Clark, Genevieve; Bergh ä user, Gunnar; Malic, Ermin; Knorr, Andreas; Xu, Xiaodong; Li, Xiaoqin

2016-01-01

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.

Excitons in insulators

International Nuclear Information System (INIS)

Grasser, R.; Scharmann, A.

1983-01-01

This chapter investigates absorption, reflectivity, and intrinsic luminescence spectra of free and/or self-trapped (localized) excitons in alkali halides and rare gas solids. Introduces the concepts underlying the Wannier-Mott and Frenkel exciton models, two extreme pictures of an exciton in crystalline materials. Discusses the theoretical and experimental background; excitons in alkali halides; and excitons in rare gas solids. Shows that the intrinsic optical behavior of wide gap insulators in the range of the fundamental absorption edge is controlled by modified Wannier-Mott excitons. Finds that while that alkali halides only show free and relaxed molecular-like exciton emission, in rare gas crystals luminescence due to free, single and double centered localized excitons is observed. Indicates that the simultaneous existence of free and self-trapped excitons in these solid requires an energy barrier for self-trapping

Strongly correlated photons generated by coupling a three- or four-level system to a waveguide

Science.gov (United States)

Zheng, Huaixiu; Gauthier, Daniel J.; Baranger, Harold U.

2012-04-01

We study the generation of strongly correlated photons by coupling an atom to photonic quantum fields in a one-dimensional waveguide. Specifically, we consider a three-level or four-level system for the atom. Photon-photon bound states emerge as a manifestation of the strong photon-photon correlation mediated by the atom. Effective repulsive or attractive interaction between photons can be produced, causing either suppressed multiphoton transmission (photon blockade) or enhanced multiphoton transmission (photon-induced tunneling). As a result, nonclassical light sources can be generated on demand by sending coherent states into the proposed system. We calculate the second-order correlation function of the transmitted field and observe bunching and antibunching caused by the bound states. Furthermore, we demonstrate that the proposed system can produce photon pairs with a high degree of spectral entanglement, which have a large capacity for carrying information and are important for large-alphabet quantum communication.

Nonlinear properties of gated graphene in a strong electromagnetic field

Energy Technology Data Exchange (ETDEWEB)

Avetisyan, A. A., E-mail: artakav@ysu.am; Djotyan, A. P., E-mail: adjotyan@ysu.am [Yerevan State University, Department of Physics (Armenia); Moulopoulos, K., E-mail: cos@ucy.ac.cy [University of Cyprus, Department of Physics (Cyprus)

2017-03-15

We develop a microscopic theory of a strong electromagnetic field interaction with gated bilayer graphene. Quantum kinetic equations for density matrix are obtained using a tight binding approach within second quantized Hamiltonian in an intense laser field. We show that adiabatically changing the gate potentials with time may produce (at resonant photon energy) a full inversion of the electron population with high density between valence and conduction bands. In the linear regime, excitonic absorption of an electromagnetic radiation in a graphene monolayer with opened energy gap is also studied.

Polariton condensation with localized excitons and propagating photons

International Nuclear Information System (INIS)

Keeling, Jonathan; Eastham, P.R.; Szymanska, M.H.; Littlewood, P.B.

2004-01-01

We estimate the condensation temperature for microcavity polaritons, allowing for their internal structure. We consider polaritons formed from localized excitons in a planar microcavity, using a generalized Dicke model. At low densities, we find a condensation temperature T c ∝ρ, as expected for a gas of structureless polaritons. However, as T c becomes of the order of the Rabi splitting, the structure of the polaritons becomes relevant, and the condensation temperature is that of a BCS-like mean-field theory. We also calculate the excitation spectrum, which is related to observable quantities such as the luminescence and absorption spectra

Triplet energy transfer and triplet exciton recycling in singlet fission sensitized organic heterojunctions

Science.gov (United States)

Hamid, Tasnuva; Yambem, Soniya D.; Crawford, Ross; Roberts, Jonathan; Pandey, Ajay K.

2017-08-01

Singlet exciton fission is a process where an excited singlet state splits into two triplets, thus leading to generation of multiple excitons per absorbed photon in organic semiconductors. Herein, we report a detailed exciton management approach for multiexciton harvesting over a broadband region of the solar spectrum in singlet fission sensitized organic photodiodes. Through systematic studies on the model cascade of pentacene/rubrene/C60, we found that efficient photocurrent generation from pentacene can still occur despite the presence of a >10nm thick interlayer of rubrene in between the pentacene/C60 heterojunction. Our results show that thin rubrene interlayers of thickness pentacene despite having a reasonably thick rubrene interlayer, that too with higher triplet energy (T1=1.12 eV) than pentacene (T1= 0.86 eV), makes its operation a rather interesting result. We discuss the role of rubrene interlayer film discontinuity, triplet exciton reflection from rubrene interlayer and triplet energy transfer from rubrene to pentacene layer followed by diffusion of triplet excitons through rubrene as plausible mechanisms that would enable triplet excitons from pentacene to generate significant photocurrent in a multilayer organic heterojunction.

Excitonic condensation of strongly correlated electrons: the case of Pr.sub.0.5./sub. Ca.sub.0.5./sub. CoO.sub.3./sub..

Czech Academy of Sciences Publication Activity Database

Kuneš, Jan; Augustinský, Pavel

2014-01-01

Roč. 90, č. 23 (2014), "235112-1"-"235112-5" ISSN 1098-0121 R&D Projects: GA ČR GA13-25251S Institutional support: RVO:68378271 Keywords : excitonic condensation * strongly correlated electrons * cobaltites Subject RIV: BM - Solid Matter Physics ; Magnetism Impact factor: 3.736, year: 2014

Nonlinear spectroscopy of the bound exciton states in CdSe single crystals

International Nuclear Information System (INIS)

Lisitsa, M.P.; Onishchenko, N.A.; Stolyarenko, A.V.; Ananchenko, V.V.; Polishchuk, S.V.

1989-01-01

The study is devoted to the pulsed laser radiation effect on the time-resolved variations of free and bound exciton bands region at the helium temperature. A gradual disappearance of the bound I 2 exciton state is observed with increase of the excitation intensity I in CdSe transmission spectra. This phenomenon is explained by the fact that despite of the shorter life of I 2 excitons as compared to the free ones, the concentration of the centres on which they localize is rather low (≤10 16 cm -3 ) while the evolution of the light-generated electron-hole pairs is such as the most probable recombination through the bound excitons. The transmission spectrum kinetics is studied. The intensity limitation of the laser pulse transmitted through the crystal in the region of the exciton ground state region is shown to be related with two-photon absorption (TPA) in which the exciton state is an intermediate level. The calculation results are in good agreement with the experiment. The estimations show the giant TPA coefficient of ∼10 3 cm/MW. The evolution of photoexcited nonequilibrium electron-hole pairs is studied. The possibility of using CdSe single crystals as spectrum-selective limiters of the laser pulses is shown. (author)

Exciton shelves for charge and energy transport in third-generation quantum-dot devices

Science.gov (United States)

Goodman, Samuel; Singh, Vivek; Noh, Hyunwoo; Casamada, Josep; Chatterjee, Anushree; Cha, Jennifer; Nagpal, Prashant

2014-03-01

Quantum dots are semiconductor nanocrystallites with size-dependent quantum-confined energy levels. While they have been intensively investigated to utilize hot-carriers for photovoltaic applications, to bridge the mismatch between incident solar photons and finite bandgap of semiconductor photocells, efficient charge or exciton transport in quantum-dot films has proven challenging. Here we show development of new coupled conjugated molecular wires with ``exciton shelves'', or different energy levels, matched with the multiple energy levels of quantum dots. Using single nanoparticle and ensemble device measurements we show successful extraction and transport of both bandedge and high-energy charge carriers, and energy transport of excitons. We demonstrate using measurements of electronic density of states, that careful matching of energy states of quantum-dot with molecular wires is important, and any mismatch can generate midgap states leading to charge recombination and reduced efficiency. Therefore, these exciton-shelves and quantum dots can lead to development of next-generation photovoltaic and photodetection devices using simultaneous transport of bandedge and hot-carriers or energy transport of excitons in these nanostructured solution-processed films.

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...

Engineering light emission of two-dimensional materials in both the weak and strong coupling regimes

Science.gov (United States)

Brotons-Gisbert, Mauro; Martínez-Pastor, Juan P.; Ballesteros, Guillem C.; Gerardot, Brian D.; Sánchez-Royo, Juan F.

2018-01-01

Two-dimensional (2D) materials have promising applications in optoelectronics, photonics, and quantum technologies. However, their intrinsically low light absorption limits their performance, and potential devices must be accurately engineered for optimal operation. Here, we apply a transfer matrix-based source-term method to optimize light absorption and emission in 2D materials and related devices in weak and strong coupling regimes. The implemented analytical model accurately accounts for experimental results reported for representative 2D materials such as graphene and MoS2. The model has been extended to propose structures to optimize light emission by exciton recombination in MoS2 single layers, light extraction from arbitrarily oriented dipole monolayers, and single-photon emission in 2D materials. Also, it has been successfully applied to retrieve exciton-cavity interaction parameters from MoS2 microcavity experiments. The present model appears as a powerful and versatile tool for the design of new optoelectronic devices based on 2D semiconductors such as quantum light sources and polariton lasers.

Excitons in InP/InAs inhomogeneous quantum dots

International Nuclear Information System (INIS)

Assaid, E; Feddi, E; Khamkhami, J El; Dujardin, F

2003-01-01

Wannier excitons confined in an InP/InAs inhomogeneous quantum dot (IQD) have been studied theoretically in the framework of the effective mass approximation. A finite-depth potential well has been used to describe the effect of the quantum confinement in the InAs layer. The exciton binding energy has been determined using the Ritz variational method. The spatial correlation between the electron and the hole has been taken into account in the expression for the wavefunction. It has been shown that for a fixed size b of the IQD, the exciton binding energy depends strongly on the core radius a. Moreover, it became apparent that there are two critical values of the core radius, a crit and a 2D , for which important changes of the exciton binding occur. The former critical value, a crit , corresponds to a minimum of the exciton binding energy and may be used to distinguish between tridimensional confinement and bidimensional confinement. The latter critical value, a 2D , corresponds to a maximum of the exciton binding energy and to the most pronounced bidimensional character of the exciton

Fluctuating exciton localization in giant π-conjugated spoked-wheel macrocycles

Science.gov (United States)

Aggarwal, A. Vikas; Thiessen, Alexander; Idelson, Alissa; Kalle, Daniel; Würsch, Dominik; Stangl, Thomas; Steiner, Florian; Jester, Stefan-S.; Vogelsang, Jan; Höger, Sigurd; Lupton, John M.

2013-11-01

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 immediately obvious. For example, where is the exciton formed within a conjugated segment and is it always situated on the same repeat units? Here, we introduce structurally rigid molecular spoked wheels, 6 nm in diameter, as a model of extended π conjugation. Single-molecule fluorescence reveals random exciton localization, which leads to temporally varying emission polarization. Initially, this random localization arises after every photon absorption event because of temperature-independent spontaneous symmetry breaking. These fast fluctuations are slowed to millisecond timescales after prolonged illumination. Intramolecular heterogeneity is revealed in cryogenic spectroscopy by jumps in transition energy, but emission polarization can also switch without a spectral jump occurring, which implies long-range homogeneity in the local dielectric environment.

Energy dissipation of free exciton polaritons in semiconducting films

International Nuclear Information System (INIS)

De Crescenzi, M.; Harbeke, G.; Tosatti, E.

1978-08-01

The effective (thickness-dependent) light absorption coefficient K(ω,d) is discussed for thin semiconducting films in the frequency range of free, spatially dispersive exciton polaritons. We find that (i) it oscillates strongly for small film thicknesses; (ii) it exhibits a slanted peak lineshape; (iii) its integrated strength also depends upon the exciton damping and extrapolates to zero for vanishing damping

Enhanced Exciton and Photon Confinement in Ruddlesden-Popper Perovskite Microplatelets for Highly Stable Low-Threshold Polarized Lasing.

Science.gov (United States)

Li, Mingjie; Wei, Qi; Muduli, Subas Kumar; Yantara, Natalia; Xu, Qiang; Mathews, Nripan; Mhaisalkar, Subodh G; Xing, Guichuan; Sum, Tze Chien

2018-06-01

At the heart of electrically driven semiconductors lasers lies their gain medium that typically comprises epitaxially grown double heterostuctures or multiple quantum wells. The simultaneous spatial confinement of charge carriers and photons afforded by the smaller bandgaps and higher refractive index of the active layers as compared to the cladding layers in these structures is essential for the optical-gain enhancement favorable for device operation. Emulating these inorganic gain media, superb properties of highly stable low-threshold (as low as ≈8 µJ cm -2 ) linearly polarized lasing from solution-processed Ruddlesden-Popper (RP) perovskite microplatelets are realized. Detailed investigations using microarea transient spectroscopies together with finite-difference time-domain simulations validate that the mixed lower-dimensional RP perovskites (functioning as cladding layers) within the microplatelets provide both enhanced exciton and photon confinement for the higher-dimensional RP perovskites (functioning as the active gain media). Furthermore, structure-lasing-threshold relationship (i.e., correlating the content of lower-dimensional RP perovskites in a single microplatelet) vital for design and performance optimization is established. Dual-wavelength lasing from these quasi-2D RP perovskite microplatelets can also be achieved. These unique properties distinguish RP perovskite microplatelets as a new family of self-assembled multilayer planar waveguide gain media favorable for developing efficient lasers. © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Colloquium: Excitons in atomically thin transition metal dichalcogenides

Science.gov (United States)

Wang, Gang; Chernikov, Alexey; Glazov, Mikhail M.; Heinz, Tony F.; Marie, Xavier; Amand, Thierry; Urbaszek, Bernhard

2018-04-01

Atomically thin materials such as graphene and monolayer transition metal dichalcogenides (TMDs) exhibit remarkable physical properties resulting from their reduced dimensionality and crystal symmetry. The family of semiconducting transition metal dichalcogenides is an especially promising platform for fundamental studies of two-dimensional (2D) systems, with potential applications in optoelectronics and valleytronics due to their direct band gap in the monolayer limit and highly efficient light-matter coupling. A crystal lattice with broken inversion symmetry combined with strong spin-orbit interactions leads to a unique combination of the spin and valley degrees of freedom. In addition, the 2D character of the monolayers and weak dielectric screening from the environment yield a significant enhancement of the Coulomb interaction. The resulting formation of bound electron-hole pairs, or excitons, dominates the optical and spin properties of the material. Here recent progress in understanding of the excitonic properties in monolayer TMDs is reviewed and future challenges are laid out. Discussed are the consequences of the strong direct and exchange Coulomb interaction, exciton light-matter coupling, and influence of finite carrier and electron-hole pair densities on the exciton properties in TMDs. Finally, the impact on valley polarization is described and the tuning of the energies and polarization observed in applied electric and magnetic fields is summarized.

Spectral properties of excitons in the bilayer graphene

Science.gov (United States)

Apinyan, V.; Kopeć, T. K.

2018-01-01

In this paper, we consider the spectral properties of the bilayer graphene with the local excitonic pairing interaction between the electrons and holes. We consider the generalized Hubbard model, which includes both intralayer and interlayer Coulomb interaction parameters. The solution of the excitonic gap parameter is used to calculate the electronic band structure, single-particle spectral functions, the hybridization gap, and the excitonic coherence length in the bilayer graphene. We show that the local interlayer Coulomb interaction is responsible for the semimetal-semiconductor transition in the double layer system, and we calculate the hybridization gap in the band structure above the critical interaction value. The formation of the excitonic band gap is reported as the threshold process and the momentum distribution functions have been calculated numerically. We show that in the weak coupling limit the system is governed by the Bardeen-Cooper-Schrieffer (BCS)-like pairing state. Contrary, in the strong coupling limit the excitonic condensate states appear in the semiconducting phase, by forming the Dirac's pockets in the reciprocal space.

Interplay of Phonon and Exciton-Mediated Superconductivity in Hybrid Semiconductor-Superconductor Structures

Science.gov (United States)

Skopelitis, Petros; Cherotchenko, Evgenia D.; Kavokin, Alexey V.; Posazhennikova, Anna

2018-03-01

We predict a strong enhancement of the critical temperature in a conventional Bardeen-Cooper-Schrieffer (BCS) superconductor in the presence of a bosonic condensate of exciton polaritons. The effect depends strongly on the ratio of the cutoff frequencies for phonon and exciton-polariton mediated BCS superconductivity, respectively. We also discuss a possible design of hybrid semiconductor-superconductor structures suitable for the experimental observation of such an effect.

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...

Programmed coherent coupling in a synthetic DNA-based excitonic circuit

Science.gov (United States)

Boulais, Étienne; Sawaya, Nicolas P. D.; Veneziano, Rémi; Andreoni, Alessio; Banal, James L.; Kondo, Toru; Mandal, Sarthak; Lin, Su; Schlau-Cohen, Gabriela S.; Woodbury, Neal W.; Yan, Hao; Aspuru-Guzik, Alán; Bathe, Mark

2018-02-01

Natural light-harvesting systems spatially organize densely packed chromophore aggregates using rigid protein scaffolds to achieve highly efficient, directed energy transfer. Here, we report a synthetic strategy using rigid DNA scaffolds to similarly program the spatial organization of densely packed, discrete clusters of cyanine dye aggregates with tunable absorption spectra and strongly coupled exciton dynamics present in natural light-harvesting systems. We first characterize the range of dye-aggregate sizes that can be templated spatially by A-tracts of B-form DNA while retaining coherent energy transfer. We then use structure-based modelling and quantum dynamics to guide the rational design of higher-order synthetic circuits consisting of multiple discrete dye aggregates within a DX-tile. These programmed circuits exhibit excitonic transport properties with prominent circular dichroism, superradiance, and fast delocalized exciton transfer, consistent with our quantum dynamics predictions. This bottom-up strategy offers a versatile approach to the rational design of strongly coupled excitonic circuits using spatially organized dye aggregates for use in coherent nanoscale energy transport, artificial light-harvesting, and nanophotonics.

Coherent detection of THz-induced sideband emission from excitons in the nonperturbative regime

Science.gov (United States)

Uchida, K.; Otobe, T.; Mochizuki, T.; Kim, C.; Yoshita, M.; Tanaka, K.; Akiyama, H.; Pfeiffer, L. N.; West, K. W.; Hirori, H.

2018-04-01

Strong interaction of a terahertz (THz) wave with excitons induces nonperturbative optical effects such as Rabi splitting and high-order sideband generation. Here, we investigated coherent properties of THz-induced sideband emissions from GaAs/AlGaAs multiquantum wells. With increasing THz electric field, optical susceptibility of the THz-dressed exciton shows a redshift with spectral broadening and extraordinary phase shift. This implies that the field ionization of the 1 s exciton modifies the THz-dressed exciton in the nonperturbative regime.

Strong coupling and polariton lasing in Te based microcavities embedding (Cd,Zn)Te quantum wells

Energy Technology Data Exchange (ETDEWEB)

Rousset, J.-G., E-mail: j-g.rousset@fuw.edu.pl; Piętka, B.; Król, M.; Mirek, R.; Lekenta, K.; Szczytko, J.; Borysiuk, J.; Suffczyński, J.; Kazimierczuk, T.; Goryca, M.; Smoleński, T.; Kossacki, P.; Nawrocki, M.; Pacuski, W. [Institute of Experimental Physics, Faculty of Physics, University of Warsaw, ul. Pasteura 5, PL-02-093 Warszawa (Poland)

2015-11-16

We report on properties of an optical microcavity based on (Cd,Zn,Mg)Te layers and embedding (Cd,Zn)Te quantum wells. The key point of the structure design is the lattice matching of the whole structure to MgTe, which eliminates the internal strain and allows one to embed an arbitrary number of unstrained quantum wells in the microcavity. We evidence the strong light-matter coupling regime already for the structure containing a single quantum well. Embedding four unstrained quantum wells results in further enhancement of the exciton-photon coupling and the polariton lasing in the strong coupling regime.

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

Energy Technology Data Exchange (ETDEWEB)

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

2017-07-19

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

Exciton diamagnetic shift and optical properties in CdSe nanocrystal quantum dots in magnetic fields

Science.gov (United States)

Wu, Shudong; Cheng, Liwen

2018-04-01

The magnetic field dependence of the optical properties of CdSe nanocrystal quantum dots (NQDs) is investigated theoretically using a perturbation method within the effective-mass approximation. The results show that the magnetic field lifts the degeneracy of the electron (hole) states. A blue-shift in the absorption spectra of m ≥ 0 exciton states is observed while the absorption peak of m attributed to the interplay of the orbital Zeeman effect and the additive confinement induced by the magnetic field. The excitonic absorption coefficient is almost independent of B in the strong confinement regime. The applied magnetic field causes the splitting of degenerated exciton states, resulting in the new absorption peaks. Based on the first-order perturbation theory, we propose the analytical expressions for the exciton binding energy, exciton transition energy and exciton diamagnetic shift of 1s, 1p-1, 1p0, 1p1, 1d-2, 1d-1, 1d0, 1d1, 1d2 and 2s exciton states on the applied magnetic field in the strong confinement regime.

Dynamic dipole-dipole interactions between excitons in quantum dots of different sizes

DEFF Research Database (Denmark)

Matsueda, Hideaki; Leosson, Kristjan; Xu, Zhangcheng

2004-01-01

A model of the resonance dynamic dipole-dipole interaction between excitons confined in quantum dots (QDs) of different sizes at close enough distance is given in terms of parity inheritance and exchange of virtual photons. Microphotoluminescence spectra of GaAs-AlGaAs coupled QDs are proposed to...

Axion-photon conversion in space and in low symmetrical dielectric crystals

International Nuclear Information System (INIS)

Gorelik, V S

2016-01-01

The opportunities of axions detection as the result of axion-photon conversion processes in the space and in low symmetrical dielectric crystals are discussed. In accordance with the modern theory predictions, axions are pseudoscalar vacuum particles having very small (0.001-1.0 meV) rest energy. The possibility of axions conversion into photons and vice-versa processes in vacuum at the presence of outer magnetic field has been analyzed before. Pseudoscalar (axion type) modes are existing in some types of crystals. Polar pseudoscalar lattice and exciton modes in low symmetrical crystals are strongly interacted with axions. In this work, optical excitation of axion-type modes in low symmetrical crystals is proposed for observation of axion - photon conversion processes. Instead of outer magnetic field, the crystalline field of such crystals may be used. The experimental schemes for axion-photon conversion processes observation with recording the secondary emission of luminescence, infrared or Stimulated Raman Scattering in some dielectric crystals are discussed. (paper)

Exciton broadening in WS2 /graphene heterostructures

International Nuclear Information System (INIS)

Hill, Heather M.; Rigosi, Albert F.; Raja, Archana

2017-01-01

Here, we have used optical spectroscopy to observe spectral broadening of WS 2 exciton reflectance peaks in heterostructures of monolayer WS 2 capped with mono- to few-layer graphene. The broadening is found to be similar for the A and B excitons and on the order of 5–10 meV. No strong dependence on the number of graphene layers was observed within experimental uncertainty. The broadening can be attributed to charge- and energy-transfer processes between the two materials, providing an observed lower bound for the corresponding time scales of 65 fs.

Towards Scalable Entangled Photon Sources with Self-Assembled InAs /GaAs Quantum Dots

Science.gov (United States)

Wang, Jianping; Gong, Ming; Guo, G.-C.; He, Lixin

2015-08-01

The biexciton cascade process in self-assembled quantum dots (QDs) provides an ideal system for realizing deterministic entangled photon-pair sources, which are essential to quantum information science. The entangled photon pairs have recently been generated in experiments after eliminating the fine-structure splitting (FSS) of excitons using a number of different methods. Thus far, however, QD-based sources of entangled photons have not been scalable because the wavelengths of QDs differ from dot to dot. Here, we propose a wavelength-tunable entangled photon emitter mounted on a three-dimensional stressor, in which the FSS and exciton energy can be tuned independently, thereby enabling photon entanglement between dissimilar QDs. We confirm these results via atomistic pseudopotential calculations. This provides a first step towards future realization of scalable entangled photon generators for quantum information applications.

Excitons in van der Waals Heterostructures: A theoretical study

DEFF Research Database (Denmark)

Latini, Simone

)electronics devices, e.g. light emitting diodes, solar cells, ultra-fast photodetectors, transistors etc., have been successfully fabricated. It is well established that for isolated 2D semiconductors and vdWHs the optical response is governed by excitonic effects. While it is understood that the reduced amount...... of electronic screening in freestanding 2D materials is the main origin of extraordinarily strongly bound excitons, a theoretical understanding of excitonic effects and of how the electronic screening is affected for the more complex case of multi-layer structures is still lacking due to the computational...... in a generalized hydrogenic model to compute exciton binding energies in isolated, supported, or encapsulated 2D semiconductors. The non-locality of the dielectric screening is inherently included in our method and we can successfully describe the non-hydrogenic Rydberg series of low-dimensional systems...

Strong Photonic-Band-Gap Effect on the Spontaneous Emission in 3D Lead Halide Perovskite Photonic Crystals.

Science.gov (United States)

Zhou, Xue; Li, Mingzhu; Wang, Kang; Li, Huizeng; Li, Yanan; Li, Chang; Yan, Yongli; Zhao, Yongsheng; Song, Yanlin

2018-03-25

Stimulated emission in perovskite-embedded polymer opal structures is investigated. A polymer opal structure is filled with a perovskite, and perovskite photonic crystals are prepared. The spontaneous emission of the perovskite embedded in the polymer opal structures exhibits clear signatures of amplified spontaneous emission (ASE) via gain modulation. The difference in refractive-index contrast between the perovskite and the polymer opal is large enough for retaining photonic-crystals properties. The photonic band gap has a strong effect on the fluorescence emission intensity and lifetime. The stimulated emission spectrum exhibits a narrow ASE rather than a wide fluorescence peak in the thin film. © 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Optical nonlinearities of excitonic states in atomically thin 2D transition metal dichalcogenides

Energy Technology Data Exchange (ETDEWEB)

Soh, Daniel Beom Soo [Sandia National Lab. (SNL-CA), Livermore, CA (United States). Proliferation Signatures Discovery and Exploitation Department

2017-08-01

We calculated the optical nonlinearities of the atomically thin monolayer transition metal dichalcogenide material (particularly MoS₂), particularly for those linear and nonlinear transition processes that utilize the bound exciton states. We adopted the bound and the unbound exciton states as the basis for the Hilbert space, and derived all the dynamical density matrices that provides the induced current density, from which the nonlinear susceptibilities can be drawn order-by-order via perturbative calculations. We provide the nonlinear susceptibilities for the linear, the second-harmonic, the third-harmonic, and the kerr-type two-photon processes.

Strong coupling of a single electron in silicon to a microwave photon

Science.gov (United States)

Mi, X.; Cady, J. V.; Zajac, D. M.; Deelman, P. W.; Petta, J. R.

2017-01-01

Silicon is vital to the computing industry because of the high quality of its native oxide and well-established doping technologies. Isotopic purification has enabled quantum coherence times on the order of seconds, thereby placing silicon at the forefront of efforts to create a solid-state quantum processor. We demonstrate strong coupling of a single electron in a silicon double quantum dot to the photonic field of a microwave cavity, as shown by the observation of vacuum Rabi splitting. Strong coupling of a quantum dot electron to a cavity photon would allow for long-range qubit coupling and the long-range entanglement of electrons in semiconductor quantum dots.

Fundamental principles of nanostructures and multiple exciton generation effect in quantum dots

International Nuclear Information System (INIS)

Turaeva, N.; Oksengendler, B.; Rashidova, S.

2011-01-01

In this work the theoretical aspects of the effect of multiple exciton generation in QDs has been studied. The statistic theory of multiple exciton generation in quantum dots is presented based on the Fermi approach to the problem of multiple generation of elementary particles at nucleon-nucleon collisions. Our calculations show that the quantum efficiencies of multiple exciton generation in various quantum dots at absorption of single photon are in a good agreement with the experimental data. The microscopic mechanism of this effect is based on the theory of electronic 'shaking'. In the work the deviation of averaged multiplicity of MEG effect from the Poisson law of fluctuations has been investigated. Besides, the role of interface electronic states of quantum dot and ligand has been considered by means of quantum mechanics. The size optimization of quantum dot has been arranged to receive the maximum multiplicity of MEG effect. (authors)

Excitons in InP/InAs inhomogeneous quantum dots

CERN Document Server

Assaid, E; Khamkhami, J E; Dujardin, F

2003-01-01

Wannier excitons confined in an InP/InAs inhomogeneous quantum dot (IQD) have been studied theoretically in the framework of the effective mass approximation. A finite-depth potential well has been used to describe the effect of the quantum confinement in the InAs layer. The exciton binding energy has been determined using the Ritz variational method. The spatial correlation between the electron and the hole has been taken into account in the expression for the wavefunction. It has been shown that for a fixed size b of the IQD, the exciton binding energy depends strongly on the core radius a. Moreover, it became apparent that there are two critical values of the core radius, a sub c sub r sub i sub t and a sub 2 sub D , for which important changes of the exciton binding occur. The former critical value, a sub c sub r sub i sub t , corresponds to a minimum of the exciton binding energy and may be used to distinguish between tridimensional confinement and bidimensional confinement. The latter critical value, a ...

Inverse Funnel Effect of Excitons in Strained Black Phosphorus

Directory of Open Access Journals (Sweden)

Pablo San-Jose

2016-09-01

Full Text Available We study the effects of strain on the properties and dynamics of Wannier excitons in monolayer (phosphorene and few-layer black phosphorus (BP, a promising two-dimensional material for optoelectronic applications due to its high mobility, mechanical strength, and strain-tunable direct band gap. We compare the results to the case of molybdenum disulphide (MoS_{2} monolayers. We find that the so-called funnel effect, i.e., the possibility of controlling exciton motion by means of inhomogeneous strains, is much stronger in few-layer BP than in MoS_{2} monolayers and, crucially, is of opposite sign. Instead of excitons accumulating isotropically around regions of high tensile strain like in MoS_{2}, excitons in BP are pushed away from said regions. This inverse funnel effect is moreover highly anisotropic, with much larger funnel distances along the armchair crystallographic direction, leading to a directional focusing of exciton flow. A strong inverse funnel effect could enable simpler designs of funnel solar cells and offer new possibilities for the manipulation and harvesting of light.

Tailoring Quantum Dot Assemblies to Extend Exciton Coherence Times and Improve Exciton Transport

Science.gov (United States)

Seward, Kenton; Lin, Zhibin; Lusk, Mark

2012-02-01

The motion of excitons through nanostructured assemblies plays a central role in a wide range of physical phenomena including quantum computing, molecular electronics, photosynthetic processes, excitonic transistors and light emitting diodes. All of these technologies are severely handicapped, though, by quasi-particle lifetimes on the order of a nanosecond. The movement of excitons must therefore be as efficient as possible in order to move excitons meaningful distances. This is problematic for assemblies of small Si quantum dots (QDs), where excitons quickly localize and entangle with dot phonon modes. Ensuing exciton transport is then characterized by a classical random walk reduced to very short distances because of efficient recombination. We use a combination of master equation (Haken-Strobl) formalism and density functional theory to estimate the rate of decoherence in Si QD assemblies and its impact on exciton mobility. Exciton-phonon coupling and Coulomb interactions are calculated as a function of dot size, spacing and termination to minimize the rate of intra-dot phonon entanglement. This extends the time over which more efficient exciton transport, characterized by partial coherence, can be maintained.

Resonant exciton-phonon coupling in ZnO nanorods at room temperature

Directory of Open Access Journals (Sweden)

Soumee Chakraborty

2011-09-01

Full Text Available Vibronic and optoelectronic properties, along with detailed studies of exciton-phonon coupling at room temperature (RT for random and aligned ZnO nanorods are reported. Excitation energy dependent Raman studies are performed for detailed analysis of multi-phonon processes in the nanorods. We report here the origin of coupling between free exciton and its associated phonon replicas, including its higher order modes, in the photoluminescence spectra at RT. Resonance of excitonic electron and resonating first order zone center LO phonon, invoked strongly by Frolich interaction, are made responsible for the observed phenomenon.

Strong-field QED processes in short laser pulses. One- and two-photon Compton scattering

Energy Technology Data Exchange (ETDEWEB)

Seipt, Daniel

2012-12-20

The purpose of this thesis is to advance the understanding of strong-field QED processes in short laser pulses. The processes of non-linear one-photon and two-photon Compton scattering are studied, that is the scattering of photons in the interaction of relativistic electrons with ultra-short high-intensity laser pulses. These investigations are done in view of the present and next generation of ultra-high intensity optical lasers which are supposed to achieve unprecedented intensities of the order of 10{sup 24} W/cm{sup 2} and beyond, with pulse lengths in the order of some femtoseconds. The ultra-high laser intensity requires a non-perturbative description of the interaction of charged particles with the laser field to allow for multi-photon interactions, which is beyond the usual perturbative expansion of QED organized in powers of the fine structure constant. This is achieved in strong-field QED by employing the Furry picture and non-perturbative solutions of the Dirac equation in the presence of a background laser field as initial and final state wave functions, as well as the laser dressed Dirac-Volkov propagator. The primary objective is a realistic description of scattering processes with regard to the finite laser pulse duration beyond the common approximation of infinite plane waves, which is made necessary by the ultra-short pulse length of modern high-intensity lasers. Non-linear finite size effects are identified, which are a result of the interplay between the ultra-high intensity and the ultra-short pulse length. In particular, the frequency spectra and azimuthal photon emission spectra are studied emphasizing the differences between pulsed and infinite laser fields. The proper description of the finite temporal duration of the laser pulse leads to a regularization of unphysical infinities (due to the infinite plane-wave description) of the laser-dressed Dirac-Volkov propagator and in the second-order strong-field process of two-photon Compton

Impacts of Coulomb Interactions on the Magnetic Responses of Excitonic Complexes in Single Semiconductor Nanostructures

Directory of Open Access Journals (Sweden)

Fu Ying-Jhe

2010-01-01

Full Text Available Abstract We report on the diamagnetic responses of different exciton complexes in single InAs/GaAs self-assembled quantum dots (QDs and quantum rings (QRs. For QDs, the imbalanced magnetic responses of inter-particle Coulomb interactions play a crucial role in the diamagnetic shifts of excitons (X, biexcitons (XX, and positive trions (X−. For negative trions (X− in QDs, anomalous magnetic responses are observed, which cannot be described by the conventional quadratic energy shift with the magnetic field. The anomalous behavior is attributed to the apparent change in the electron wave function extent after photon emission due to the strong Coulomb attraction by the hole in its initial state. In QRs, the diamagnetic responses of X and XX also show different behaviors. Unlike QDs, the diamagnetic shift of XX in QRs is considerably larger than that of X. The inherent structural asymmetry combined with the inter-particle Coulomb interactions makes the wave function distribution of XX very different from that of X in QRs. Our results suggest that the phase coherence of XX in QRs may survive from the wave function localization due to the structural asymmetry or imperfections.

Near-unity efficiency, single-photon sources based on tapered photonic nanowires

DEFF Research Database (Denmark)

Bleuse, Joël; Munsch, Mathieu; Claudon, Julien

2012-01-01

Single-photon emission from excitons in InAs Quantum Dots (QD) embedded in GaAs Tapered Photonic Wires (TPW) already demonstrated a 0.72 collection efficiency, with TPWs were the apex is the sharp end of the cone. Going to alternate designs, still based on the idea of the adiabatic deconfinement...... of the quasi-Gaussian emission mode, but with inverted TPW where the apex is the cone's base, leads to even larger efficiencies. In addition, these inverted TPWs make the electric pumping of the emitters compatible with these large efficiencies....

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.

Perovskite Excitonics : Primary Exciton Creation and Crossover from Free Carriers to a Secondary Exciton Phase

NARCIS (Netherlands)

Sarritzu, Valerio; Sestu, Nicola; Marongiu, Daniela; Chang, Xueqing; Wang, Qingqian; Loi, Maria Antonietta; Quochi, Francesco; Saba, Michele; Mura, Andrea; Bongiovanni, Giovanni

2018-01-01

Understanding exciton formation is of fundamental importance for emerging optoelectronic materials, like hybrid organic-inorganic perovskites, as excitons are the lowest-energy photoexcitations in semiconductors, are electrically neutral, and do not directly contribute to charge transport, but can

Excitonic processes at organic heterojunctions

Science.gov (United States)

He, ShouJie; Lu, ZhengHong

2018-02-01

Understanding excitonic processes at organic heterojunctions is crucial for development of organic semiconductor devices. This article reviews recent research on excitonic physics that involve intermolecular charge transfer (CT) excitons, and progress on understanding relationships between various interface energy levels and key parameters governing various competing interface excitonic processes. These interface excitonic processes include radiative exciplex emission, nonradiative recombination, Auger electron emission, and CT exciton dissociation. This article also reviews various device applications involving interface CT excitons, such as organic light-emitting diodes (OLEDs), organic photovoltaic cells, organic rectifying diodes, and ultralow-voltage Auger OLEDs.

Spin-dependent exciton-exciton interaction potential in two- and three-dimensional structure semiconductors under excitation

International Nuclear Information System (INIS)

Nguyen Ba An; Hoang Ngoc Cam; Nguyen Trung Dan

1990-08-01

Analytical expressions of the exciton-exciton interaction potentials have been approximately derived in both 2D and 3D structure materials exhibiting explicit dependences on exciton momentum difference, momentum transfer, electron-hole effective mass ratio and two-exciton state spin symmetry. Numerical calculations show that the character of the exciton-exciton interaction is determined by all of the above-mentioned dependences. (author). 32 refs, 7 figs

Few-Photon Multiple Ionization of Ne and Ar by Strong Free-Electron-Laser Pulses

International Nuclear Information System (INIS)

Moshammer, R.; Jiang, Y. H.; Rudenko, A.; Ergler, Th.; Schroeter, C. D.; Luedemann, S.; Zrost, K.; Dorn, A.; Ferger, T.; Kuehnel, K. U.; Ullrich, J.; Foucar, L.; Titze, J.; Jahnke, T.; Schoeffler, M.; Doerner, R.; Fischer, D.; Weber, T.; Zouros, T. J. M.; Duesterer, S.

2007-01-01

Few-photon multiple ionization of Ne and Ar atoms by strong vacuum ultraviolet laser pulses from the free-electron laser at Hamburg was investigated differentially with the Heidelberg reaction microscope. The light-intensity dependence of Ne 2+ production reveals the dominance of nonsequential two-photon double ionization at intensities of I 12 W/cm 2 and significant contributions of three-photon ionization as I increases. Ne 2+ recoil-ion-momentum distributions suggest that two electrons absorbing ''instantaneously'' two photons are ejected most likely into opposite hemispheres with similar energies

Single photon emission and quantum ring-cavity coupling in InAs/GaAs quantum rings

International Nuclear Information System (INIS)

Gallardo, E; Nowak, A K; Sanvitto, D; Meulen, H P van der; Calleja, J M; MartInez, L J; Prieto, I; Alija, A R; Granados, D; Taboada, A G; GarcIa, J M; Postigo, P A; Sarkar, D

2010-01-01

Different InAs/GaAs quantum rings embedded in a photonic crystal microcavity are studied by quantum correlation measurements. Single photon emission, with g (2) (0) values around 0.3, is demonstrated for a quantum ring not coupled to the microcavity. Characteristic rise-times are found to be longer for excitons than for biexcitons, resulting in the time asymmetry of the exciton-biexciton cross-correlation. No antibunching is observed in another quantum ring weakly coupled to the microcavity.

Exciton Rydberg series in mono- and few-layer WS2

Science.gov (United States)

Chernikov, Alexey; Berkelbach, Timothy C.; Hill, Heather M.; Rigosi, Albert; Li, Yilei; Aslan, Özgur B.; Hybertsen, Mark S.; Reichman, David R.; Heinz, Tony F.

2014-03-01

Considered a long-awaited semiconducting analogue to graphene, the family of atomically thin transition metal dichalcogenides (TMDs) attracted intense interest in the scientific community due to their remarkable physical properties resulting from the reduced dimensionality. A fundamental manifestation of the two-dimensional nature is a strong increase in the Coulomb interaction. The resulting formation of tightly bound excitons plays a crucial role for a majority of optical and transport phenomena. In our work, we investigate the excitons in atomically thin TMDs by optical micro-spectroscopy and apply a microscopic, ab-initio theoretical approach. We observe a full sequence of excited exciton states, i.e., the Rydberg series, in the monolayer WS2, identifying tightly bound excitons with energies exceeding 0.3 eV - almost an order of magnitude higher than in the corresponding, three-dimensional crystal. We also find significant deviations of the excitonic properties from the conventional hydrogenic physics - a direct evidence of a non-uniform dielectric environment. Finally, an excellent quantitative agreement is obtained between the experimental findings and the developed theoretical approach.

Co-existence of free and self-trapped excitons in J-aggregates

International Nuclear Information System (INIS)

Malyukin, Yu.V.; Lebedenko, A.N.; Sorokin, A.V.; Yefimova, S.L.

2005-01-01

Nature of excited electronic states of amphi-PIC J-aggregates, which are the source of the self-trapping states, have been investigated using low-temperature site-selective, time-resolved spectroscopy techniques. The self-trapping states are shown to evolve from the delocalized exciton states within the J-band. The strongly localized electronic states located on the low-frequency edge of the J-band, are not able to form polaronic states and, hence, the polaronic relaxation process is particularly collective one. The exciton self-trapping is more effective in J-aggregates with strong disorder, requires overcoming a self-trapping barrier

Wannier-Mott Excitons in Nanoscale Molecular Ices

Science.gov (United States)

Chen, Y.-J.; Muñoz Caro, G. M.; Aparicio, S.; Jiménez-Escobar, A.; Lasne, J.; Rosu-Finsen, A.; McCoustra, M. R. S.; Cassidy, A. M.; Field, D.

2017-10-01

The absorption of light to create Wannier-Mott excitons is a fundamental feature dictating the optical and photovoltaic properties of low band gap, high permittivity semiconductors. Such excitons, with an electron-hole separation an order of magnitude greater than lattice dimensions, are largely limited to these semiconductors but here we find evidence of Wannier-Mott exciton formation in solid carbon monoxide (CO) with a band gap of >8 eV and a low electrical permittivity. This is established through the observation that a change of a few degrees K in deposition temperature can shift the electronic absorption spectra of solid CO by several hundred wave numbers, coupled with the recent discovery that deposition of CO leads to the spontaneous formation of electric fields within the film. These so-called spontelectric fields, here approaching 4 ×107 V m-1 , are strongly temperature dependent. We find that a simple electrostatic model reproduces the observed temperature dependent spectral shifts based on the Stark effect on a hole and electron residing several nm apart, identifying the presence of Wannier-Mott excitons. The spontelectric effect in CO simultaneously explains the long-standing enigma of the sensitivity of vacuum ultraviolet spectra to the deposition temperature.

Characterization of Strong Light-Matter Coupling in Semiconductor Quantum-Dot Microcavities via Photon-Statistics Spectroscopy

Science.gov (United States)

Schneebeli, L.; Kira, M.; Koch, S. W.

2008-08-01

It is shown that spectrally resolved photon-statistics measurements of the resonance fluorescence from realistic semiconductor quantum-dot systems allow for high contrast identification of the two-photon strong-coupling states. Using a microscopic theory, the second-rung resonance of Jaynes-Cummings ladder is analyzed and optimum excitation conditions are determined. The computed photon-statistics spectrum displays gigantic, experimentally robust resonances at the energetic positions of the second-rung emission.

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...

Exploring the physics of superconducting qubits strongly coupled to microwave frequency photons

Energy Technology Data Exchange (ETDEWEB)

Wallraff, Andreas [ETH Zurich (Switzerland)

2013-07-01

Using modern micro and nano-fabrication techniques combined with superconducting materials we realize electronic circuits the properties of which are governed by the laws of quantum mechanics. In such circuits the strong interaction of photons with superconducting quantum two-level systems allows us to probe fundamental quantum properties of light and to develop components for applications in quantum information technology. Here, I present experiments in which we have created and probed entanglement between stationary qubits and microwave photons freely propagating down a transmission line. In these experiments we use superconducting parametric amplifiers realized in our lab to detect both qubit and photon states efficiently. Using similar techniques we aim at demonstrating a deterministic scheme for teleportation of quantum states in a macroscopic system based on superconducting circuits.

Biexciton formation and exciton coherent coupling in layered GaSe

Science.gov (United States)

Dey, P.; Paul, J.; Moody, G.; Stevens, C. E.; Glikin, N.; Kovalyuk, Z. D.; Kudrynskyi, Z. R.; Romero, A. H.; Cantarero, A.; Hilton, D. J.; Karaiskaj, D.

2015-06-01

Nonlinear two-dimensional Fourier transform (2DFT) and linear absorption spectroscopy are used to study the electronic structure and optical properties of excitons in the layered semiconductor GaSe. At the 1s exciton resonance, two peaks are identified in the absorption spectra, which are assigned to splitting of the exciton ground state into the triplet and singlet states. 2DFT spectra acquired for co-linear polarization of the excitation pulses feature an additional peak originating from coherent energy transfer between the singlet and triplet. At cross-linear polarization of the excitation pulses, the 2DFT spectra expose a new peak likely originating from bound biexcitons. The polarization dependent 2DFT spectra are well reproduced by simulations using the optical Bloch equations for a four level system, where many-body effects are included phenomenologically. Although biexciton effects are thought to be strong in this material, only moderate contributions from bound biexciton creation can be observed. The biexciton binding energy of ˜2 meV was estimated from the separation of the peaks in the 2DFT spectra. Temperature dependent absorption and 2DFT measurements, combined with "ab initio" theoretical calculations of the phonon spectra, indicate strong interaction with the A1 ' phonon mode. Excitation density dependent 2DFT measurements reveal excitation induced dephasing and provide a lower limit for the homogeneous linewidth of the excitons in the present GaSe crystal.

Impact of the glass transition on exciton dynamics in polymer thin films

Science.gov (United States)

Ehrenreich, Philipp; Proepper, Daniel; Graf, Alexander; Jores, Stefan; Boris, Alexander V.; Schmidt-Mende, Lukas

2017-11-01

In the development of organic electronics, unlimited design possibilities of conjugated polymers offer a wide variety of mechanical and electronic properties. Thereby, it is crucially important to reveal universal physical characteristics that allow efficient and forward developments of new chemical compounds. In particular for organic solar cells, a deeper understanding of exciton dynamics in polymer films can help to improve the charge generation process further. For this purpose, poly(3-hexylthiophene) (P3HT) is commonly used as a model system, although exciton decay kinetics have found different interpretations. Using temperature-dependent time-resolved photoluminescence spectroscopy in combination with low-temperature spectroscopic ellipsometry, we can show that P3HT is indeed a model system in which excitons follow a simple diffusion/hopping model. Based on our results we can exclude the relevance of hot-exciton emission as well as a dynamic torsional relaxation upon photoexcitation on a ps time scale. Instead, we depict the glass transition temperature of polymers to strongly affect exciton dynamics.

Wannier-Frenkel hybrid exciton in organic-semiconductor quantum dot heterostructures

International Nuclear Information System (INIS)

Birman, Joseph L.; Huong, Nguyen Que

2007-01-01

The formation of a hybridization state of Wannier Mott exciton and Frenkel exciton in different hetero-structure configurations involving quantum dots is investigated. The hybrid excitons exist at the interfaces of the semiconductors quantum dots and the organic medium, having unique properties and a large optical non-linearity. The coupling at resonance is very strong and tunable by changing the parameters of the systems (dot radius, dot-dot distance, generation of the organic dendrites and the materials of the system etc...). Different semiconductor quantum dot-organic material combination systems have been considered such as a semiconductor quantum dot lattice embedded in an organic host, a semiconductor quantum dot at the center of an organic dendrite, a semiconductor quantum dot coated by an organic shell

Electrons, holes, and excitons in GaAs polytype quantum dots

Energy Technology Data Exchange (ETDEWEB)

Climente, Juan I.; Segarra, Carlos; Rajadell, Fernando; Planelles, Josep, E-mail: josep.planelles@uji.es [Departament de Química Física i Analítica, Universitat Jaume I, E-12080 Castelló (Spain)

2016-03-28

Single and multi-band k⋅p Hamiltonians for GaAs crystal phase quantum dots are used to assess ongoing experimental activity on the role of such factors as quantum confinement, spontaneous polarization, valence band mixing, and exciton Coulomb interaction. Spontaneous polarization is found to be a dominating term. Together with the control of dot thickness [Vainorius et al., Nano Lett. 15, 2652 (2015)], it enables wide exciton wavelength and lifetime tunability. Several new phenomena are predicted for small diameter dots [Loitsch et al., Adv. Mater. 27, 2195 (2015)], including non-heavy hole ground state, strong hole spin admixture, and a type-II to type-I exciton transition, which can be used to improve the absorption strength and reduce the radiative lifetime of GaAs polytypes.

The strong will of the photon

International Nuclear Information System (INIS)

Schuler, Gerhard

1993-01-01

Among today's elementary particles, the photon, the massless carrier of the electromagnetic force, plays a special role. At high energy, it has a dual character - sometimes pointlike and structureless, elsewhere with a hadronic structure. This is reminiscent of the duality of radiation and matter established at the beginning of the century. But while this wave-particle duality is understood in quantum mechanics, we have no complete description of high energy hadronic interactions. Quantum chromodynamics, the field theory of quarks and gluons, comes nearest, but calculations are not always possible. Physicists have to resort to intuitive pictures and models to supplement formal theory. The hadronic Side of the photon is a rich field, both theoretically and experimentally, studied using a range of reactions at all the major front-line accelerators and storage rings, culminating most recently with first data from the new HERA electron proton collider at DESY, Hamburg. The photon was first regarded as structureless. The first hint of photon structure was probably electronpositron pair creation by photons in an electromagnetic field. In relativistic quantum field theory, a particle contains not only its 'bare' state, but also contributions from all states coupled to it by the interaction. Thus in quantum terms the photon also contains electron-positron pairs, which can materialize in high-energy reactions

Intense coherent longitudinal optical phonons in CuI thin films under exciton-excitation conditions

International Nuclear Information System (INIS)

Kojima, O.; Mizoguchi, K.; Nakayama, M..

2005-01-01

We have investigated the dynamical properties of the coherent longitudinal optical (LO) phonon in CuI thin films grown on a NaCl substrate by vacuum deposition. The intense coherent LO phonon in the CuI thin film is observed under the exciton-excitation conditions. Moreover, the pump-energy dependence of the amplitude of the coherent LO phonon shows peaks at the heavy-hole and light-hole exciton energies. The enhancement of the coherent LO phonon under the exciton-resonance condition is much larger than that in an ordinary semiconductor quantum well system such as a GaAs/AlAs one. These facts demonstrate that the intense coherent LO phonon is generated under the exciton-excitation condition in a material with a strong exciton-phonon interaction such as CuI

Circuit electromechanics with single photon strong coupling

Energy Technology Data Exchange (ETDEWEB)

Xue, Zheng-Yuan, E-mail: zyxue@scnu.edu.cn; Yang, Li-Na [Guangdong Provincial Key Laboratory of Quantum Engineering and Quantum Materials, and School of Physics and Telecommunication Engineering, South China Normal University, Guangzhou 510006 (China); Zhou, Jian, E-mail: jianzhou8627@163.com [Department of Electronic Communication Engineering, Anhui Xinhua University, Hefei 230088 (China); Guangdong Provincial Key Laboratory of Quantum Engineering and Quantum Materials, and School of Physics and Telecommunication Engineering, South China Normal University, Guangzhou 510006 (China)

2015-07-13

In circuit electromechanics, the coupling strength is usually very small. Here, replacing the capacitor in circuit electromechanics by a superconducting flux qubit, we show that the coupling among the qubit and the two resonators can induce effective electromechanical coupling which can attain the strong coupling regime at the single photon level with feasible experimental parameters. We use dispersive couplings among two resonators and the qubit while the qubit is also driven by an external classical field. These couplings form a three-wave mixing configuration among the three elements where the qubit degree of freedom can be adiabatically eliminated, and thus results in the enhanced coupling between the two resonators. Therefore, our work constitutes the first step towards studying quantum nonlinear effect in circuit electromechanics.

Reconstructing Space- and Energy-Dependent Exciton Generation in Solution-Processed Inverted Organic Solar Cells.

Science.gov (United States)

Wang, Yuheng; Zhang, Yajie; Lu, Guanghao; Feng, Xiaoshan; Xiao, Tong; Xie, Jing; Liu, Xiaoyan; Ji, Jiahui; Wei, Zhixiang; Bu, Laju

2018-04-25

Photon absorption-induced exciton generation plays an important role in determining the photovoltaic properties of donor/acceptor organic solar cells with an inverted architecture. However, the reconstruction of light harvesting and thus exciton generation at different locations within organic inverted device are still not well resolved. Here, we investigate the film depth-dependent light absorption spectra in a small molecule donor/acceptor film. Including depth-dependent spectra into an optical transfer matrix method allows us to reconstruct both film depth- and energy-dependent exciton generation profiles, using which short-circuit current and external quantum efficiency of the inverted device are simulated and compared with the experimental measurements. The film depth-dependent spectroscopy, from which we are able to simultaneously reconstruct light harvesting profile, depth-dependent composition distribution, and vertical energy level variations, provides insights into photovoltaic process. In combination with appropriate material processing methods and device architecture, the method proposed in this work will help optimizing film depth-dependent optical/electronic properties for high-performance solar cells.

Excitonic Order and Superconductivity in the Two-Orbital Hubbard Model: Variational Cluster Approach

Science.gov (United States)

Fujiuchi, Ryo; Sugimoto, Koudai; Ohta, Yukinori

2018-06-01

Using the variational cluster approach based on the self-energy functional theory, we study the possible occurrence of excitonic order and superconductivity in the two-orbital Hubbard model with intra- and inter-orbital Coulomb interactions. It is known that an antiferromagnetic Mott insulator state appears in the regime of strong intra-orbital interaction, a band insulator state appears in the regime of strong inter-orbital interaction, and an excitonic insulator state appears between them. In addition to these states, we find that the s±-wave superconducting state appears in the small-correlation regime, and the dx2 - y2-wave superconducting state appears on the boundary of the antiferromagnetic Mott insulator state. We calculate the single-particle spectral function of the model and compare the band gap formation due to the superconducting and excitonic orders.

Strongly-Refractive One-Dimensional Photonic Crystal Prisms

Science.gov (United States)

Ting, David Z. (Inventor)

2004-01-01

One-dimensional (1D) photonic crystal prisms can separate a beam of polychromatic electromagnetic waves into constituent wavelength components and can utilize unconventional refraction properties for wavelength dispersion over significant portions of an entire photonic band rather than just near the band edges outside the photonic band gaps. Using a ID photonic crystal simplifies the design and fabrication process and allows the use of larger feature sizes. The prism geometry broadens the useful wavelength range, enables better optical transmission, and exhibits angular dependence on wavelength with reduced non-linearity. The properties of the 1 D photonic crystal prism can be tuned by varying design parameters such as incidence angle, exit surface angle, and layer widths. The ID photonic crystal prism can be fabricated in a planar process, and can be used as optical integrated circuit elements.

Multiple exciton generation in quantum dot-based solar cells

Science.gov (United States)

Goodwin, Heather; Jellicoe, Tom C.; Davis, Nathaniel J. L. K.; Böhm, Marcus L.

2018-01-01

Multiple exciton generation (MEG) in quantum-confined semiconductors is the process by which multiple bound charge-carrier pairs are generated after absorption of a single high-energy photon. Such charge-carrier multiplication effects have been highlighted as particularly beneficial for solar cells where they have the potential to increase the photocurrent significantly. Indeed, recent research efforts have proved that more than one charge-carrier pair per incident solar photon can be extracted in photovoltaic devices incorporating quantum-confined semiconductors. While these proof-of-concept applications underline the potential of MEG in solar cells, the impact of the carrier multiplication effect on the device performance remains rather low. This review covers recent advancements in the understanding and application of MEG as a photocurrent-enhancing mechanism in quantum dot-based photovoltaics.

Phonon effects on the radiative recombination of excitons in double quantum dots

Science.gov (United States)

Karwat, Paweł; Sitek, Anna; Machnikowski, Paweł

2011-11-01

We study theoretically the radiative recombination of excitons in double quantum dots in the presence of carrier-phonon coupling. We show that the phonon-induced pure dephasing effects and transitions between the exciton states strongly modify the spontaneous emission process and make it sensitive to temperature, which may lead to nonmonotonic temperature dependence of the time-resolved luminescence. We show also that, under specific resonance conditions, the biexcitonic interband polarization can be coherently transferred to the excitonic one, leading to an extended lifetime of the total coherent polarization, which is reflected in the nonlinear optical spectrum of the system. We study the stability of this effect against phonon-induced decoherence.

Density of states and excitonic condensation in the double layer correlated systems

Energy Technology Data Exchange (ETDEWEB)

Apinyan, V., E-mail: v.apinyan@int.pan.wroc.pl; Kopeć, T.K.

2016-01-15

We consider the single-particle density of states (DOS) in the strongly correlated double layer (DL) system, without applied external fields. We demonstrate an unusual collapse effect in the spectrum of the normal single-particle spectral function at the particular high-symmetry point corresponding to the specific bunching-point solution of the chemical potential in the Frenkel channel. We show that at the low-temperature limit the anomalous spectral function obeys a concave like structure, which is directly related to the interlayer pair formation and condensation. We calculate the normal DOS functions, and we find their temperature dependence for different values of the interlayer Coulomb interaction parameter. We show that the normal electron and hole DOS functions demonstrate typical condensates double peak structures on the background of the excitonic pair formation quasiparticle spectra and we have found the evidence of the hybridization gap in the case of high-temperature limit, and small interlayer coupling parameter. Meanwhile, we show a possible crossover from the excitonic condensate regime into the band insulator state. The structure of the normal DOS spectra, in the Frenkel channel and for the strong interlayer coupling regime, is found gapless for all temperature limits, which clearly indicates the strong coherence effects in the DL structure, and the excitonic condensates therein. We have shown that the excitonic pair formation and pair condensation occur simultaneously in the DL system, in contrast with the purely three-dimensional (3D) or two-dimensional cases (2D), discussed previously.

Fermi-edge exciton-polaritons in doped semiconductor microcavities with finite hole mass

Science.gov (United States)

Pimenov, Dimitri; von Delft, Jan; Glazman, Leonid; Goldstein, Moshe

2017-10-01

The coupling between a 2D semiconductor quantum well and an optical cavity gives rise to combined light-matter excitations, the exciton-polaritons. These were usually measured when the conduction band is empty, making the single polariton physics a simple single-body problem. The situation is dramatically different in the presence of a finite conduction-band population, where the creation or annihilation of a single exciton involves a many-body shakeup of the Fermi sea. Recent experiments in this regime revealed a strong modification of the exciton-polariton spectrum. Previous theoretical studies concerned with nonzero Fermi energy mostly relied on the approximation of an immobile valence-band hole with infinite mass, which is appropriate for low-mobility samples only; for high-mobility samples, one needs to consider a mobile hole with large but finite mass. To bridge this gap, we present an analytical diagrammatic approach and tackle a model with short-ranged (screened) electron-hole interaction, studying it in two complementary regimes. We find that the finite hole mass has opposite effects on the exciton-polariton spectra in the two regimes: in the first, where the Fermi energy is much smaller than the exciton binding energy, excitonic features are enhanced by the finite mass. In the second regime, where the Fermi energy is much larger than the exciton binding energy, finite mass effects cut off the excitonic features in the polariton spectra, in qualitative agreement with recent experiments.

Optical nonlinearity and bistability in the bound exciton energy range of CdS

International Nuclear Information System (INIS)

Hoenig, T.; Gutowski, J.

1988-01-01

Under high excitation conditions thick CdS samples show pronounced broad-band nonlinear transmission in the bound exciton region and up to a wavelength of about 515 nm at cryo-temperatures. This behavior is only explainable in a model based on impurity neutralization and bound exciton creation. The suitability of these nonlinearities to yield optical bistability will be shown. Bistable operation is investigated in dependence of crystal thickness, impurity concentration, excitation density, wavelength, and temperature. A strong correlation to acceptor-bound exciton generation is obtained, and the explanation of this bistable operation fits well with that of the above mentioned transmission behavior. (author)

Structural tunability and switchable exciton emission in inorganic-organic hybrids with mixed halides

Science.gov (United States)

Ahmad, Shahab; Baumberg, Jeremy J.; Vijaya Prakash, G.

2013-12-01

Room-temperature tunable excitonic photoluminescence is demonstrated in alloy-tuned layered Inorganic-Organic (IO) hybrids, (C12H25NH3)2PbI4(1-y)Br4y (y = 0 to 1). These perovskite IO hybrids adopt structures with alternating stacks of low-dimensional inorganic and organic layers, considered to be naturally self-assembled multiple quantum wells. These systems resemble stacked monolayer 2D semiconductors since no interlayer coupling exists. Thin films of IO hybrids exhibit sharp and strong photoluminescence (PL) at room-temperature due to stable excitons formed within the low-dimensional inorganic layers. Systematic variation in the observed exciton PL from 510 nm to 350 nm as the alloy composition is changed, is attributed to the structural readjustment of crystal packing upon increase of the Br content in the Pb-I inorganic network. The energy separation between exciton absorption and PL is attributed to the modified exciton density of states and diffusion of excitons from relatively higher energy states corresponding to bromine rich sites towards the lower energy iodine sites. Apart from compositional fluctuations, these excitons show remarkable reversible flips at temperature-induced phase transitions. All the results are successfully correlated with thermal and structural studies. Such structural engineering flexibility in these hybrids allows selective tuning of desirable exciton properties within suitable operating temperature ranges. Such wide-range PL tunability and reversible exciton switching in these novel IO hybrids paves the way to potential applications in new generation of optoelectronic devices.

Biexciton formation and exciton coherent coupling in layered GaSe

Energy Technology Data Exchange (ETDEWEB)

Dey, P.; Paul, J.; Stevens, C. E.; Glikin, N.; Karaiskaj, D., E-mail: karaiskaj@usf.edu [Department of Physics, University of South Florida, 4202 East Fowler Ave., Tampa, Florida 33620 (United States); Moody, G. [National Institute of Standards and Technology, 325 Broadway, Boulder, Colarado 80305 (United States); Kovalyuk, Z. D.; Kudrynskyi, Z. R. [Chernivtsi Department, Frantsevich Institute of Material Sciences Problems, The National Academy of Sciences of Ukraine, 5, Iryna Vilde St., 58001 Chernivtsi (Ukraine); Romero, A. H. [Physics Department, West Virginia University, Morgantown, West Virginia 26506-6315 (United States); Cantarero, A. [Materials Science Institute, University of Valencia, P.O. Box 2205, 46071 Valencia (Spain); Hilton, D. J. [Department of Physics, University of Alabama at Birmingham, Birmingham, Alabama 35294 (United States)

2015-06-07

Nonlinear two-dimensional Fourier transform (2DFT) and linear absorption spectroscopy are used to study the electronic structure and optical properties of excitons in the layered semiconductor GaSe. At the 1s exciton resonance, two peaks are identified in the absorption spectra, which are assigned to splitting of the exciton ground state into the triplet and singlet states. 2DFT spectra acquired for co-linear polarization of the excitation pulses feature an additional peak originating from coherent energy transfer between the singlet and triplet. At cross-linear polarization of the excitation pulses, the 2DFT spectra expose a new peak likely originating from bound biexcitons. The polarization dependent 2DFT spectra are well reproduced by simulations using the optical Bloch equations for a four level system, where many-body effects are included phenomenologically. Although biexciton effects are thought to be strong in this material, only moderate contributions from bound biexciton creation can be observed. The biexciton binding energy of ∼2 meV was estimated from the separation of the peaks in the 2DFT spectra. Temperature dependent absorption and 2DFT measurements, combined with “ab initio” theoretical calculations of the phonon spectra, indicate strong interaction with the A{sub 1}{sup ′} phonon mode. Excitation density dependent 2DFT measurements reveal excitation induced dephasing and provide a lower limit for the homogeneous linewidth of the excitons in the present GaSe crystal.

Biexciton formation and exciton coherent coupling in layered GaSe

International Nuclear Information System (INIS)

Dey, P.; Paul, J.; Stevens, C. E.; Glikin, N.; Karaiskaj, D.; Moody, G.; Kovalyuk, Z. D.; Kudrynskyi, Z. R.; Romero, A. H.; Cantarero, A.; Hilton, D. J.

2015-01-01

Nonlinear two-dimensional Fourier transform (2DFT) and linear absorption spectroscopy are used to study the electronic structure and optical properties of excitons in the layered semiconductor GaSe. At the 1s exciton resonance, two peaks are identified in the absorption spectra, which are assigned to splitting of the exciton ground state into the triplet and singlet states. 2DFT spectra acquired for co-linear polarization of the excitation pulses feature an additional peak originating from coherent energy transfer between the singlet and triplet. At cross-linear polarization of the excitation pulses, the 2DFT spectra expose a new peak likely originating from bound biexcitons. The polarization dependent 2DFT spectra are well reproduced by simulations using the optical Bloch equations for a four level system, where many-body effects are included phenomenologically. Although biexciton effects are thought to be strong in this material, only moderate contributions from bound biexciton creation can be observed. The biexciton binding energy of ∼2 meV was estimated from the separation of the peaks in the 2DFT spectra. Temperature dependent absorption and 2DFT measurements, combined with “ab initio” theoretical calculations of the phonon spectra, indicate strong interaction with the A 1 ′ phonon mode. Excitation density dependent 2DFT measurements reveal excitation induced dephasing and provide a lower limit for the homogeneous linewidth of the excitons in the present GaSe crystal

Electrical control of optical orientation of neutral and negatively charged excitons in an n -type semiconductor quantum well

Science.gov (United States)

Dzhioev, R. I.; Korenev, V. L.; Lazarev, M. V.; Sapega, V. F.; Gammon, D.; Bracker, A. S.

2007-01-01

We report electric field induced increase of spin orientation of negatively charged excitons (trions) localized in n -type GaAs/AlGaAs quantum well. Under resonant excitation of free neutral heavy-hole excitons, the polarization of trions increases dramatically with electrical injection of electrons. The polarization enhancement correlates strongly with trion/exciton luminescence intensity ratio. This effect results from a very efficient trapping of free neutral excitons by the quantum well interfacial fluctuations (“natural” quantum dots) containing resident electrons.

Exciton modeling of energy-transfer dynamics in the LHCII complex of higher plants: a Redfield theory approach

NARCIS (Netherlands)

Novoderezhkin, V.; Salverda, J.M.; Amerongen, van H.; Grondelle, van R.

2003-01-01

We propose an exciton model for the peripheral plant light-harvesting complex LHCII that allows us to explain the absorption (OD) and linear dichroism (LD) spectra, the superradiance (SR), the pump-probe transient absorption (TA), the three-pulse photon echo peak shift (3PEPS), and transient grating

Exciton modeling of energy-transfer dynamics in the LHCII complex of higher plants: A redfield theory approach

NARCIS (Netherlands)

Novoderezhkin, V.; Salverda, J.M.; van Amerongen, H.; van Grondelle, R.

2003-01-01

We propose an exciton model for the peripheral plant light-harvesting complex LHCII that allows us to explain the absorption (OD) and linear dichroism (LD) spectra, the superradiance (SR), the pump-probe transient absorption (TA), the three-pulse photon echo peak shift (3PEPS), and transient grating

Identification of excitons, trions and biexcitons in single-layer WS{sub 2}

Energy Technology Data Exchange (ETDEWEB)

Plechinger, Gerd; Nagler, Philipp; Kraus, Julia; Paradiso, Nicola; Strunk, Christoph; Schueller, Christian; Korn, Tobias [Institut fuer Experimentelle und Angewandte Physik, Universitaet Regensburg, 93040, Regensburg (Germany)

2015-08-15

Single-layer WS{sub 2} is a direct-gap semiconductor showing strong excitonic photoluminescence features in the visible spectral range. Here, we present temperature-dependent photoluminescence measurements on mechanically exfoliated single-layer WS{sub 2}, revealing the existence of neutral and charged excitons at low temperatures as well as at room temperature. By applying a gate voltage, we can electrically control the ratio of excitons and trions and assert a residual n-type doping of our samples. At high excitation densities and low temperatures, an additional peak at energies below the trion dominates the photoluminescence, which we identify as biexciton emission. (copyright 2015 WILEY-VCH Verlag GmbH and Co. KGaA, Weinheim)

Spin-exciton interaction and related micro-photoluminescence spectra of ZnSe:Mn DMS nanoribbon.

Science.gov (United States)

Hou, Lipeng; Zhou, Weichang; Zou, Bingsuo; Zhang, Yu; Han, Junbo; Yang, Xinxin; Gong, Zhihong; Li, Jingbo; Xie, Sishen; Shi, Li-Jie

2017-03-10

For their spintronic applications the magnetic and optical properties of diluted magnetic semiconductors (DMS) have been studied widely. However, the exact relationships between the magnetic interactions and optical emission behaviors in DMS are not well understood yet due to their complicated microstructural and compositional characters from different growth and preparation techniques. Manganese (Mn) doped ZnSe nanoribbons with high quality were obtained by using the chemical vapor deposition (CVD) method. Successful Mn ion doping in a single ZnSe nanoribbon was identified by elemental energy-dispersive x-ray spectroscopy mapping and micro-photoluminescence (PL) mapping of intrinsic d-d optical transition at 580 nm, i.e. the transition of 4 T 1 ( 4 G) →  6 A 1 ( 6 s),. Besides the d-d transition PL peak at 580 nm, two other PL peaks related to Mn ion aggregates in the ZnSe lattice were detected at 664 nm and 530 nm, which were assigned to the d-d transitions from the Mn 2+ -Mn 2+ pairs with ferromagnetic (FM) coupling and antiferromagnetic (AFM) coupling, respectively. Moreover, AFM pair formation goes along with strong coupling with acoustic phonon or structural defects. These arguments were supported by temperature-dependent PL spectra, power-dependent PL lifetimes, and first-principle calculations. Due to the ferromagnetic pair existence, an exciton magnetic polaron (EMP) is formed and emits at 460 nm. Defect existence favors the AFM pair, which also can account for its giant enhancement of spin-orbital coupling and the spin Hall effect observed in PRL 97, 126603(2006) and PRL 96, 196404(2006). These emission results of DMS reflect their relation to local sp-d hybridization, spin-spin magnetic coupling, exciton-spin or phonon interactions covering structural relaxations. This kind of material can be used to study the exciton-spin interaction and may find applications in spin-related photonic devices besides spintronics.

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

Structural tunability and switchable exciton emission in inorganic-organic hybrids with mixed halides

International Nuclear Information System (INIS)

Ahmad, Shahab; Vijaya Prakash, G.; Baumberg, Jeremy J.

2013-01-01

Room-temperature tunable excitonic photoluminescence is demonstrated in alloy-tuned layered Inorganic-Organic (IO) hybrids, (C 12 H 25 NH 3 ) 2 PbI 4(1−y) Br 4y (y = 0 to 1). These perovskite IO hybrids adopt structures with alternating stacks of low-dimensional inorganic and organic layers, considered to be naturally self-assembled multiple quantum wells. These systems resemble stacked monolayer 2D semiconductors since no interlayer coupling exists. Thin films of IO hybrids exhibit sharp and strong photoluminescence (PL) at room-temperature due to stable excitons formed within the low-dimensional inorganic layers. Systematic variation in the observed exciton PL from 510 nm to 350 nm as the alloy composition is changed, is attributed to the structural readjustment of crystal packing upon increase of the Br content in the Pb-I inorganic network. The energy separation between exciton absorption and PL is attributed to the modified exciton density of states and diffusion of excitons from relatively higher energy states corresponding to bromine rich sites towards the lower energy iodine sites. Apart from compositional fluctuations, these excitons show remarkable reversible flips at temperature-induced phase transitions. All the results are successfully correlated with thermal and structural studies. Such structural engineering flexibility in these hybrids allows selective tuning of desirable exciton properties within suitable operating temperature ranges. Such wide-range PL tunability and reversible exciton switching in these novel IO hybrids paves the way to potential applications in new generation of optoelectronic devices

Theory of few photon dynamics in light emitting quantum dot devices

Science.gov (United States)

Carmele, Alexander; Richter, Marten; Sitek, Anna; Knorr, Andreas

2009-10-01

We present a modified cluster expansion to describe single-photon emitters in a semiconductor environment. We calculate microscopically to what extent semiconductor features in quantum dot-wetting layer systems alter the exciton and photon dynamics in comparison to the atom-like emission dynamics. We access these systems by the photon-probability-cluster-expansion: a reliable approach for few photon dynamics in many body electron systems. As a first application, we show that the amplitude of vacuum Rabi flops determines the number of electrons in the quantum dot.

Excitonic Behavior of Rhodamine Dimers: A Single-Molecule Study

NARCIS (Netherlands)

Hernando Campos, J.; van der Schaaf, Martijn; van Dijk, E.M.H.P.; Sauer, Markus; Garcia Parajo, M.F.; van Hulst, N.F.

2003-01-01

The optical behavior of a dimer of tetramethylrhodamine-5-isothiocyanate has been investigated by means of single-molecule measurements. Bulk absorption and fluorescence spectra show the existence of two populations of the dimer molecule that exhibit distinct excitonic interactions (strong and weak

Atomistic tight-binding theory of excitonic splitting energies in CdX(X = Se, S and Te)/ZnS core/shell nanocrystals

Science.gov (United States)

Sukkabot, Worasak; Pinsook, Udomsilp

2017-01-01

Using the atomistic tight-binding theory (TB) and a configuration interaction description (CI), we numerically compute the excitonic splitting of CdX(X = Se, S and Te)/ZnS core/shell nanocrystals with the objective to explain how types of the core materials and growth shell thickness can provide the detailed manipulation of the dark-dark (DD), dark-bright (DB) and bright-bright (BB) excitonic splitting, beneficial for the active application of quantum information. To analyze the splitting of the excitonic states, the optical band gaps, ground-state wave function overlaps and atomistic electron-hole interactions tend to be numerically demonstrated. Based on the atomistic computations, the single-particle and excitonic gaps are mainly reduced with the increasing ZnS shell thickness owing to the quantum confinement. In the range of the higher to lower energies, the order of the single-particle gaps is CdSe/ZnS, CdS/ZnS and CdTe/ZnS core/shell nanocrystals, while one of the excitonic gaps is CdS/ZnS, CdSe/ZnS and CdTe/ZnS core/shell nanocrystals because of the atomistic electron-hole interaction. The strongest electron-hole interactions are mainly observed in CdSe/ZnS core/shell nanocrystals. In addition, the computational results underline that the energies of the dark-dark (DD), dark-bright (DB) and bright-bright (BB) excitonic splitting are generally reduced with the increasing ZnS growth shell thickness as described by the trend of the electron-hole exchange interaction. The high-to-low splitting of the excitonic states is demonstrated in CdSe/ZnS, CdTe/ZnS and CdS/ZnS core/shell nanocrystals because of the fashion in the electron-hole exchange interaction and overlaps of the electron-hole wave functions. As the resulting calculations, it is expected that CdS/ZnS core/shell nanocrystals are the best candidates to be the source of entangled photons. Finally, the comprehensive information on the excitonic splitting can enable the use of suitable core

Giant nonlinear interaction between two optical beams via a quantum dot embedded in a photonic wire

Science.gov (United States)

Nguyen, H. A.; Grange, T.; Reznychenko, B.; Yeo, I.; de Assis, P.-L.; Tumanov, D.; Fratini, F.; Malik, N. S.; Dupuy, E.; Gregersen, N.; Auffèves, A.; Gérard, J.-M.; Claudon, J.; Poizat, J.-Ph.

2018-05-01

Optical nonlinearities usually appear for large intensities, but discrete transitions allow for giant nonlinearities operating at the single-photon level. This has been demonstrated in the last decade for a single optical mode with cold atomic gases, or single two-level systems coupled to light via a tailored photonic environment. Here, we demonstrate a two-mode giant nonlinearity with a single semiconductor quantum dot (QD) embedded in a photonic wire antenna. We exploit two detuned optical transitions associated with the exciton-biexciton QD level scheme. Owing to the broadband waveguide antenna, the two transitions are efficiently interfaced with two free-space laser beams. The reflection of one laser beam is then controlled by the other beam, with a threshold power as low as 10 photons per exciton lifetime (1.6 nW ). Such a two-color nonlinearity opens appealing perspectives for the realization of ultralow-power logical gates and optical quantum gates, and could also be implemented in an integrated photonic circuit based on planar waveguides.

Molecular plasmonics: The role of rovibrational molecular states in exciton-plasmon materials under strong-coupling conditions

Science.gov (United States)

Sukharev, Maxim; Charron, Eric

2017-03-01

We extend the model of exciton-plasmon materials to include a rovibrational structure of molecules using wave-packet propagations on electronic potential energy surfaces. Our model replaces conventional two-level emitters with more complex molecules, allowing us to examine the influence of alignment and vibrational dynamics on strong coupling with surface plasmon-polaritons. We apply the model to a hybrid system comprising a thin layer of molecules placed on top of a periodic array of slits. Rigorous simulations are performed for two types of molecular systems described by vibrational bound-bound and bound-continuum electronic transitions. Calculations reveal new features in transmission, reflection, and absorption spectra, including the observation of significantly higher values of the Rabi splitting and vibrational patterns clearly seen in the corresponding spectra. We also examine the influence of anisotropic initial conditions on optical properties of hybrid materials, demonstrating that the optical response of the system is significantly affected by an initial prealignment of the molecules. Our work demonstrates that prealigned molecules could serve as an efficient probe for the subdiffraction characterization of the near-field near metal interfaces.

The Cascade-Exciton Approach to Nuclear Reactions. (Foundation and Achievements)

International Nuclear Information System (INIS)

Mashnik, S.G.

1994-01-01

The relativistic kinetic equations describing nuclear reactions at intermediate energies are obtained on the dynamical basis. These equations are analyzed and realized in several versions of the Cascade Exciton Model (CEM). The CEM assumes that reactions occur in three stages: the intranuclear cascade, pre-equilibrium and the evaporative ones. A large variety of experimental data on hadron- and photonuclear reactions in the bombarding energy range up to several GeV are analyzed in this approach. The contributions of different pion and photon absorption mechanisms and the relative role of different particle and photon production mechanisms in these reactions are estimated. The CEM describes adequately nuclear reactions at intermediate energies and has one of the best predictive powers as compared to other available modern models. 55 refs., 10 figs., 1 tab

Exciton emissions in alkali cyanides

International Nuclear Information System (INIS)

Weid, J.P. von der.

1979-10-01

The emissions of Alkali Cyanides X irradiated at low temperature were measured. In addition to the molecular (Frenkel Type) exciton emissions, another emitting centre was found and tentatively assigned to a charge transfer self trapped exciton. The nature of the molecular exciton emitting state is discussed. (Author) [pt

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

Light-trapping for room temperature Bose-Einstein condensation in InGaAs quantum wells.

Science.gov (United States)

Vasudev, Pranai; Jiang, Jian-Hua; John, Sajeev

2016-06-27

We demonstrate the possibility of room-temperature, thermal equilibrium Bose-Einstein condensation (BEC) of exciton-polaritons in a multiple quantum well (QW) system composed of InGaAs quantum wells surrounded by InP barriers, allowing for the emission of light near telecommunication wavelengths. The QWs are embedded in a cavity consisting of double slanted pore (SP2) photonic crystals composed of InP. We consider exciton-polaritons that result from the strong coupling between the multiple quantum well excitons and photons in the lowest planar guided mode within the photonic band gap (PBG) of the photonic crystal cavity. The collective coupling of three QWs results in a vacuum Rabi splitting of 3% of the bare exciton recombination energy. Due to the full three-dimensional PBG exhibited by the SP2 photonic crystal (16% gap to mid-gap frequency ratio), the radiative decay of polaritons is eliminated in all directions. Due to the short exciton-phonon scattering time in InGaAs quantum wells of 0.5 ps and the exciton non-radiative decay time of 200 ps at room temperature, polaritons can achieve thermal equilibrium with the host lattice to form an equilibrium BEC. Using a SP2 photonic crystal with a lattice constant of a = 516 nm, a unit cell height of 2a=730nm and a pore radius of 0.305a = 157 nm, light in the lowest planar guided mode is strongly localized in the central slab layer. The central slab layer consists of 3 nm InGaAs quantum wells with 7 nm InP barriers, in which excitons have a recombination energy of 0.944 eV, a binding energy of 7 meV and a Bohr radius of aB = 10 nm. We take the exciton recombination energy to be detuned 35 meV above the lowest guided photonic mode so that an exciton-polariton has a photonic fraction of approximately 97% per QW. This increases the energy range of small-effective-mass photonlike states and increases the critical temperature for the onset of a Bose-Einstein condensate. With three quantum wells in the central slab layer

Visualising Berry phase and diabolical points in a quantum exciton-polariton billiard.

Science.gov (United States)

Estrecho, E; Gao, T; Brodbeck, S; Kamp, M; Schneider, C; Höfling, S; Truscott, A G; Ostrovskaya, E A

2016-11-25

Diabolical points (spectral degeneracies) can naturally occur in spectra of two-dimensional quantum systems and classical wave resonators due to simple symmetries. Geometric Berry phase is associated with these spectral degeneracies. Here, we demonstrate a diabolical point and the corresponding Berry phase in the spectrum of hybrid light-matter quasiparticles-exciton-polaritons in semiconductor microcavities. It is well known that sufficiently strong optical pumping can drive exciton-polaritons to quantum degeneracy, whereby they form a macroscopically populated quantum coherent state similar to a Bose-Einstein condensate. By pumping a microcavity with a spatially structured light beam, we create a two-dimensional quantum billiard for the exciton-polariton condensate and demonstrate a diabolical point in the spectrum of the billiard eigenstates. The fully reconfigurable geometry of the potential walls controlled by the optical pump enables a striking experimental visualization of the Berry phase associated with the diabolical point. The Berry phase is observed and measured by direct imaging of the macroscopic exciton-polariton probability densities.

PCBM : P3HT polymer composites for photonic crystal all-optical switching applications

International Nuclear Information System (INIS)

Li Zhiqiang; Hu Xiaoyong; Zhang Jiaxiang; Yang Hong; Gong Qihuang

2010-01-01

An all-optical switching with an operating pump intensity of 1 MW cm -2 is realized in a one-dimensional nonlinear organic photonic crystal made of poly(3-hexylthiophene) doped with 1-(3-methoxycarbonyl)propyl-1-phenyl-(6,6)C 61 , fabricated by focused ion-beam etching. The femtosecond pump and probe method is adopted to measure the transmittance changes of the probe laser based on the photonic bandgap shift induced by the pump laser. Under resonant excitation, a large nonlinear refractive index of the order of 10 -9 cm 2 W -1 is obtained for the polymer composite. A switching time of 58.9 ps is maintained due to intermolecular charge transfer and exciton-exciton annihilation.

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.

Strongly nonexponential time-resolved fluorescence of quantum-dot ensembles in three-dimensional photonic crystals

DEFF Research Database (Denmark)

Nikolaev, Ivan S.; Lodahl, Peter; van Driel, A. Floris

2007-01-01

We observe experimentally that ensembles of quantum dots in three-dimensional 3D photonic crystals reveal strongly nonexponential time-resolved emission. These complex emission decay curves are analyzed with a continuous distribution of decay rates. The log-normal distribution describes the decays...... parameter. This interpretation qualitatively agrees with the calculations of the 3D projected local density of states. We therefore conclude that fluorescence decay of ensembles of quantum dots is highly nonexponential to an extent that is controlled by photonic crystals....

Relativistic quantum dynamics in strong fields: Photon emission from heavy, few-electron ions

International Nuclear Information System (INIS)

Fritzsche, S.; Stoehlker, T.

2005-03-01

Recent progress in the study of the photon emission from highly-charged heavy ions is reviewed. These investigations show that high-Z ions provide a unique tool for improving the understanding of the electron-electron and electron-photon interaction in the presence of strong fields. Apart from the bound-state transitions, which are accurately described in the framework of quantum electrodynamics, much information has been obtained also from the radiative capture of (quasi-) free electrons by high-Z ions. Many features in the observed spectra hereby confirm the inherently relativistic behavior of even the simplest compound quantum systems in nature. (orig.)

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.

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.

Coherence properties of exciton polariton OPO condensates in one and two dimensions

International Nuclear Information System (INIS)

Spano, R; Cuadra, J; Tosi, G; Antón, C; Lingg, C A; Sanvitto, D; Martín, M D; Viña, L; Eastham, P R; Van der Poel, M; Hvam, J M

2012-01-01

We give an overview of the coherence properties of exciton-polariton condensates generated by optical parametric scattering. Different aspects of the first-order coherence (g (1) ) have been investigated. The spatial coherence extension of a two-dimensional (2D) polariton system, below and at the parametric threshold, demonstrates the development of a constant phase coherence over the entire condensate, once the condensate phase transition takes place. The effect on coherence of the photonic versus excitonic nature of the condensates is also examined. The coherence of a quasi-1D trap, composed of a line defect, is studied, showing the detrimental effect of reduced dimensionality on the establishment of the long range order. In addition, the temporal coherence decay, g (1) (τ), reveals a fast decay in contrast with the 2D case. The situation of a quasi-1D condensate coexisting with a 2D one is also presented. (paper)

Giant nonlinear interaction between two optical beams via a quantum dot embedded in a photonic wire

DEFF Research Database (Denmark)

Nguyen, H.A.; Grange, T.; Reznychenko, B.

2018-01-01

a tailored photonic environment. Here, we demonstrate a two-mode giant nonlinearity with a single semiconductor quantum dot (QD) embedded in a photonic wire antenna. We exploit two detuned optical transitions associated with the exciton-biexciton QD level scheme. Owing to the broadband waveguide antenna...

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.

Bose-Einstein condensation and indirect excitons: a review.

Science.gov (United States)

Combescot, Monique; Combescot, Roland; Dubin, François

2017-06-01

We review recent progress on Bose-Einstein condensation (BEC) of semiconductor excitons. The first part deals with theory, the second part with experiments. This Review is written at a time where the problem of exciton Bose-Einstein condensation has just been revived by the understanding that the exciton condensate must be dark because the exciton ground state is not coupled to light. Here, we theoretically discuss this missed understanding before providing its experimental support through experiments that scrutinize indirect excitons made of spatially separated electrons and holes. The theoretical part first discusses condensation of elementary bosons. In particular, the necessary inhibition of condensate fragmentation by exchange interaction is stressed, before extending the discussion to interacting bosons with spin degrees of freedom. The theoretical part then considers composite bosons made of two fermions like semiconductor excitons. The spin structure of the excitons is detailed, with emphasis on the crucial fact that ground-state excitons are dark: indeed, this imposes the exciton Bose-Einstein condensate to be not coupled to light in the dilute regime. Condensate fragmentations are then reconsidered. In particular, it is shown that while at low density, the exciton condensate is fully dark, it acquires a bright component, coherent with the dark one, beyond a density threshold: in this regime, the exciton condensate is 'gray'. The experimental part first discusses optical creation of indirect excitons in quantum wells, and the detection of their photoluminescence. Exciton thermalisation is also addressed, as well as available approaches to estimate the exciton density. We then switch to specific experiments where indirect excitons form a macroscopic fragmented ring. We show that such ring provides efficient electrostatic trapping in the region of the fragments where an essentially-dark exciton Bose-Einstein condensate is formed at sub-Kelvin bath

PCBM : P3HT polymer composites for photonic crystal all-optical switching applications

Energy Technology Data Exchange (ETDEWEB)

Li Zhiqiang; Hu Xiaoyong; Zhang Jiaxiang; Yang Hong; Gong Qihuang, E-mail: xiaoyonghu@pku.edu.c, E-mail: qhgong@pku.edu.c [State Key Laboratory for Mesoscopic Physics and Department of Physics, Peking University, Beijing 100871 (China)

2010-09-29

An all-optical switching with an operating pump intensity of 1 MW cm{sup -2} is realized in a one-dimensional nonlinear organic photonic crystal made of poly(3-hexylthiophene) doped with 1-(3-methoxycarbonyl)propyl-1-phenyl-(6,6)C{sub 61}, fabricated by focused ion-beam etching. The femtosecond pump and probe method is adopted to measure the transmittance changes of the probe laser based on the photonic bandgap shift induced by the pump laser. Under resonant excitation, a large nonlinear refractive index of the order of 10{sup -9} cm{sup 2} W{sup -1} is obtained for the polymer composite. A switching time of 58.9 ps is maintained due to intermolecular charge transfer and exciton-exciton annihilation.

Fluctuations of tunneling currents in photonic and polaritonic systems

Science.gov (United States)

Mantsevich, V. N.; Glazov, M. M.

2018-04-01

Here we develop the nonequilibrium Green's function formalism to analyze the fluctuation spectra of the boson tunneling currents. The approach allows us to calculate the noise spectra in both equilibrium and nonequilibrium conditions. The proposed general formalism is applied to several important realizations of boson transport, including the tunneling transport between two reservoirs and the case where the boson current flows through the intermediate region between the reservoirs. Developed theory can be applied for the analysis of the current noise in waveguides, coupled optical resonators, quantum microcavities, etc., where the tunneling of photons, exciton-polaritons, or excitons can be realized.

Triplet exciton dynamics

International Nuclear Information System (INIS)

Strien, A.J. van.

1981-01-01

Results are presented of electron spin echo experiments combined with laser flash excitation on triplet states of aromatic molecules. Some of the theoretical and experimental aspects of the photoexcited triplet state are discussed in detail and the electron spin echo spectrometers and laser systems are described. All the experiments described in this thesis were performed at liquid helium temperatures. An account is given of the ESE experiments performed on the photoexcited, non-radiative, triplet state of pentacene in napthalene. This is an example of the ESE technique being used to ascertain the zero-field splitting parameters, the populating and depopulating rates, and the orientation of the pentacene molecules in the naphthalene host. A combination of high resolution laser flash excitation and electron-spin echoes in zero-magnetic field allowed the author to observe directly k(vector)→k(vector)' exciton scattering processes in the one-dimensional triplet excitons in tetrachlorobenzene for the first time. Additional experimental data about exciton scattering is provided and a study of the orientational dependence of the spin-lattice relaxation of the triplet excitons in an external magnetic field is described. (Auth.)

Geometrical-confinement effects on excitons in quantum disks

International Nuclear Information System (INIS)

Song, J.; Ulloa, S.E.

1995-01-01

Excitons confined to flat semiconductor quantum dots with elliptical cross sections are considered as we study geometrical effects on exciton binding energy, electron-hole separation, and the resulting linear optical properties. We use numerical matrix diagonalization techniques with appropriately large and optimized basis sets in an effective-mass Hamiltonian approach. The linear optical susceptibilities of GaAs and InAs dots for several different size ratios are discussed and compared to experimental photoluminescence spectra obtained on GaAs/Al x Ga 1-x As and InAs/GaAs quantum dots. For quantum dots of several nm in size, there is a strong blueshift of the luminescence due to geometrical-confinement effects. Also, transition peaks are split and shifted towards higher energy, in comparison with dots with circular cross sections

Exciton and biexciton signatures in femtosecond transient absorption of π-conjugated oligomers

Science.gov (United States)

Klimov, Victor I.; McBranch, Duncan W.; Barashkov, Nikolay N.; Ferraris, John P.

1997-12-01

We report femtosecond transient-absorption studies of a five-ring oligomer of polyphenylenevinylene prepared in two different forms: as solid-state films and dilute solutions. Both types of samples exhibit a photoinduced absorption (PA) band with dynamics which closely match those of the stimulated emission (SE), demonstrating unambiguously that these features originate from the same species, namely from intrachain singlet excitons. Photochemical degradation of the solid-state samples is demonstrated to dramatically shorten the SE dynamics above a moderate incident pump fluence, whereupon the dynamics of the SE and the long- wavelength PA no longer coincide. In contrast to solutions, solid-state films exhibit an additional short-wavelength PA band with pump-independent dynamics, indicating the efficient formation of non-emissive inter-chain excitons. Correlations in the subpicosecond dynamics of the two PA features, as well as the pump intensity-dependence provide strong evidence that the formation of inter-chain excitons is mediated by intrachain two-exciton states. At high pump levels, we see a clear indication of interaction between excited states also in dilute solutions. This is manifested as a superlinear pump-dependence and shortening of the decay dynamics of the SE. We attribute this behavior to the formation of biexcitons resulting from coherent interaction between two excitons on a single chain.

Rotational symmetry breaking and topological phase transition in the exciton-polariton condensate of gapped 2D Dirac material

Science.gov (United States)

Lee, Ki Hoon; Lee, Changhee; Jeong, Jae-Seung; Min, Hongki; Chung, Suk Bum

For the quantum well in an optical microcavity, the interplay of the Coulomb interaction and the electron-photon coupling can lead to the emergence of bosonic quasiparticles consisting of the exciton and the cavity photon known as polariton, which can form the Bose-Einstein condensate above a threshold density. Additional physics due to the nontrivial Berry phase comes into play when the quantum well consists of the gapped Dirac material such as the transition metal dichalcogenide (TMD) MoS2 or WTe2. Specifically, in forming excitons, the electron-photon coupling from the optical selection rule due to the Berry phase competes against, rather than cooperates with, the Coulomb interaction. We find that this competition gives rise to the spontaneous breaking of the rotational symmetry in the polariton condensate and also drives topological phase transition, both novel features in polariton condensation. We also investigate the possible detection of this competition through photoluminescence. This work was supported in part by the Institute for Basic Science of Korea (IBS) under Grant IBS-R009-Y1 and by the National Research Foundation of Korea (NRF) under the Basic Science Research Program Grant No. 2015R1D1A1A01058071.

Photon-photon interactions

International Nuclear Information System (INIS)

Gilman, F.J.

1980-01-01

A brief summary of the present status of photon-photon interactions is presented. Stress is placed on the use of two-photon collisions to test present ideas on the quark constituents of hadrons and on the theory of strong interactions

Theoretical study of excitonic complexes in semiconductors quantum wells

International Nuclear Information System (INIS)

Dacal, Luis Carlos Ogando

2001-08-01

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

Real-Time Observation of Ultrafast Intraband Relaxation and Exciton Multiplication in PbS Quantum Dots

KAUST Repository

El-Ballouli, Ala’a O.

2014-03-19

We examine ultrafast intraconduction band relaxation and multiple-exciton generation (MEG) in PbS quantum dots (QDs) using transient absorption spectroscopy with 120 fs temporal resolution. The intraconduction band relaxation can be directly and excellently resolved spectrally and temporally by applying broadband pump-probe spectroscopy to excite and detect the wavelengths around the exciton absorption peak, which is located in the near-infrared region. The time-resolved data unambiguously demonstrate that the intraband relaxation time progressively increases as the pump-photon energy increases. Moreover, the relaxation time becomes much shorter as the size of the QDs decreases, indicating the crucial role of spatial confinement in the intraband relaxation process. Additionally, our results reveal the systematic scaling of the intraband relaxation time with both excess energy above the effective energy band gap and QD size. We also assess MEG in different sizes of the QDs. Under the condition of high-energy photon excitation, which is well above the MEG energy threshold, ultrafast bleach recovery due to the nonradiative Auger recombination of the multiple electron-hole pairs provides conclusive experimental evidence for the presence of MEG. For instance, we achieved quantum efficiencies of 159, 129 and 106% per single-absorbed photon at pump photoexcition of three times the band gap for QDs with band gaps of 880 nm (1.41 eV), 1000 nm (1.24 eV) and 1210 nm (1.0 eV), respectively. These findings demonstrate clearly that the efficiency of transferring excess photon energy to carrier multiplication is significantly increased in smaller QDs compared with larger ones. Finally, we discuss the Auger recombination dynamics of the multiple electron-hole pairs as a function of QD size.

Effects of multi-photon interferences from internally generated fields in strongly resonant systems

International Nuclear Information System (INIS)

Deng, Lu; Payne, Marvin G.; Garrett, William R.

2006-01-01

In studies of various nonlinear optical phenomena, strong resonant features in the atomic or molecular response to multi-photon driven processes have been used to greatly enhance the visibility of otherwise weak higher-order processes. However, there are well defined circumstances where a multi-photon-resonant response of a target system leads to the generation of one or more new electromagnetic fields that can drastically change the overall system response from what would be expected from the imposed laser fields alone. New effects can occur and dominate some aspects of the nonlinear optical response because of the constructive or destructive interference between transition amplitudes along multiple excitation pathways between a given set of optically coupled states, where one of the pathways involve internally generated field(s). Under destructive interference some resonant enhancements can become completely canceled (suppressed). This review focuses on the class of optical interference effects associated with internally generated fields, that have been found to be capable of influencing a very significant number of basic physical phenomena in gas or vapor phase systems. It provides a historical overview of experimental and theoretical developments and a modern understanding of the underlying physics and its various manifestations that include: suppression of multi-photon excitation processes, suppression of stimulated emissions (Raman, hyper-Raman, and optically pumped stimulated emissions), saturation of parametric wave-mixing, pressure and beam-geometry dependent shifting of multi-photon-resonant absorption lines, and the suppression of Autler-Townes splitting and ac-stark shifts. Additionally, optical interference effects in some modern contexts, such as achieving multi-photon induced transparency, establishing single-photon self-interference based induced transparency, and generating entangled single photon states, are reviewed

Visualization of Excitonic Structure in the Fenna-Matthews-Olson Photosynthetic Complex by Polarization-Dependent Two-Dimensional Electronic Spectroscopy

International Nuclear Information System (INIS)

Fleming, Graham; Read, Elizabeth L.; Schlau-Cohen, Gabriela S.; Engel, Gregory S.; Wen, Jianzhong; Blankenship, Robert E.; Fleming, Graham R.

2008-01-01

Photosynthetic light-harvesting proceeds by the collection and highly efficient transfer of energy through a network of pigment-protein complexes. Inter-chromophore electronic couplings and interactions between pigments and the surrounding protein determine energy levels of excitonic states and dictate the mechanism of energy flow. The excitonic structure (orientation of excitonic transition dipoles) of pigment-protein complexes is generally deduced indirectly from x-ray crystallography in combination with predictions of transition energies and couplings in the chromophore site basis. Here, we demonstrate that coarse-grained excitonic structural information in the form of projection angles between transition dipole moments can be obtained from polarization-dependent two-dimensional electronic spectroscopy of an isotropic sample, particularly when the nonrephasing or free polarization decay signal rather than the photon echo signal is considered. The method provides an experimental link between atomic and electronic structure and accesses dynamical information with femtosecond time resolution. In an investigation of the Fenna-Matthews-Olson complex from green sulfur bacteria, energy transfer connecting two particular exciton states in the protein is isolated as being the primary contributor to a cross peak in the nonrephasing 2D spectrum at 400 fs under a specific sequence of polarized excitation pulses. The results suggest the possibility of designing experiments using combinations of tailored polarization sequences to separate and monitor individual relaxation pathways

Generalized bipolariton model. propagation of a ultrashort laser pulse through a thin semiconductor film in the conditions of two-photon generation of biexcitons

International Nuclear Information System (INIS)

Igor Beloussov

2013-01-01

A generalized bipolariton model is proposed. Bipolaritons is formed from virtual excitons of four kinds. There exists both attractive and repulsive interaction between these excitons, though only excitons of a specific type can interact with light. A substantial difference between conventional and our models is shown for the case of nonlinear transmission/reflection of ultrashort laser pulses by a thin semiconductor film under two-photon generation of biexcitons. (author)

Band-Edge Exciton Fine Structure and Recombination Dynamics in InP/ZnS Colloidal Nanocrystals.

Science.gov (United States)

Biadala, Louis; Siebers, Benjamin; Beyazit, Yasin; Tessier, Mickaël D; Dupont, Dorian; Hens, Zeger; Yakovlev, Dmitri R; Bayer, Manfred

2016-03-22

We report on a temperature-, time-, and spectrally resolved study of the photoluminescence of type-I InP/ZnS colloidal nanocrystals with varying core size. By studying the exciton recombination dynamics we assess the exciton fine structure in these systems. In addition to the typical bright-dark doublet, the photoluminescence stems from an upper bright state in spite of its large energy splitting (∼100 meV). This striking observation results from dramatically lengthened thermalization processes among the fine structure levels and points to optical-phonon bottleneck effects in InP/ZnS nanocrystals. Furthermore, our data show that the radiative recombination of the dark exciton scales linearly with the bright-dark energy splitting for CdSe and InP nanocrystals. This finding strongly suggests a universal dangling bonds-assisted recombination of the dark exciton in colloidal nanostructures.

Excitons in the rare gas solids

International Nuclear Information System (INIS)

1988-01-01

Excitons play a prominent role in the chemistry and physics of condensed matter. Excitons in the rare gas solids, the prototypical van der Waals insulators, will be the focus of the remainder of this report. The goal here is to investigate the controversies surrounding the description of excitons in insulators and, therefore the simplest class of these solids, namely the rare gas solids, is chosen as the exemplary system. Specific problems associated with molecular crystals are, therefore, avoided and only the salient features of excitons are thus considered. 47 refs., 9 figs., 4 tabs

Electron-photon and electron-electron interactions in the presence of strong electromagnetic fields

International Nuclear Information System (INIS)

Surzhykov, A.; Fritzsche, S.; Stoehlker, Th.

2010-01-01

During the last decade, photon emission from highly-charged, heavy ions has been in the focus of intense studies at the GSI accelerator and storage ring facility in Darmstadt. These studies have revealed unique information about the electron-electron and electron-photon interactions in the presence of extremely strong nuclear fields. Apart from the radiative electron capture processes, characteristic photon emission following collisional excitation of projectile ions has also attracted much interest. In this contribution, we summarize the recent theoretical studies on the production of excited ionic states and their subsequent radiative decay. We will pay special attention to the angular and polarization properties of Kα emission from helium-like ions produced by means of dielectronic recombination. The results obtained for this (resonant) capture process will be compared with the theoretical predictions for the characteristic X-rays following Coulomb excitation and radiative recombination of few-electron, heavy ions. Work is supported by Helmholtz Association and GSl under the project VH-NG--421. (author)

Dynamics in terahertz semiconductor microcavity: quantum noise spectra

Science.gov (United States)

Jabri, H.; Eleuch, H.

2018-05-01

We investigate the physics of an optical semiconductor microcavity containing a coupled double quantum well interacting with cavity photons. The photon statistics of the transmitted light by the cavity is explored. We show that the nonlinear interactions in the direct and indirect excitonic modes generate an important squeezing despite the weak nonlinearities. When the strong coupling regime is achieved, the noise spectra of the system is dominated by the indirect exciton distribution. At the opposite, in the weak regime, direct excitons contribute much larger in the noise spectra.

Photon and spin dependence of the resonance line shape in the strong coupling regime

NARCIS (Netherlands)

Miyashita, Seiji; Shirai, Tatsuhiko; Mori, Takashi; De Raedt, Hans; Bertaina, Sylvain; Chiorescu, Irinel

2012-01-01

We study the quantum dynamics of a spin ensemble coupled to cavity photons. Recently, related experimental results have been reported, showing the existence of the strong coupling regime in such systems. We study the eigenenergy distribution of the multi-spin system (following the Tavis-Cummings

Excitons

Energy Technology Data Exchange (ETDEWEB)

Kozhushner, M

1975-06-01

The theory of quasi particles is explained to layman readers and the significance of the discovery of excitons is pointed out. New possibilities of the study of electron-hole interactions and of superconductivity are indicated.

Probing exciton density of states through phonon-assisted emission in GaN epilayers: A and B exciton contributions

Science.gov (United States)

Cavigli, Lucia; Gabrieli, Riccardo; Gurioli, Massimo; Bogani, Franco; Feltin, Eric; Carlin, Jean-François; Butté, Raphaël; Grandjean, Nicolas; Vinattieri, Anna

2010-09-01

A detailed experimental investigation of the phonon-assisted emission in a high-quality c -plane GaN epilayer is presented up to 200 K. By performing photoluminescence and reflectivity measurements, we find important etaloning effects in the phonon-replica spectra, which have to be corrected before addressing the lineshape analysis. Direct experimental evidence for free exciton thermalization is found for the whole temperature range investigated. A close comparison with existing models for phonon replicas originating from a thermalized free exciton distribution shows that the simplified and commonly adopted description of the exciton-phonon interaction with a single excitonic band leads to a large discrepancy with experimental data. Only the consideration of the complex nature of the excitonic band in GaN, including A and B exciton contributions, allows accounting for the temperature dependence of the peak energy, intensity, and lineshape of the phonon replicas.

Dispersion anisotropy of plasmon-exciton-polaritons in lattices of metallic nanoparticles

NARCIS (Netherlands)

Ramezani, Mohammad; Halpin, Alexei; Feist, Johannes; Van Hoof, Niels; Fernández-Domínguez, Antonio I.; Garcia-Vidal, Francisco J.; Gómez Rivas, Jaime

2018-01-01

When the electromagnetic modes supported by plasmonic-based cavities interact strongly with molecules located within the cavity, new hybrid states known as plasmon-exciton-polaritons (PEPs) are formed. The properties of PEPs, such as group velocity, effective mass, and lifetime, depend on the

Spectral and Dynamical Properties of Single Excitons, Biexcitons, and Trions in Cesium-Lead-Halide Perovskite Quantum Dots.

Science.gov (United States)

Makarov, Nikolay S; Guo, Shaojun; Isaienko, Oleksandr; Liu, Wenyong; Robel, István; Klimov, Victor I

2016-04-13

Organic-inorganic lead-halide perovskites have been the subject of recent intense interest due to their unusually strong photovoltaic performance. A new addition to the perovskite family is all-inorganic Cs-Pb-halide perovskite nanocrystals, or quantum dots, fabricated via a moderate-temperature colloidal synthesis. While being only recently introduced to the research community, these nanomaterials have already shown promise for a range of applications from color-converting phosphors and light-emitting diodes to lasers, and even room-temperature single-photon sources. Knowledge of the optical properties of perovskite quantum dots still remains vastly incomplete. Here we apply various time-resolved spectroscopic techniques to conduct a comprehensive study of spectral and dynamical characteristics of single- and multiexciton states in CsPbX3 nanocrystals with X being either Br, I, or their mixture. Specifically, we measure exciton radiative lifetimes, absorption cross-sections, and derive the degeneracies of the band-edge electron and hole states. We also characterize the rates of intraband cooling and nonradiative Auger recombination and evaluate the strength of exciton-exciton coupling. The overall conclusion of this work is that spectroscopic properties of Cs-Pb-halide quantum dots are largely similar to those of quantum dots of more traditional semiconductors such as CdSe and PbSe. At the same time, we observe some distinctions including, for example, an appreciable effect of the halide identity on radiative lifetimes, considerably shorter biexciton Auger lifetimes, and apparent deviation of their size dependence from the "universal volume scaling" previously observed for many traditional nanocrystal systems. The high efficiency of Auger decay in perovskite quantum dots is detrimental to their prospective applications in light-emitting devices and lasers. This points toward the need for the development of approaches for effective suppression of Auger

Quantum-well exciton polariton emission from multi-quantum-well wire structures

Science.gov (United States)

Kohl, M.; Heitmann, D.; Grambow, P.; Ploog, K.

The radiative decay of quantum-well exciton (QWE) polaritons in microstructured Al0.3Ga0.7As - GaAs multi-quantum wells (MQW) has been studied by photoluminescence spectroscopy. Periodic wire structures with lateral periodicities a = 250-500 nm and lateral widths t = 100-200 nm have been fabricated by plasma etching. The thickness of the QWs was 13 nm. In the QW wire samples the free-exciton photoluminescence was strongly reduced and the QWE polariton emission was observed as a maximum peaked at a 3 meV higher energy than the free QWE transition. In samples which had only a microstructured cladding layer, the free-exciton photoluminescence was dominant in the spectrum and the QWE polariton emission was observed as a shoulder on the high-energy side of the free QWE transition. In addition, two transitions at the low energy side of the free QWE photoluminescence were present in the microstructured samples, which were related to etching induced states.

Excitonic pathway to photoinduced magnetism in colloidal nanocrystals with nonmagnetic dopants.

Science.gov (United States)

Pinchetti, Valerio; Di, Qiumei; Lorenzon, Monica; Camellini, Andrea; Fasoli, Mauro; Zavelani-Rossi, Margherita; Meinardi, Francesco; Zhang, Jiatao; Crooker, Scott A; Brovelli, Sergio

2018-02-01

Electronic doping of colloidal semiconductor nanostructures holds promise for future device concepts in optoelectronic and spin-based technologies. Ag + is an emerging electronic dopant in III-V and II-VI nanostructures, introducing intragap electronic states optically coupled to the host conduction band. With its full 4d shell Ag + is nonmagnetic, and the dopant-related luminescence is ascribed to decay of the conduction-band electron following transfer of the photoexcited hole to Ag + . This optical activation process and the associated modification of the electronic configuration of Ag + remain unclear. Here, we trace a comprehensive picture of the excitonic process in Ag-doped CdSe nanocrystals and demonstrate that, in contrast to expectations, capture of the photohole leads to conversion of Ag + to paramagnetic Ag 2+ . The process of exciton recombination is thus inextricably tied to photoinduced magnetism. Accordingly, we observe strong optically activated magnetism and diluted magnetic semiconductor behaviour, demonstrating that optically switchable magnetic nanomaterials can be obtained by exploiting excitonic processes involving nonmagnetic impurities.

Scaling laws of Rydberg excitons

Science.gov (United States)

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

2017-09-01

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

Exciton and biexciton signatures in femotosecond transient absorption of {pi}-conjugated oligomers

Energy Technology Data Exchange (ETDEWEB)

Klimov, V.; McBranch, D. [Los Alamos National Lab., NM (United States); Barashkov, N.; Ferraris, J. [Univ. of Texas, Dallas, TX (United States)

1997-10-01

The authors report femotosecond transient-absorption studies of a five-ring oligomer of polyphenylenevinylene (PPV) prepared in two different forms: as solid-state films and dilute solutions. Both types of samples exhibit a photoinduced absorption (PA) band with dynamics which closely match those of the stimulated emission (SE), demonstrating unambiguously that these features originate from the same species, namely from intrachain singlet excitons. Photo-chemical degradation of the solid-state samples is demonstrated to dramatically shorten the SE dynamics above a moderate incident pump fluence, whereupon the dynamics of the SE and the long-wavelength PA no longer coincide. In contrast to solutions, solid-state films exhibit an additional short-wavelength PA band with pump-independent dynamics, indicating the efficient formation of non-emissive inter-chain excitons. Correlations in the subpicosecond dynamics of the two PA features, as well as the pump intensity-dependence provide strong evidence that the formation of inter-chain excitons is mediated by intrachain two-exciton states. At high pump levels, the authors see a clear indication of interaction between excited states also in dilute solutions. This is manifested as a superlinear pump-dependence and shortening of the decay dynamics of the SE. They attribute this behavior to the formation of biexcitons resulting from coherent interaction between two excitons on a single chain.

Large photonic band gaps and strong attenuations of two-segment-connected Peano derivative networks

International Nuclear Information System (INIS)

Lu, Jian; Yang, Xiangbo; Zhang, Guogang; Cai, Lianzhang

2011-01-01

In this Letter, based on ancient Peano curves we construct four kinds of interesting Peano derivative networks composed of one-dimensional (1D) waveguides and investigate the optical transmission spectra and photonic attenuation behavior of electromagnetic (EM) waves in one- and two-segment-connected networks. It is found that for some two-segment-connected networks large photonic band gaps (PBGs) can be created and the widths of large PBGs can be controlled by adjusting the matching ratio of waveguide length and are insensitive to generation number. Diamond- and hexagon-Peano networks are good selectable structures for the designing of optical devices with large PBG(s) and strong attenuation(s). -- Highlights: → Peano and Peano derivative networks composed of 1D waveguides are designed. → Large PBGs with strong attenuations have been created by these fractal networks. → New approach for designing optical devices with large PBGs is proposed. → Diamond- and hexagon-Peano networks with d2:d1=2:1 are good selectable structures.

Strong photonic crystal behavior in regular arrays of core-shell and quantum disc InGaN/GaN nanorod light-emitting diodes

Energy Technology Data Exchange (ETDEWEB)

Lewins, C. J., E-mail: c.j.lewins@bath.ac.uk; Le Boulbar, E. D.; Lis, S. M.; Shields, P. A.; Allsopp, D. W. E., E-mail: d.allsopp@bath.ac.uk [Department of Electronic and Electrical Engineering, University of Bath, Claverton Down, Bath BA2 7AY (United Kingdom); Edwards, P. R.; Martin, R. W. [Department of Physics, SUPA, University of Strathclyde, Glasgow G4 0NG (United Kingdom)

2014-07-28

We show that arrays of emissive nanorod structures can exhibit strong photonic crystal behavior, via observations of the far-field luminescence from core-shell and quantum disc InGaN/GaN nanorods. The conditions needed for the formation of directional Bloch modes characteristic of strong photonic behavior are found to depend critically upon the vertical shape of the nanorod sidewalls. Index guiding by a region of lower volume-averaged refractive index near the base of the nanorods creates a quasi-suspended photonic crystal slab at the top of the nanorods which supports Bloch modes. Only diffractive behavior could be observed without this region. Slab waveguide modelling of the vertical structure shows that the behavioral regime of the emissive nanorod arrays depends strongly upon the optical coupling between the nanorod region and the planar layers below. The controlled crossover between the two regimes of photonic crystal operation enables the design of photonic nanorod structures formed on planar substrates that exploit either behavior depending on device requirements.

Excitons

International Nuclear Information System (INIS)

Kozhushner, M.

1975-01-01

The theory of quasi particles is explained to layman readers and the significance of the discovery of excitons is pointed out. New possibilities of the study of electron-hole interactions and of superconductivity are indicated. (L.O.)

Tunneling Photocurrent Assisted by Interlayer Excitons in Staggered van der Waals Hetero-Bilayers.

Science.gov (United States)

Luong, Dinh Hoa; Lee, Hyun Seok; Neupane, Guru Prakash; Roy, Shrawan; Ghimire, Ganesh; Lee, Jin Hee; Vu, Quoc An; Lee, Young Hee

2017-09-01

Vertically stacked van der Waals (vdW) heterostructures have been suggested as a robust platform for studying interfacial phenomena and related electric/optoelectronic devices. While the interlayer Coulomb interaction mediated by the vdW coupling has been extensively studied for carrier recombination processes in a diode transport, its correlation with the interlayer tunneling transport has not been elucidated. Here, a contrast is reported between tunneling and drift photocurrents tailored by the interlayer coupling strength in MoSe 2 /MoS 2 hetero-bilayers (HBs). The interfacial coupling modulated by thermal annealing is identified by the interlayer phonon coupling in Raman spectra and the emerging interlayer exciton peak in photoluminescence spectra. In strongly coupled HBs, positive photocurrents are observed owing to the inelastic band-to-band tunneling assisted by interlayer excitons that prevail over exciton recombinations. By contrast, weakly coupled HBs exhibit a negative photovoltaic diode behavior, manifested as a drift current without interlayer excitonic emissions. This study sheds light on tailoring the tunneling transport for numerous optoelectronic HB devices. © 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Role of many-body effects in the coherent dynamics of excitons in low-temperature-grown GaAs

Energy Technology Data Exchange (ETDEWEB)

Webber, D.; Hacquebard, L.; Hall, K. C. [Department of Physics and Atmospheric Science, Dalhousie University, Halifax, Nova Scotia B3H 4R2 (Canada); Liu, X.; Dobrowolska, M.; Furdyna, J. K. [Department of Physics, University of Notre Dame, Notre Dame, Indiana 46556 (United States)

2015-10-05

Femtosecond four-wave mixing experiments on low-temperature-grown (LT-) GaAs indicate a polarization-dependent nonlinear optical response at the exciton, which we attribute to Coulomb-mediated coupling between excitons and electron-hole pairs simultaneously excited by the broad-bandwidth laser pulses. Strong suppression of the exciton response through screening by carriers injected by a third pump pulse was observed, an effect that is transient due to rapid carrier trapping. Our findings highlight the need to account for the complex interplay of disorder and many-body effects in the design of ultrafast optoelectronic devices using this material.

Strong-coupling of WSe2 in ultra-compact plasmonic nanocavities at room temperature.

Science.gov (United States)

Kleemann, Marie-Elena; Chikkaraddy, Rohit; Alexeev, Evgeny M; Kos, Dean; Carnegie, Cloudy; Deacon, Will; de Pury, Alex Casalis; Große, Christoph; de Nijs, Bart; Mertens, Jan; Tartakovskii, Alexander I; Baumberg, Jeremy J

2017-11-03

Strong coupling of monolayer metal dichalcogenide semiconductors with light offers encouraging prospects for realistic exciton devices at room temperature. However, the nature of this coupling depends extremely sensitively on the optical confinement and the orientation of electronic dipoles and fields. Here, we show how plasmon strong coupling can be achieved in compact, robust, and easily assembled gold nano-gap resonators at room temperature. We prove that strong-coupling is impossible with monolayers due to the large exciton coherence size, but resolve clear anti-crossings for greater than 7 layer devices with Rabi splittings exceeding 135 meV. We show that such structures improve on prospects for nonlinear exciton functionalities by at least 10 4 , while retaining quantum efficiencies above 50%, and demonstrate evidence for superlinear light emission.

Elastic strain engineering of quantum dot excitonic emission in nanomembranes and optical resonators

Energy Technology Data Exchange (ETDEWEB)

Ding, Fei; Plumhof, Johannes; Rastelli, Armando; Schmidt, Oliver [Institute for Integrative Nanosciences, IFW Dresden (Germany); Singh, Ranber; Zander, Tim; Bester, Gabriel [Max-Planck-Institut fuer Festkoerperforschung, Stuttgart (Germany)

2010-07-01

We study the effect of an external biaxial stress on the light emission of single InGaAs/GaAs(001) quantum dots (QD) embedded in a 200 nm-thick-membrane. Reversible and bi-directional spectral tuning of QD excitonic emission is demonstrated via a simple electro-mechanical device. The most intriguing finding is that biaxial strain is a reliable tool to engineer the QD electronic structure and reach color coincidence between exciton and biexciton emission, providing a vital prerequisite for the generation of polarization entangled photon pairs through a time reordering strategy. The physical origin of this new phenomenon is discussed based on the empirical pseudopotential calculations. With similar technique we study the effect of biaxial stress on single QDs embedded in microring resonators. The microrings can be reversibly stretched or squeezed, resulting in a controllable engineering of both QD emissions and optical modes. Our results open up a new tuning strategy to study cQED with semiconductor quantum dots.

Models of coherent exciton condensation

International Nuclear Information System (INIS)

Littlewood, P B; Eastham, P R; Keeling, J M J; Marchetti, F M; Simons, B D; Szymanska, M H

2004-01-01

That excitons in solids might condense into a phase-coherent ground state was proposed about 40 years ago, and has been attracting experimental and theoretical attention ever since. Although experimental confirmation has been hard to come by, the concepts released by this phenomenon have been widely influential. This tutorial review discusses general aspects of the theory of exciton and polariton condensates, focusing on the reasons for coherence in the ground state wavefunction, the BCS to Bose crossover(s) for excitons and for polaritons, and the relationship of the coherent condensates to standard lasers

Models of coherent exciton condensation

Energy Technology Data Exchange (ETDEWEB)

Littlewood, P B [Theory of Condensed Matter, Cavendish Laboratory, Cambridge CB3 0HE (United Kingdom); Eastham, P R [Theory of Condensed Matter, Cavendish Laboratory, Cambridge CB3 0HE (United Kingdom); Keeling, J M J [Theory of Condensed Matter, Cavendish Laboratory, Cambridge CB3 0HE (United Kingdom); Marchetti, F M [Theory of Condensed Matter, Cavendish Laboratory, Cambridge CB3 0HE (United Kingdom); Simons, B D [Theory of Condensed Matter, Cavendish Laboratory, Cambridge CB3 0HE (United Kingdom); Szymanska, M H [Theory of Condensed Matter, Cavendish Laboratory, Cambridge CB3 0HE (United Kingdom)

2004-09-08

That excitons in solids might condense into a phase-coherent ground state was proposed about 40 years ago, and has been attracting experimental and theoretical attention ever since. Although experimental confirmation has been hard to come by, the concepts released by this phenomenon have been widely influential. This tutorial review discusses general aspects of the theory of exciton and polariton condensates, focusing on the reasons for coherence in the ground state wavefunction, the BCS to Bose crossover(s) for excitons and for polaritons, and the relationship of the coherent condensates to standard lasers.

Characterization of InP and InGaN quantum dots for single photon sources and AlGaInAs quantum dots in intermediate band solar cells

International Nuclear Information System (INIS)

Kremling, Stefan

2014-01-01

single QDs. Finally, the emission of single photons has been demonstrated using autocorrelation measurements. For a more efficient diffraction-limited output coupling of photons, the InP QDs grown by cyclic material deposition were embedded in micropillar resonator structures and investigated by means of spectroscopy. First, structures with different diameters were characterized by photoluminescence spectroscopy. Second, the energy of a single QD exciton and the energy of the cavity were tuned into resonance by changing the temperature. In the regime of weak coupling a luminescence enhancement due to the Purcell Effect was observed. Finally, also in the regime of weak coupling, the emission of single photons has been demonstrated by autocorrelation measurements. In terms of applications, electrical operations are desirable. Therefore, the Bragg mirrors of the micropillar resonator were doped for an efficient current injection and electrical contacts were deposited. After basic electrical characterization, the regime of weak coupling of a single QD exciton and the cavity resulting in a luminescence enhancement were demonstrated by the Purcell effect. Finally, the emission of single photons based on autocorrelation measurements is shown. In this chapter, the luminescence properties of single InGaN QD were investigated. Based on the wurtzite crystal structure of nitrite-compound semiconductors strong piezoelectric fields occur that lead to strongly linearly polarized luminescence. Several QDs were investigated and statistical studies were performed. Excitation power depending measurements allows one to identify the different exciton states of a single QD. In addition, the emission of single photons of InGaN QDs up to a temperature of 50 K was demonstrated for the first time. In the final chapter, an application of QDs in solar cells is presented to specifically exploit the unique properties of QDs in optical devices. The concept of the intermediate band solar cell utilizes

Solid state photon upconversion utilizing thermally activated delayed fluorescence molecules as triplet sensitizer

Energy Technology Data Exchange (ETDEWEB)

Wu, Tony C.; Congreve, Daniel N.; Baldo, Marc A., E-mail: baldo@mit.edu [Department of Electrical Engineering and Computer Science, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139 (United States)

2015-07-20

The ability to upconvert light is useful for a range of applications, from biological imaging to solar cells. But modern technologies have struggled to upconvert incoherent incident light at low intensities. Here, we report solid state photon upconversion employing triplet-triplet exciton annihilation in an organic semiconductor, sensitized by a thermally activated-delayed fluorescence (TADF) dye. Compared to conventional phosphorescent sensitizers, the TADF dye maximizes the wavelength shift in upconversion due to its small singlet-triplet splitting. The efficiency of energy transfer from the TADF dye is 9.1%, and the conversion yield of sensitizer exciton pairs to singlet excitons in the annihilator is 1.1%. Our results demonstrate upconversion in solid state geometries and with non-heavy metal-based sensitizer materials.

Measurement of Coherent Emission and Linear Polarization of Photons by Electrons in the Strong Fields of Aligned Crystals

CERN Document Server

Apyan, A.; Badelek, B.; Ballestrero, S.; Biino, C.; Birol, I.; Cenci, P.; Connell, S.H.; Eichblatt, S.; Fonseca, T.; Freund, A.; Gorini, B.; Groess, R.; Ispirian, K.; Ketel, T.J.; Kononets, Yu.V.; Lopez, A.; Mangiarotti, A.; van Rens, B.; Sellschop, J.P.F.; Shieh, M.; Sona, P.; Strakhovenko, V.; Uggerhoj, E.; Uggerhj, Ulrik Ingerslev; Unel, G.; Velasco, M.; Vilakazi, Z.Z.; Wessely, O.; Kononets, Yu.V.

2004-01-01

We present new results regarding the features of high energy photon emission by an electron beam of 178 GeV penetrating a 1.5 cm thick single Si crystal aligned at the Strings-Of-Strings (SOS) orientation. This concerns a special case of coherent bremsstrahlung where the electron interacts with the strong fields of successive atomic strings in a plane and for which the largest enhancement of the highest energy photons is expected. The polarization of the resulting photon beam was measured by the asymmetry of electron-positron pair production in an aligned diamond crystal analyzer. By the selection of a single pair the energy and the polarization of individual photons could be measured in an the environment of multiple photons produced in the radiator crystal. Photons in the high energy region show less than 20% linear polarization at the 90% confidence level.

Tailoring double Fano profiles with plasmon-assisted quantum interference in hybrid exciton-plasmon system

International Nuclear Information System (INIS)

Zhao, Dongxing; Wu, Jiarui; Gu, Ying; Gong, Qihuang

2014-01-01

We propose tailoring of the double Fano profiles via plasmon-assisted quantum interference in a hybrid exciton-plasmon system. Tailoring is performed by the interference between two exciton channels interacting with a common localized surface plasmon. Using an applied field of low intensity, the absorption spectrum of the hybrid system reveals a double Fano lineshape with four peaks. For relatively large field intensity, a broad flat window in the absorption spectrum appears which results from the destructive interference between excitons. Because of strong constructive interference, this window vanishes as intensity is further increased. We have designed a nanometer bandpass optical filter for visible light based on tailoring of the optical spectrum. This study provides a platform for quantum interference that may have potential applications in ultracompact tunable quantum devices.

Exciton-dopant and exciton-charge interactions in electronically doped OLEDs

International Nuclear Information System (INIS)

Williams, Christopher; Lee, Sergey; Ferraris, John; Zakhidov, A. Anvar

2004-01-01

The electronic dopants, like tetrafluorocyanoquinodimethane (F 4 -TCNQ) molecules, used for p-doping of hole transport layers in organic light-emitting diodes (OLEDs) are found to quench the electroluminescence (EL) if they diffuse into the emissive layer. We observed EL quenching in OLED with F 4 -TCNQ doped N,N'-diphenyl-N'N'-bis(1-naphthyl)-1,1'-biphenyl-4,4'-diamine hole transport layer at large dopant concentrations, >5%. To separate the effects of exciton-dopant quenching, from exciton-polaron quenching we have intentionally doped the emissive layer of (8-tris-hydroxyquinoline) with three acceptors (A) of different electron affinities: F 4 -TCNQ, TCNQ, and C 60 , and found that C 60 is the strongest EL-quencher, while F 4 -TCNQ is the weakest, contrary to intuitive expectations. The new effects of charge transfer and usually considered energy transfer from exciton to neutral (A) and charged acceptors (A - ) are compared as channels for non-radiative Ex-A decay. At high current loads the EL quenching is observed, which is due to decay of Ex on free charge carriers, hole polarons P + . We consider contributions to Ex-P + interaction by short-range charge transfer and describe the structure of microscopic charge transfer (CT)-processes responsible for it. The formation of metastable states of 'charged excitons' (predicted and studied by Agranovich et al. Chem. Phys. 272 (2001) 159) by electron transfer from a P to an Ex is pointed out, and ways to suppress non-radiative Ex-P decay are suggested

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...

Fractional Solitons in Excitonic Josephson Junctions

OpenAIRE

Hsu, Ya-Fen; Su, Jung-Jung

2015-01-01

The Josephson effect is especially appealing to physicists because it reveals macroscopically the quantum order and phase. In excitonic bilayers the effect is even subtler due to the counterflow of supercurrent as well as the tunneling between layers (interlayer tunneling). Here we study, in a quantum Hall bilayer, the excitonic Josephson junction: a conjunct of two exciton condensates with a relative phase ? 0 applied. The system is mapped into a pseudospin ferromagnet then described numeric...

Stable biexcitons in two-dimensional metal-halide perovskites with strong dynamic lattice disorder

Science.gov (United States)

Thouin, Félix; Neutzner, Stefanie; Cortecchia, Daniele; Dragomir, Vlad Alexandru; Soci, Cesare; Salim, Teddy; Lam, Yeng Ming; Leonelli, Richard; Petrozza, Annamaria; Kandada, Ajay Ram Srimath; Silva, Carlos

2018-03-01

With strongly bound and stable excitons at room temperature, single-layer, two-dimensional organic-inorganic hybrid perovskites are viable semiconductors for light-emitting quantum optoelectronics applications. In such a technological context, it is imperative to comprehensively explore all the factors—chemical, electronic, and structural—that govern strong multiexciton correlations. Here, by means of two-dimensional coherent spectroscopy, we examine excitonic many-body effects in pure, single-layer (PEA) 2PbI4 (PEA = phenylethylammonium). We determine the binding energy of biexcitons—correlated two-electron, two-hole quasiparticles—to be 44 ±5 meV at room temperature. The extraordinarily high values are similar to those reported in other strongly excitonic two-dimensional materials such as transition-metal dichalcogenides. Importantly, we show that this binding energy increases by ˜25 % upon cooling to 5 K. Our work highlights the importance of multiexciton correlations in this class of technologically promising, solution-processable materials, in spite of the strong effects of lattice fluctuations and dynamic disorder.

Energy-level repulsion by spin-orbit coupling in two-dimensional Rydberg excitons

Science.gov (United States)

Stephanovich, V. A.; Sherman, E. Ya.; Zinner, N. T.; Marchukov, O. V.

2018-05-01

We study the effects of Rashba spin-orbit coupling on two-dimensional Rydberg exciton systems. Using analytical and numerical arguments we demonstrate that this coupling considerably modifies the wave functions and leads to a level repulsion that results in a deviation from the Poissonian statistics of the adjacent level distance distribution. This signifies the crossover to nonintegrability of the system and hints at the possibility of quantum chaos emerging. Such behavior strongly differs from the classical realization, where spin-orbit coupling produces highly entangled, chaotic electron trajectories in an exciton. We also calculate the oscillator strengths and show that randomization appears in the transitions between states with different total momenta.

Precise single-qubit control of the reflection phase of a photon mediated by a strongly-coupled ancilla–cavity system

Science.gov (United States)

Motzoi, F.; Mølmer, K.

2018-05-01

We propose to use the interaction between a single qubit atom and a surrounding ensemble of three level atoms to control the phase of light reflected by an optical cavity. Our scheme employs an ensemble dark resonance that is perturbed by the qubit atom to yield a single-atom single photon gate. We show here that off-resonant excitation towards Rydberg states with strong dipolar interactions offers experimentally-viable regimes of operations with low errors (in the 10‑3 range) as required for fault-tolerant optical-photon, gate-based quantum computation. We also propose and analyze an implementation within microwave circuit-QED, where a strongly-coupled ancilla superconducting qubit can be used in the place of the atomic ensemble to provide high-fidelity coupling to microwave photons.

Chiral topological excitons in a Chern band insulator

Science.gov (United States)

Chen, Ke; Shindou, Ryuichi

2017-10-01

A family of semiconductors called Chern band insulators are shown to host exciton bands with nonzero topological Chern integers and chiral exciton edge modes. Using a prototypical two-band Chern insulator model, we calculate a cross-correlation function to obtain the exciton bands and their Chern integers. The lowest exciton band acquires Chern integers such as ±1 and ±2 in the electronic Chern insulator phase. The nontrivial topology can be experimentally observed both by a nonlocal optoelectronic response of exciton edge modes and by a phase shift in the cross-correlation response due to the bulk mode. Our result suggests that magnetically doped HgTe, InAs/GaSb quantum wells, and (Bi,Sb)2Te3 thin films are promising candidates for a platform of topological excitonics.

Directed emission of CdSe nanoplatelets originating from strongly anisotropic 2D electronic structure

Science.gov (United States)

Scott, Riccardo; Heckmann, Jan; Prudnikau, Anatol V.; Antanovich, Artsiom; Mikhailov, Aleksandr; Owschimikow, Nina; Artemyev, Mikhail; Climente, Juan I.; Woggon, Ulrike; Grosse, Nicolai B.; Achtstein, Alexander W.

2017-12-01

Intrinsically directional light emitters are potentially important for applications in photonics including lasing and energy-efficient display technology. Here, we propose a new route to overcome intrinsic efficiency limitations in light-emitting devices by studying a CdSe nanoplatelets monolayer that exhibits strongly anisotropic, directed photoluminescence. Analysis of the two-dimensional k-space distribution reveals the underlying internal transition dipole distribution. The observed directed emission is related to the anisotropy of the electronic Bloch states governing the exciton transition dipole moment and forming a bright plane. The strongly directed emission perpendicular to the platelet is further enhanced by the optical local density of states and local fields. In contrast to the emission directionality, the off-resonant absorption into the energetically higher 2D-continuum of states is isotropic. These contrasting optical properties make the oriented CdSe nanoplatelets, or superstructures of parallel-oriented platelets, an interesting and potentially useful class of semiconductor-based emitters.

Field-induced exciton dissociation in PTB7-based organic solar cells

Science.gov (United States)

Gerhard, Marina; Arndt, Andreas P.; Bilal, Mühenad; Lemmer, Uli; Koch, Martin; Howard, Ian A.

2017-05-01

The physics of charge separation in organic semiconductors is a topic of ongoing research of relevance to material and device engineering. Herein, we present experimental observations of the field and temperature dependence of charge separation from singlet excitons in PTB7 and PC71BM , and from charge-transfer states created across interfaces in PTB 7 /PC71BM bulk heterojunction solar cells. We obtain this experimental data by time-resolving the near infrared emission of the states from 10 K to room temperature and electric fields from 0 to 2.5 MVcm -1 . Examining how the luminescence is quenched by field and temperature gives direct insight into the underlying physics. We observe that singlet excitons can be split by high fields, and that disorder broadens the high threshold fields needed to split the excitons. Charge-transfer (CT) states, on the other hand, can be separated by both field and temperature. Also, the data imply a strong reduction of the activation barrier for charge splitting from the CT state relative to the exciton state. The observations provided herein of the field-dependent separation of CT states as a function of temperature offer a rich data set against which theoretical models of charge separation can be rigorously tested; it should be useful for developing the more advanced theoretical models of charge separation.

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...

Excitonic effects in gain and index in GaAlAs quantum well lasers

Energy Technology Data Exchange (ETDEWEB)

Kesler, M.P.; Harder, C. (IBM Research Division, Zurich Research Laboratory, 8803 Rueschlikon (Switzerland))

1990-07-09

Spontaneous emission and gain measurements in GaAlAs single quantum well lasers are presented. The gain is derived from the spontaneous emission detected through an opening in the top metallic contact of the lasers. Excitonic effects are seen in the gain (absorption) spectra for low carrier densities, and the step-like nature of the two-dimensional density of states is evident. From the gain spectra, refractive index changes are derived via a Kramers--Kronig transformation, and this is used to evaluate the linewidth enhancement factor as a function of photon energy.

Excitonic optical bistability in n-type doped semiconductors

International Nuclear Information System (INIS)

Nguyen Ba An; Le Thi Cat Tuong

1991-07-01

A resonant monochromatic pump laser generates coherent excitons in an n-type doped semiconductor. Both exciton-exciton and exciton-donor interactions come into play. The former interaction can give rise to the appearance of optical bistability which is heavily influenced by the latter one. When optical bistability occurs at a fixed laser frequency both its holding intensity and hysteresis loop size are shown to decrease with increasing donor concentration. Two possibilities are suggested for experimentally determining one of the two parameters of the system - the exciton-donor coupling constant and the donor concentration, if the other parameter is known beforehand. (author). 36 refs, 2 figs

Strongly interacting photons and atoms

International Nuclear Information System (INIS)

Alge, W.

1999-05-01

This thesis contains the main results of the research topics I have pursued during the my PhD studies at the University of Innsbruck and partly in collaboration with the Institut d' Optique in Orsay, France. It is divided into three parts. The first and largest part discusses the possibility of using strong standing waves as a tool to cool and trap neutral atoms in optical cavities. This is very important in the field of nonlinear optics where several successful experiments with cold atoms in cavities have been performed recently. A discussion of the optical parametric oscillator in a regime where the nonlinearity dominates the evolution is the topic of the second part. We investigated mainly the statistical properties of the cavity output of the three interactive cavity modes. Very recently a system has been proposed which promises fantastic properties. It should exhibit a giant Kerr nonlinearity with negligible absorption thus leading to a photonic turnstile device based on cold atoms in cavity. We have shown that this model suffers from overly simplistic assumptions and developed several more comprehensive approaches to study the behavior of this system. Apart from the division into three parts of different contents the thesis is divided into publications, supplements and invisible stuff. The intention of the supplements is to reach researchers which work in related areas and provide them with more detailed information about the concepts and the numerical tools we used. It is written especially for diploma and PhD students to give them a chance to use the third part of our work which is actually the largest one. They consist of a large number of computer programs we wrote to investigate the behavior of the systems in parameter regions where no hope exists to solve the equations analytically. (author)

Generation and control of polarization-entangled photons from GaAs island quantum dots by an electric field.

Science.gov (United States)

Ghali, Mohsen; Ohtani, Keita; Ohno, Yuzo; Ohno, Hideo

2012-02-07

Semiconductor quantum dots are potential sources for generating polarization-entangled photons efficiently. The main prerequisite for such generation based on biexciton-exciton cascaded emission is to control the exciton fine-structure splitting. Among various techniques investigated for this purpose, an electric field is a promising means to facilitate the integration into optoelectronic devices. Here we demonstrate the generation of polarization-entangled photons from single GaAs quantum dots by an electric field. In contrast to previous studies, which were limited to In(Ga)As quantum dots, GaAs island quantum dots formed by a thickness fluctuation were used because they exhibit a larger oscillator strength and emit light with a shorter wavelength. A forward voltage was applied to a Schottky diode to control the fine-structure splitting. We observed a decrease and suppression in the fine-structure splitting of the studied single quantum dot with the field, which enabled us to generate polarization-entangled photons with a high fidelity of 0.72 ± 0.05.

Two-color single-photon emission from InAs quantum dots: toward logic information management using quantum light.

Science.gov (United States)

Rivas, David; Muñoz-Matutano, Guillermo; Canet-Ferrer, Josep; García-Calzada, Raúl; Trevisi, Giovanna; Seravalli, Luca; Frigeri, Paola; Martínez-Pastor, Juan P

2014-02-12

In this work, we propose the use of the Hanbury-Brown and Twiss interferometric technique and a switchable two-color excitation method for evaluating the exciton and noncorrelated electron-hole dynamics associated with single photon emission from indium arsenide (InAs) self-assembled quantum dots (QDs). Using a microstate master equation model we demonstrate that our single QDs are described by nonlinear exciton dynamics. The simultaneous detection of two-color, single photon emission from InAs QDs using these nonlinear dynamics was used to design a NOT AND logic transference function. This computational functionality combines the advantages of working with light/photons as input/output device parameters (all-optical system) and that of a nanodevice (QD size of ∼ 20 nm) while also providing high optical sensitivity (ultralow optical power operational requirements). These system features represent an important and interesting step toward the development of new prototypes for the incoming quantum information technologies.

The mean energy loss by neutrino with magnetic moment in strong magnetic field with consideration of positronium contribution to photon dispersion

Science.gov (United States)

Mosichkin, A. F.

2017-11-01

The process of radiative decay of the neutrino with a magnetic moment in a strong magnetic field with consideration of positronium influence on photon dispersion has been studied. Positronium contribution to the photon polarization operator induces significant modifications of the photon dispersion law and neutrino radiative decay amplitude. It has been shown that the mean energy loss of a neutrino with magnetic a moment significantly increases, when the positronium contribution to photon dispersion is taken into account.

Strongly Iridescent Hybrid Photonic Sensors Based on Self-Assembled Nanoparticles for Hazardous Solvent Detection

Directory of Open Access Journals (Sweden)

Ayaka Sato

2018-03-01

Full Text Available Facile detection and the identification of hazardous organic solvents are essential for ensuring global safety and avoiding harm to the environment caused by industrial wastes. Here, we present a simple method for the fabrication of silver-coated monodisperse polystyrene nanoparticle photonic structures that are embedded into a polydimethylsiloxane (PDMS matrix. These hybrid materials exhibit a strong green iridescence with a reflectance peak at 550 nm that originates from the close-packed arrangement of the nanoparticles. This reflectance peak measured under Wulff-Bragg conditions displays a 20 to 50 nm red shift when the photonic sensors are exposed to five commonly employed and highly hazardous organic solvents. These red-shifts correlate well with PDMS swelling ratios using the various solvents, which suggests that the observable color variations result from an increase in the photonic crystal lattice parameter with a similar mechanism to the color modulation of the chameleon skin. Dynamic reflectance measurements enable the possibility of clearly identifying each of the tested solvents. Furthermore, as small amounts of hazardous solvents such as tetrahydrofuran can be detected even when mixed with water, the nanostructured solvent sensors we introduce here could have a major impact on global safety measures as innovative photonic technology for easily visualizing and identifying the presence of contaminants in water.

Acousto-exciton interaction in a gas of 2D indirect dipolar excitons in the presence of disorder

Energy Technology Data Exchange (ETDEWEB)

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

2016-03-15

A theory for the linear and quadratic responses of a 2D gas of indirect dipolar excitons to an external surface acoustic wave perturbation in the presence of a static random potential is considered. The theory is constructed both for high temperatures, definitely greater than the exciton gas condensation temperature, and at zero temperature by taking into account the Bose–Einstein condensation effects. The particle Green functions, the density–density correlation function, and the quadratic response function are calculated by the “cross” diagram technique. The results obtained are used to calculate the absorption of Rayleigh surface waves and the acoustic exciton gas drag by a Rayleigh wave. The damping of Bogoliubov excitations in an exciton condensate due to theirs scattering by a random potential has also been determined.

Stabilizing strongly correlated photon fluids with non-Markovian reservoirs

Science.gov (United States)

Lebreuilly, José; Biella, Alberto; Storme, Florent; Rossini, Davide; Fazio, Rosario; Ciuti, Cristiano; Carusotto, Iacopo

2017-09-01

We introduce a frequency-dependent incoherent pump scheme with a square-shaped spectrum as a way to study strongly correlated photons in arrays of coupled nonlinear resonators. This scheme can be implemented via a reservoir of population-inverted two-level emitters with a broad distribution of transition frequencies. Our proposal is predicted to stabilize a nonequilibrium steady state sharing important features with a zero-temperature equilibrium state with a tunable chemical potential. We confirm the efficiency of our proposal for the Bose-Hubbard model by computing numerically the steady state for finite system sizes: first, we predict the occurrence of a sequence of incompressible Mott-insulator-like states with arbitrary integer densities presenting strong robustness against tunneling and losses. Secondly, for stronger tunneling amplitudes or noninteger densities, the system enters a coherent regime analogous to the superfluid state. In addition to an overall agreement with the zero-temperature equilibrium state, exotic nonequilibrium processes leading to a finite entropy generation are pointed out in specific regions of parameter space. The equilibrium ground state is shown to be recovered by adding frequency-dependent losses. The promise of this improved scheme in view of quantum simulation of the zero-temperature many-body physics is highlighted.

Communication: Broad manifold of excitonic states in light-harvesting complex 1 promotes efficient unidirectional energy transfer in vivo

Science.gov (United States)

Sohail, Sara H.; Dahlberg, Peter D.; Allodi, Marco A.; Massey, Sara C.; Ting, Po-Chieh; Martin, Elizabeth C.; Hunter, C. Neil; Engel, Gregory S.

2017-10-01

In photosynthetic organisms, the pigment-protein complexes that comprise the light-harvesting antenna exhibit complex electronic structures and ultrafast dynamics due to the coupling among the chromophores. Here, we present absorptive two-dimensional (2D) electronic spectra from living cultures of the purple bacterium, Rhodobacter sphaeroides, acquired using gradient assisted photon echo spectroscopy. Diagonal slices through the 2D lineshape of the LH1 stimulated emission/ground state bleach feature reveal a resolvable higher energy population within the B875 manifold. The waiting time evolution of diagonal, horizontal, and vertical slices through the 2D lineshape shows a sub-100 fs intra-complex relaxation as this higher energy population red shifts. The absorption (855 nm) of this higher lying sub-population of B875 before it has red shifted optimizes spectral overlap between the LH1 B875 band and the B850 band of LH2. Access to an energetically broad distribution of excitonic states within B875 offers a mechanism for efficient energy transfer from LH2 to LH1 during photosynthesis while limiting back transfer. Two-dimensional lineshapes reveal a rapid decay in the ground-state bleach/stimulated emission of B875. This signal, identified as a decrease in the dipole strength of a strong transition in LH1 on the red side of the B875 band, is assigned to the rapid localization of an initially delocalized exciton state, a dephasing process that frustrates back transfer from LH1 to LH2.

Quantum Dot Photonics

Science.gov (United States)

Kinnischtzke, Laura A.

We report on several experiments using single excitons confined to single semiconductor quantum dots (QDs). Electric and magnetic fields have previously been used as experimental knobs to understand and control individual excitons in single quantum dots. We realize new ways of electric field control by changing materials and device geometry in the first two experiments with strain-based InAs QDs. A standard Schottky diode heterostructure is demonstrated with graphene as the Schottky gate material, and its performance is bench-marked against a diode with a standard gate material, semi-transparent nickel-chromium (NiCr). This change of materials increases the photon collection rate by eliminating absorption in the metallic NiCr layer. A second set of experiments investigates the electric field response of QDs as a possible metrology source. A linear voltage potential drop in a plane near the QDs is used to describe how the spatially varying voltage profile is also imparted on the QDs. We demonstrate a procedure to map this voltage profile as a preliminary route towards a full quantum sensor array. Lastly, InAs QDs are explored as potential spin-photon interfaces. We describe how a magnetic field is used to realize a reversible exchange of information between light and matter, including a discussion of the polarization-dependence of the photoluminesence, and how that can be linked to the spin of a resident electron or hole. We present evidence of this in two wavelength regimes for InAs quantum dots, and discuss how an external magnetic field informs the spin physics of these 2-level systems. This thesis concludes with the discovery of a new class of quantum dots. As-yet unidentified defect states in single layer tungsten diselenide (WSe 2 ) are shown to host quantum light emission. We explore the spatial extent of electron confinement and tentatively identify a radiative lifetime of 1 ns for these single photon emitters.

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...... was coated with a metal mask containing special openings (windows) of a micron size or smaller. Both photoexcitation and observation of luminescence were performed through these windows by the fiber optic technique. At low pumping powers, the interwell excitons were strongly localized because of the residual...... charged impurities, and the corresponding photoluminescence line was nonuniformly broadened. As the laser excitation power increased, a narrow line due to delocalized excitons arose in a threshold-like manner, after which its intensity rapidly increased with growing pumping and the line itself narrowed...

Magnetic field effect on the energy levels of an exciton in a GaAs quantum dot: Application for excitonic lasers.

Science.gov (United States)

Jahan, K Luhluh; Boda, A; Shankar, I V; Raju, Ch Narasimha; Chatterjee, Ashok

2018-03-22

The problem of an exciton trapped in a Gaussian quantum dot (QD) of GaAs is studied in both two and three dimensions in the presence of an external magnetic field using the Ritz variational method, the 1/N expansion method and the shifted 1/N expansion method. The ground state energy and the binding energy of the exciton are obtained as a function of the quantum dot size, confinement strength and the magnetic field and compared with those available in the literature. While the variational method gives the upper bound to the ground state energy, the 1/N expansion method gives the lower bound. The results obtained from the shifted 1/N expansion method are shown to match very well with those obtained from the exact diagonalization technique. The variation of the exciton size and the oscillator strength of the exciton are also studied as a function of the size of the quantum dot. The excited states of the exciton are computed using the shifted 1/N expansion method and it is suggested that a given number of stable excitonic bound states can be realized in a quantum dot by tuning the quantum dot parameters. This can open up the possibility of having quantum dot lasers using excitonic states.

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.

Hot exciton relaxation in multiple layers CdSe/ZnSe self-assembled quantum dots separated by thick ZnSe barriers

International Nuclear Information System (INIS)

Eremenko, M; Budkin, G; Reznitsky, A

2015-01-01

We have studied PL and PLE spectra of two samples (A and B) of MBE grown CdSe/ZnSe asymmetric double quantum wells with different amount of deposited CdSe layers separated by 14 nm ZnSe barrier. It has been found that PLE spectra of the states forming short wavelength side of the PL spectra of both deep and shallow QWs of the sample A as well as that of deep QW of the sample B demonstrate oscillating structure in the spectral ranges corresponding to exciton states of self-assembled quantum dots only. Meanwhile PLE spectra of the short wavelength states of shallow QW the sample B revealed pronounced oscillating structure with energy period of ZnSe LO phonon under excitation with photons in a wide energy range both in the regions of quantum-dot states and in that of free states in the ZnSe barrier. In these spectra creating of excitons with kinetic energies more than 0.3 eV was observed which considerably exceed the exciton binding energy as well as LO phonon energy (both appr. 0.03 eV). It has been concluded that oscillating structure of the PLE spectra arises due to cascade relaxation of hot excitons. We discuss the model which explains these experimental findings. (paper)

Hot exciton relaxation in multiple layers CdSe/ZnSe self-assembled quantum dots separated by thick ZnSe barriers

Science.gov (United States)

Eremenko, M.; Budkin, G.; Reznitsky, A.

2015-11-01

We have studied PL and PLE spectra of two samples (A and B) of MBE grown CdSe/ZnSe asymmetric double quantum wells with different amount of deposited CdSe layers separated by 14 nm ZnSe barrier. It has been found that PLE spectra of the states forming short wavelength side of the PL spectra of both deep and shallow QWs of the sample A as well as that of deep QW of the sample B demonstrate oscillating structure in the spectral ranges corresponding to exciton states of self-assembled quantum dots only. Meanwhile PLE spectra of the short wavelength states of shallow QW the sample B revealed pronounced oscillating structure with energy period of ZnSe LO phonon under excitation with photons in a wide energy range both in the regions of quantum-dot states and in that of free states in the ZnSe barrier. In these spectra creating of excitons with kinetic energies more than 0.3 eV was observed which considerably exceed the exciton binding energy as well as LO phonon energy (both appr. 0.03 eV). It has been concluded that oscillating structure of the PLE spectra arises due to cascade relaxation of hot excitons. We discuss the model which explains these experimental findings.

Nonboson treatment of excitonic nonlinearity in optically excited media

International Nuclear Information System (INIS)

Nguyen Ba An.

1990-11-01

The present article shortly reviews some recent results in the study of excitonic nonlinearity in optically excited media using a nonboson treatment for many-exciton systems. After a brief discussion of the exciton nonbosonity the closed commutation relations are given for exciton operators which hold for any exciton density and type. The nonboson treatment is then applied to the problems of intrinsic optical bistability and nonlinear polariton yielding quite interesting and new effects, e.g. new shapes of hysteresis loops of intrinsic optical bistability or anomalies of polariton dispersion. (author). 71 refs, 4 figs

Atomic lattice excitons: from condensates to crystals

International Nuclear Information System (INIS)

Kantian, A; Daley, A J; Toermae, P; Zoller, P

2007-01-01

We discuss atomic lattice excitons (ALEs), bound particle-hole pairs formed by fermionic atoms in two bands of an optical lattice. Such a system provides a clean set-up, with tunable masses and interactions, to study fundamental properties of excitons including exciton condensation. We also find that for a large effective mass ratio between particles and holes, effective long-range interactions can mediate the formation of an exciton crystal, for which superfluidity is suppressed. Using a combination of mean-field treatments, bosonized theory based on a Born-Oppenheimer approximation, and one-dimensional (1D) numerical computation, we discuss the properties of ALEs under varying conditions, and discuss in particular their preparation and measurement

Atomic lattice excitons: from condensates to crystals

Energy Technology Data Exchange (ETDEWEB)

Kantian, A [Institute for Quantum Optics and Quantum Information of the Austrian Academy of Sciences, A-6020 Innsbruck (Austria); Daley, A J [Institute for Quantum Optics and Quantum Information of the Austrian Academy of Sciences, A-6020 Innsbruck (Austria); Toermae, P [Nanoscience Center, Department of Physics, University of Jyvaeskylae, PO Box 35, FIN-40014 (Finland); Zoller, P [Institute for Quantum Optics and Quantum Information of the Austrian Academy of Sciences, A-6020 Innsbruck (Austria)

2007-11-15

We discuss atomic lattice excitons (ALEs), bound particle-hole pairs formed by fermionic atoms in two bands of an optical lattice. Such a system provides a clean set-up, with tunable masses and interactions, to study fundamental properties of excitons including exciton condensation. We also find that for a large effective mass ratio between particles and holes, effective long-range interactions can mediate the formation of an exciton crystal, for which superfluidity is suppressed. Using a combination of mean-field treatments, bosonized theory based on a Born-Oppenheimer approximation, and one-dimensional (1D) numerical computation, we discuss the properties of ALEs under varying conditions, and discuss in particular their preparation and measurement.

Silver Nanoshell Plasmonically Controlled Emission of Semiconductor Quantum Dots in the Strong Coupling Regime.

Science.gov (United States)

Zhou, Ning; Yuan, Meng; Gao, Yuhan; Li, Dongsheng; Yang, Deren

2016-04-26

Strong coupling between semiconductor excitons and localized surface plasmons (LSPs) giving rise to hybridized plexciton states in which energy is coherently and reversibly exchanged between the components is vital, especially in the area of quantum information processing from fundamental and practical points of view. Here, in photoluminescence spectra, rather than from common extinction or reflection measurements, we report on the direct observation of Rabi splitting of approximately 160 meV as an indication of strong coupling between excited states of CdSe/ZnS quantum dots (QDs) and LSP modes of silver nanoshells under nonresonant nanosecond pulsed laser excitation at room temperature. The strong coupling manifests itself as an anticrossing-like behavior of the two newly formed polaritons when tuning the silver nanoshell plasmon energies across the exciton line of the QDs. Further analysis substantiates the essentiality of high pump energy and collective strong coupling of many QDs with the radiative dipole mode of the metallic nanoparticles for the realization of strong coupling. Our finding opens up interesting directions for the investigation of strong coupling between LSPs and excitons from the perspective of radiative recombination under easily accessible experimental conditions.

Triplet exciton diffusion in organic semiconductors

Energy Technology Data Exchange (ETDEWEB)

Koehler, Anna [Department of Physics, University of Bayreuth (Germany)

2010-07-01

Efficient triplet exciton emission has allowed improved operation of organic light-emitting diodes (LEDs). To enhance the device performance, it is necessary to understand what governs the motion of triplet excitons through the organic semiconductor. We use a series of poly(p-phenylene)-type conjugated polymers and oligomers of variable degree of molecular distortion (i.e. polaron formation) and energetic disorder as model systems to study the Dexter-type triplet exciton diffusion in thin films. We show that triplet diffusion can be quantitatively described in the framework of a Holstein small polaron model (Marcus theory) that is extended to include contributions from energetic disorder. The model predicts a tunnelling process at low temperatures followed by a thermally activated hopping process above a transition temperature. In contrast to charge transfer, the activation energy required for triplet exciton transfer can be deduced from the optical spectra. We discuss the implications for device architecture.

Photon Splitting in a Strong Magnetic Field: Recalculation and Comparison with Previous Calculations

International Nuclear Information System (INIS)

Adler, S.L.; Schubert, C.

1996-01-01

We recalculate the amplitude for photon splitting in a strong magnetic field below the pair production threshold, using the world line path integral variant of the Bern-Kosower formalism. Numerical comparison (using programs that we have made available for public access on the Internet) shows that the results of the recalculation are identical to the earlier calculations of Adler and later of Stoneham, and to the recent recalculation by Baier, Milstein, and Shaisultanov. copyright 1996 The American Physical Society

Scientific/Technical Report

Energy Technology Data Exchange (ETDEWEB)

Bommissetty, Venkat [Materials Research Society, Warrendale, PA (United States)

2012-11-21

This symposium aimed to bring together researchers working on quantifying nanoscale carrier transport processes in excitonic solar cells. 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 efforts 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.

Exciton binding energy in a pyramidal quantum dot

Science.gov (United States)

Anitha, A.; Arulmozhi, M.

2018-05-01

The effects of spatially dependent effective mass, non-parabolicity of the conduction band and dielectric screening function on exciton binding energy in a pyramid-shaped quantum dot of GaAs have been investigated by variational method as a function of base width of the pyramid. We have assumed that the pyramid has a square base with area a× a and height of the pyramid H=a/2. The trial wave function of the exciton has been chosen according to the even mirror boundary condition, i.e. the wave function of the exciton at the boundary could be non-zero. The results show that (i) the non-parabolicity of the conduction band affects the light hole (lh) and heavy hole (hh) excitons to be more bound than that with parabolicity of the conduction band, (ii) the dielectric screening function (DSF) affects the lh and hh excitons to be more bound than that without the DSF and (iii) the spatially dependent effective mass (SDEM) affects the lh and hh excitons to be less bound than that without the SDEM. The combined effects of DSF and SDEM on exciton binding energy have also been calculated. The results are compared with those available in the literature.

Effect of exciton polaritons of absorption edge of GaTe

International Nuclear Information System (INIS)

Kurbatov, L.N.; Dirochka, A.I.; Sosin, V.A.

1979-01-01

The experimental results, pointing to the dependence of spectral and integral coefficients of exciton absorption as well as to the exciton relaxation parameter γsub(0) over the exciton zone on the sample thickness, are presented. It is tried to explain the inverse dependences of absorption intensity in the maximum of αsub(max) and γsub(0) exciton line within the limits of polariton theory. The values of polariton free path length in GaTe at various temperatures, as well as the volume γsub(vol.) and surface γsub(surf.) parameters of exciton relaxation over the exciton zone are discussed

Switching Exciton Pulses Through Conical Intersections

Science.gov (United States)

Leonhardt, K.; Wüster, S.; Rost, J. M.

2014-11-01

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 nonadiabatic 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. The fundamental ideas discussed here have general implications for excitons on a dynamic network.

Mapping the Local Density of Optical States of a Photonic Crystal with Single Quantum Dots

DEFF Research Database (Denmark)

Wang, Qin; Stobbe, Søren; Lodahl, Peter

2011-01-01

We use single self-assembled InGaAs quantum dots as internal probes to map the local density of optical states of photonic crystal membranes. The employed technique separates contributions from nonradiative recombination and spin-flip processes by properly accounting for the role of the exciton...... fine structure. We observe inhibition factors as high as 70 and compare our results to local density of optical states calculations available from the literature, thereby establishing a quantitative understanding of photon emission in photonic crystal membranes. © 2011 American Physical Society....

Phonon-assisted exciton formation in ZnO/(Zn, Mg)O single quantum wells grown on C-plane oriented substrates

International Nuclear Information System (INIS)

Béaur, L.; Bretagnon, T.; Guillet, T.; Brimont, C.; Gallart, M.; Gil, B.; Gilliot, P.; Morhain, C.

2013-01-01

We report on absorption phenomena in ZnO/(Zn, Mg)O quantum wells grown along the c-axis by molecular beam epitaxy. The optical properties of such quantum wells are affected by a huge internal electric field. For wide quantum wells the absorption is driven by Quantum Confined Stark Effect. Phonon-assisted formation of excitons is observed in the case of thin quantum wells. The physical origin of these hot excitons is determined by using both low temperature (T=10 K) photoluminescence excitation spectroscopy and reflectivity measurements. -- Highlights: ► High structural quality ZnO/(Zn, Mg)O quantum wells are growth along the polar c-direction. ► Indirect phonon-assisted formation of excitons in the thin single quantum wells. ► Strong internal electric field present in polar heterostructures prevents the observation of hot excitons

Exceptionally slow rise in differential reflectivity spectra of excitons in GaN: effect of excitation-induced dephasing

International Nuclear Information System (INIS)

Stanton, C.J.; Kenrow, J.; El Sayed, K.; Jho, Y.D.; Kim, D.S.; Song, J.J.; Fischer, Arthur Joseph

2004-01-01

Femtosecond differential reflectivity spectroscopy (DRS) and four-wave mixing (FWM) experiments were performed simultaneously to study the initial temporal dynamics of the exciton line-shapes in GaN epilayers. Beats between the A-B excitons were found only for positive time delay in both DRS and FWM experiments. The rise time at negative time delay for the DRS was much slower than the FWM signal or differential transmission spectroscopy at the exciton resonance. A numerical solution of a six band semiconductor Bloch equation model including nonlinearities at the Hartree-Fock level shows that this slow rise in the DRS results from excitation induced dephasing, that is, the strong density dependence of the dephasing time which changes with the laser excitation energy.

Experimental demonstration of highly anisotropic decay rates of single quantum dots inside photonic crystals

DEFF Research Database (Denmark)

Wang, Qin; Stobbe, Søren; Nielsen, Henri Thyrrestrup

We have systematically measured the variation of the spontaneous emission rate with polarization for self-assembled single quantum dots in two-dimensional photonic crystal membranes and obtained a maximum anisotropy factor of 6 between the decay rates of the two nondegenerate bright exciton states....

Excitonic effects in the luminescence of quantum wells

International Nuclear Information System (INIS)

Deveaud, B.; Kappei, L.; Berney, J.; Morier-Genoud, F.; Portella-Oberli, M.T.; Szczytko, J.; Piermarocchi, C.

2005-01-01

We report on the origin of the excitonic luminescence in quantum wells. This study is carried out by time-resolved photoluminescence experiments performed on a very high-quality InGaAs quantum well sample in which the photoluminescence contributions at the energy of the exciton and at the band edge can be clearly separated and traced over a broad range of times and densities. This allows us to compare the two conflicting theoretical approaches to the question of the origin of the excitonic luminescence in quantum wells: the model of the exciton population and the model of the Coulomb correlated plasma. We measure the exciton formation time and we show the fast exciton formation and its dependence with carrier density. We are also able to give the boundaries of the Mott transition in our system, and to show the absence of observable renormalization of the gap below the onset of this transition. We detail the characteristics of the trion formation and evidence the possible formation of both positive and negative trions in the absence of any resident free carrier populations

Characterization of scintillating CaWO{sub 4} crystals for the CRESST experiment using two-photon excitation

Energy Technology Data Exchange (ETDEWEB)

Hampf, Raphael; Dandl, Thomas; Muenster, Andrea; Oberauer, Lothar; Roth, Sabine; Schoenert, Stefan; Ulrich, Andreas [Physik-Department and Excellence Cluster Universe, Technische Universitaet Muenchen, D-85747 Garching (Germany)

2016-07-01

In the CRESST experiment for direct dark matter search, phonon and photon signals from cryogenic CaWO{sub 4} crystals are used to search for WIMP-induced nuclear recoil events. We present a novel table-top setup in which the scintillation of CaWO{sub 4} is induced by 0.7 ns laser pulses of 355 nm wavelength. The excitation occurs via two-photon absorption in the bulk material. The scintillation light is observed by time resolved optical spectroscopy. By varying the focusing of the laser-beam the excitation density can be made high enough to study quenching effects due to exciton-exciton annihilation. This allows to perform experiments to test models for the quenching factors of different ionizing projectiles in CaWO{sub 4} which are used to identify these projectiles on an event by event basis.

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.

Role of excitons in the energy resolution of scintillators used for medical imaging

Energy Technology Data Exchange (ETDEWEB)

Singh, Jai [School of Engineering and IT, B-purple-12, Faculty of EHS, Charles Darwin University, Darwin NT 0909 (Australia)

2010-11-01

Theoretical investigations suggest that the nonproportionality in a scintillator is caused by the high excitation density created within the track of an X-ray or {gamma} ray photon entering in a scintillating crystal. In this paper an analytical expression for the scintillator yield is derived. For the case of BaF{sub 2} scintillator the role of excitons created within the {gamma}-ray track in the scintillator yield is studied. By comparing the results of two theories an analytical expression is also derived for an energy parameter which could otherwise only be determined by fitting the theoretical yield to the experimental data.

Role of excitons in the energy resolution of scintillators used for medical imaging

International Nuclear Information System (INIS)

Singh, Jai

2010-01-01

Theoretical investigations suggest that the nonproportionality in a scintillator is caused by the high excitation density created within the track of an X-ray or γ ray photon entering in a scintillating crystal. In this paper an analytical expression for the scintillator yield is derived. For the case of BaF 2 scintillator the role of excitons created within the γ-ray track in the scintillator yield is studied. By comparing the results of two theories an analytical expression is also derived for an energy parameter which could otherwise only be determined by fitting the theoretical yield to the experimental data.

Interaction and dephasing of center-of-mass quantized excitons in wide ZnSe/Zn0.94Mg0.06Se quantum wells

DEFF Research Database (Denmark)

Wagner, Hans Peter; Schätz, A.; Maier, R.

1998-01-01

We investigate the interaction and dephasing of the excitons in wide ZnSe/Zn0.94Mg0.06Se quantum wells by spectrally resolved, femtosecond four-wave mixing (FWM). Polarization-dependent measurements indicate that excitation-induced dephasing is the dominant FWM process. The biexcitons of the center...... repulsion for coherent excitons. The exciton interaction rates with acoustic and optical phonons are deduced by their temperature dependencies. The acoustic-phonon scattering is found to be strongly reduced in the investigated wide wells due to the reduced accessible phonon wave vector....

Exploring exciton relaxation and multiexciton generation in PbSe nanocrystals using hyperspectral near-IR probing.

Science.gov (United States)

Gdor, Itay; Sachs, Hanan; Roitblat, Avishy; Strasfeld, David B; Bawendi, Moungi G; Ruhman, Sanford

2012-04-24

Hyperspectral femtosecond transient absorption spectroscopy is employed to record exciton relaxation and recombination in colloidal lead selenide (PbSe) nanocrystals in unprecedented detail. Results obtained with different pump wavelengths and fluences are scrutinized with regard to three issues: (1) early subpicosecond spectral features due to "hot" excitons are analyzed in terms of suggested underlying mechanisms; (2) global kinetic analysis facilitates separation of the transient difference spectra into single, double, and triple exciton state contributions, from which individual band assignments can be tested; and (3) the transient spectra are screened for signatures of multiexciton generation (MEG) by comparing experiments with excitation pulses both below and well above the theoretical threshold for multiplication. For the latter, a recently devised ultrafast pump-probe spectroscopic approach is employed. Scaling sample concentrations and pump pulse intensities inversely with the extinction coefficient at each excitation wavelength overcomes ambiguities due to direct multiphoton excitation, uncertainties of absolute absorption cross sections, and low signal levels. As observed in a recent application of this method to InAs core/shell/shell nanodots, no sign of MEG was detected in this sample up to photon energy 3.7 times the band gap. Accordingly, numerous reports of efficient MEG in other samples of PbSe suggest that the efficiency of this process varies from sample to sample and depends on factors yet to be determined.

Phase diagram of incoherently driven strongly correlated photonic lattices

Science.gov (United States)

Biella, Alberto; Storme, Florent; Lebreuilly, José; Rossini, Davide; Fazio, Rosario; Carusotto, Iacopo; Ciuti, Cristiano

2017-08-01

We explore theoretically the nonequilibrium photonic phases of an array of coupled cavities in presence of incoherent driving and dissipation. In particular, we consider a Hubbard model system where each site is a Kerr nonlinear resonator coupled to a two-level emitter, which is pumped incoherently. Within a Gutzwiller mean-field approach, we determine the steady-state phase diagram of such a system. We find that, at a critical value of the intercavity photon hopping rate, a second-order nonequilibrium phase transition associated with the spontaneous breaking of the U(1 ) symmetry occurs. The transition from an incompressible Mott-like photon fluid to a coherent delocalized phase is driven by commensurability effects and not by the competition between photon hopping and optical nonlinearity. The essence of the mean-field predictions is corroborated by finite-size simulations obtained with matrix product operators and corner-space renormalization methods.

Excitonic polaritons of zinc diarsenide single crystals

Energy Technology Data Exchange (ETDEWEB)

Syrbu, N.N., E-mail: sirbunn@yahoo.com [Technical University of Moldova, Chisinau, Republic of Moldova (Moldova, Republic of); Stamov, I.G. [T.G. Shevchenko State University of Pridnestrovie, Tiraspol, Republic of Moldova (Moldova, Republic of); Zalamai, V.V. [Institute of Applied Physics, Academy of Sciences of Moldova, Chisinau, Republic of Moldova (Moldova, Republic of); Dorogan, A. [Technical University of Moldova, Chisinau, Republic of Moldova (Moldova, Republic of)

2017-02-01

Excitonic polaritons of ZnAs{sub 2} single crystals had been investigated. Parameters of singlet excitons with Г{sub 2}¯(z) symmetry and orthoexcitons 2Г{sub 1}¯(y)+Г{sub 2}¯(x) had been determined. Spectral dependencies of ordinary and extraordinary dispersion of refractive index had been calculated using interferential reflection and transmittance spectra. It was shown, that A excitonic series were due to hole (V{sub 1}) and electron (C{sub 1}) bands. The values of effective masses of electrons (m{sub c}{sup *}=0.10 m{sub 0}) and holes (m{sub v1}{sup *}=0.89 m{sub 0}) had been estimated. It was revealed that the hole mass m{sub v1}{sup *} changes from 1.03 m{sub 0} to 0.55 m{sub 0} at temperature increasing from 10 K up to 230 K and that the electron mass m{sub c}{sup *} does not depend on temperature. The integral absorption A (eV cm{sup −1}) of the states n=1, 2 and 3 of Г{sub 2}¯(z) excitons depends on the A{sub n}≈n{sup −3} equality, which it is characteristic for S-type excitonic functions. Temperature dependences of the integral absorption of ground states for Г{sub 2}¯(z) and Г{sub 2}¯(Ñ…) excitons differ. The ground states of B and C excitons formed by V{sub 3} – C{sub 1} and V{sub 4} – C{sub 1} bands and its parameters had been determined.

Enhanced magneto-plasmonic effect in Au/Co/Au multilayers caused by exciton–plasmon strong coupling

Energy Technology Data Exchange (ETDEWEB)

Hamidi, S.M., E-mail: m_hamidi@sbu.ac.ir; Ghaebi, O.

2016-09-15

In this paper, we have investigated magneto optical Kerr rotation using the strong coupling of exciton–plasmon. For this purpose, we have demonstrated strong coupling phenomenon using reflectometry measurements. These measurements revealed the formation of two split polaritonic extrema in reflectometry as a function of wavelength. Then we have shown exciton–plasmon coupling in dispersion diagram which presented an anti-crossing between the polaritonic branches. To assure the readers of strong coupling, we have shown an enhanced magneto-optical Kerr rotation by comparing the reflectometry results of strong coupling of surface Plasmon polariton of Au/Co/Au multilayer and R6G excitons with surface Plasmon polariton magneto-optical kerr effect experimental setup. - Highlights: • The magneto optical Kerr rotation has been investigated by using the strong coupling of exciton–plasmon. • We have shown exciton–plasmon coupling in dispersion diagram which presented an anti-crossing between the polaritonic branches. • Strong coupling of surface plasmon polariton and exciton have been yielded to the enhanced magneto-optical Kerr effect. • Plasmons in Au/Co/Au multilayer and exciton in R6G have been coupled to enhance magneto-optical activity.

Construction of Nanowire Heterojunctions: Photonic Function-Oriented Nanoarchitectonics.

Science.gov (United States)

Li, Yong Jun; Yan, Yongli; Zhao, Yong Sheng; Yao, Jiannian

2016-02-10

Nanophotonics has received broad research interest because it may provide an alternative opportunity to overcome the fundamental limitations of electronic circuits. So far, diverse photonic functions, such as light generation, modulation, and detection, have been realized based on various nano-materials. The exact structural features of these material systems, including geometric characteristics, surface morphology, and material composition, play a key role in determining the photonic functions. Therefore, rational designs and constructions of materials on both morphological and componential levels, namely nanoarchitectonics, are indispensable for any photonic device with specific functionalities. Recently, a series of nanowire heterojunctions (NWHJs), which are usually made from two or more kinds of material compositions, were constructed for novel photonic applications based on various interactions between different materials at the junctions, for instance, energy transfer, exciton-plasmon coupling, or photon-plasmon coupling. A summary of these works is necessary to get a more comprehensive understanding of the relationship between photonic functions and architectonics of NWHJs, which will be instructive for designing novel photonic devices towards integrated circuits. Here, photonic function oriented nanoarchitectonics based on recent breakthroughs in nanophotonic devices are discussed, with emphasis on the design mechanisms, fabrication strategies, and excellent performances. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Growth of self-assembled (Ga)InAs/GaAs quantum dots and realization of high quality microcavities for experiments in the field of strong exciton photon coupling

International Nuclear Information System (INIS)

Loeffler, Andreas

2008-01-01

the exciton could be observed. A Rabi-splitting of about 60 μeV was measured for circular GaInAs dots with an indium content of 43 % and diameters between 20 and 25 nm. we could conclude an oscillator strength of approximately 40-50 for the enlarged quantum dot structures. In contrast to that, the slightly smaller dots with an indium content of 43 % only show an oscillator strength of about 15-20. Furthermore, doped microcavities were realized with regard to electrically driven devices. The investigated electrically driven mircocavities with embedded GaInAs quantum dots were operating in the weak coupling regime and showed a clear Purcell effect with a Purcell factor in resonance of about 10. Due to the use of enlarged GaInAs quantum dots, we were able to reach the strong coupling regime with a vacuum Rabi-splitting of 85 μeV also for electrically driven micropillars. (orig.)

F-center and self-trapped exciton formation in strongly excited alkali halide crystals

International Nuclear Information System (INIS)

Kravchenko, V.A.; Yakovlev, V.Yu.

1988-01-01

Method of luminescent and absorption spectroscopy with time resolution was used to study the effect of density of electron pulse excitation (t p =10 -8 s, P=(10 5 -10 8 ) WXcm -2 ) on efficiency of η ε two-halide autolocalized exciton (TALE) and F-centers (η F ) formation in CsI, CsBr, KBr, KI alkali halide crystals. It was established that for all studied systems the elevation of P power of electron beam (EB) from 10 5 up to 5X10 7 WXcm -2 resulted to sufficient decrease of production efficiency and yield of TALE luminescence. In the case when F-centers of colour are induced predominantly by pulsed irradiation in crystals, F-center yield is independent of P. If F-centers and TALE are produced in comparable amounts (CsBr crystals, T=80 K), η ε decrease with P growth is accompanied by η F growth

Energetic disorder and exciton states of individual molecular rings

International Nuclear Information System (INIS)

Herman, Pavel; Barvik, Ivan; Zapletal, David

2006-01-01

Exciton states in molecular rings (resembling, e.g. the B850 ring from LH2 complexes of purple bacterium Rhodopseudomonas acidophila) with strong intermolecular interaction are still a question of interest [V. Sundstrom, T. Pullerits, R. van Grondelle, J. Phys. Chem. B 103 (1999) 2327]. In our theoretical model we use the ring of two-level systems, simulating, e.g., the bacteriochlorophylls B850. The dynamical aspects in ensemble of rings are reflected in optical line shapes of electronic transitions. The observed linewidths reflect the combined influence of different types of static and dynamic disorder. To avoid the broadening of lines due to ensemble averaging one uses the single-molecule spectroscopy technique to obtain a fluorescence-excitation spectrum. For zero disorder the exciton manifold features two non-degenerate and eight pairwise degenerate states. In the presence of energetic disorder the degeneracy of the exciton states is lifted and oscillator strength is redistributed among the exciton states. A satisfactory understanding of the nature of static disorder in light-harvesting systems has not been reached [S. Jang, S.F. Dempster, R.J. Silbey, J. Phys. Chem. B 105 (2001) 6655]. In the local site basis, there can be present static disorder in both diagonal and off-diagonal Hamiltonian matrix elements. Silbey et al. [J. Phys. Chem. B 105 (2001) 6655] pointed out several questions: is former enough or the latter should be included as well? If both are considered, then there remains a question about whether they are independent or correlated. The distribution of the energetic separation E(k=+/-1) and relative orientation of the transition-dipole moments has been recently investigated [S. Jang, et al., J. Phys. Chem. B 105 (2001) 6655; C. Hofmann, T.J. Aartsma, J. Koehler, Chem. Phys. Lett. 395 (2004) 373]. In our present contribution we have extended such a type of investigation to four models of noncorrelated static disorder: (A) Gaussian disorder in the

Bragg polaritons in a ZnSe-based unfolded microcavity at elevated temperatures

Energy Technology Data Exchange (ETDEWEB)

Sebald, K.; Rahman, SK. S.; Cornelius, M.; Kaya, T.; Gutowski, J. [Semiconductor Optics, Institute of Solid State Physics, University of Bremen, 28334 Bremen (Germany); Klein, T.; Gust, A.; Hommel, D. [Semiconductor Epitaxy, Institute of Solid State Physics, University of Bremen, 28334 Bremen (Germany); Klembt, S. [Institut Néel, Université Grenoble Alpes and CNRS, B.P. 166, 38042 Grenoble (France)

2016-03-21

In this contribution, we present strong coupling of ZnSe quantum well excitons to Bragg modes resulting in the formation of Bragg polariton eigenstates, characterized by a small effective mass in comparison to a conventional microcavity. We observe an anticrossing of the excitonic and the photonic component in our sample being a clear signature for the strong-coupling regime. The anticrossing is investigated by changing the detuning between the excitonic components and the Bragg mode. We find anticrossings between the first Bragg mode and the heavy- as well as light-hole exciton, respectively, resulting in three polariton branches. The observed Bragg-polariton branches are in good agreement with theoretical calculations. The strong indication for the existence of strong coupling is traceable up to a temperature of 200 K, with a Rabi-splitting energy of 24 meV and 13 meV for the Bragg mode with the heavy- and light-hole exciton, respectively. These findings demonstrate the advantages of this sample configuration for ZnSe-based devices for the strong coupling regime.

Excitons in single-walled carbon nanotubes: environmental effect

International Nuclear Information System (INIS)

Smyrnov, O.A.

2010-01-01

The properties of excitons in semiconducting single-walled carbon nanotubes (SWCNTs) isolated in vacuum or a medium and their contributions to the optical spectra of nanotubes are studied within the elementary potential model, in which an exciton is represented as a bound state of two oppositely charged quasiparticles confined to the nanotube surface. The emphasis is given on the influence of the dielectric environment surrounding a nanotube on the exciton spectra. For nanotubes in the environment with a permittivity less than ∼ 1:8; the ground-state exciton binding energies exceed the respective energy gaps, whereas the obtained binding energies of excitons in nanotubes in a medium with permittivity greater than ∼ 4 are in good accordance with the corresponding experimental data and consistent with the known scaling relation for the environmental effect. The stabilization of a single-electron spectrum in SWCNTs in media with rather low permittivities is discussed.

Accelerating FRET between Near-Infrared Emitting Quantum Dots Using a Molecular J-Aggregate as an Exciton Bridge.

Science.gov (United States)

Wang, Chen; Weiss, Emily A

2017-09-13

Fast energy transfer (EnT) among quantum dots (QDs) with near-infrared (NIR) emission is essential for fully exploiting their light harvesting and photon downconversion (multiexciton generation) abilities. This paper demonstrates a relayed EnT mechanism that accelerates the migration of NIR excitons between PbS QDs by a factor of 20 from that of one-step EnT through a polyelectrolyte and even a factor of ∼2 from that of one-step EnT between QDs in direct contact, by employing a J-aggregate (J-agg) of a cyanine dye as an exciton bridge. The donor QDs, acceptor QDs, and J-agg are electrostatically assembled into a sandwich structure with layer-by-layer deposition. Estimates of EnT rate and yield from transient and steady-state absorption and photoluminescence spectroscopies show that the rate-limiting step in the relay is EnT from the donor QD to the J-agg, while EnT from the J-agg to the acceptor QD occurs in J-agg with more intermolecular order. This work demonstrates the viability of relayed EnT through a molecular bridge as a strategy for accelerating long-distance exciton migration in assemblies of QDs, in particular in the near-infrared.

Effects of surface and interface traps on exciton and multi-exciton dynamics in core/shell quantum dots

Science.gov (United States)

Bozio, Renato; Righetto, Marcello; Minotto, Alessandro

2017-08-01

Exciton interactions and dynamics are the most important factors determining the exceptional photophysical properties of semiconductor quantum dots (QDs). In particular, best performances have been obtained for ingeniously engineered core/shell QDs. We have studied two factors entering in the exciton decay dynamics with adverse effects for the luminescence efficiency: exciton trapping at surface and interface traps, and non-radiative Auger recombination in QDs carrying either net charges or multiple excitons. In this work, we present a detailed study into the optical absorption, fluorescence dynamics and quantum yield, as well as ultrafast transient absorption properties of CdSe/CdS, CdSe/Cd0.5Zn0.5S, and CdSe/ZnS QDs as a function of shell thickness. It turns out that de-trapping processes play a pivotal role in determining steady state emission properties. By studying the excitation dependent photoluminescence quantum yields (PLQY) in different CdSe/CdxZn1-xS (x = 0, 0.5, 1) QDs, we demonstrate the different role played by hot and cold carrier trapping rates in determining fluorescence quantum yields. Finally, the use of global analysis allows us untangling the complex ultrafast transient absorption signals. Smoothing of interface potential, together with effective surface passivation, appear to be crucial factors in slowing down both Auger-based and exciton trapping recombination processes.

Exciton spectra of mixed LiH1-xDx crystals

International Nuclear Information System (INIS)

Plekhanov, V.G.

1989-01-01

The results of low-tempertaure experimental investigation of exciton spectra of pure surface of mixed crystals LiH 1-x d x forming the continuous series of a solved solution are presented. The long-wave reflection spectra is formed, as in pure crystals, by excitons of a large radius. The developed structure of spectra of exciton luminiscence consisting mainly of LO-lines, testifies to the intraband Frelich mechanism of free exciton scattering by LO-phonos, playing the considerable role in renormalization of the exciton Rydberg and the energy of interband transitions. Increase of the concentration of deuterium in mixed crystals causes a short-wave shift in the reflection spectrum and luminescence and continuous decrease of LO-phonon energy together with the increase of Rydberg exciton

Triplet exciton formation in organic photovoltaics

Energy Technology Data Exchange (ETDEWEB)

Yang, Xudong; Westenhoff, Sebastian; Howard, Ian; Ford, Thomas; Friend, Richard; Hodgkiss, Justin; Greenham, Neil [Cavendish Laboratory, University of Cambridge (United Kingdom)

2009-07-01

We have recently found that the formation of triplet excitons can be an important loss mechanism in organic photovoltaics, particularly in donor-acceptor blends designed to have high open-circuit voltages. This can occur when the intrachain triplet state lies lower in energy than the charge-transfer state formed at the heterojunction. We find that in a blend based on the polyfluorene derivatives F8BT and PFB, triplet excitons are formed after photoexcitation with much higher efficiency than in the component polymers. We use transient absorption spectroscopy to study the dynamics of charges and triplet excitons on timescales from picoseconds to microseconds. This allows us to determine a characteristic time of {proportional_to} 40 ns for intersystem crossing in the charge-separated state, and to estimate that as many as 75% of photoexcitations lead to the formation of triplet states. To avoid losses to triplet excitons in photovoltaic devices, it is necessary to separate charge pairs before intersystem crossing can occur. We also present photophysical measurements of saturation and relaxation of the triplet excited state absorption used to quantify triplet populations.

Photon-exchange energy transfer of an electron–hole plasma between quasi-two-dimensional semiconductor layers

International Nuclear Information System (INIS)

Lyo, S.K.

2012-01-01

Photon-mediated energy transfer is shown to play an important role for transfer of an electron–hole plasma between two quasi-two-dimensional quantum wells separated by a wide barrier. The magnitude and the dependence of the transfer rate of an electron–hole plasma on the temperature, the well-to-well distance, and the plasma density are compared with those of the standard Förster (i.e., dipolar) rate and also with the exciton transfer rate. The plasma transfer rate through the photon-exchange mechanism decays very slowly as a function of the well-to-well distance and is larger than the dipolar rate except for short distances. The transfer rate of plasmas saturates at high densities and decays rapidly with the temperature. - Highlights: ► We study energy transfer (ET) between two two-dimensional semiconductor quantum wells. ► We compare the ET rates of an electron–hole plasma (at a high density) and Mott excitons. ► We show that the proposed photon-exchange rate is practically dominant over the Förster rate. ► We examine the dependences of the ET rate on the temperature, density, and well-to-well distance.

Magneto-optical quantum interferences in a system of spinor excitons

Science.gov (United States)

Kuan, Wen-Hsuan; Gudmundsson, Vidar

2018-04-01

In this work we investigate magneto-optical properties of two-dimensional semiconductor quantum-ring excitons with Rashba and Dresselhaus spin-orbit interactions threaded by a magnetic flux perpendicular to the plane of the ring. By calculating the excitonic Aharonov-Bohm spectrum, we study the Coulomb and spin-orbit effects on the Aharonov-Bohm features. From the light-matter interactions of the excitons, we find that for scalar excitons, there are open channels for spontaneous recombination resulting in a bright photoluminescence spectrum, whereas the forbidden recombination of dipolar excitons results in a dark photoluminescence spectrum. We investigate the generation of persistent charge and spin currents. The exploration of spin orientations manifests that by adjusting the strength of the spin-orbit interactions, the exciton can be constructed as a squeezed complex with specific spin polarization. Moreover, a coherently moving dipolar exciton acquires a nontrivial dual Aharonov-Casher phase, creating the possibility to generate persistent dipole currents and spin dipole currents. Our study reveals that in the presence of certain spin-orbit generated fields, the manipulation of the magnetic field provides a potential application for quantum-ring spinor excitons to be utilized in nano-scaled magneto-optical switches.

Separate observation of ballistic and scattered photons in the propagation of short laser pulses through a strongly scattering medium

International Nuclear Information System (INIS)

Tereshchenko, Sergei A; Podgaetskii, Vitalii M; Vorob'ev, Nikolai S; Smirnov, A V

1998-01-01

The conditions are identified for simultaneous observation of the peaks of scattered and unscattered (ballistic) photons in a narrow pulsed laser beam crossing a strongly scattering medium. The experimental results are explained on the basis of a nonstationary two-flux model of radiation transport. An analytic expression is given for the contribution of ballistic photons to the transmitted radiation, as a function of the characteristics of the scattering medium. It is shown that the ballistic photon contribution can be increased by the use of high-contrast substances which alter selectively the absorption and scattering coefficients of the medium. (laser applications and other topics in quantum electronics)

Plexcitons: The Role of Oscillator Strengths and Spectral Widths in Determining Strong Coupling

Energy Technology Data Exchange (ETDEWEB)

Thomas, Reshmi [School; Thomas, Anoop [School; Pullanchery, Saranya [School; Joseph, Linta [School; Somasundaran, Sanoop Mambully [School; Swathi, Rotti Srinivasamurthy [School; Gray, Stephen K. [Center; Thomas, K. George [School

2018-01-05

Strong coupling interactions between plasmon and exciton-based excitations have been proposed to be useful in the design of optoelectronic systems. However, the role of various optical parameters dictating the plasmon-exciton (plexciton) interactions is less understood. Herein, we propose an inequality for achieving strong coupling between plasmons and excitons through appropriate variation of their oscillator strengths and spectral widths. These aspects are found to be consistent with experiments on two sets of free-standing plexcitonic systems obtained by (i) linking fluorescein isothiocyanate on Ag nanoparticles of varying sizes through silane coupling and (ii) electrostatic binding of cyanine dyes on polystyrenesulfonate-coated Au nanorods of varying aspect ratios. Being covalently linked on Ag nanoparticles, fluorescein isothiocyanate remains in monomeric state, and its high oscillator strength and narrow spectral width enable us to approach the strong coupling limit. In contrast, in the presence of polystyrenesulfonate, monomeric forms of cyanine dyes exist in equilibrium with their aggregates: Coupling is not observed for monomers and H-aggregates whose optical parameters are unfavorable. The large aggregation number, narrow spectral width, and extremely high oscillator strength of J-aggregates of cyanines permit effective delocalization of excitons along the linear assembly of chromophores, which in turn leads to efficient coupling with the plasmons. Further, the results obtained from experiments and theoretical models are jointly employed to describe the plexcitonic states, estimate the coupling strengths, and rationalize the dispersion curves. The experimental results and the theoretical analysis presented here portray a way forward to the rational design of plexcitonic systems attaining the strong coupling limits.

Hadronic photon-photon interactions at high energies

International Nuclear Information System (INIS)

Engel, R.; Siegen Univ.; Ranft, J.

1996-01-01

Photon-photon collisions are investigated in the framework of the two-component Dual Parton Model. The model contains contributions from direct, resolved soft and resolved hard interactions. All free parameters of the model are determined in fits to hadron-hadron and photon-hadron cross section data. The model is shown to agree well to hadron production data from hadron-hadron and photon-hadron collisions. The multiparticle production in hadron-hadron, photon-hadron and photon-photon collisions as predicted by the model is compared. Strong differences are only found as function of the transverse momentum variable. (author)

Optical and Excitonic Properties of Atomically Thin Transition-Metal Dichalcogenides

Science.gov (United States)

Berkelbach, Timothy C.; Reichman, David R.

2018-03-01

Starting with the isolation of a single sheet of graphene, the study of layered materials has been one of the most active areas of condensed matter physics, chemistry, and materials science. Single-layer transition-metal dichalcogenides are direct-gap semiconducting analogs of graphene that exhibit novel electronic and optical properties. These features provide exciting opportunities for the discovery of both new fundamental physical phenomena as well as innovative device platforms. Here, we review the progress associated with the creation and use of a simple microscopic framework for describing the optical and excitonic behavior of few-layer transition-metal dichalcogenides, which is based on symmetry, band structure, and the effective interactions between charge carriers in these materials. This approach provides an often quantitative account of experiments that probe the physics associated with strong electron–hole interactions in these quasi two-dimensional systems and has been successfully employed by many groups to both describe and predict emergent excitonic behavior in these layered semiconducting systems.

Competing role of Interactions in Synchronization of Exciton-Polariton condensates

Science.gov (United States)

Khan, Saeed; Tureci, Hakan E.

We present a theoretical study of synchronization dynamics in incoherently pumped exciton-polariton condensates in coupled traps. Our analysis is based on an expansion in non-Hermitian modes that take into account the trapping potential and the pump-induced complex-valued potential. We find that polariton-polariton and reservoir-polariton interactions play competing roles in the emergence of a synchronized phase as pumping power is increased, leading to qualitatively different synchronized phases. Crucially, these interactions can also act against each other to hinder synchronization. We present a phase diagram and explain the general characteristics of these phases using a generalized Adler equation. Our work sheds light on dynamics strongly influenced by competing interactions particular to incoherently pumped exciton-polariton condensates, which can lead to interesting features in recently engineered polariton lattices. This work was supported by the US Department of Energy, Office of Basic Energy Sciences, Division of Materials Sciences and Engineering.

Anisotropy of exciton spectrum and spin-orbit interactions in quantum wells in tilted magnetic field

International Nuclear Information System (INIS)

Olendski, Oleg; Shahbazyan, Tigran V

2006-01-01

We study theoretically excitonic energy spectrum and optical absorption in narrowgap semiconductor quantum wells in strong magnetic field. We show that, in the presence of an in-plane field component, the absorption coefficient exhibit a double-peak structure due to hybridization of bright and dark excitons. If both Rashba and Dresselhaus spin-orbit terms are present, the spectrum is anisotropic in in-plane field orientation with respect to [100] axis. In particular, the magnitude of the splitting can be tuned in a wide interval by varying the azimuthal angle of the in-plane field. The absorption spectrrum anisotropy would allow simultaneous measurement Dresselhaus and Rashba spin-orbit coefficients

Ultrastrong exciton-photon coupling in single and coupled organic microcavities

Science.gov (United States)

Liu, Bin; Bramante, Rosemary; Valle, Brent; Singer, Kenneth; Khattab, Tawfik; Williams, Jarrod; Twieg, Robert

2015-03-01

We have demonstrated ultrastrong light-matter coupling in organic planar microcavities composed of a neat glassy organic dye film between two metallic (aluminum) mirrors in a half-cavity configuration. Such cavities are characterized by Q factors around 10. Tuning the thickness of the organic layer enables the observation of the ultrastrong coupling regime. Via reflectivity measurements, we observe a very large Rabi splitting around 1.227 eV between upper and lower polariton branches at room temperature, and we detect polariton emission from the lower polariton branch via photoluminescence measurements. The large splitting is due to the large oscillator strength of the neat dye glass, and to the match of the low-Q cavity spectral width to the broad absorption width of the dye film material. We also study the interaction between excitonic states of neat glassy organic dye and cavity modes within coupled microcavity structures. The high-reflectivity mirrors are formed from distributed Bragg reflectors (DBR), which are multilayer films fabricated using the coextrusion process, containing alternating layers of high (SAN25, n =1.57) and low (Dyneon THV 220G, n =1.37) refractive index dielectric polymers. Nonlinear optical measurements will be discussed. This research was supported by the National Science Foundation Center for Layered Polymer Systems (CLiPS) under Grant Number DMR-0423914.

Probing long-lived dark excitons in self-assembled quantum dots

DEFF Research Database (Denmark)

Johansen, Jeppe; Julsgaard, Brian; Stobbe, Søren

2010-01-01

Long-lived dark exciton states are formed in self-assembled quantum dots due to the combination of the angular momentum of electrons and holes. The lifetime of dark excitons are determined by spin-flip processes that transfer dark excitons into radiative bright excitons. We employ time......-resolved spontaneous emission measurements in a modified local density of optical states to unambiguously record the spin-flip rate. Pronounced variations in the spin-flip rate with the quantum dot emission energy are observed demonstrating that the exciton storage time can be extended by controlling the quantum dot......, which illustrates the important role of interfaces for quantum dot based nanophotonic structures....

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.

Influence of excitonic effects on luminescence quantum yield in silicon

Energy Technology Data Exchange (ETDEWEB)

Sachenko, A.V.; Kostylyov, V.P.; Vlasiuk, V.M. [V. Lashkaryov Institute of Semiconductor Physics, NAS of Ukraine, 41 prospect Nauky, 03028 Kyiv (Ukraine); Sokolovskyi, I.O., E-mail: isokolovskyi@mun.ca [V. Lashkaryov Institute of Semiconductor Physics, NAS of Ukraine, 41 prospect Nauky, 03028 Kyiv (Ukraine); Department of Physics and Physical Oceanography, Memorial University of Newfoundland, St. John' s, NL, A1B 3X7 Canada (Canada); Evstigneev, M. [Department of Physics and Physical Oceanography, Memorial University of Newfoundland, St. John' s, NL, A1B 3X7 Canada (Canada)

2017-03-15

Nonradiative exciton lifetime in silicon is determined by comparison of the experimental and theoretical curves of bulk minority charge carriers lifetime on doping and excitation levels. This value is used to analyze the influence of excitonic effects on internal luminescence quantum yield at room temperature, taking into account both nonradiative and radiative exciton lifetimes. A range of Shockley-Hall-Reed lifetimes is found, where excitonic effects lead to an increase of internal luminescence quantum yield.

Strong Quantum Confinement Effects and Chiral Excitons in Bio-Inspired ZnO–Amino Acid Cocrystals

KAUST Repository

Muhammed, Madathumpady Abubaker Habeeb

2018-02-20

Elucidating the underlying principles behind band gap engineering is paramount for the successful implementation of semiconductors in photonic and optoelectronic devices. Recently it has been shown that the band gap of a wide and direct band gap semiconductor, such as ZnO, can be modified upon cocrystallization with amino acids, with the role of the biomolecules remaining unclear. Here, by probing and modeling the light-emitting properties of ZnO-amino acid cocrystals, we identify the amino acids\\' role on this band gap modulation and demonstrate their effective chirality transfer to the interband excitations in ZnO. Our 3D quantum model suggests that the strong band edge emission blue-shift in the cocrystals can be explained by a quasi-periodic distribution of amino acid potential barriers within the ZnO crystal lattice. Overall, our findings indicate that biomolecule cocrystallization can be used as a truly bio-inspired means to induce chiral quantum confinement effects in quasi-bulk semiconductors.

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

Energy Technology Data Exchange (ETDEWEB)

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

2015-05-15

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

Fractional Solitons in Excitonic Josephson Junctions

Science.gov (United States)

Su, Jung-Jung; Hsu, Ya-Fen

The Josephson effect is especially appealing because it reveals macroscopically the quantum order and phase. Here we study this effect in an excitonic Josephson junction: a conjunct of two exciton condensates with a relative phase ϕ0 applied. Such a junction is proposed to take place in the quantum Hall bilayer (QHB) that makes it subtler than in superconductor because of the counterflow of excitonic supercurrent and the interlayer tunneling in QHB. We treat the system theoretically by first mapping it into a pseudospin ferromagnet then describing it by the Landau-Lifshitz-Gilbert equation. In the presence of interlayer tunneling, the excitonic Josephson junction can possess a family of fractional sine-Gordon solitons that resemble the static fractional Josephson vortices in the extended superconducting Josephson junctions. Interestingly, each fractional soliton carries a topological charge Q which is not necessarily a half/full integer but can vary continuously. The resultant current-phase relation (CPR) shows that solitons with Q =ϕ0 / 2 π are the lowest energy states for small ϕ0. When ϕ0 > π , solitons with Q =ϕ0 / 2 π - 1 take place - the polarity of CPR is then switched.

Donor bound excitons in ZnSe nanoresonators - Applications in quantum information science

Energy Technology Data Exchange (ETDEWEB)

Pawlis, A. [Department of Physics, University of Paderborn, Warburger Str. 100, 33098 Paderborn, Germany and Edward L. Ginzton Laboratory, Stanford University, Stanford, California 94305-4088 (United States); Lischka, K. [Department of Physics, University of Paderborn, Warburger Str. 100, 33098 Paderborn (Germany); Sanaka, K.; Yamamoto, Y. [Edward L. Ginzton Laboratory, Stanford University, Stanford, California 94305-4088, USA and National Institute of Informatics, 2-1-2 Hitotsubashi, Chiyoda-ku, Tokyo 101-8430 (Japan); Sleiter, D. [Edward L. Ginzton Laboratory, Stanford University, Stanford, California 94305-4088 (United States)

2014-05-15

Here we summarize the advantages of excitons bound to isolated fluorine donor in ZnSe/ZnMgSe quantum well nano-structures. Devices based on these semiconductors, are particularly suited to implement concepts of the optical manipulation of quantum states in solid-state material. The fluorine donor in ZnSe provides a physical qubit with potential advantages over previously researched qubits. In this context we show several initial demonstrations of devices, such as a low-threshold microdisk laser and an indistinguishable single photon source. Additionally we demonstrate the realization of a controllable three-level-system qubit consisting of a single Fluorine donor in a ZnSe nano-pillar, which provides an optical accessible single electon spin qubit.

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...

Excitons and continuum transitions of rubidium halides in the 10 - 26 eV photon energy range at low temperatures

International Nuclear Information System (INIS)

Zierau, W.; Skibowski, M.

1975-04-01

The reflection spectra of RbCl, RbBr and RbI single crystals were investigated for temperatures between 300 K and 8 K in order to study excitations from the Rb + 4p level (> approximately 16 eV) as well as the higher continuum transitions from the valence band (> approximately 10 eV). The measurements were performed by use of the synchrotron radiation of DESY. The sensitivity for detecting details of the fine structure was increased by simultaneously measuring the wavelength modulated spectra. The experimental procedure is briefly described. New spectral features have been resolved for the exciton multiplets from the Rb + 4p level. They are discussed in light of the predictions of a recent model for the Rb + 4p excitons based on ligand field theory. The continuum transitions associated with the valence band and the Rb + 4p level show characteristic structure which is compared with calculations of the joint density of states. (orig.) [de

Angular momentum transport with twisted exciton wave packets

Science.gov (United States)

Zang, Xiaoning; Lusk, Mark T.

2017-10-01

A chain of cofacial molecules with CN or CN h symmetry supports excitonic states with a screwlike structure. These can be quantified with the combination of an axial wave number and an azimuthal winding number. Combinations of these states can be used to construct excitonic wave packets that spiral down the chain with well-determined linear and angular momenta. These twisted exciton wave packets can be created and annihilated using laser pulses, and their angular momentum can be optically modified during transit. This allows for the creation of optoexcitonic circuits in which information, encoded in the angular momentum of light, is converted into excitonic wave packets that can be manipulated, transported, and then reemitted. A tight-binding paradigm is used to demonstrate the key ideas. The approach is then extended to quantify the evolution of twisted exciton wave packets in a many-body, multilevel time-domain density functional theory setting. In both settings, numerical methods are developed that allow the site-to-site transfer of angular momentum to be quantified.

Exciton Transport Simulations in Phenyl Cored Thiophene Dendrimers

Science.gov (United States)

Kim, Kwiseon; Erkan Kose, Muhammet; Graf, Peter; Kopidakis, Nikos; Rumbles, Garry; Shaheen, Sean E.

2009-03-01

Phenyl cored 3-arm and 4-arm thiophene dendrimers are promising materials for use in photovoltaic devices. It is important to understand the energy transfer mechanisms in these molecules to guide the synthesis of novel dendrimers with improved efficiency. A method is developed to estimate the exciton diffusion lengths for the dendrimers and similar chromophores in amorphous films. The approach exploits Fermi's Golden Rule to estimate the energy transfer rates for an ensemble of bimolecular complexes in random orientations. Using Poisson's equation to evaluate Coulomb integrals led to efficient calculation of excitonic couplings between the transition densities. Monte-Carlo simulations revealed the dynamics of energy transport in the dendrimers. Experimental exciton diffusion lengths of the dendrimers range 10 ˜ 20 nm, increasing with the size of the dendrimer. Simulated diffusion lengths correlate well with experiments. The chemical structure of the chromophore, the shape of the transition densities and the exciton lifetime are found to be the most important factors that determine the exciton diffusion length in amorphous films.

Excitonic terahertz photoconductivity in intrinsic semiconductor nanowires

Science.gov (United States)

Yan, Jie-Yun

2018-06-01

Excitonic terahertz photoconductivity in intrinsic semiconductor nanowires is studied. Based on the excitonic theory, the numerical method to calculate the photoconductivity spectrum in the nanowires is developed, which can simulate optical pump terahertz-probe spectroscopy measurements on real nanowires and thereby calculate the typical photoconductivity spectrum. With the help of the energetic structure deduced from the calculated linear absorption spectrum, the numerically observed shift of the resonant peak in the photoconductivity spectrum is found to result from the dominant exciton transition between excited or continuum states to the ground state, and the quantitative analysis is in good agreement with the quantum plasmon model. Besides, the dependence of the photoconductivity on the polarization of the terahertz field is also discussed. The numerical method and supporting theoretical analysis provide a new tool for experimentalists to understand the terahertz photoconductivity in intrinsic semiconductor nanowires at low temperatures or for nanowires subjected to below bandgap photoexcitation, where excitonic effects dominate.

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.

Hopping approach towards exciton dissociation in conjugated polymers

International Nuclear Information System (INIS)

Emelianova, E. V.; Auweraer, M. van der; Baessler, H.

2008-01-01

By employing random walk an analytic theory for the dissociation of singlet excitons in a random organic solid, for instance, a conjugated polymer, has been developed. At variance of conventional three-dimensional Onsager theory, it is assumed that an exciton with finite lifetime can first transfer endothermically an electron to an adjacent site, thereby generating a charge transfer state whose energy is above the energy of that of the initial exciton. In a second step the latter can fully dissociate in accordance with Onsager's concept Brownian motion. The results indicate that, depending of the energy required for the first jump, the first jump contributes significantly to the field dependence of the dissociation yield. Disorder weakens the temperature dependence of the yield dramatically and precludes extracting information on the exciton binding energy from it

Resonant transfer of excitons and quantum computation

International Nuclear Information System (INIS)

Lovett, Brendon W.; Reina, John H.; Nazir, Ahsan; Kothari, Beeneet; Briggs, G. Andrew D.

2003-01-01

Resonant energy transfer mechanisms have been observed in the sensitized luminescence of solids, and in quantum dots, molecular nanostructures, and photosynthetic organisms. We demonstrate that such mechanisms, together with the exciton-exciton binding energy shift typical of these nanostructures, can be used to perform universal quantum logic and generate quantum entanglement

Exciton dephasing in ZnSe quantum wires

DEFF Research Database (Denmark)

Wagner, Hans Peter; Langbein, Wolfgang Werner; Hvam, Jørn Märcher

1998-01-01

The homogeneous linewidths of excitons in wet-etched ZnSe quantum wires of lateral sizes down to 23 nm are studied by transient four-wave mixing. The low-density dephasing time is found to increase with decreasing wire width. This is attributed mainly to a reduction of electron-exciton scattering...

Entangled exciton states in quantum dot molecules

Science.gov (United States)

Bayer, Manfred

2002-03-01

Currently there is strong interest in quantum information processing(See, for example, The Physics of Quantum Information, eds. D. Bouwmeester, A. Ekert and A. Zeilinger (Springer, Berlin, 2000).) in a solid state environment. Many approaches mimic atomic physics concepts in which semiconductor quantum dots are implemented as artificial atoms. An essential building block of a quantum processor is a gate which entangles the states of two quantum bits. Recently a pair of vertically aligned quantum dots has been suggested as optically driven quantum gate(P. Hawrylak, S. Fafard, and Z. R. Wasilewski, Cond. Matter News 7, 16 (1999).)(M. Bayer, P. Hawrylak, K. Hinzer, S. Fafard, M. Korkusinski, Z.R. Wasilewski, O. Stern, and A. Forchel, Science 291, 451 (2001).): The quantum bits are individual carriers either on dot zero or dot one. The different dot indices play the same role as a "spin", therefore we call them "isospin". Quantum mechanical tunneling between the dots rotates the isospin and leads to superposition of these states. The quantum gate is built when two different particles, an electron and a hole, are created optically. The two particles form entangled isospin states. Here we present spectrocsopic studies of single self-assembled InAs/GaAs quantum dot molecules that support the feasibility of this proposal. The evolution of the excitonic recombination spectrum with varying separation between the dots allows us to demonstrate coherent tunneling of carriers across the separating barrier and the formation of entangled exciton states: Due to the coupling between the dots the exciton states show a splitting that increases with decreasing barrier width. For barrier widths below 5 nm it exceeds the thermal energy at room temperature. For a given barrier width, we find only small variations of the tunneling induced splitting demonstrating a good homogeneity within a molecule ensemble. The entanglement may be controlled by application of electromagnetic field. For

Photoluminescence dynamics of weakly confined excitons in GaAs thin films

International Nuclear Information System (INIS)

Kanno, Atsushi; Katouf, Redouane; Kojima, Osamu; Ishi-Hayase, Junko; Sasaki, Masahide; Tsuchiya, Masahiro; Isu, Toshiro

2008-01-01

We investigate the dynamics of weakly confined excitons in GaAs thin films measured by time-resolved photoluminescence (PL) technique. When excitation energy was above the resonant energy of the exciton, a long PL rise time of about 200 ps was observed. It is considered that an exciton formation process from excited continuum energy states to discrete energy states of the exciton in the thin film causes the slow PL rise. The observed PL decay time constant was about 14 ns due to high quality fabricated samples. The observed population dynamics can be surely ascribed to the specific features of weakly confined excitons

Integration of Single-Photon Sources and Detectors on GaAs

Directory of Open Access Journals (Sweden)

Giulia Enrica Digeronimo

2016-10-01

Full Text Available Quantum photonic integrated circuits (QPICs on a GaAs platform allow the generation, manipulation, routing, and detection of non-classical states of light, which could pave the way for quantum information processing based on photons. In this article, the prototype of a multi-functional QPIC is presented together with our recent achievements in terms of nanofabrication and integration of each component of the circuit. Photons are generated by excited InAs quantum dots (QDs and routed through ridge waveguides towards photonic crystal cavities acting as filters. The filters with a transmission of 20% and free spectral range ≥66 nm are able to select a single excitonic line out of the complex emission spectra of the QDs. The QD luminescence can be measured by on-chip superconducting single photon detectors made of niobium nitride (NbN nanowires patterned on top of a suspended nanobeam, reaching a device quantum efficiency up to 28%. Moreover, two electrically independent detectors are integrated on top of the same nanobeam, resulting in a very compact autocorrelator for on-chip g(2(τ measurements.

Tailorable Exciton Transport in Doped Peptide–Amphiphile Assemblies

Energy Technology Data Exchange (ETDEWEB)

Solomon, Lee A. [Center; Sykes, Matthew E. [Center; Wu, Yimin A. [Center; Schaller, Richard D. [Center; Department; Wiederrecht, Gary P. [Center; Fry, H. Christopher [Center

2017-08-29

Light-harvesting biomaterials are an attractive target in photovoltaics, photocatalysis, and artificial photosynthesis. Through peptide self-assembly, complex nanostructures can be engineered to study the role of chromophore organization during light absorption and energy transport. To this end, we demonstrate the one-dimensional transport of excitons along naturally occurring, light-harvesting, Zn-protoporphyrin IX chromophores within self-assembled peptide-amphiphile nanofibers. The internal structure of the nanofibers induces packing of the porphyrins into linear chains. We find that this peptide assembly can enable long-range exciton diffusion, yet it also induces the formation of excimers between adjacent molecules, which serve as exciton traps. Electronic coupling between neighboring porphyrin molecules is confirmed by various spectroscopic methods. The exciton diffusion process is then probed through transient photoluminescence and absorption measurements and fit to a model for one-dimensional hopping. Because excimer formation impedes exciton hopping, increasing the interchromophore spacing allows for improved diffusivity, which we control through porphyrin doping levels. We show that diffusion lengths of over 60 nm are possible at low porphyrin doping, representing an order of magnitude improvement over the highest doping fractions.

Sample-averaged biexciton quantum yield measured by solution-phase photon correlation.

Science.gov (United States)

Beyler, Andrew P; Bischof, Thomas S; Cui, Jian; Coropceanu, Igor; Harris, Daniel K; Bawendi, Moungi G

2014-12-10

The brightness of nanoscale optical materials such as semiconductor nanocrystals is currently limited in high excitation flux applications by inefficient multiexciton fluorescence. We have devised a solution-phase photon correlation measurement that can conveniently and reliably measure the average biexciton-to-exciton quantum yield ratio of an entire sample without user selection bias. This technique can be used to investigate the multiexciton recombination dynamics of a broad scope of synthetically underdeveloped materials, including those with low exciton quantum yields and poor fluorescence stability. Here, we have applied this method to measure weak biexciton fluorescence in samples of visible-emitting InP/ZnS and InAs/ZnS core/shell nanocrystals, and to demonstrate that a rapid CdS shell growth procedure can markedly increase the biexciton fluorescence of CdSe nanocrystals.

2D optical photon echo spectroscopy of a self-assembled quantum dot

International Nuclear Information System (INIS)

Fingerhut, Benjamin P.; Mukamel, Shaul; Richter, Marten; Luo, Jun-Wei; Zunger, Alex

2013-01-01

Simulations of two dimensional coherent photon echo (2D-PE) spectra of self-assembled InAs/GaAs quantum dots (QD) in different charged states are presented revealing the coupling between the individual mono-exciton X q transitions and contributions of bi-excitons XX q . The information about the XX q states is crucial for various application scenarios of QDs, like e.g. highly efficient solar cells. The simulations rely on a microscopic description of the electronic structure by high-level atomistic many-body pseudopotential calculations. It is shown that asymmetric diagonal peak shapes and double cross-peaks are the result of XX q state contributions to the PE signal by analyzing the contributions of the individual pathways excited state emission, ground state bleach and excited state absorption. The results show that from the detuned X q and XX q contributions the bi-exciton binding energies of the XX q manifold are revealed in 2D-PE signals. (copyright 2012 by WILEY-VCH Verlag GmbH and Co. KGaA, Weinheim)

Excitonic AND Logic Gates on DNA Brick Nanobreadboards

Science.gov (United States)

2015-01-01

A promising application of DNA self-assembly is the fabrication of chromophore-based excitonic devices. DNA brick assembly is a compelling method for creating programmable nanobreadboards on which chromophores may be rapidly and easily repositioned to prototype new excitonic devices, optimize device operation, and induce reversible switching. Using DNA nanobreadboards, we have demonstrated each of these functions through the construction and operation of two different excitonic AND logic gates. The modularity and high chromophore density achievable via this brick-based approach provide a viable path toward developing information processing and storage systems. PMID:25839049

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.

Radiative recombination of excitons in amorphous semiconductors

International Nuclear Information System (INIS)

Singh, Jai

2005-01-01

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

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.

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...... times slower in the lateral direction between aggregates. Exciton hopping between aggregates is found to show a subtle dependence on interchain coupling, aggregate size, and Boltzmann statistics. Additionally, a clear correlation is observed between the effective exciton diffusion coefficient...

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.

Pool-Frenkel thermoelectric modulation of exciton photoluminescence in GaSe crystals

International Nuclear Information System (INIS)

Ertap, H.; Mamedov, G.M.; Karabulut, M.; Bacioglu, A.

2011-01-01

Effect of external field on the exciton photoluminescence of GaSe crystals has been investigated and it has been observed that the PL is quenched with the applied field. The changes observed in the PL spectra have been analyzed with impact exciton, Franz-Keldysh and Pool-Frenkel effects. From the analyses of the experimental data, it has been found that the intensity of direct free, indirect free and bound exciton peaks decreased exponentially with the square root of applied field as I∼exp-β√E. The energy positions of emission peaks were found to shift to longer wavelength with the applied field as ΔE∼β√E. From these findings, the Pool-Frenkel thermoelectric field effect is seen to be the dominant mechanism in the variation of exciton PL with the applied field even though the impact exciton and Franz-Keldysh effects contribute. - Highlights: → Exciton PL intensity varies with the applied field. It decreases with the square root of E in accordance with Pool-Frenkel effect. → In the intrinsic region of PL spectrum, lines belonging to direct and indirect free/bound excitons were observed. → Line positions shifted to longer wavelengths with the applied field. → It was shown that amplitude modulation of exciton PL with electric field was possible.

Photon-photon and photon-hadron processes in relativistic heavy ion collisions

International Nuclear Information System (INIS)

Baron, N.C.

1993-11-01

Photon-photon and photon-hadron interactions in relativistic heavy ion collisions are studied in the framework of the impact parameter dependent equivalent photon approximation. Improvements of this method, like formfactor inclusion and geometrical modifications are developed. In disruptive relativistic heavy ion collisions where the heavy ions overlapp during the collision, electromagnetic processes are an important background to other mechanisms. In peripheral (non-disruptive) relativistic heavy ion collisions where the ions pass each other without strong interactions, the electromagnetic processes can be studied in their pure form. The lepton pair production is an important diagnostic tool in relativistic heavy ion collisions. The coherent γγ lepton pair production is therefore extensively studied in disruptive but also in non-disruptive collisions. The effects of strong interactions on the coherent γγ lepton pair production in disruptive collisions are discussed in terms of a simple stopping model. Coherent γγ dielectron production contributes to the dilepton production in high energy hadron-hadron collisions. As an example, the coherent dielectron production in π - p collisions is studied in terms of the equivalent photon approximation. Peripheral ultrarelativistic heavy ion collisions open up new possibilities for γγ physics. Taking into account γA background reactions, typical γγ processes in the relevant invariant mass ranges are discussed. The extreme high energy part of the equivalent photon spectrum leads to hard photon-parton reactions. As a potential tool to investigate the gluon distribution function of nucleons, thee q anti q production via the γg fusion in ultrarelativistic heavy ion collisions is studied. It is the purpose of this work to investigate how photon-photon and photon-hadron reactions in relativistic heavy ion collisions may contribute to the understanding of QCD and the standard model. (orig.) [de

Extension of the radiative lifetime of Wannier-Mott excitons in semiconductor nanoclusters

International Nuclear Information System (INIS)

Kukushkin, V. A.

2015-01-01

The purpose of the study is to calculate the radiative lifetime of Wannier-Mott excitons in three-dimensional potential wells formed of direct-gap narrow-gap semiconductor nanoclusters in wide-gap semiconductors and assumed to be large compared to the exciton radius. Calculations are carried out for the InAs/GaAs heterosystem. It is shown that, as the nanocluster dimensions are reduced to values on the order of the exciton radius, the exciton radiative lifetime becomes several times longer compared to that in a homogeneous semiconductor. The increase in the radiative lifetime is more pronounced at low temperatures. Thus, it is established that the placement of Wannier-Mott excitons into direct-gap semiconductor nanoclusters, whose dimensions are of the order of the exciton radius, can be used for considerable extension of the exciton radiative lifetime

Correction of the exciton Bohr radius in monolayer transition metal dichalcogenides

Science.gov (United States)

Li, Run-Ze; Dong, Xi-Ying; Li, Zhi-Qing; Wang, Zi-Wu

2018-07-01

We theoretically investigate the correction of exciton Bohr radius in monolayer transition metal dichalcogenides (TMDCs) on different polar substrates arising from the exciton-optical phonon coupling, in which both the intrinsic longitudinal optical phonon and surface optical phonon modes couple with the exciton are taken into account. We find that the exciton Bohr radius is enlarged markedly due to these coupling. Moreover, it can be changed on a large scale by modulating the polarizability of polar substrate and the internal distance between the monolayer TMDCs and polar substrate. Theoretical result provides a potential explanation for the variation of the exciton Bohr radius in experimental measurement.

Quantum optical signatures in strong-field laser physics: Infrared photon counting in high-order-harmonic generation.

Science.gov (United States)

Gonoskov, I A; Tsatrafyllis, N; Kominis, I K; Tzallas, P

2016-09-07

We analytically describe the strong-field light-electron interaction using a quantized coherent laser state with arbitrary photon number. We obtain a light-electron wave function which is a closed-form solution of the time-dependent Schrödinger equation (TDSE). This wave function provides information about the quantum optical features of the interaction not accessible by semi-classical theories. With this approach we can reveal the quantum optical properties of high harmonic generation (HHG) process in gases by measuring the photon statistics of the transmitted infrared (IR) laser radiation. This work can lead to novel experiments in high-resolution spectroscopy in extreme-ultraviolet (XUV) and attosecond science without the need to measure the XUV light, while it can pave the way for the development of intense non-classical light sources.

Exciton diffusion in WSe2 monolayers embedded in a van der Waals heterostructure

Science.gov (United States)

Cadiz, F.; Robert, C.; Courtade, E.; Manca, M.; Martinelli, L.; Taniguchi, T.; Watanabe, K.; Amand, T.; Rowe, A. C. H.; Paget, D.; Urbaszek, B.; Marie, X.

2018-04-01

We have combined spatially resolved steady-state micro-photoluminescence with time-resolved photoluminescence to investigate the exciton diffusion in a WSe2 monolayer encapsulated with hexagonal boron nitride. At 300 K, we extract an exciton diffusion length of LX = 0.36 ± 0.02 μm and an exciton diffusion coefficient of DX = 14.5 ± 2 cm2/s. This represents a nearly 10-fold increase in the effective mobility of excitons with respect to several previously reported values on nonencapsulated samples. At cryogenic temperatures, the high optical quality of these samples has allowed us to discriminate the diffusion of the different exciton species: bright and dark neutral excitons, as well as charged excitons. The longer lifetime of dark neutral excitons yields a larger diffusion length of LXD=1.5 ±0.02 μ m.

Photon antibunching in single-walled carbon nanotubes at telecommunication wavelengths and room temperature

Energy Technology Data Exchange (ETDEWEB)

Endo, Takumi, E-mail: endou@az.appi.keio.ac.jp; Ishi-Hayase, Junko; Maki, Hideyuki, E-mail: maki@appi.keio.ac.jp [Department of Applied Physics and Physico-Informatics, Keio University, Yokohama 223-8522 (Japan)

2015-03-16

We investigated the photoluminescence of individual air-suspended single-walled carbon nanotubes (SWNTs) from 6 to 300 K. Time-resolved and antibunching measurements over the telecommunication wavelength range were performed using a superconducting single-photon detector. We detected moderate temperature independent antibunching behavior over the whole temperature range studied. To investigate the exciton dynamics, which is responsible for the antibunching behavior, we measured excitation-power and temperature dependence of the photoluminescence spectra and lifetime decay curves. These measurements suggested an exciton confinement effect that is likely caused by high-dielectric amorphous carbon surrounding the SWNTs. These results indicate that SWNTs are good candidates for light sources in quantum communication technologies operating in the telecommunication wavelength range and at room temperature.

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......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...

Stark effect of optical properties of excitons in a quantum nanorod with parabolic confinement

Energy Technology Data Exchange (ETDEWEB)

Lyo, S.K., E-mail: sklyo@uci.edu

2014-01-15

We study the quantum Stark effect of optical properties of a quasi-one-dimensional quantum rod with parabolic confinement. Interplays between the competing/cooperative forces from confinement, electron–hole (e–h) attraction, and an external field are examined by studying the binding energy, the oscillator strength, and the root-mean-square (RMS) average of the e–h separation in a nonlinear electric field. In a long rod with weak confinement, the e–h interaction dominates over the confinement effect, yielding an abrupt drop of the exciton binding energy, oscillator strength, and a sudden increase of the RMS average e–h separation as the excitons are dissociated at the threshold field as the field increases. The exciton-dissociation transition is gradual in a short rod, where the confinement force dominates over the e–h attraction. We show that a DC field can induce an optically active excited exciton state in a narrow field range, causing a sharp peak in the oscillator strength and a dip in the RMS average of the e–h separation as the field increases. The Stark effects are also investigated as a function of the linear confinement length (i.e., rod length) at fixed fields. -- Highlights: • Study the dependence of optical properties of nanorods on the rod size and field. • Study the interplay between forces of confinement, Coulomb attraction, and field. • A strong field induces an optically active excited state observed in quantum dots.

The effect of excitons on CdTe solar cells

International Nuclear Information System (INIS)

Karazhanov, S. Zh.; Zhang, Y.; Mascarenhas, A.; Deb, S.

2000-01-01

Temperature and doping-level dependence of CdTe solar cells is investigated, taking into account the involvement of excitons on photocurrent transport. We show that the density of excitons in CdTe is comparable with that of minority carriers at doping levels ≥10 15 cm -3 . From the investigation of the dark-saturation current, we show that the product of electron and hole concentrations at equilibrium is several orders of magnitude more than the square of the intrinsic carrier concentration. With this assumption, we have studied the effect of excitons on CdTe solar cells, and the effect is negative. CdTe solar cell performance with excitons included agrees well with existing experimental results. (c) 2000 American Institute of Physics

Porous silicon: silicon quantum dots for photonic applications

International Nuclear Information System (INIS)

Pavesi, L.; Guardini, R.

1996-01-01

Porous silicon formation and structure characterization are briefly illustrated. Its luminescence properties rae presented and interpreted on the basis of exciton recombination in quantum dot structures: the trap-controlled hopping mechanism is used to describe the recombination dynamics. Porous silicon application to photonic devices is considered: porous silicon multilayer in general, and micro cavities in particular are described. The present situation in the realization of porous silicon LEDs is considered, and future developments in this field of research are suggested. (author). 30 refs., 30 figs., 13 tabs

Radiative recombination process of high density excitons in CdS crystals

Energy Technology Data Exchange (ETDEWEB)

Dneprovskij, V.S.; Klimov, V.I.; Martynenko, E.D.; Stadnik, V.A.

1983-11-01

The behaviour of the P-, E-, L- and Q-lines of luminescence in CdS is compared with calculated results for the processes of exciton-exciton scattering, exciton-electron scattering, annihilation of equilibrium electron-hole fluid (EHF), annihilation of electron-hole plasma (processes of amplification and reabsorption are taken into account). The comparison permitted to determine parameters of high density exciton gas and EHF. Spectral-kinetic properties of generation are investigated, and amplification factor in CdS is estimated.

Effect of disorder on exciton dissociation in conjugated polymers

International Nuclear Information System (INIS)

Feng Yuwen; Zhao Hui; Chen Yuguang; Yan Yonghong

2017-01-01

By using a multi-configurational time-dependent Hartree–Fock (MCTDHF) method for the time-dependent Schrödinger equation and a Newtonian equation of motion for lattice, we investigate the disorder effects on the dissociation process of excitons in conjugated polymer chains. The simulations are performed within the framework of an extended version of the Su–Schrieffer–Heeger model modified to include on-site disorder, off-diagonal, electron–electron interaction, and an external electric field. Our results show that Coulomb correlation effects play an important role in determining the exciton dissociation process. The electric field required to dissociate an exciton can practically impossibly occur in a pure polymer chain, especially in the case of triplet exciton. However, when the on-site disorder effects are taken into account, this leads to a reduction in mean dissociation electric fields. As the disorder strength increases, the dissociation field decreases effectively. On the contrary, the effects of off-diagonal disorder are negative in most cases. Moreover, the dependence of exciton dissociation on the conjugated length is also discussed. (paper)

Phosphorene/ZnO Nano-Heterojunctions for Broadband Photonic Nonvolatile Memory Applications.

Science.gov (United States)

Hu, Liang; Yuan, Jun; Ren, Yi; Wang, Yan; Yang, Jia-Qin; Zhou, Ye; Zeng, Yu-Jia; Han, Su-Ting; Ruan, Shuangchen

2018-06-10

High-performance photonic nonvolatile memory combining photosensing and data storage with low power consumption ensures the energy efficiency of computer systems. This study first reports in situ derived phosphorene/ZnO hybrid heterojunction nanoparticles and their application in broadband-response photonic nonvolatile memory. The photonic nonvolatile memory consistently exhibits broadband response from ultraviolet (380 nm) to near infrared (785 nm), with controllable shifts of the SET voltage. The broadband resistive switching is attributed to the enhanced photon harvesting, a fast exciton separation, as well as the formation of an oxygen vacancy filament in the nano-heterojunction. In addition, the device exhibits an excellent stability under air exposure compared with reported pristine phosphorene-based nonvolatile memory. The superior antioxidation capacity is believed to originate from the fast transfer of lone-pair electrons of phosphorene. The unique assembly of phosphorene/ZnO nano-heterojunctions paves the way toward multifunctional broadband-response data-storage techniques. © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

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

Rigorous numerical study of strong microwave photon-magnon coupling in all-dielectric magnetic multilayers

Energy Technology Data Exchange (ETDEWEB)

Maksymov, Ivan S., E-mail: ivan.maksymov@uwa.edu.au [School of Physics M013, The University of Western Australia, 35 Stirling Highway, Crawley, WA 6009 (Australia); ARC Centre of Excellence for Nanoscale BioPhotonics, School of Applied Sciences, RMIT University, Melbourne, VIC 3001 (Australia); Hutomo, Jessica; Nam, Donghee; Kostylev, Mikhail [School of Physics M013, The University of Western Australia, 35 Stirling Highway, Crawley, WA 6009 (Australia)

2015-05-21

We demonstrate theoretically a ∼350-fold local enhancement of the intensity of the in-plane microwave magnetic field in multilayered structures made from a magneto-insulating yttrium iron garnet (YIG) layer sandwiched between two non-magnetic layers with a high dielectric constant matching that of YIG. The enhancement is predicted for the excitation regime when the microwave magnetic field is induced inside the multilayer by the transducer of a stripline Broadband Ferromagnetic Resonance (BFMR) setup. By means of a rigorous numerical solution of the Landau-Lifshitz-Gilbert equation consistently with the Maxwell's equations, we investigate the magnetisation dynamics in the multilayer. We reveal a strong photon-magnon coupling, which manifests itself as anti-crossing of the ferromagnetic resonance magnon mode supported by the YIG layer and the electromagnetic resonance mode supported by the whole multilayered structure. The frequency of the magnon mode depends on the external static magnetic field, which in our case is applied tangentially to the multilayer in the direction perpendicular to the microwave magnetic field induced by the stripline of the BFMR setup. The frequency of the electromagnetic mode is independent of the static magnetic field. Consequently, the predicted photon-magnon coupling is sensitive to the applied magnetic field and thus can be used in magnetically tuneable metamaterials based on simultaneously negative permittivity and permeability achievable thanks to the YIG layer. We also suggest that the predicted photon-magnon coupling may find applications in microwave quantum information systems.

Effects of excitation spectral width on decay profile of weakly confined excitons

International Nuclear Information System (INIS)

Kojima, O.; Isu, T.; Ishi-Hayase, J.; Kanno, A.; Katouf, R.; Sasaki, M.; Tsuchiya, M.

2008-01-01

We report the effect due to a simultaneous excitation of several exciton states on the radiative decay profiles on the basis of the nonlocal response of weakly confined excitons in GaAs thin films. In the case of excitation of single exciton state, the transient grating signal has two decay components. The fast decay component comes from nonlocal response, and the long-lived component is attributed to free exciton decay. With an increase of excitation spectral width, the nonlocal component becomes small in comparison with the long-lived component, and disappears under irradiation of a femtosecond-pulse laser with broader spectral width. The transient grating spectra clearly indicates the contribution of the weakly confined excitons to the signal, and the exciton line width hardly changes by excitation spectral width. From these results, we concluded that the change of decay profile is attributed not to the many-body effect but to the effect of simultaneous excitation of several exciton states

Large-k exciton dynamics in GaN epilayers: Nonthermal and thermal regimes

Science.gov (United States)

Vinattieri, Anna; Bogani, Franco; Cavigli, Lucia; Manzi, Donatella; Gurioli, Massimo; Feltin, Eric; Carlin, Jean-François; Martin, Denis; Butté, Raphaël; Grandjean, Nicolas

2013-02-01

We present a detailed investigation performed at low temperature (T<50 K) concerning the exciton dynamics in GaN epilayers grown on c-plane sapphire substrates, focusing on the exciton formation and the transition from the nonthermal to the thermal regime. The time-resolved kinetics of longitudinal-optical-phonon replicas is used to address the energy relaxation in the excitonic band. From picosecond time-resolved spectra, we bring evidence for a long lasting nonthermal excitonic distribution, which accounts for the first 50 ps. Such a behavior is confirmed in different experimental conditions when both nonresonant and resonant excitations are used. At low excitation power density, the exciton formation and their subsequent thermalization are dominated by impurity scattering rather than by acoustic phonon scattering. The estimate of the average energy of the excitons as a function of delay after the excitation pulse provides information on the relaxation time, which describes the evolution of the exciton population to the thermal regime.

Highly mobile charge-transfer excitons in two-dimensional WS2/tetracene heterostructures

Science.gov (United States)

Zhu, Tong; Yuan, Long; Zhao, Yan; Zhou, Mingwei; Wan, Yan; Mei, Jianguo; Huang, Libai

2018-01-01

Charge-transfer (CT) excitons at heterointerfaces play a critical role in light to electricity conversion using organic and nanostructured materials. However, how CT excitons migrate at these interfaces is poorly understood. We investigate the formation and transport of CT excitons in two-dimensional WS2/tetracene van der Waals heterostructures. Electron and hole transfer occurs on the time scale of a few picoseconds, and emission of interlayer CT excitons with a binding energy of ~0.3 eV has been observed. Transport of the CT excitons is directly measured by transient absorption microscopy, revealing coexistence of delocalized and localized states. Trapping-detrapping dynamics between the delocalized and localized states leads to stretched-exponential photoluminescence decay with an average lifetime of ~2 ns. The delocalized CT excitons are remarkably mobile with a diffusion constant of ~1 cm2 s−1. These highly mobile CT excitons could have important implications in achieving efficient charge separation. PMID:29340303

Exciton luminescence in CdxMn1-xTe compounds

International Nuclear Information System (INIS)

Caraman, M.; Gashin, P.; Metelitsa, Snejana; Nicorici, Valentina; Nicorici, A.

2002-01-01

The Cd x Mn 1-x Te (0.5 7 W/cm 2 . The luminescence spectra were observed at 78 K. The results of the study had shown that the presence of relatively narrow luminescence peaks localized in the region of the fundamental absorption edge is characteristic for these spectra and for the majority of the crystals a wide maximum in the long wavelength region is observed. The luminescence maxima with an accuracy of ∼ 5 meV correspond to the resonance energy of the excitons of the state with n=1 determined from the absorption spectra. Hence, these maxima can be considered as exciton luminescence stimulated either by the excitons of the state n=1 or bounded to the exciton ionization centers. From the analysis of the absorption and exciton luminescence spectra one can make a conclusion about the fact that the homogeneity extent of the crystals decreases from CdTe to the compounds with x= 0.8 - 0.7 and slightly increases at the x decrease to 0.5. The exciton luminescence lines in CdTe and Cd 0.99 Mn 0.01 Te crystals is shifting by 7 - 10 meV relatively to the lines of free excitons absorption. This fact is explained by the fact that in these crystals, probably, excitons bounding to the lattice inherited defects with the binding energy of 7 - 10 meV participate in the luminescence. In the long wavelength region a wide peak is observed on which the impurity lines are not displayed. In the luminescence spectra of CdTe with 0.1%. As crystals three maxima at 1.51 eV, 1.46 eV and 1.42 eV are revealed. For pure CdTe the maximum at 1.4 eV is also revealed. These maxima are explained by the luminescence through the recombination levels localized at 0.46 eV. (authors)

Anisotropic Exciton Rabi Oscillation in Single Telecommunication-Band Quantum Dot

Science.gov (United States)

Toshiyuki Miyazawa,; Toshihiro Nakaoka,; Katsuyuki Watanabe,; Naoto Kumagai,; Naoki Yokoyama,; Yasuhiko Arakawa,

2010-06-01

Anisotropic Rabi oscillation in the exciton state in a single InAs/GaAs quantum dot (QD) was demonstrated in the telecommunication-band by selecting two orthogonal polarization angles of the excitation laser. Our InAs QDs were embedded in an intrinsic layer of an n-i-Schottky diode, which provides an electric field to extract photoexcited carriers from QDs. Owing to the potential anisotropy of QDs, the fine structure splitting (FSS) energy in the exciton state in single InAs QDs was ˜110 μeV, measured by polarization-resolved photocurrent spectroscopy. The ratio between two different Rabi frequencies, which reflect anisotropic dipole moments of two orthogonal exciton states, was estimated to be ˜1.2. This demonstrates that the selective control of two orthogonal polarized exciton states is a promising technique for exciton-based-quantum information devices compatible with fiber optics.

Dynamics of exciton relaxation in LH2 antenna probed by multipulse nonlinear spectroscopy.

Science.gov (United States)

Novoderezhkin, Vladimir I; Cohen Stuart, Thomas A; van Grondelle, Rienk

2011-04-28

We explain the relaxation dynamics in the LH2-B850 antenna as revealed by multipulse pump-dump-probe spectroscopy (Th. A. Cohen Stuart, M. Vengris, V. I. Novoderezhkin, R. J. Cogdell, C. N. Hunter, R. van Grondelle, submitted). The theory of pump-dump-probe response is evaluated using the doorway-window approach in combination with the modified Redfield theory. We demonstrate that a simultaneous fit of linear spectra, pump-probe, and pump-dump-probe kinetics can be obtained at a quantitative level using the disordered exciton model, which is essentially the same as used to model the spectral fluctuations in single LH2 complexes (Novoderezhkin, V.; Rutkauskas, D.; van Grondelle, R. Biophys. J. 2006, 90, 2890). The present studies suggest that the observed relaxation rates are strongly dependent on the realization of the disorder. A big spread of the rates (exceeding 3 orders of magnitude) is correlated with the disorder-induced changes in delocalization length and overlap of the exciton wave functions. We conclude that the bulk kinetics reflect a superposition of many pathways corresponding to different physical limits of energy transfer, varying from sub-20 fs relaxation between delocalized and highly spatially overlapping exciton states to >20 ps jumps between states localized at the opposite sides of the ring.

Ultrafast terahertz electrodynamics of photonic and electronic nanostructures

Energy Technology Data Exchange (ETDEWEB)

Luo, Liang [Iowa State Univ., Ames, IA (United States)

2015-01-01

This thesis summarizes my work on using ultrafast laser pulses to study Terahertz (THz) electrodynamics of photonic and electronic nanostructures and microstructures. Ultrafast timeresolved (optical, NIR, MIR, THz) pump-probe spectroscopy setup has been successfully built, which enables me to perform a series of relevant experiments. Firstly, a novel high e ciency and compact THz wave emitter based on split-ring-resonators has been developed and characterized. The emitter can be pumped at any wavelength by tailoring the magnetic resonance and could generate gapless THz waves covering the entire THz band. Secondly, two kinds of new photonic structures for THz wave manipulation have been successfully designed and characterized. One is based on the 1D and 2D photo-imprinted di ractive elements. The other is based on the photoexcited double-split-ring-resonator metamaterials. Both structures are exible and can modulate THz waves with large tunability. Thirdly, the dark excitons in semiconducting singlewalled carbon nanotubes are studied by optical pump and THz probe spectroscopy, which provides the rst insights into the THz responses of nonequilibrium excitonic correlations and dynamics from the dark ground states in carbon nanotubes. Next, several on-going projects are brie y presented such as the study of ultrafast THz dynamics of Dirac fermions in topological insulator Bi₂Se₃ with Mid-infrared excitation. Finally, the thesis ends with a summary of the completed experiments and an outlook of the future plan.

Engineering and manipulating exciton wave packets

Science.gov (United States)

Zang, Xiaoning; Montangero, Simone; Carr, Lincoln D.; Lusk, Mark T.

2017-05-01

When a semiconductor absorbs light, the resulting electron-hole superposition amounts to a uncontrolled quantum ripple that eventually degenerates into diffusion. If the conformation of these excitonic superpositions could be engineered, though, they would constitute a new means of transporting information and energy. We show that properly designed laser pulses can be used to create such excitonic wave packets. They can be formed with a prescribed speed, direction, and spectral make-up that allows them to be selectively passed, rejected, or even dissociated using superlattices. Their coherence also provides a handle for manipulation using active, external controls. Energy and information can be conveniently processed and subsequently removed at a distant site by reversing the original procedure to produce a stimulated emission. The ability to create, manage, and remove structured excitons comprises the foundation for optoexcitonic circuits with application to a wide range of quantum information, energy, and light-flow technologies. The paradigm is demonstrated using both tight-binding and time-domain density functional theory simulations.

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...

Modeling loss and backscattering in a photonic-bandgap fiber using strong perturbation

Science.gov (United States)

Zamani Aghaie, Kiarash; Digonnet, Michel J. F.; Fan, Shanhui

2013-02-01

We use coupled-mode theory with strong perturbation to model the loss and backscattering coefficients of a commercial hollow-core fiber (NKT Photonics' HC-1550-02 fiber) induced by the frozen-in longitudinal perturbations of the fiber cross section. Strong perturbation is used, for the first time to the best of our knowledge, because the large difference between the refractive indices of the two fiber materials (silica and air) makes conventional weak-perturbation less accurate. We first study the loss and backscattering using the mathematical description of conventional surface-capillary waves (SCWs). This model implicitly assumes that the mechanical waves on the core wall of a PBF have the same power spectral density (PSD) as the waves that develop on an infinitely thick cylindrical tube with the same diameter as the PBF core. The loss and backscattering coefficients predicted with this thick-wall SCW roughness are 0.5 dB/km and 1.1×10-10 mm-1, respectively. These values are more than one order of magnitude smaller than the measured values (20-30 dB/km and ~1.5×10-9 mm-1, respectively). This result suggests that the thick-wall SCW PSD is not representative of the roughness of our fiber. We found that this discrepancy occurs at least in part because the effect of the finite thickness of the silica membranes (only ~120 nm) is neglected. We present a new expression for the PSD that takes into account this finite thickness and demonstrates that the finite thickness substantially increases the roughness. The predicted loss and backscattering coefficients predicted with this thin-film SCW PSD are 30 dB/km and 1.3×10-9 mm-1, which are both close to the measured values. We also show that the thin-film SCW PSD accurately predicts the roughness PSD measured by others in a solid-core photonic-crystal fiber.

Synthesis and Exciton Dynamics of Triplet Sensitized Conjugated Polymers

KAUST Repository

Andernach, Rolf; Utzat, Hendrik; Dimitrov, Stoichko; McCulloch, Iain; Heeney, Martin; Durrant, James; Bronstein, Hugo

2015-01-01

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

Resolving ultrafast exciton migration in organic solids at the nanoscale

Science.gov (United States)

Ginsberg, Naomi

The migration of Frenkel excitons, tightly-bound electron-hole pairs, in photosynthesis and in organic semiconducting films is critical to the efficiency of natural and artificial light harvesting. While these materials exhibit a high degree of structural heterogeneity on the nanoscale, traditional measurements of exciton migration lengths are performed on bulk samples. Since both the characteristic length scales of structural heterogeneity and the reported bulk diffusion lengths are smaller than the optical diffraction limit, we adapt far-field super-resolution fluorescence imaging to uncover the correlations between the structural and energetic landscapes that the excitons explore. By combining the ultrafast super-resolved measurements with exciton hopping simulations we furthermore specify the nature (in addition to the extent) of exciton migration as a function of the intrinsic and ensemble chromophore energy scales that determine a spatio-energetic landscape for migration. In collaboration with: Samuel Penwell, Lucas Ginsberg, University of California, Berkeley and Rodrigo Noriega University of Utah.

The creation of defects in ammonium halides by excitons

International Nuclear Information System (INIS)

Kim, L.M.

2002-01-01

The ammonium halides crystals and alkali halides crystals are analogous by kind chemical bonds and crystalline lattices. The anionic sublattice is identical in this crystals. It is known the main mechanism of defect creation by irradiation is radiationless decay of excitons in alkali halides crystals. The F-, H-centers are formation in this processes. However, F, H-centres are not detected in ammonium halides. The goal of this work is investigation the creation of defects in ammonium halides by excitons. We established that excitons in ammonium chlorides and bromides are similar to excitons in alkali halides. It is known excitons are self-trapped and have identical parameters of the exciton-phonon interaction in both kind crystals. It is supposed, that processes of radiationless disintegration of excitons are identical in ammonium and alkali halides. It is necessary to understand why F-, H-centers are absent in ammonium halides. V k -centres are created by the excitation of the ammonium halides crystals in the absorption band of excitons. It was established by thermoluminescence and spectrums of absorption. The V k -centers begin to migrate at 110-120 K in ammonium chlorides and bromides. The curve of thermoluminescence have peak with maximum at this temperatures. It is known V k -centers in ammonium chlorides have the absorption band at 380 nm. We discovered this absorption band after irradiation of crystals by ultra-violet. In alkali halides F-center is anionic vacancy with electron. The wave function of electron are spread ed at the cations around anionic vacancy. We established the cation NH 4 + in ammonium halides can to capture electron. The ion NH 4 2+ is unsteady. It is disintegrated to NH 3 + and H + . We suppose that excitons in ammonium and alkali halides are disintegrated identically. When cation NH 4 + capture electron, in the anionic sublattice the configuration are created in a direction (100) The indicated configuration is unsteady in relation to a

Room temperature current injection polariton light emitting diode with a hybrid microcavity.

Science.gov (United States)

Lu, Tien-Chang; Chen, Jun-Rong; Lin, Shiang-Chi; Huang, Si-Wei; Wang, Shing-Chung; Yamamoto, Yoshihisa

2011-07-13

The strong light-matter interaction within a semiconductor high-Q microcavity has been used to produce half-matter/half-light quasiparticles, exciton-polaritons. The exciton-polaritons have very small effective mass and controllable energy-momentum dispersion relation. These unique properties of polaritons provide the possibility to investigate the fundamental physics including solid-state cavity quantum electrodynamics, and dynamical Bose-Einstein condensates (BECs). Thus far the polariton BEC has been demonstrated using optical excitation. However, from a practical viewpoint, the current injection polariton devices operating at room temperature would be most desirable. Here we report the first realization of a current injection microcavity GaN exciton-polariton light emitting diode (LED) operating under room temperature. The exciton-polariton emission from the LED at photon energy 3.02 eV under strong coupling condition is confirmed through temperature-dependent and angle-resolved electroluminescence spectra.

Bose-Einstein condensation of excitons in Cu2O

International Nuclear Information System (INIS)

Snoke, D.W.

1990-01-01

Free excitons provide the only experimental system other than helium in which the behavior of particles with mass is known to follow Bose-Einstein statistics. Experimental observations are presented of the kinetic energy distribution of excitons in the direct-gap semiconductor Cu 2 O, both the triplet orthoexciton state and the singlet paraexciton state. The density and temperature of the exciton gas closely follow the phase boundary for Bose-Einstein condensation. At the highest densities, the lower-lying paraexcitons take on an anomalous energy distribution with a sharp, high-energy edge. This odd distribution of particle energies may be associated with Bose-Einstein condensation into a state with nonzero momentum. Indeed, the excitons leave the region of their creation at supersonic velocities. In addition to the experimental observations, theoretical models are presented for several aspects of this nonequilibrium system. The equilibration of a nearly-ideal boson gas is modeled, finding that a significant time is required for the approach to condensation. The temperature and density of the excitons in steady state are modeled based on known classical kinetic effects in semiconductors, and the effects of Bose-Einstein statistics on these processes estimated

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

Some evidence for the high density phase of excitons in CdS

International Nuclear Information System (INIS)

Rueckmann, I.; May, V.; Voigt, J.

1980-01-01

Reflection spectra without and with additional pumping are measured in CdS at 1.8 and 77 K, respectively, starting from very low pump intensities. At low pump intensities a special behaviour of the reflection minimum is found indicating the importance of an exciton dead layer. The experimental spectra up to the highest pump intensities can be fitted very well taking into account spatial dispersion, exciton dead layer, and density dependent excitonic parameters. Polarizability, damping, and layer thickness change continuously in the whole range of excitation intensities. On the other side, the transverse dielectric function of a high density gas of interacting 1s excitons is calculated. A comparison between theoretically and experimentally obtained excitonic parameters at different densities shows good agreement. Hence, the importance of many-exciton interaction for the reflection spectra up to vanishing at highest pump intensities is concluded. (author)

Self-trapped excitons in LH2 bacteriochlorophyll-protein complexes under high pressure

International Nuclear Information System (INIS)

Timpmann, K.; Ellervee, Aleksandr; Kuznetsov, Anatoli; Laisaar, Arlentin; Trinkunas, Gediminas; Freiberg, Arvi

2003-01-01

The absorption and emission spectra of excitons in LH2 antenna complexes from the photosynthetic purple bacterium Rhodobacter sphaeroides have been studied under hydrostatic pressure. The measurements made between ambient pressure and 6 kbar over a broad temperature range reveal largely different rates of the pressure-induced shifts for the absorption and emission bands. Numerical calculations based on exciton polaron model provide evidence for the exciton self-trapping at ambient pressure as well as for the pressure stabilization of the self-trapped exciton states responsible for the emission, whereas the light absorbing states belong to nearly free excitons over the whole pressure and temperature ranges studied

Nonlinear silicon photonics

Science.gov (United States)

Borghi, M.; Castellan, C.; Signorini, S.; Trenti, A.; Pavesi, L.

2017-09-01

Silicon photonics is a technology based on fabricating integrated optical circuits by using the same paradigms as the dominant electronics industry. After twenty years of fervid development, silicon photonics is entering the market with low cost, high performance and mass-manufacturable optical devices. Until now, most silicon photonic devices have been based on linear optical effects, despite the many phenomenologies associated with nonlinear optics in both bulk materials and integrated waveguides. Silicon and silicon-based materials have strong optical nonlinearities which are enhanced in integrated devices by the small cross-section of the high-index contrast silicon waveguides or photonic crystals. Here the photons are made to strongly interact with the medium where they propagate. This is the central argument of nonlinear silicon photonics. It is the aim of this review to describe the state-of-the-art in the field. Starting from the basic nonlinearities in a silicon waveguide or in optical resonator geometries, many phenomena and applications are described—including frequency generation, frequency conversion, frequency-comb generation, supercontinuum generation, soliton formation, temporal imaging and time lensing, Raman lasing, and comb spectroscopy. Emerging quantum photonics applications, such as entangled photon sources, heralded single-photon sources and integrated quantum photonic circuits are also addressed at the end of this review.

Enhancement of exciton radiative recombination for In-doped ZnO nanowires with aluminum cylindrical micropillars

Energy Technology Data Exchange (ETDEWEB)

Wang, Jen-Cheng; Liang, Yu-Ting; Cheng, Fang-Ching; Fang, Chia-Hui; Chen, Hung-Ing; Tsai, Chung-Yuan [Graduate Institute of Electro-Optical Engineering and Department of Electronic Engineering, Chang Gung University, 259 Wen-Hwa 1st Road, Kwei-Shan, Tao-Yuan 333, Taiwan, ROC (China); Jiang, Joe-Air [Department of Bio-Industrial Mechatronics Engineering, National Taiwan University, Taipei 106, Taiwan, ROC (China); Nee, Tzer-En, E-mail: neete@mail.cgu.edu.tw [Graduate Institute of Electro-Optical Engineering and Department of Electronic Engineering, Chang Gung University, 259 Wen-Hwa 1st Road, Kwei-Shan, Tao-Yuan 333, Taiwan, ROC (China)

2013-04-15

Zinc oxide (ZnO) has attracted intensive research effort in recent years, due to its unique properties and versatile applications. Recent work on the conservation of surface plasmon (SP) and light through period metal arrays has elucidated the propagation of SP resonance behavior. In this paper, we discuss the enhancement of exciton radiative recombination of the ZnO nanowires with Al cylindrical micropillars. Optical characterization of exciton interacted with SP resonance for indium-doped ZnO nanowires with Al cylindrical micropillars has been also investigated. From photoluminescence spectra of In-doped ZnO nanowires, it is found that the In-doped ZnO nanowires have a blue emission at 425 nm, which resulted from the ZnO band-to-band transition. Prior to the arrays of samples were annealed, a broad green emission centered at 500 nm was observed, which is attributed to ZnO native point defects. The relatively strong green band emission results from the radiative recombination that arises from the ionized oxygen vacancy and surface-defect related luminescence. Compare the In-doped ZnO on Si substrate, the enhancement of PL intensity for In-doped ZnO with deposited Al pattern film can be attributed to strong interaction with SP resonance and exciton over a broad temperature range. These experimental results indicate that Al cylindrical micropillars can significantly enhance carrier confinement and increase the quantum efficiency of In-doped ZnO/Al heterostructures due to the interaction of SP resonance between the In-doped ZnO nanowires and Al cylindrical micropillar structures, the surface-defect related luminescence, and the auxiliary test structures with variable micropillar parameters. -- Highlights: ► We examine the exciton radiative recombination of the ZnO nanowires. ► Al cylindrical micropillars affect the carrier recombination of ZnO/Al structures. ► The interaction of SP resonance between In-doped ZnO nanowire and Al pattern film. ► The carrier

Quantum photonics with quantum dots in photonic wires

DEFF Research Database (Denmark)

Munsch, Mathieu; Kuhlmann, Andreas; Cadeddu, Davide

2016-01-01

We present results from the spectroscopy of a single quantum dot in a photonic wire. The device presents a high photon extraction efficiency, and strong hybrid coupling to mechanical modes. We use resonance fluorescence to probe the emitter’s properties with the highest sensitivity. Weperform...

Exciton diffusion coefficient measurement in ZnO nanowires under electron beam irradiation

Science.gov (United States)

Donatini, Fabrice; Pernot, Julien

2018-03-01

In semiconductor nanowires (NWs) the exciton diffusion coefficient can be determined using a scanning electron microscope fitted with a cathodoluminescence system. High spatial and temporal resolution cathodoluminescence experiments are needed to measure independently the exciton diffusion length and lifetime in single NWs. However, both diffusion length and lifetime can be affected by the electron beam bombardment during observation and measurement. Thus, in this work the exciton lifetime in a ZnO NW is measured versus the electron beam dose (EBD) via a time-resolved cathodoluminescence experiment with a temporal resolution of 50 ps. The behavior of the measured exciton lifetime is consistent with our recent work on the EBD dependence of the exciton diffusion length in similar NWs investigated under comparable SEM conditions. Combining the two results, the exciton diffusion coefficient in ZnO is determined at room temperature and is found constant over the full span of EBD.

Decay of orientational grating of weakly confined excitons in GaAs thin films

International Nuclear Information System (INIS)

Kojima, O.; Isu, T.; Ishi-Hayase, J.; Kanno, A.; Katouf, R.; Sasaki, M.; Tsuchiya, M.

2008-01-01

We report the dynamical properties of the exciton orientation in GaAs thin films using the orientational grating (OG) technique. From the results of excitation-power dependence of OG signal, we confirmed that the OG signal comes from the optical nonlinearity of weakly confined excitons. In addition, the OG-decay time decreases with an increase of excitation power due to exciton-exciton interaction, and the shortest decay time is below 1 ps. Our results may imply the potential application of optical nonlinearity of weakly confined exciton to ultrafast switching devices operating at 1 Tbit/s

Photonic engineering of highly linearly polarized quantum dot emission at telecommunication wavelengths

Science.gov (United States)

Mrowiński, P.; Emmerling, M.; Schneider, C.; Reithmaier, J. P.; Misiewicz, J.; Höfling, S.; Sek, G.

2018-04-01

In this work, we discuss a method to control the polarization anisotropy of spontaneous emission from neutral excitons confined in quantum-dot-like nanostructures, namely single epitaxial InAs quantum dashes emitting at telecom wavelengths. The nanostructures are embedded inside lithographically defined, in-plane asymmetric photonic mesa structures, which generate polarization-dependent photonic confinement. First, we study the influence of the photonic confinement on the polarization anisotropy of the emission by photoluminescence spectroscopy, and we find evidence of different contributions to a degree of linear polarization (DOLP), i.e., from the quantum dash and the photonic mesa, in total giving rise to DOLP =0.85 . Then, we perform finite-difference time-domain simulations of photonic confinement, and we calculate the DOLP in a dipole approximation showing well-matched results for the established model. Furthermore, by using numerical calculations, we demonstrate several types of photonic confinements where highly linearly polarized emission with DOLP of about 0.9 is possible by controlling the position of a quantum emitter inside the photonic structure. Then, we elaborate on anisotropic quantum emitters allowing for exceeding DOLP =0.95 in an optimized case, and we discuss the ways towards efficient linearly polarized single photon source at telecom bands.

Intrinsic and environmental effects on the interference properties of a high-performance quantum dot single-photon source

DEFF Research Database (Denmark)

Gerhardt, Stefan; Iles-Smith, Jake; McCutcheon, Dara

2018-01-01

We report a joint experimental and theoretical study of the interference properties of a single-photon source based on a In(Ga)As quantum dot embedded in a quasiplanar GaAs microcavity. Using resonant laser excitation with a pulse separation of 2 ns, we find near-perfect interference of the emitt...... in excitonic Rabi oscillations....

Modeling temperature dependent singlet exciton dynamics in multilayered organic nanofibers

Science.gov (United States)

de Sousa, Leonardo Evaristo; de Oliveira Neto, Pedro Henrique; Kjelstrup-Hansen, Jakob; da Silva Filho, Demétrio Antônio

2018-05-01

Organic nanofibers have shown potential for application in optoelectronic devices because of the tunability of their optical properties. These properties are influenced by the electronic structure of the molecules that compose the nanofibers and also by the behavior of the excitons generated in the material. Exciton diffusion by means of Förster resonance energy transfer is responsible, for instance, for the change with temperature of colors in the light emitted by systems composed of different types of nanofibers. To study in detail this mechanism, we model temperature dependent singlet exciton dynamics in multilayered organic nanofibers. By simulating absorption and emission spectra, the possible Förster transitions are identified. Then, a kinetic Monte Carlo model is employed in combination with a genetic algorithm to theoretically reproduce time-resolved photoluminescence measurements for several temperatures. This procedure allows for the obtainment of different information regarding exciton diffusion in such a system, including temperature effects on the Förster transfer efficiency and the activation energy of the Förster mechanism. The method is general and may be employed for different systems where exciton diffusion plays a role.

Two exciton states in discrete and continuum alpha-helical proteins

International Nuclear Information System (INIS)

Latha, M.M.; Merlin, G.

2012-01-01

The dynamics of alpha-helical proteins is described by proposing a model Hamiltonian representing two exciton bound states. The dynamics is studied by constructing the equations of motion using a two exciton eigen-function in the discrete level. A numerical analysis shows the existence of two excitons in alpha-helical proteins and its propagation as solitons along the hydrogen bonding spines. The lattice model is also treated in the continuum limit which is a valid approximation in the low temperature, long wavelength limit. The resulting equation is studied using the multiple scale perturbation analysis which also shows the transfer of two exciton energy through alpha-helical proteins in the form of solitons with no change in velocity and amplitude. -- Highlights: ► The dynamics of alpha-helical proteins with two exciton states is studied. ► The dynamics is studied both in the discrete and continuum levels. ► The resulting equations are solved numerically and analytically. ► The solution supports the propagation of the energy in the form of solitons.

Photon and photon reactions: elementary theoretical introduction

International Nuclear Information System (INIS)

Diu, B.

The electromagnetic field and associated quanta, the photons, are simply and briefly studied. The conventional electromagnetism laws are recalled. Fundamental concepts such as gauge invariance, the electromagnetic current conservation, and photon behavior against the internal symmetries of strong interactions are simply introduced. Results and notations are applied to analysis of reactions where photons intervene in initial or final states (photoproduction) within the limits of amplitude properties in the conventional space-time. The helicity and invariant amplitude formalisms are compared [fr

Ultrafast electric phase control of a single exciton qubit

Science.gov (United States)

Widhalm, Alex; Mukherjee, Amlan; Krehs, Sebastian; Sharma, Nandlal; Kölling, Peter; Thiede, Andreas; Reuter, Dirk; Förstner, Jens; Zrenner, Artur

2018-03-01

We report on the coherent phase manipulation of quantum dot excitons by electric means. For our experiments, we use a low capacitance single quantum dot photodiode which is electrically controlled by a custom designed SiGe:C BiCMOS chip. The phase manipulation is performed and quantified in a Ramsey experiment, where ultrafast transient detuning of the exciton energy is performed synchronous to double pulse π/2 ps laser excitation. We are able to demonstrate electrically controlled phase manipulations with magnitudes up to 3π within 100 ps which is below the dephasing time of the quantum dot exciton.

Tunable photonic crystal for THz radiation in layered superconductors: Strong magnetic-field dependence of the transmission coefficient

International Nuclear Information System (INIS)

Savel'ev, Sergey; Rakhmanov, A.L.; Nori, Franco

2006-01-01

Josephson plasma waves are scattered by the Josephson vortex lattice. This scattering results in a strong dependence, on the in-plane magnetic-field H ab , of the reflection and transmission of THz radiation propagating in layered superconductors. In particular, a tunable band-gap structure (THz photonic crystal) occurs in such a medium. These effects can be used, by varying H ab , for the selective frequency-filtering of THz radiation

Excitons in Core-Shell Nanowires with Polygonal Cross Sections.

Science.gov (United States)

Sitek, Anna; Urbaneja Torres, Miguel; Torfason, Kristinn; Gudmundsson, Vidar; Bertoni, Andrea; Manolescu, Andrei

2018-04-11

The distinctive prismatic geometry of semiconductor core-shell nanowires leads to complex localization patterns of carriers. Here, we describe the formation of optically active in-gap excitonic states induced by the interplay between localization of carriers in the corners and their mutual Coulomb interaction. To compute the energy spectra and configurations of excitons created in the conductive shell, we use a multielectron numerical approach based on the exact solution of the multiparticle Hamiltonian for electrons in the valence and conduction bands, which includes the Coulomb interaction in a nonperturbative manner. We expose the formation of well-separated quasidegenerate levels, and focus on the implications of the electron localization in the corners or on the sides of triangular, square, and hexagonal cross sections. We obtain excitonic in-gap states associated with symmetrically distributed electrons in the spin singlet configuration. They acquire large contributions due to Coulomb interaction, and thus are shifted to much higher energies than other states corresponding to the conduction electron and the vacancy localized in the same corner. We compare the results of the multielectron method with those of an electron-hole model, and we show that the latter does not reproduce the singlet excitonic states. We also obtain the exciton lifetime and explain selection rules which govern the recombination process.

Excitonic and electron-hole mechanisms of the creation of Frenkel defect in alkali halides

International Nuclear Information System (INIS)

Lushchik, A.; Kirm, M.; Lushchik, Ch.; Vasil'chenko, E.

2000-01-01

Excitonic and electron-hole (e-h) mechanisms of stable F centre creation by VUV radiation in alkali halide crystals are discussed. In KCl at 4.2 K, the efficiency of stable F-H pair creation is especially high at the direct optical formation of triplet excitons with n=1. At 200-400 K, the creation processes of stable F centres in KCl are especially efficient at the formation of one-halide exciton in the Urbach tail of an exciton absorption. In KCl and KBr, the decay of a cation exciton (∼20 eV) causes the formation of two e-h pairs, while in NaCl a cation exciton (33.5 eV) decays into two e-h and an anion exciton. An elastic uniaxial stress of a crystal excited by VUV radiation decreases the mean free path of excitons before their self-trapping (KI) and increases the mean free path of hot holes before self-trapping (NaCl)

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...

Photogenerated Exciton Dissociation in Highly Coupled Lead Salt Nanocrystal Assemblies

KAUST Repository

Choi, Joshua J.; Luria, Justin; Hyun, Byung-Ryool; Bartnik, Adam C.; Sun, Liangfeng; Lim, Yee-Fun; Marohn, John A.; Wise, Frank W.; Hanrath, Tobias

2010-01-01

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.

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.

Highly Anisotropic in-Plane Excitons in Atomically Thin and Bulklike 1T '-ReSe₂

DEFF Research Database (Denmark)

Arora, Ashish; Noky, Jonathan; Drueppel, Matthias

2017-01-01

and photoluminescence spectroscopy of excitons in 1T '-ReSe2. On reducing the crystal thickness from bulk to a monolayer, we observe a strong blue shift of the optical band gap from 1.37 to 1.50 eV. The excitons are strongly polarized with dipole vectors along different crystal directions, which persist from bulk down......Atomically thin materials such as graphene or MoS2 are of high in-plane symmetry. Crystals with reduced symmetry hold the promise for novel optoelectronic devices based on their anisotropy in current flow or light polarization. Here, we present polarization-resolved optical transmission...... crystal. In addition, we find in our calculations a direct band gap in 1T '-ReSe2 regardless of crystal thickness, indicating weak interlayer coupling effects on the band gap characteristics. Our results pave the way for polarization-sensitive applications, such as optical logic circuits operating...

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...

Almost real photons

International Nuclear Information System (INIS)

Fujii, H.

1977-01-01

High energy photon-proton scattering is expected to bring an important information on strong and electromagnetic interaction, and is discussed in this paper. When the ''mass'' of the photon is less than that of the lightest hadron, it is said ''the photon is almost real''. The photon energy is sufficiently high to check the energy dependence of the gamma-proton total cross section, even in the first stage of TRISTAN. The tagging system consists of four multi-wire proportional chambers (MWPC) and a lead glass Cerenkov counter. The energy of scattered electrons is determined with the Cerenkov counter. The equivalent-photon approximation is a useful method to obtain the counting rates. The estimation of the counting rate was made under the expected value of the total cross section. The estimated counting rate is strong enough for the experiment of the gamma-proton total cross section measurement. (Kato, T.)

Single-crystal charge transfer interfaces for efficient photonic devices (Conference Presentation)

Science.gov (United States)

Alves, Helena; Pinto, Rui M.; Maçôas, Ermelinda M. S.; Baleizão, Carlos; Santos, Isabel C.

2016-09-01

Organic semiconductors have unique optical, mechanical and electronic properties that can be combined with customized chemical functionality. In the crystalline form, determinant features for electronic applications such as molecular purity, the charge mobility or the exciton diffusion length, reveal a superior performance when compared with materials in a more disordered form. Combining crystals of two different conjugated materials as even enable a new 2D electronic system. However, the use of organic single crystals in devices is still limited to a few applications, such as field-effect transistors. In 2013, we presented the first system composed of single-crystal charge transfer interfaces presenting photoconductivity behaviour. The system composed of rubrene and TCNQ has a responsivity reaching 1 A/W, corresponding to an external quantum efficiency of nearly 100%. A similar approach, with a hybrid structure of a PCBM film and rubrene single crystal also presents high responsivity and the possibility to extract excitons generated in acceptor materials. This strategy led to an extended action towards the near IR. By adequate material design and structural organisation of perylediimides, we demonstrate that is possible to improve exciton diffusion efficiency. More recently, we have successfully used the concept of charge transfer interfaces in phototransistors. These results open the possibility of using organic single-crystal interfaces in photonic applications.

Direct observation of the lowest indirect exciton state in the bulk of hexagonal boron nitride

Science.gov (United States)

Schuster, R.; Habenicht, C.; Ahmad, M.; Knupfer, M.; Büchner, B.

2018-01-01

We combine electron energy-loss spectroscopy and first-principles calculations based on density-functional theory (DFT) to identify the lowest indirect exciton state in the in-plane charge response of hexagonal boron nitride (h-BN) single crystals. This remarkably sharp mode forms a narrow pocket with a dispersion bandwidth of ˜100 meV and, as we argue based on a comparison to our DFT calculations, is predominantly polarized along the Γ K direction of the hexagonal Brillouin zone. Our data support the recent report by Cassabois et al. [Nat. Photonics 10, 262 (2016), 10.1038/nphoton.2015.277] who indirectly inferred the existence of this mode from the photoluminescence signal, thereby establishing h-BN as an indirect semiconductor.

Vacuum ultraviolet synchrotron measurements of excitons in NaMgF{sub 3}:Yb{sup 2+}

Energy Technology Data Exchange (ETDEWEB)

Hughes-Currie, Rosa B. [Department of Physics and Astronomy, University of Canterbury, PB 4800, Christchurch 8140 (New Zealand); Ivanovskikh, Konstantin V. [ANK Service Ltd., PB 58, Novouralsk 624131, Sverdlovsk Region (Russian Federation); Ural Federal University, 19 Mira st., Ekaterinburg 620002 (Russian Federation); Reid, Michael F., E-mail: mike.reid@canterbury.ac.nz [Department of Physics and Astronomy, University of Canterbury, PB 4800, Christchurch 8140 (New Zealand); MacDiarmid Institute for Advanced Materials and Nanotechnology (New Zealand); Wells, Jon-Paul R. [Department of Physics and Astronomy, University of Canterbury, PB 4800, Christchurch 8140 (New Zealand); Dodd-Walls Centre for Quantum and Photonic Technologies (New Zealand); Reeves, Roger J. [Department of Physics and Astronomy, University of Canterbury, PB 4800, Christchurch 8140 (New Zealand); MacDiarmid Institute for Advanced Materials and Nanotechnology (New Zealand); Meijerink, Andries [Debye Institute, Utrecht University, P.O. Box 80 000, 3508 TA Utrecht (Netherlands)

2016-01-15

Results of a vacuum ultraviolet spectroscopic characterization of NaMgF{sub 3}:Yb{sup 2+} are presented. The material demonstrates emission features associated with self-trapped excitons and impurity-trapped excitons. The emission features noticeably overlap giving rise to a broad emission band from 17 000 to 35 000 cm{sup −1} at a sample temperature of 8 K. To identify the true profiles of the emission features we have used a deconvolution procedure. The deconvolution was possible due to the thermal quenching of self-trapped excitons at room temperature that allowed for direct observations of the impurity trapped exciton emission band. Energy transfer between host electronic excitations (excitons and e–h pairs) and Yb{sup 2+} ions leading to the formation of impurity-trapped excitons is evident from excitation spectra. - Highlights: • We present VUV emission and excitation spectra of NaMgF{sub 3}:Yb{sup 2+}. • Formation of free excitons leads to emission from intrinsic and extrinsic excitons. • We deconvolute the emission to separate the two overlapping exciton bands. • The excitation spectra show two mechanisms for forming impurity-trapped excitons.

Complete quantum control of exciton qubits bound to isoelectronic centres.

Science.gov (United States)

Éthier-Majcher, G; St-Jean, P; Boso, G; Tosi, A; Klem, J F; Francoeur, S

2014-05-30

In recent years, impressive demonstrations related to quantum information processing have been realized. The scalability of quantum interactions between arbitrary qubits within an array remains however a significant hurdle to the practical realization of a quantum computer. Among the proposed ideas to achieve fully scalable quantum processing, the use of photons is appealing because they can mediate long-range quantum interactions and could serve as buses to build quantum networks. Quantum dots or nitrogen-vacancy centres in diamond can be coupled to light, but the former system lacks optical homogeneity while the latter suffers from a low dipole moment, rendering their large-scale interconnection challenging. Here, through the complete quantum control of exciton qubits, we demonstrate that nitrogen isoelectronic centres in GaAs combine both the uniformity and predictability of atomic defects and the dipole moment of semiconductor quantum dots. This establishes isoelectronic centres as a promising platform for quantum information processing.

Decoherence suppression of excitons by bang-bang control

International Nuclear Information System (INIS)

Kishimoto, T.; Hasegawa, A.; Mitsumori, Y.; Ishi-Hayase, J.; Sasaki, M.; Minami, F.

2007-01-01

We report the demonstration of decoherence control of excitons on a layered compound semiconductor GaSe by using successive three femtosecond pulses, i.e., the six-wave mixing configuration. The second pulse acts as a π pulse which reverses the time evolution of non-Markovian dynamics. By changing the pulse interval conditions, we confirmed for the first time the suppression of exciton decoherence by π pulse irradiation

Interplay of Cu and oxygen vacancy in optical transitions and screening of excitons in ZnO:Cu films

International Nuclear Information System (INIS)

Darma, Yudi; Rusydi, Andrivo; Seng Herng, Tun; Marlina, Resti; Fauziah, Resti; Ding, Jun

2014-01-01

We study room temperature optics and electronic structures of ZnO:Cu films as a function of Cu concentration using a combination of spectroscopic ellipsometry, photoluminescence, and ultraviolet-visible absorption spectroscopy. Mid-gap optical states, interband transitions, and excitons are observed and distinguishable. We argue that the mid-gap states are originated from interactions of Cu and oxygen vacancy (Vo). They are located below conduction band (Zn4s) and above valence band (O2p) promoting strong green emission and narrowing optical band gap. Excitonic states are screened and its intensities decrease upon Cu doping. Our results show the importance of Cu and Vo driving the electronic structures and optical transitions in ZnO:Cu films

Interplay of Cu and oxygen vacancy in optical transitions and screening of excitons in ZnO:Cu films

Science.gov (United States)

Darma, Yudi; Seng Herng, Tun; Marlina, Resti; Fauziah, Resti; Ding, Jun; Rusydi, Andrivo

2014-02-01

We study room temperature optics and electronic structures of ZnO:Cu films as a function of Cu concentration using a combination of spectroscopic ellipsometry, photoluminescence, and ultraviolet-visible absorption spectroscopy. Mid-gap optical states, interband transitions, and excitons are observed and distinguishable. We argue that the mid-gap states are originated from interactions of Cu and oxygen vacancy (Vo). They are located below conduction band (Zn4s) and above valence band (O2p) promoting strong green emission and narrowing optical band gap. Excitonic states are screened and its intensities decrease upon Cu doping. Our results show the importance of Cu and Vo driving the electronic structures and optical transitions in ZnO:Cu films.

Interconversion between Free Charges and Bound Excitons in 2D Hybrid Lead Halide Perovskites.

Science.gov (United States)

Gélvez-Rueda, María C; Hutter, Eline M; Cao, Duyen H; Renaud, Nicolas; Stoumpos, Constantinos C; Hupp, Joseph T; Savenije, Tom J; Kanatzidis, Mercouri G; Grozema, Ferdinand C

2017-11-30

The optoelectronic properties of hybrid perovskites can be easily tailored by varying their components. Specifically, mixing the common short organic cation (methylammonium (MA)) with a larger one (e.g., butyl ammonium (BA)) results in 2-dimensional perovskites with varying thicknesses of inorganic layers separated by the large organic cation. In both of these applications, a detailed understanding of the dissociation and recombination of electron-hole pairs is of prime importance. In this work, we give a clear experimental demonstration of the interconversion between bound excitons and free charges as a function of temperature by combining microwave conductivity techniques with photoluminescence measurements. We demonstrate that the exciton binding energy varies strongly (between 80 and 370 meV) with the thickness of the inorganic layers. Additionally, we show that the mobility of charges increases with the layer thickness, in agreement with calculated effective masses from electronic structure calculations.

Interconversion between Free Charges and Bound Excitons in 2D Hybrid Lead Halide Perovskites

International Nuclear Information System (INIS)

Gélvez-Rueda, María C.; Hutter, Eline M.; Cao, Duyen H.; Renaud, Nicolas; Stoumpos, Constantinos C.

2017-01-01

The optoelectronic properties of hybrid perovskites can be easily tailored by varying their components. Specifically, mixing the common short organic cation (methylammonium (MA)) with a larger one (e.g., butyl ammonium (BA)) results in 2-dimensional perovskites with varying thicknesses of inorganic layers separated by the large organic cation. In both of these applications, a detailed understanding of the dissociation and recombination of electron–hole pairs is of prime importance. Here in this work, we give a clear experimental demonstration of the interconversion between bound excitons and free charges as a function of temperature by combining microwave conductivity techniques with photoluminescence measurements. We demonstrate that the exciton binding energy varies strongly (between 80 and 370 meV) with the thickness of the inorganic layers. Additionally, we show that the mobility of charges increases with the layer thickness, in agreement with calculated effective masses from electronic structure calculations.

Broadband Light Collection Efficiency Enhancement of Carbon Nanotube Excitons Coupled to Metallo-Dielectric Antenna Arrays

Energy Technology Data Exchange (ETDEWEB)

Shayan, Kamran [Department; Rabut, Claire [Department; Kong, Xiaoqing [Department; Li, Xiangzhi [Department; Luo, Yue [Department; Mistry, Kevin S. [National Renewable; Blackburn, Jeffrey L. [National Renewable; Lee, Stephanie S. [Department; Strauf, Stefan [Department

2017-11-09

The realization of on-chip quantum networks ideally requires lossless interfaces between photons and solid-state quantum emitters. We propose and demonstrate on-chip arrays of metallo-dielectric antennas (MDA) that are tailored toward efficient and broadband light collection from individual embedded carbon nanotube quantum emitters by trapping air gaps on chip that form cavity modes. Scalable implementation is realized by employing polymer layer dry-transfer techniques that avoid solvent incompatibility issues, as well as a planar design that avoids solid-immersion lenses. Cryogenic measurements demonstrate 7-fold enhanced exciton intensity when compared to emitters located on bare wafers, corresponding to a light collection efficiency (LCE) up to 92% in the best case (average LCE of 69%) into a narrow output cone of +/-15 degrees that enables a priori fiber-to-chip butt coupling. The demonstrated MDA arrays are directly compatible with other quantum systems, particularly 2D materials, toward enabling efficient on-chip quantum light sources or spin-photon interfaces requiring unity light collection, both at cryogenic or room temperature.

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

Science.gov (United States)

Mullenbach, Tyler K.

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

Employing exciton transfer molecules to increase the lifetime of phosphorescent red organic light emitting diodes

Science.gov (United States)

Lindla, Florian; Boesing, Manuel; van Gemmern, Philipp; Bertram, Dietrich; Keiper, Dietmar; Heuken, Michael; Kalisch, Holger; Jansen, Rolf H.

2011-04-01

The lifetime of phosphorescent red organic light emitting diodes (OLEDs) is investigated employing either N,N'-diphenyl-N,N'-bis(1-naphthylphenyl)-1,1'-biphenyl-4,4'-diamine (NPB), TMM117, or 4,4',4″-tris(N-carbazolyl)-triphenylamine (TCTA) as hole-conducting host material (mixed with an electron conductor). All OLED (organic vapor phase deposition-processed) show similar efficiencies around 30 lm/W but strongly different lifetimes. Quickly degrading OLED based on TCTA can be stabilized by doping exciton transfer molecules [tris-(phenyl-pyridyl)-Ir (Ir(ppy)3)] to the emission layer. At a current density of 50 mA/cm2 (12 800 cd/m2), a lifetime of 387 h can be achieved. Employing exciton transfer molecules is suggested to prevent the degradation of the red emission layer in phosphorescent white OLED.

Optical Selection Rule of Excitons in Gapped Chiral Fermion Systems

Science.gov (United States)

Zhang, Xiaoou; Shan, Wen-Yu; Xiao, Di

2018-02-01

We show that the exciton optical selection rule in gapped chiral fermion systems is governed by their winding number w , a topological quantity of the Bloch bands. Specifically, in a CN-invariant chiral fermion system, the angular momentum of bright exciton states is given by w ±1 +n N with n being an integer. We demonstrate our theory by proposing two chiral fermion systems capable of hosting dark s -like excitons: gapped surface states of a topological crystalline insulator with C4 rotational symmetry and biased 3 R -stacked MoS2 bilayers. In the latter case, we show that gating can be used to tune the s -like excitons from bright to dark by changing the winding number. Our theory thus provides a pathway to electrical control of optical transitions in two-dimensional material.

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

Science.gov (United States)

Sato, Yoshihiro; Doolittle, Brian

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.

Influence of intra-pigment vibrations on dynamics of photosynthetic exciton

International Nuclear Information System (INIS)

Sato, Yoshihiro; Doolittle, Brian

2014-01-01

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

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.

Room-Temperature Exciton Lasing in Ultrathin Film of Coupled Nanocrystals

International Nuclear Information System (INIS)

Appavoo, Kannatassen; Xiaoze, Liu; Menon, Vinod; Sfeir, Matthew Y.

2015-01-01

We demonstrate exciton lasing in sub-wavelength coupled nanostructures at ultralow fluence threshold, as probed by femtosecond broadband emission and absorption spectroscopy. The complex spectrotemporal dynamics reveal for the first time an excitonic-to-electron-hole plasma lasing mechanism.

Interacting Electrons and Holes in Quasi-2D Quantum Dots in Strong Magnetic Fields

Science.gov (United States)

Hawrylak, P.; Sheng, W.; Cheng, S.-J.

2004-09-01