Nonlinear optical spectra having characteristics of Fano interferences in coherently coupled lowest exciton biexciton states in semiconductor quantum dots

Directory of Open Access Journals (Sweden)

Hideki Gotoh

2014-10-01

Full Text Available Optical nonlinear effects are examined using a two-color micro-photoluminescence (micro-PL method in a coherently coupled exciton-biexciton system in a single quantum dot (QD. PL and photoluminescence excitation spectroscopy (PLE are employed to measure the absorption spectra of the exciton and biexciton states. PLE for Stokes and anti-Stokes PL enables us to clarify the nonlinear optical absorption properties in the lowest exciton and biexciton states. The nonlinear absorption spectra for excitons exhibit asymmetric shapes with peak and dip structures, and provide a distinct contrast to the symmetric dip structures of conventional nonlinear spectra. Theoretical analyses with a density matrix method indicate that the nonlinear spectra are caused not by a simple coherent interaction between the exciton and biexciton states but by coupling effects among exciton, biexciton and continuum states. These results indicate that Fano quantum interference effects appear in exciton-biexciton systems at QDs and offer important insights into their physics.

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)

Theory of Transient Excited State Absorptions in Pentacene and Derivatives: Triplet-Triplet Biexciton versus Free Triplets.

Science.gov (United States)

Khan, Souratosh; Mazumdar, Sumit

2017-12-07

Recent experiments in several singlet-fission materials have found that the triplet-triplet biexciton either is the primary product of photoexcitation or has a much longer lifetime than believed until now. It thus becomes essential to determine the difference in the spectroscopic signatures of the bound triplet-triplet and free triplets to distinguish between them optically. We report calculations of excited state absorptions (ESAs) from the singlet and triplet excitons and from the triplet-triplet biexciton for a pentacene crystal with the herringbone structure and for nanocrystals of bis(triisopropylsilylethynyl) (TIPS)-pentacene. The triplet-triplet biexciton absorbs in both the visible and the near-infrared (NIR), while the monomer free triplet absorbs only in the visible. The intensity of the NIR absorption depends on the extent of intermolecular coupling, in agreement with observations in TIPS-pentacene nanocrystals. We predict additional weak ESA from the triplet-triplet but not from the triplet, at still lower energy.

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...

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.

Stability and signatures of biexcitons in carbon nanotubes

DEFF Research Database (Denmark)

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

2005-01-01

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

Optical instabilities and chaos due to the virtual formation of biexcitons

International Nuclear Information System (INIS)

Nguyen Trung Dan.

1994-07-01

Optical instabilities and chaos due to virtual formation of biexcitons in optically excited semiconductors are investigated. A complete linear stability analysis of steady-state bistable solutions of nonlinear coupled differential equations describing the nonlinear dynamics of semiconductors is carried out. The dynamical solutions are studied numerically using an iterative procedure. (author). 20 refs, 3 figs

Biexciton Auger Recombination Differs in Hybrid and Inorganic Halide Perovskite Quantum Dots.

Science.gov (United States)

Eperon, Giles E; Jedlicka, Erin; Ginger, David S

2018-01-04

We use time-resolved photoluminescence measurements to determine the biexciton Auger recombination rate in both hybrid organic-inorganic and fully inorganic halide perovskite nanocrystals as a function of nanocrystal volume. We find that the volume scaling of the biexciton Auger rate in the hybrid perovskites, containing a polar organic A-site cation, is significantly shallower than in the fully inorganic Cs-based nanocrystals. As the nanocrystals become smaller, the Auger rate in the hybrid nanocrystals increases even less than expected, compared to the fully inorganic nanocrystals, which already show a shallower volume dependence than other material systems such as chalcogenide quantum dots. This finding suggests there may be differences in the strength of Coulombic interactions between the fully inorganic and hybrid perovskites, which may prove to be crucial in selecting materials to obtain the highest performing devices in the future, and hints that there could be something "special" about the hybrid materials.

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.

Dark trions and biexcitons in WS2 and WSe2 made bright by e-e scattering

Science.gov (United States)

Danovich, Mark; Zólyomi, Viktor; Fal'Ko, Vladimir I.

2017-04-01

The direct band gap character and large spin-orbit splitting of the valence band edges (at the K and K’ valleys) in monolayer transition metal dichalcogenides have put these two-dimensional materials under the spot-light of intense experimental and theoretical studies. In particular, for Tungsten dichalcogenides it has been found that the sign of spin splitting of conduction band edges makes ground state excitons radiatively inactive (dark) due to spin and momentum mismatch between the constituent electron and hole. One might similarly assume that the ground states of charged excitons and biexcitons in these monolayers are also dark. Here, we show that the intervalley (K ⇆ K‧) electron-electron scattering mixes bright and dark states of these complexes, and estimate the radiative lifetimes in the ground states of these “semi-dark” trions and biexcitons to be ~10 ps, and analyse how these complexes appear in the temperature-dependent photoluminescence spectra of WS2 and WSe2 monolayers.

Coherent dynamics of exciton and biexciton resonances in InGaAs/GaAs single quantum wells

DEFF Research Database (Denmark)

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

1999-01-01

The coherent dynamics of both exciton and biexciton resonances have been investigated in In0.18Ga0.82As/GaAs single quantum wells with thicknesses ranging from 1 to 4 nm, using time-integrated and spectrally-resolved transient four-wave mixing. From the temperature dependence of the exciton...

Self-reflection in a system of excitons and biexcitons in semiconductors

International Nuclear Information System (INIS)

Khadzhi, P I; Lyakhomskaya, K D

1999-01-01

The characteristic features of the self-reflection of a powerful electromagnetic wave in a system of coherent excitons and biexcitons in semiconductors were investigated as one of the manifestations of the nonlinear optical skin effect. It was found that a monotonically decreasing standing wave with an exponentially falling spatial tail is formed in the surface region of a semiconductor. Under the influence of the field of a powerful pulse, an optically homogeneous medium is converted into one with distributed feedback. The appearance of spatially separated narrow peaks of the refractive index, extinction coefficient, and reflection coefficient is predicted. (nonlinear optical phenomena)

Biexciton binding energy in ZnSe quantum wells and quantum wires

DEFF Research Database (Denmark)

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

2002-01-01

The biexciton binding energy E-XX is investigated in ZnSe/ZnMgSe quantum wells and quantum wires as a function of the lateral confinement by transient four-wave mixing. In the quantum wells one observes for decreasing well width a significant increase in the relative binding energy, saturating...... for well widths less than 8 nm. In the quantum wires an increase of 30% is found in the smallest quantum wire structures compared to the corresponding quantum well value. A simple analytical model taking into account the quantum confinement in these low-dimensional systems is used to explain...

Biexcitons in π-conjugated oligomers: Intensity-dependent femtosecond transient-absorption study

Science.gov (United States)

Klimov, V. I.; McBranch, D. W.; Barashkov, N.; Ferraris, J.

1998-09-01

We report femtosecond transient-absorption (TA) studies of a five-ring oligomer of poly(para-phenylene vinylene) prepared in two different forms: solid-state films and dilute solutions. At high pump fluences, in both types of samples, we observe generation of two-exciton states, which are detected by the evolution of TA spectra and dynamics with increasing pump intensity. In solutions, double excitation of molecules results in the formation of stable biexcitons with enhanced oscillator strength, leading to an increased efficiency of the radiative decay and a superlinear pump dependence of the stimulated emission. In solid-state samples, the two-exciton states are unstable and decay on the subpicosecond time scale due to ultrafast charge transfer, accompanied by generation of interchain excitons.

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)

Biexcitons in {pi}-conjugated oligomers: Intensity-dependent femtosecond transient-absorption study

Energy Technology Data Exchange (ETDEWEB)

Klimov, V.I.; McBranch, D.W. [Chemical Science and Technology Division, CST-6, Mail Stop J585, Los Alamos National Laboratory, Los Alamos, New Mexico 87545 (United States); Barashkov, N.; Ferraris, J. [Chemistry Department, University of Texas, Dallas, Texas 75083 (United States)

1998-09-01

We report femtosecond transient-absorption (TA) studies of a five-ring oligomer of poly({ital para}-phenylene vinylene) prepared in two different forms: solid-state films and dilute solutions. At high pump fluences, in both types of samples, we observe generation of two-exciton states, which are detected by the evolution of TA spectra and dynamics with increasing pump intensity. In solutions, double excitation of molecules results in the formation of stable biexcitons with enhanced oscillator strength, leading to an increased efficiency of the radiative decay and a superlinear pump dependence of the stimulated emission. In solid-state samples, the two-exciton states are unstable and decay on the subpicosecond time scale due to ultrafast charge transfer, accompanied by generation of interchain excitons. {copyright} {ital 1998} {ital The American Physical Society}

NONLINEAR OPTICAL PHENOMENA: Self-reflection in a system of excitons and biexcitons in semiconductors

Science.gov (United States)

Khadzhi, P. I.; Lyakhomskaya, K. D.

1999-10-01

The characteristic features of the self-reflection of a powerful electromagnetic wave in a system of coherent excitons and biexcitons in semiconductors were investigated as one of the manifestations of the nonlinear optical skin effect. It was found that a monotonically decreasing standing wave with an exponentially falling spatial tail is formed in the surface region of a semiconductor. Under the influence of the field of a powerful pulse, an optically homogeneous medium is converted into one with distributed feedback. The appearance of spatially separated narrow peaks of the refractive index, extinction coefficient, and reflection coefficient is predicted.

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)

Ultrafast spectral interferometry of resonant secondary emission from quantum wells: From Rayleigh scattering to coherent emission from biexcitons

DEFF Research Database (Denmark)

Birkedal, Dan; Shah, Jagdeep; Pfeiffer, L. N.

1999-01-01

Recent investigations of secondary emission from quantum well excitons following ultrafast resonant excitation have demonstrated an intricate interplay of coherent Rayleigh scattering and incoherent luminescence. We have very recently demonstrated that it is possible to isolate and time resolve...... the coherent field associated with Rayleigh component using ultrafast spectral interferometry or Tadpole, thus, obtaining substantial and new information of the nature of resonant secondary emission. Our observation demonstrates that Rayleigh scattering from static disorder is inherently a non-ergodic process...... invalidating the use of current theories using ensemble averages to describe our observations. Furthermore, we report here a new and hitherto unknown coherent scattering mechanism involving the two-photon coherence associated with the biexciton transition. The process leaves an exciton behind taking up...

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.

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.

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

Exciton molecule in semiconductors by two-photon absorption

International Nuclear Information System (INIS)

Arya, K.; Hassan, A.R.

1976-07-01

Direct creation of bi-exciton states by two-photon absorption in direct gap semiconductors is investigated theoretically. A numerical application to the case of CuCl shows that the two-photon absorption coefficient for bi-excitonic transitions is larger than that for two-photon interband transitions by three orders of magnitude. It becomes comparable to that for one-photon excitonic transitions for available laser intensities. The main contribution to this enhancement of the absorption coefficient for the transitions to the bi-exciton states is found to be from the resonance effect

Amplification of electromagnetic radiation in the exciton region of the spectrum of a semiconductor

International Nuclear Information System (INIS)

Nerkararyan, Kh.V.

1989-01-01

The problem of amplification of electromagnetic radiation in the exciton region of the spectrum of a semiconductor was first discussed by Haken. The possibility of amplification of an electromagnetic wave under conditions of Bose condensation of biexcitons was considered in Ref. 2. However, the difficulties encountered in the creation of a Bose condensed state of biexcitons complicate greatly the performance of an experiment of this kind. The authors shall show that amplification is possible also in a gaseous mixture of excitons and biexcitons which is in thermal equilibrium and can be described by the Maxwellian distribution function of the velocities

Interaction and Dephasing of Excitons in ZnSe Quantum Wires

DEFF Research Database (Denmark)

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

1999-01-01

We study the coherent formation of biexcitons in wet-etched ZnSe quantum wires of lateral sizes down to 23 nm by transient degenerate four-wave mixing. We observe an increase of the biexciton binding energy with decreasing wire width reaching 30% energy enhancement in the smallest wire structure...

Two-Photon Rabi Splitting in a Coupled System of a Nanocavity and Exciton Complexes

Science.gov (United States)

Qian, Chenjiang; Wu, Shiyao; Song, Feilong; Peng, Kai; Xie, Xin; Yang, Jingnan; Xiao, Shan; Steer, Matthew J.; Thayne, Iain G.; Tang, Chengchun; Zuo, Zhanchun; Jin, Kuijuan; Gu, Changzhi; Xu, Xiulai

2018-05-01

Two-photon Rabi splitting in a cavity-dot system provides a basis for multiqubit coherent control in a quantum photonic network. Here we report on two-photon Rabi splitting in a strongly coupled cavity-dot system. The quantum dot was grown intentionally large in size for a large oscillation strength and small biexciton binding energy. Both exciton and biexciton transitions couple to a high-quality-factor photonic crystal cavity with large coupling strengths over 130 μ eV . Furthermore, the small binding energy enables the cavity to simultaneously couple with two exciton states. Thereby, two-photon Rabi splitting between the biexciton and cavity is achieved, which can be well reproduced by theoretical calculations with quantum master equations.

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

DEFF Research Database (Denmark)

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

2001-01-01

-biexciton beating at the exciton resonance is observed that is vanishing for long negative delays owing to the faster dephasing in the two-exciton continuum compared with the bound biexciton state. These results are in qualitative agreement with microscopic model calculations that include the coherent dynamics...... of one- and two-exciton resonances up to the fifth order in the optical field....

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.

Complexes of dipolar excitons in layered quasi-two-dimensional nanostructures

Science.gov (United States)

Bondarev, Igor V.; Vladimirova, Maria R.

2018-04-01

We discuss neutral and charged complexes (biexcitons and trions) formed by indirect excitons in layered quasi-two-dimensional semiconductor heterostructures. Indirect excitons—long-lived neutral Coulomb-bound pairs of electrons and holes of different layers—have been known for semiconductor coupled quantum wells and have recently been reported for van der Waals heterostructures such as double bilayer graphene and transition-metal dichalcogenides. Using the configuration space approach, we derive the analytical expressions for the trion and biexciton binding energies as a function of interlayer distance. The method captures essential kinematics of complex formation to reveal significant binding energies, up to a few tens of meV for typical interlayer distances ˜3 -5 Å , with the trion binding energy always being greater than that of the biexciton. Our results can contribute to the understanding of more complex many-body phenomena such as exciton Bose-Einstein condensation and Wigner-like electron-hole crystallization in layered semiconductor heterostructures.

Development of a scanning nearfield optical microscope for low-temperature investigations of semiconductor nanostructures

International Nuclear Information System (INIS)

Hodeck, Kai Friedrich

2009-01-01

In the present work the electronic structure of MOCVD-grown InGaAs/GaAs and InAs/GaAs quantum dots which are characterized by a particularly low ground state transition energy, was investigated using Scanning Nearfield Optical Microscopy (SNOM). The pivotal question of the presented investigations is, which influence the interaction of the confined carriers has on the energy states of the biexcitons and the multiexcitons in a quantum dot. Therefore, photoluminescence spectra of single quantum dots were investigated under varying excitation intensity at different temperatures between 5 K and 300 K. The construction of a novel scanning nearfield microscope especially for low temperatures allowed the investigation of single quantum dots. Due to significant improvements of the positioning technology and the shear-force distance control between the sample and the nearfield probe a stable scanning of the quantum dot samples at 5 K could be demonstrated, showing a lateral optical resolution of 200 nm. This way, in the photoluminescence spectroscopy of single quantum dots the thermal linewidth broadening of the detected light was reduced down to a value of less than 1 meV, which allowed the identification of the transitions of biexcitons and multiexcitons. On the basis of the performed measurements, for the InGaAs/GaAs quantum dots a biexciton state was identified, with variable binding energies of 2-7 meV. Furthermore, a positively charged trion state with a binding energy of 11 meV was observed, showing high emission intensity, which can be assigned to the sample doping. Accordingly, for the positively charged biexciton state a binding energy of 11 meV can be announced. For the investigated InAs/GaAs quantum dots a biexciton state with binding energies of 3-4 meV was found. Some of the investigated InAs/GaAs quantum dots showed the formation of positively charged states, in particular of a trion state with a binding energy of 3 meV, and of the positively charged

Development of a scanning nearfield optical microscope for low-temperature investigations of semiconductor nanostructures

Energy Technology Data Exchange (ETDEWEB)

Hodeck, Kai Friedrich

2009-02-19

In the present work the electronic structure of MOCVD-grown InGaAs/GaAs and InAs/GaAs quantum dots which are characterized by a particularly low ground state transition energy, was investigated using Scanning Nearfield Optical Microscopy (SNOM). The pivotal question of the presented investigations is, which influence the interaction of the confined carriers has on the energy states of the biexcitons and the multiexcitons in a quantum dot. Therefore, photoluminescence spectra of single quantum dots were investigated under varying excitation intensity at different temperatures between 5 K and 300 K. The construction of a novel scanning nearfield microscope especially for low temperatures allowed the investigation of single quantum dots. Due to significant improvements of the positioning technology and the shear-force distance control between the sample and the nearfield probe a stable scanning of the quantum dot samples at 5 K could be demonstrated, showing a lateral optical resolution of 200 nm. This way, in the photoluminescence spectroscopy of single quantum dots the thermal linewidth broadening of the detected light was reduced down to a value of less than 1 meV, which allowed the identification of the transitions of biexcitons and multiexcitons. On the basis of the performed measurements, for the InGaAs/GaAs quantum dots a biexciton state was identified, with variable binding energies of 2-7 meV. Furthermore, a positively charged trion state with a binding energy of 11 meV was observed, showing high emission intensity, which can be assigned to the sample doping. Accordingly, for the positively charged biexciton state a binding energy of 11 meV can be announced. For the investigated InAs/GaAs quantum dots a biexciton state with binding energies of 3-4 meV was found. Some of the investigated InAs/GaAs quantum dots showed the formation of positively charged states, in particular of a trion state with a binding energy of 3 meV, and of the positively charged

Many-body effects in transport through a quantum-dot cavity system

Science.gov (United States)

Dinu, I. V.; Moldoveanu, V.; Gartner, P.

2018-05-01

We theoretically describe electric transport through an optically active quantum dot embedded in a single-mode cavity, and coupled to source-drain particle reservoirs. The populations of various many-body configurations (e.g., excitons, trions, biexciton) and the photon-number occupancies are calculated from a master equation which is derived in the basis of dressed states. These take into account both the Coulomb and the light-matter interaction. The former is essential in the description of the transport, while for the latter we identify situations in which it can be neglected in the expression of tunneling rates. The fermionic nature of the particle reservoirs plays an important role in the argument. The master equation is numerically solved for the s -shell many-body configurations of disk-shaped quantum dots. If the cavity is tuned to the biexciton-exciton transition, the most efficient optical processes take place in a three-level Λ system. The alternative exciton-ground-state route is inhibited as nonresonant due to the biexciton binding energy. The steady-state current is analyzed as a function of the photon frequency and the coupling to the leads. An unexpected feature appears in its dependence on the cavity loss rate, which turns out to be nonmonotonic.

Slow Auger Relaxation in HgTe Colloidal Quantum Dots.

Science.gov (United States)

Melnychuk, Christopher; Guyot-Sionnest, Philippe

2018-05-03

The biexciton lifetimes in HgTe colloidal quantum dots are measured as a function of particle size. Samples produced by two synthetic methods, leading to partially aggregated or well-dispersed particles, exhibit markedly different dynamics. The relaxation characteristics of partially aggregated HgTe inhibit reliable determinations of the Auger lifetime. In well-dispersed HgTe quantum dots, the biexciton lifetime increases approximately linearly with particle volume, confirming trends observed in other systems. The extracted Auger coefficient is three orders of magnitude smaller than that for bulk HgCdTe materials with similar energy gaps. We discuss these findings in the context of understanding Auger relaxation in quantum-confined systems and their relevance to mid-infrared optoelectronic devices based on HgTe colloidal quantum dots.

Coherent dynamics in semiconductors

DEFF Research Database (Denmark)

Hvam, Jørn Märcher

1998-01-01

enhanced in quantum confined lower-dimensional systems, where exciton and biexciton effects dominate the spectra even at room temperature. The coherent dynamics of excitons are at modest densities well described by the optical Bloch equations and a number of the dynamical effects known from atomic......Ultrafast nonlinear optical spectroscopy is used to study the coherent dynamics of optically excited electron-hole pairs in semiconductors. Coulomb interaction implies that the optical inter-band transitions are dominated, at least at low temperatures, by excitonic effects. They are further...... and molecular systems are found and studied in the exciton-biexciton system of semiconductors. At densities where strong exciton interactions, or many-body effects, become dominant, the semiconductor Bloch equations present a more rigorous treatment of the phenomena Ultrafast degenerate four-wave mixing is used...

Understanding the features in the ultrafast transient absorption spectra of CdSe quantum dots

Energy Technology Data Exchange (ETDEWEB)

Zhang, Cheng; Do, Thanh Nhut [Division of Chemistry and Biological Chemistry, School of Physical and Mathematical Sciences, Nanyang Technological University, 21 Nanyang Link, Singapore 637371 (Singapore); Ong, Xuanwei [Department of Chemistry, National University of Singapore, 3 Science Drive 3, Singapore 117543 (Singapore); Chan, Yinthai [Department of Chemistry, National University of Singapore, 3 Science Drive 3, Singapore 117543 (Singapore); Institute of Materials Research & Engineering, A*STAR, 2 Fusionopolis Way, Innovis, Singapore 138634 (Singapore); Tan, Howe-Siang, E-mail: howesiang@ntu.edu.sg [Division of Chemistry and Biological Chemistry, School of Physical and Mathematical Sciences, Nanyang Technological University, 21 Nanyang Link, Singapore 637371 (Singapore)

2016-12-20

We describe a model to explain the features of the ultrafast transient absorption (TA) spectra of CdSe core type quantum dots (QDs). The measured TA spectrum consists of contributions by the ground state bleach (GSB), stimulated emission (SE) and excited state absorption (ESA) processes associated with the three lowest energy transition of the QDs. We model the shapes of the GSB, SE and ESA spectral components after fits to the linear absorption. The spectral positions of the ESA components take into account the biexcitonic binding energy. In order to obtain the correct weightage of the GSB, SE and ESA components to the TA spectrum, we enumerate the set of coherence transfer pathways associated with these processes. From our fits of the experimental TA spectra of 65 Å diameter QDs, biexcitonic binding energies for the three lowest energy transitions are obtained.

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.

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...

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.

Suppressed Blinking and Auger Recombination in Near-Infrared Type-II InP/CdS Nanocrystal Quantum Dots

Science.gov (United States)

Dennis, Allison M.; Mangum, Benjamin D.; Piryatinski, Andrei; Park, Young-Shin; Hannah, Daniel C.; Casson, Joanna L.; Williams, Darrick J.; Schaller, Richard D.; Htoon, Han; Hollingsworth, Jennifer A.

2012-01-01

Non-blinking excitonic emission from near-infrared and type-II nanocrystal quantum dots (NQDs) is reported for the first time. To realize this unusual degree of stability at the single-dot level, novel InP/CdS core/shell NQDs were synthesized for a range of shell thicknesses (~1–11 monolayers of CdS). Ensemble spectroscopy measurements (photoluminescence peak position and radiative lifetimes) and electronic structure calculations established the transition from type-I to type-II band alignment in these heterostructured NQDs. More significantly, single-NQD studies revealed clear evidence for blinking suppression that was not strongly shell-thickness dependent, while photobleaching and biexciton lifetimes trended explicitly with extent of shelling. Specifically, very long biexciton lifetimes—up to >7 ns—were obtained for the thickest-shell structures, indicating dramatic suppression of non-radiative Auger recombination. This new system demonstrates that electronic structure and shell thickness can be employed together to effect control over key single-dot and ensemble NQD photophysical properties. PMID:23030497

Monotonicity and concavity in Coulomb systems

International Nuclear Information System (INIS)

Englisch, R.; Englisch, H.; Karl-Marx-Universitaet, Leipzig

1986-01-01

The eigenvalues of H(α) = H 0 + αH * , where H * is an arbitrary Coulomb potential, decrease with increasing α ≥ 0. Linear and parabolic bounds for the ground state energy are presented. These bounds are applied to the biexciton and the exciton at a neutral donor. (orig.)

Transient four-wave mixing in T-shaped GaAs quantum wires

DEFF Research Database (Denmark)

Langbein, Wolfgang Werner; Gislason, Hannes; Hvam, Jørn Märcher

1999-01-01

The binding energy of excitons and biexcitons and the exciton dephasing in T-shaped GaAs quantum wires is investigated by transient four-wave mixing. The T-shaped structure is fabricated by cleaved-edge overgrowth, and its geometry is engineered to optimize the one-dimensional confinement. In thi...

Spectroscopy of size dependent many-particle effects in single self-assembled semiconductor quantum dots

Energy Technology Data Exchange (ETDEWEB)

Dal Savio, C.

2006-02-20

Single InAs quantum dots (QDs) grown with the Stranski-Krastanov method in a In{sub 0.12}Ga{sub 0.88}As quantum well embedded in GaAs and emitting in the near infrared have been optically investigated. To perform QD spectroscopy at low temperatures a very stable micro-photoluminescence ({mu}-PL) microscope set-up fully integrated in a liquid helium (LHe) cryostate has been successfully developed. The system is based on the cold finger technique and a Fourier Transform (FT) spectrometer combined with a nitrogen cooled Ge detector. Photoluminescence of the QDs was excited non resonantly with a He-Ne laser and single dot spectroscopy was carried out at temperatures below 60 K. The experimental set-up allows mapping of the optical emission by recording spectra for every point of a scan grid. This mapping mode is used to acquire optical images and to locate a particular dot for investigation. Series of measurement on a single QD were normally performed over a long time (from a few days to a week), with the need of daily adjustment in the sub-micrometer range. At low excitation power a single sharp line (E{sub x}) arising from recombination of a single exciton in the dot is observed. Varying the excitation density the spectra become more complex, with appearance of the biexciton emission line (E{sub xx}) on the lower energies side of the E{sub x} line, followed by emission from excitons occupying higher shells in the dot. Measured biexciton binding energies and power dependence are in good agreement with values reported in the literature. The temperature dependence of the optical emission was investigated. The energy shows the characteristic decrease related to the shrinking of the semiconductor band gap, while the linewidth evolution is compatible with broadening due to coupling with acoustic and optical phonons. A statistics of biexciton binding energies over a dozen of dots was acquired and the results compared with single QD spectroscopy data available in the

Superposition Principle in Auger Recombination of Charged and Neutral Multicarrier States in Semiconductor Quantum Dots.

Science.gov (United States)

Wu, Kaifeng; Lim, Jaehoon; Klimov, Victor I

2017-08-22

Application of colloidal semiconductor quantum dots (QDs) in optical and optoelectronic devices is often complicated by unintentional generation of extra charges, which opens fast nonradiative Auger recombination pathways whereby the recombination energy of an exciton is quickly transferred to the extra carrier(s) and ultimately dissipated as heat. Previous studies of Auger recombination have primarily focused on neutral and, more recently, negatively charged multicarrier states. Auger dynamics of positively charged species remains more poorly explored due to difficulties in creating, stabilizing, and detecting excess holes in the QDs. Here we apply photochemical doping to prepare both negatively and positively charged CdSe/CdS QDs with two distinct core/shell interfacial profiles ("sharp" versus "smooth"). Using neutral and charged QD samples we evaluate Auger lifetimes of biexcitons, negative and positive trions (an exciton with an extra electron or a hole, respectively), and multiply negatively charged excitons. Using these measurements, we demonstrate that Auger decay of both neutral and charged multicarrier states can be presented as a superposition of independent elementary three-particle Auger events. As one of the manifestations of the superposition principle, we observe that the biexciton Auger decay rate can be presented as a sum of the Auger rates for independent negative and positive trion pathways. By comparing the measurements on the QDs with the "sharp" versus "smooth" interfaces, we also find that while affecting the absolute values of Auger lifetimes, manipulation of the shape of the confinement potential does not lead to violation of the superposition principle, which still allows us to accurately predict the biexciton Auger lifetimes based on the measured negative and positive trion dynamics. These findings indicate considerable robustness of the superposition principle as applied to Auger decay of charged and neutral multicarrier states

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)

Development of Highly Ordered Heterostructured Semiconductor Nanowire Arrays for Sub-Wavelength Optical Devices

Science.gov (United States)

2007-06-01

properties of nanowires" J. Appl. Phys 98, 094306 (2005) 9. Harry E. Ruda and Alexander Shik, "Polarization-sensitive optical properties of metallic and...34Biexcitons in parabolic quantum dots", Phys. Rev. B. 73, 125321 (2006). 11. M. Blumin, H.E. Ruda, I. Savelyev , A Shik and H. Wang, "Self-assembled InAs

Many-body effects in valleytronics: direct measurement of valley lifetimes in single-layer MoS2.

Science.gov (United States)

Mai, Cong; Barrette, Andrew; Yu, Yifei; Semenov, Yuriy G; Kim, Ki Wook; Cao, Linyou; Gundogdu, Kenan

2014-01-08

Single layer MoS2 is an ideal material for the emerging field of "valleytronics" in which charge carrier momentum can be finely controlled by optical excitation. This system is also known to exhibit strong many-body interactions as observed by tightly bound excitons and trions. Here we report direct measurements of valley relaxation dynamics in single layer MoS2, by using ultrafast transient absorption spectroscopy. Our results show that strong Coulomb interactions significantly impact valley population dynamics. Initial excitation by circularly polarized light creates electron-hole pairs within the K-valley. These excitons coherently couple to dark intervalley excitonic states, which facilitate fast electron valley depolarization. Hole valley relaxation is delayed up to about 10 ps due to nondegeneracy of the valence band spin states. Intervalley biexciton formation reveals the hole valley relaxation dynamics. We observe that biexcitons form with more than an order of magnitude larger binding energy compared to conventional semiconductors. These measurements provide significant insight into valley specific processes in 2D semiconductors. Hence they could be used to suggest routes to design semiconducting materials that enable control of valley polarization.

Theory of Spin States of Quantum Dot Molecules

Science.gov (United States)

Ponomarev, I. V.; Reinecke, T. L.; Scheibner, M.; Stinaff, E. A.; Bracker, A. S.; Doty, M. F.; Gammon, D.; Korenev, V. L.

2007-04-01

The photoluminescence spectrum of an asymmetric pair of coupled InAs quantum dots in an applied electric field shows a rich pattern of level anticrossings, crossings and fine structure that can be understood as a superposition of charge and spin configurations. We present a theoretical model that provides a description of the energy positions and intensities of the optical transitions in exciton, biexciton and charged exciton states of coupled quantum dots molecules.

Monotonicity of energy eigenvalues for Coulomb systems

International Nuclear Information System (INIS)

Englisch, R.

1983-01-01

Generalising results by earlier workers for a large class of Hamiltonians (among others, Hamiltonians of Coulomb systems) which can be written in the form H(α) = H 0 + αH' the present works shows that their eigenvalues decrease with increasing α. This result is applied to Coulomb systems in which the distances between the infinitely heavy particles are varying and also is used to obtain a completion and simplification of proof for the stability of the biexciton. (author)

Fabrication of cuprous chloride films on copper substrate by chemical bath deposition

Energy Technology Data Exchange (ETDEWEB)

Lin, Yu-Ting; Ci, Ji-Wei; Tu, Wei-Chen [Department of Electronic Engineering, College of Electrical Engineering and Computer Science, Chung Yuan Christian University, Chung-Li 32023, Taiwan (China); Uen, Wu-Yih, E-mail: uenwuyih@ms37.hinet.net [Department of Electronic Engineering, College of Electrical Engineering and Computer Science, Chung Yuan Christian University, Chung-Li 32023, Taiwan (China); Lan, Shan-Ming [Department of Electronic Engineering, College of Electrical Engineering and Computer Science, Chung Yuan Christian University, Chung-Li 32023, Taiwan (China); Yang, Tsun-Neng; Shen, Chin-Chang; Wu, Chih-Hung [Institute of Nuclear Energy Research, P.O. Box 3-11, Lungtan 32500, Taiwan (China)

2015-09-30

Polycrystalline CuCl films were fabricated by chemical bath deposition (CBD) on a Cu substrate at a low solution temperature of 90 °C. Continuous CuCl films were prepared using the copper (II) chloride (CuCl{sub 2}) compound as the precursor for both the Cu{sup 2+} and Cl{sup −} sources, together with repeated HCl dip treatments. An HCl dip pretreatment of the substrate favored the nucleation of CuCl crystallites. Further, interrupting the film deposition and including an HCl dip treatment of the film growth surface facilitated the deposition of a full-coverage CuCl film. A dual beam (FIB/SEM) system with energy dispersive spectrometry facilities attached revealed a homogeneous CuCl layer with a flat-top surface and an average thickness of about 1 μm. Both the excitonic and biexcitonic emission lines were well-resolved in the 6.4 K photoluminescence spectra. In particular, the free exciton emission line was observable at room temperature, indicating the good quality of the CuCl films prepared by CBD. - Highlights: • Cuprous chloride (CuCl) was prepared on Cu substrate by chemical bath deposition. • HCl dip treatments facilitated the deposition of a full-coverage CuCl film. • A homogeneous elemental distribution was recognized for the deposited CuCl layer. • Excitonic and biexcitonic photoluminescence lines of CuCl films were well-resolved. • The free exciton emission line of CuCl films was observable at room temperature.

Valley dynamics of intravalley and intervalley multiexcitonic states in monolayer WS2

Science.gov (United States)

Fu, Jiyong; Bezerra, Andre; Qu, Fanyao

2018-03-01

We present a comprehensive model comprising of a complete set of rate equations, which account for charge transfer among multiexcitonic channels including excitons, trions, and biexcitons, to investigate valley (locked with spin) dynamics in monolayer WS2. The steady-state photoluminescence (PL) spectra, underlying the laser power dependence of excitonic populations, are also determined. Our computed PL for all excitonic states agrees with the experimental data of Paradisanos et al. [Appl. Phys. Lett. 110, 193102 (2017), 10.1063/1.4983285]. We find that the relative weight of PL, stemmed from different excitonic channels, strongly depends on the laser power even under dynamical conditions. Remarkably, the biexciton channel, having the weakest PL intensity at low laser powers, tends to prevail in PL over other excitonic states as the power strengthens. In addition, by accounting for intervalley scatterings, which enable transfer of excitonic states from one valley to the other, we determine the valley polarization, which strongly depends on intervalley scatterings and the exciton generation rates in the two valleys. On the other hand, the valley polarization for all excitonic channels is found almost independent of the laser power, consistent with experimental measurements as well. Finally, the valley dynamics involving both intra- and intervalley trions is discussed. Our model and numerical outcome should be beneficial to experiments especially featuring the interplay of multiexcitonic channels in, e.g., elucidating experimental data, estimating central excitonic quantities including recombination times and transition rates, and in widening possible new experimental scopes.

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.

Onion like growth and inverted many-particle energies in quantum dots

International Nuclear Information System (INIS)

Bimberg, D.

2008-01-01

Use of surfactants like antimony in MOCVD growth enables novel growth regimes for quantum dots (QDs). The quantum dot ensemble luminescence no longer appears as a single inhomogeneously broadened peak but shows a multi-modal structure. Quantum dot subensembles are forming which differ in height by exactly one monolayer. For the first time the systematic dependence of excitonic properties on quantum dot size and shape can be investigated in detail. Both biexcitonic binding energy and excitonic fine-structure splitting vary from large positive through zero to negative values. Correlation and piezoelectric effects explain the observations

Multicomponent exciton gas in cuprous oxide: cooling behaviour and the role of Auger decay

Science.gov (United States)

Semkat, D.; Sobkowiak, S.; Schöne, F.; Stolz, H.; Koch, Th; Fehske, H.

2017-10-01

In this paper we present a hydrodynamic model to describe the dynamics of para- and orthoexcitons in cuprous oxide at ultralow temperatures inside a stress induced potential trap. We take into account the finite lifetime of the excitons, the excitation process and exciton-phonon as well as exciton-exciton interaction. Furthermore, we model the two-body loss mechanism assuming an Auger-like effect and compare it to an alternative explanation which relies on the formation of biexcitons. We discuss in detail the influence on the numerical results and compare the predictions to experimental data.

Entangled-photon generation from a quantum dot in cavity QED

International Nuclear Information System (INIS)

Ajiki, Hiroshi; Ishihara, Hajime

2009-01-01

We theoretically study polarization-entangled photon generation from a single quantum dot in a microcavity. Entangled-photon pairs with singlet or triplet Bell states are generated in the resonant-hyperparametric scattering via dressed states in the cavity QED. Although co-polarized non-entangled photons are also generated, the generation is dramatically suppressed in the strong-coupling limit owing to the photon blockade effect. Finite binding energy of biexciton is also important for the generation of photon pairs with high degree of entanglement. (copyright 2009 WILEY-VCH Verlag GmbH and Co. KGaA, Weinheim) (orig.)

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....

Influence of multi-exciton correlations on nonlinear polariton dynamics in semiconductor microcavities

International Nuclear Information System (INIS)

Wen, P; Nelson, Keith A; Christmann, G; Baumberg, J J

2013-01-01

Using two-dimensional spectroscopy, we resolve multi-polariton coherences in quantum wells embedded inside a semiconductor microcavity and elucidate how multi-exciton correlations mediate polariton nonlinear dynamics. We find that polariton correlation strengths depend on spectral overlap with the biexciton resonance and that up to at least four polaritons can be correlated, a higher-order correlation than observed to date among excitons in bare quantum wells. The high-order correlations can be attributed to coupling through the cavity mode, although the role of high-order Coulomb correlations cannot be excluded. (paper)

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.

Effect of the depolarization field on coherent optical properties in semiconductor quantum dots

Science.gov (United States)

Mitsumori, Yasuyoshi; Watanabe, Shunta; Asakura, Kenta; Seki, Keisuke; Edamatsu, Keiichi; Akahane, Kouichi; Yamamoto, Naokatsu

2018-06-01

We study the photon echo spectrum of self-assembled semiconductor quantum dots using femtosecond light pulses. The spectrum shape changes from a single-peaked to a double-peaked structure as the time delay between the two excitation pulses is increased. The spectrum change is reproduced by numerical calculations, which include the depolarization field induced by the biexciton-exciton transition as well as the conventional local-field effect for the exciton-ground-state transition in a quantum dot. Our findings suggest that various optical transitions in tightly localized systems generate a depolarization field, which renormalizes the resonant frequency with a change in the polarization itself, leading to unique optical properties.

Excitons, biexcitons, and phonons in ultrathin CdSe/ZnSe quantum structures

DEFF Research Database (Denmark)

Gindele, F.; Woggon, Ulrike; Langbein, Wolfgang Werner

1999-01-01

The optical properties of CdSe nanostructures grown by migration-enhanced epitaxy of CdSe on ZnSe are studied by time-, energy-, and temperature-dependent photoluminescence and excitation spectroscopy, as well as by polarization-dependent four-wave mixing and two-photon absorption experiments...

Single-dot Spectroscopy of GaAs Quantum Dots Fabricated by Filling of Self-assembled Nanoholes

Directory of Open Access Journals (Sweden)

Heyn Ch

2010-01-01

Full Text Available Abstract We study the optical emission of single GaAs quantum dots (QDs. The QDs are fabricated by filling of nanoholes in AlGaAs and AlAs which are generated in a self-assembled fashion by local droplet etching with Al droplets. Using suitable process parameters, we create either uniform QDs in partially filled deep holes or QDs with very broad size distribution in completely filled shallow holes. Micro photoluminescence measurements of single QDs of both types establish sharp excitonic peaks. We measure a fine-structure splitting in the range of 22–40μeV and no dependence on QD size. Furthermore, we find a decrease in exciton–biexciton splitting with increasing QD size.

Photoluminescence of a single InAs/AlAs quantum dot

International Nuclear Information System (INIS)

Shamirzaev, T.S.; Zhuravlev, K.S.; Larsson, M.; Holtz, P.O.

2008-01-01

Micro-photoluminescence (μ-PL) of a simple InAs/AlAs quantum dot (QD) has been studied. It has been found that the μ-PL emission related to the recombination in a single QD is strongly broadened probably due to spectral diffusion. Emissions related to the recombination of biexcitons and excitons occupying excited levels of the QD are observed in μ-PL spectra at high excitation power densities. A red shift of the μ-PL emissions related to recombination of excitons in the ground and excited levels of the QD with increasing excitation power gives clear evidence for type I alignment of the InAs/AlAs QD. (copyright 2008 WILEY-VCH Verlag GmbH and Co. KGaA, Weinheim) (orig.)

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.

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

DEFF Research Database (Denmark)

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

1999-01-01

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

Dicke states in multiple quantum dots

Science.gov (United States)

Sitek, Anna; Manolescu, Andrei

2013-10-01

We present a theoretical study of the collective optical effects which can occur in groups of three and four quantum dots. We define conditions for stable subradiant (dark) states, rapidly decaying super-radiant states, and spontaneous trapping of excitation. Each quantum dot is treated like a two-level system. The quantum dots are, however, realistic, meaning that they may have different transition energies and dipole moments. The dots interact via a short-range coupling which allows excitation transfer across the dots, but conserves the total population of the system. We calculate the time evolution of single-exciton and biexciton states using the Lindblad equation. In the steady state the individual populations of each dot may have permanent oscillations with frequencies given by the energy separation between the subradiant eigenstates.

Vector pulsing soliton of self-induced transparency in waveguide

International Nuclear Information System (INIS)

Adamashvili, G.T.

2015-01-01

A theory of an optical resonance vector pulsing soliton in waveguide is developed. A thin transition layer containing semiconductor quantum dots forms the boundary between the waveguide and one of the connected media. Analytical and numerical solutions for the optical vector pulsing soliton in waveguide are obtained. The vector pulsing soliton in the presence of excitonic and bi-excitonic excitations is compared with the soliton for waveguide TM-modes with parameters that can be used in modern optical experiments. It is shown that these nonlinear waves have significantly different parameters and shapes. - Highlights: • An optical vector pulsing soliton in a planar waveguide is presented. • Explicit form of the optical vector pulsing soliton are obtained. • The vector pulsing soliton and the soliton have different parameters and profiles

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.

Pairing mechanism in Bi-O superconductors: A finite-size chain calculation

International Nuclear Information System (INIS)

Aligia, A.A.; Nunez Regueiro, M.D.; Gagliano, E.R.

1989-01-01

We have studied the pairing mechanism in BiO 3 systems by calculating the binding energy of a pair of holes in finite Bi-O chains, for parameters that simulate three-dimensional behavior. In agreement with previous results using perturbation theory in the hopping t, for covalent Bi-O binding and parameters for which the parent compound has a disproportionate ground state, pairing induced by the presence of biexcitons is obtained for sufficiently large interatomic Coulomb repulsion. The analysis of appropriate correlation functions shows a rapid metallization of the system as t and the number of holes increase. This fact shrinks the region of parameters for which the finite-size calculations can be trusted without further study. The same model for other parameters yields pairing in two other regimes: bipolaronic and magnetic excitonic

Electric field induced removal of the biexciton binding energy in a single quantum dot

NARCIS (Netherlands)

Reimer, M.E.; Kouwen, Van M.P.; Hidma, A.W.; Weert, van M.H.M.; Bakkers, E.P.A.M.; Kouwenhoven, L.P.; Zwiller, V.

2011-01-01

We control the electrostatic environment of a single InAsP quantum dot in an InP nanowire with two contacts and two lateral gates positioned to an individual nanowire. We empty the quantum dot of excess charges and apply an electric field across its radial dimension. A large tuning range for the

Using biharmonic laser pumping for preparation of pure and entangled multiexciton states in clusters of resonantly interacting fluorescent centres

International Nuclear Information System (INIS)

Basieva, I.T.; Basiev, T.T.; Dietler, G.; Pukhov, K.K.; Sekatskii, S.K.

2007-01-01

Use of a biharmonic laser pumping for preparation of pure and entangled multiexciton states in dimers and tetramers of resonantly interacting fluorescent particles is analysed. Special emphasis is given to the preparation of all possible pure exciton states and their maximally entangled Bell states. The general results are illustrated using as an example the pair and quartet centres of neodymium ions in calcium fluoride (M- and N-centres), where all necessary experimental information concerning the interactions and decoherence is available, and experimental preparation of Bell vacuum-single exciton and vacuum-biexciton states has been recently demonstrated. These results can be easily rescaled for the cases of quantum dots and dye molecules. Numerical results are compared with the analytical results obtained for a particular case of the biharmonic excitation of dimers. Excellent agreement between these approaches is demonstrated

Comportamiento óptico no-lineal de nanocristales semiconductores de CdS en una matriz de gel de sílice

Directory of Open Access Journals (Sweden)

de la Rosa-Fox, N.

2000-06-01

Full Text Available Nanocrystals embedded in a dielectric matrix can be obtained through sol-gel method, it permits the control of several kinetic parameters during the nanocrystal growth. The size and size distribution have been studied by means small-angle neutron scattering techniques (SANS, that allow a spatial resolution from 1 to 50 nm. High intensity optical excitation from a Nd:YAG laser (6 ns pulse at 10 Hz repetition rate was focused on the sample to study the photoluminescence yield at rigth angle. The spectrum shows radiative process from intrinsic transitions (2.76 eV and a broad band in the lower energy side (1.65 eV that correspond to crystal surface traps. The photoluminescence yield grows superlineary giving rise to amplified intensity (60 cm-1 due to biexciton species, this fact can be interpreted as a non-linear optical behaviour coming from the CdS nanocrystals.

La inclusión de nanocristales en una matriz dieléctrica puede realizarse mediante el método sol-gel, permitiendo el control de parámetros cinéticos en el crecimiento de los cristales. El tamaño y distribución de dichos nanocristales se han estudiado por medio de difusión de neutrones a bajo ángulo (SANS, con una resolución espacial entre 1 y 50 nm. Bajo excitación óptica de alta intensidad, usando un láser (Nd:YAG con pulsos de 6 ns y una frecuencia de repetición de 10 Hz, se focalizó en la muestra para registrar la señal de fotoluminiscencia en la dirección perpendicular. El espectro indica procesos radiativos debidos a transiciones intrínsecas (2.76 eV y una banda ancha a más baja energía (1.65 eV correspondiente a recombinaciones en los defectos superficiales. La señal de fotoluminiscencia crece superlinealmente dando lugar a una amplificación (60 cm-1 debida principalmente a biexcitones que indican un comportamiento óptico no-lineal de los nanocristales de CdS.

A quantum light-emitting diode for the standard telecom window around 1,550 nm.

Science.gov (United States)

Müller, T; Skiba-Szymanska, J; Krysa, A B; Huwer, J; Felle, M; Anderson, M; Stevenson, R M; Heffernan, J; Ritchie, D A; Shields, A J

2018-02-28

Single photons and entangled photon pairs are a key resource of many quantum secure communication and quantum computation protocols, and non-Poissonian sources emitting in the low-loss wavelength region around 1,550 nm are essential for the development of fibre-based quantum network infrastructure. However, reaching this wavelength window has been challenging for semiconductor-based quantum light sources. Here we show that quantum dot devices based on indium phosphide are capable of electrically injected single photon emission in this wavelength region. Using the biexciton cascade mechanism, they also produce entangled photons with a fidelity of 87 ± 4%, sufficient for the application of one-way error correction protocols. The material system further allows for entangled photon generation up to an operating temperature of 93 K. Our quantum photon source can be directly integrated with existing long distance quantum communication and cryptography systems, and provides a promising material platform for developing future quantum network hardware.

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.

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.

Tuning Single Quantum Dot Emission with a Micromirror.

Science.gov (United States)

Yuan, Gangcheng; Gómez, Daniel; Kirkwood, Nicholas; Mulvaney, Paul

2018-02-14

The photoluminescence of single quantum dots fluctuates between bright (on) and dark (off) states, also termed fluorescence intermittency or blinking. This blinking limits the performance of quantum dot-based devices such as light-emitting diodes and solar cells. However, the origins of the blinking remain unresolved. Here, we use a movable gold micromirror to determine both the quantum yield of the bright state and the orientation of the excited state dipole of single quantum dots. We observe that the quantum yield of the bright state is close to unity for these single QDs. Furthermore, we also study the effect of a micromirror on blinking, and then evaluate excitation efficiency, biexciton quantum yield, and detection efficiency. The mirror does not modify the off-time statistics, but it does change the density of optical states available to the quantum dot and hence the on times. The duration of the on times can be lengthened due to an increase in the radiative recombination rate.

Evolution in time of an N-atom system. I. A physical basis set for the projection of the master equation

International Nuclear Information System (INIS)

Freedhoff, Helen

2004-01-01

We study an aggregate of N identical two-level atoms (TLA's) coupled by the retarded interatomic interaction, using the Lehmberg-Agarwal master equation. First, we calculate the entangled eigenstates of the system; then, we use these eigenstates as a basis set for the projection of the master equation. We demonstrate that in this basis the equations of motion for the level populations, as well as the expressions for the emission and absorption spectra, assume a simple mathematical structure and allow for a transparent physical interpretation. To illustrate the use of the general theory in emission processes, we study an isosceles triangle of atoms, and present in the long wavelength limit the (cascade) emission spectrum for a hexagon of atoms fully excited at t=0. To illustrate its use for absorption processes, we tabulate (in the same limit) the biexciton absorption frequencies, linewidths, and relative intensities for polygons consisting of N=2,...,9 TLA's

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.

Origins of Singlet Fission in Solid Pentacene from an ab initio Green's Function Approach

Science.gov (United States)

Refaely-Abramson, Sivan; da Jornada, Felipe H.; Louie, Steven G.; Neaton, Jeffrey B.

2017-12-01

We develop a new first-principles approach to predict and understand rates of singlet fission with an ab initio Green's-function formalism based on many-body perturbation theory. Starting with singlet and triplet excitons computed from a G W plus Bethe-Salpeter equation approach, we calculate the exciton-biexciton coupling to lowest order in the Coulomb interaction, assuming a final state consisting of two noninteracting spin-correlated triplets with finite center-of-mass momentum. For crystalline pentacene, symmetries dictate that the only purely Coulombic fission decay process from a bright singlet state requires a final state consisting of two inequivalent nearly degenerate triplets of nonzero, equal and opposite, center-of-mass momenta. For such a process, we predict a singlet lifetime of 30-70 fs, in very good agreement with experimental data, indicating that this process can dominate singlet fission in crystalline pentacene. Our approach is general and provides a framework for predicting and understanding multiexciton interactions in solids.

Temperature-dependent properties of semiconductor quantum dots in coherent regime; Temperaturabhaengige Eigenschaften einzelner Halbleiter-Quantenpunkte im Kohaerenten Regime

Energy Technology Data Exchange (ETDEWEB)

Huebner, Marc C.

2009-10-15

Recently, the public has become aware of keywords like ''Quantum computer'' or ''Quantum cryptography''. Regarding their potential application in solid state based quantum information processing and their overall benefit in fundamental research quantum dots have gained more and more public interest. In this context, quantum dots are often referred to as ''artificial atoms'', a term subsuming their physical properties quite nicely and emphasizing the huge potential for further investigations. The basic mechanism to be considered is the theoretical model of a two-level system. A quantum dot itself represents this kind of system quite nicely, provided that only the presence or absence of a single exciton in the ground state of that structure is regarded. This concept can also be expanded to the presence of two excitons (bi-exciton). Transitions between the relevant levels can be induced by optical stimulation. When integrating quantum dots in diode like structures measurements of this phenomena can be accomplished regarding photo currents. This means of detection is highly sensitive and allows for tuning of the energy levels with respect to the energy of an exciting laser utilizing the Stark effect (via an external electric field). The photo current then shows narrow resonances representing those transitions. By this, the system can be used as a highly sensitive nano-spectrometer. The examination of coherent interactions between quantum dots and an electromagnetic field uses laser pulses that are much shorter than the dephasing time of the system (2 ps). The basic study to be done on two level systems is the measurement of Rabi oscillations allowing for the selection of an arbitrary superposition of states. In this work, the existing setup was improved regarding the possibility to control the temperature of the sample. Up to now, only investigations at 4,2 K have been possible. Even at 70 K Rabi oscillations

All-inorganic perovskite nanocrystal assisted extraction of hot electrons and biexcitons from photoexcited CdTe quantum dots.

Science.gov (United States)

Mondal, Navendu; De, Apurba; Samanta, Anunay

2018-01-03

Excitation of semiconductor quantum dots (QDs) by photons possessing energy higher than the band-gap creates a hot electron-hole pair, which releases its excess energy as waste heat or under certain conditions (when hν > 2E g ) produces multiple excitons. Extraction of these hot carriers and multiple excitons is one of the key strategies for enhancing the efficiency of QD-based photovoltaic devices. However, this is a difficult task as competing carrier cooling and relaxation of multiple excitons (through Auger recombination) are ultrafast processes. Herein, we study the potential of all-inorganic perovskite nanocrystals (NCs) of CsPbX 3 (X = Cl, Br) as harvesters of these short-lived species from photo-excited CdTe QDs. The femtosecond transient absorption measurements show CsPbX 3 mediated extraction of both hot and thermalized electrons of the QDs (under a low pump power) and (under a high pump fluence) extraction of multiple excitons prior to their Auger assisted recombination. A faster timescale of thermalized electron transfer (∼2 ps) and a higher extraction efficiency of hot electrons (∼60%) are observed in the presence of CsPbBr 3 . These observations demonstrate the potential of all-inorganic perovskite NCs in the extraction of these short-lived energy rich species implying that complexes of the QDs and perovskite NCs are better suited for improving the efficiency of QD-sensitized solar cells.

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.

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.

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.

Violet-to-Blue Gain and Lasing from Colloidal CdS Nanoplatelets: Low-Threshold Stimulated Emission Despite Low Photoluminescence Quantum Yield

Energy Technology Data Exchange (ETDEWEB)

Diroll, Benjamin T.; Talapin, Dmitri V.; Schaller, Richard D.

2017-02-13

Amplified spontaneous emission (ASE) and lasing from solution-processed materials are demonstrated in the challenging violet-to-blue (430–490 nm) spectral region for colloidal nanoplatelets of CdS and newly synthesized core/shell CdS/ZnS nanoplatelets. Despite modest band-edge photoluminescence quantum yields of 2% or less for single excitons, which we show results from hole trapping, the samples exhibit low ASE thresholds. Furthermore, four-monolayer CdS samples show ASE at shorter wavelengths than any reported film of colloidal quantum-confined material. This work underlines that low quantum yields for single excitons do not necessarily lead to a poor gain medium. The low ASE thresholds originate from negligible dispersion in thickness, large absorption cross sections of 2.8 × 10–14 cm–2, and rather slow (150 to 300 ps) biexciton recombination. We show that under higher-fluence excitation, ASE can kinetically outcompete hole trapping. Using nanoplatelets as the gain medium, lasing is observed in a linear optical cavity. This work confirms the fundamental advantages of colloidal quantum well structures as gain media, even in the absence of high photoluminescence efficiency.

Highly Enhanced Many-Body Interactions in Anisotropic 2D Semiconductors.

Science.gov (United States)

Sharma, Ankur; Yan, Han; Zhang, Linglong; Sun, Xueqian; Liu, Boqing; Lu, Yuerui

2018-05-15

Atomically thin two-dimensional (2D) semiconductors have presented a plethora of opportunities for future optoelectronic devices and photonics applications, made possible by the strong light matter interactions at the 2D quantum limit. Many body interactions between fundamental particles in 2D semiconductors are strongly enhanced compared with those in bulk semiconductors because of the reduced dimensionality and, thus, reduced dielectric screening. These enhanced many body interactions lead to the formation of robust quasi-particles, such as excitons, trions, and biexcitons, which are extremely important for the optoelectronics device applications of 2D semiconductors, such as light emitting diodes, lasers, and optical modulators, etc. Recently, the emerging anisotropic 2D semiconductors, such as black phosphorus (termed as phosphorene) and phosphorene-like 2D materials, such as ReSe 2 , 2D-perovskites, SnS, etc., show strong anisotropic optical and electrical properties, which are different from conventional isotropic 2D semiconductors, such as transition metal dichalcogenide (TMD) monolayers. This anisotropy leads to the formation of quasi-one-dimensional (quasi-1D) excitons and trions in a 2D system, which results in even stronger many body interactions in anisotropic 2D materials, arising from the further reduced dimensionality of the quasi-particles and thus reduced dielectric screening. Many body interactions have been heavily investigated in TMD monolayers in past years, but not in anisotropic 2D materials yet. The quasi-particles in anisotropic 2D materials have fractional dimensionality which makes them perfect candidates to serve as a platform to study fundamental particle interactions in fractional dimensional space. In this Account, we present our recent progress related to 2D phosphorene, a 2D system with quasi-1D excitons and trions. Phosphorene, because of its unique anisotropic properties, provides a unique 2D platform for investigating the

Excitation intensity dependence of photoluminescence spectra of SiGe quantum dots grown on prepatterned Si substrates: Evidence for biexcitonic transition

Czech Academy of Sciences Publication Activity Database

Klenovský, P.; Brehm, M.; Křápek, Vlastimil; Lausecker, E.; Munzar, D.; Hackl, F.; Steiner, H.; Fromherz, T.; Bauer, G.; Humlíček, J.

2012-01-01

Roč. 86, č. 11 (2012), "115305-1"-"115305-8" ISSN 1098-0121 Institutional research plan: CEZ:AV0Z10100521 Keywords : semiconductors nanocrystals * cyclotron resonance * uniaxial-stress * band alignment * Ge islands * germanium * wells * silicon * Si(001) * luminescence Subject RIV: BM - Solid Matter Physics ; Magnetism Impact factor: 3.767, year: 2012 http://prb.aps.org/abstract/PRB/v86/i11/e115305

Optical manipulation of electron spin in quantum dot systems

Science.gov (United States)

Villas-Boas, Jose; Ulloa, Sergio; Govorov, Alexander

2006-03-01

Self-assembled quantum dots (QDs) are of particular interest for fundamental physics because of their similarity with atoms. Coupling two of such dots and addressing them with polarized laser light pulses is perhaps even more interesting. In this paper we use a multi-exciton density matrix formalism to model the spin dynamics of a system with single or double layers of QDs. Our model includes the anisotropic electron-hole exchange in the dots, the presence of wetting layer states, and interdot tunneling [1]. Our results show that it is possible to switch the spin polarization of a single self-assembled quantum dot under elliptically polarized light by increasing the laser intensity. In the nonlinear mechanism described here, intense elliptically polarized light creates an effective exchange channel between the exciton spin states through biexciton states, as we demonstrate by numerical and analytical methods. We further show that the effect persists in realistic ensembles of dots, and we propose alternative ways to detect it. We also extend our study to a double layer of quantum dots, where we find a competition between Rabi frequency and tunneling oscillations. [1] J. M. Villas-Boas, S. E. Ulloa, and A. O. Govorov, Phys. Rev. Lett. 94, 057404 (2005); Phys. Rev. B 69, 125342 (2004).

Temperature dependent empirical pseudopotential theory for self-assembled quantum dots.

Science.gov (United States)

Wang, Jianping; Gong, Ming; Guo, Guang-Can; He, Lixin

2012-11-28

We develop a temperature dependent empirical pseudopotential theory to study the electronic and optical properties of self-assembled quantum dots (QDs) at finite temperature. The theory takes the effects of both lattice expansion and lattice vibration into account. We apply the theory to InAs/GaAs QDs. For the unstrained InAs/GaAs heterostructure, the conduction band offset increases whereas the valence band offset decreases with increasing temperature, and there is a type-I to type-II transition at approximately 135 K. Yet, for InAs/GaAs QDs, the holes are still localized in the QDs even at room temperature, because the large lattice mismatch between InAs and GaAs greatly enhances the valence band offset. The single-particle energy levels in the QDs show a strong temperature dependence due to the change of confinement potentials. Because of the changes of the band offsets, the electron wavefunctions confined in QDs increase by about 1-5%, whereas the hole wavefunctions decrease by about 30-40% when the temperature increases from 0 to 300 K. The calculated recombination energies of excitons, biexcitons and charged excitons show red shifts with increasing temperature which are in excellent agreement with available experimental data.

Ultrafast Single and Multiexciton Energy Transfer in Semiconductor Nanoplatelets

Science.gov (United States)

Schaller, Richard

Photophysical processes such as fluorescence resonance energy transfer (FRET) enable optical antennas, wavelength down-conversion in light-emitting diodes (LEDs), and optical bio-sensing schemes. The rate and efficiency of this donor to acceptor transfer of excitation between chromophores dictates the utility of FRET and can unlock new device operation motifs including quantum-funnel solar cells and reduced gain thresholds. However, the fastest reported FRET time constants involving spherical quantum dots (QDs) (0.12-1 ns), do not outpace biexciton Auger recombination (0.01-0.1 ns), which impedes multiexciton-driven applications including electrically-pumped lasers and carrier-multiplication-enhanced photovoltaics. Precisely controlled, few-monolayer thick semiconductor nano-platelets with tens-of-nanometer diameters exhibit intense optical transitions and hundreds-of-picosecond Auger recombination, but heretofore lack FRET characterizations. We examine binary CdSe NPL solids and show that inter-plate FRET (~6-23 ps, presumably for co-facial arrangements) can occur 15-50 times faster than Auger recombination and demonstrate multiexcitonic FRET, making such materials ideal candidates for advanced technologies. This work was performed at the Center for Nanoscale Materials, a U.S. Department of Energy Office of Science User Facility under Contract No. DE-AC02-06CH11357.

Chemical Structure, Ensemble and Single-Particle Spectroscopy of Thick-Shell InP-ZnSe Quantum Dots.

Science.gov (United States)

Reid, Kemar R; McBride, James R; Freymeyer, Nathaniel J; Thal, Lucas B; Rosenthal, Sandra J

2018-02-14

Thick-shell (>5 nm) InP-ZnSe colloidal quantum dots (QDs) grown by a continuous-injection shell growth process are reported. The growth of a thick crystalline shell is attributed to the high temperature of the growth process and the relatively low lattice mismatch between the InP core and ZnSe shell. In addition to a narrow ensemble photoluminescence (PL) line-width (∼40 nm), ensemble and single-particle emission dynamics measurements indicate that blinking and Auger recombination are reduced in these heterostructures. More specifically, high single-dot ON-times (>95%) were obtained for the core-shell QDs, and measured ensemble biexciton lifetimes, τ 2x ∼ 540 ps, represent a 7-fold increase compared to InP-ZnS QDs. Further, high-resolution energy dispersive X-ray (EDX) chemical maps directly show for the first time significant incorporation of indium into the shell of the InP-ZnSe QDs. Examination of the atomic structure of the thick-shell QDs by high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) reveals structural defects in subpopulations of particles that may mitigate PL efficiencies (∼40% in ensemble), providing insight toward further synthetic refinement. These InP-ZnSe heterostructures represent progress toward fully cadmium-free QDs with superior photophysical properties important in biological labeling and other emission-based technologies.

Phonon-Assisted Two-Photon Interference from Remote Quantum Emitters.

Science.gov (United States)

Reindl, Marcus; Jöns, Klaus D; Huber, Daniel; Schimpf, Christian; Huo, Yongheng; Zwiller, Val; Rastelli, Armando; Trotta, Rinaldo

2017-07-12

Photonic quantum technologies are on the verge of finding applications in everyday life with quantum cryptography and quantum simulators on the horizon. Extensive research has been carried out to identify suitable quantum emitters and single epitaxial quantum dots have emerged as near-optimal sources of bright, on-demand, highly indistinguishable single photons and entangled photon-pairs. In order to build up quantum networks, it is essential to interface remote quantum emitters. However, this is still an outstanding challenge, as the quantum states of dissimilar "artificial atoms" have to be prepared on-demand with high fidelity and the generated photons have to be made indistinguishable in all possible degrees of freedom. Here, we overcome this major obstacle and show an unprecedented two-photon interference (visibility of 51 ± 5%) from remote strain-tunable GaAs quantum dots emitting on-demand photon-pairs. We achieve this result by exploiting for the first time the full potential of a novel phonon-assisted two-photon excitation scheme, which allows for the generation of highly indistinguishable (visibility of 71 ± 9%) entangled photon-pairs (fidelity of 90 ± 2%), enables push-button biexciton state preparation (fidelity of 80 ± 2%) and outperforms conventional resonant two-photon excitation schemes in terms of robustness against environmental decoherence. Our results mark an important milestone for the practical realization of quantum repeaters and complex multiphoton entanglement experiments involving dissimilar artificial atoms.

Optical and electronic properties of InGaAs and nitride quantum dots

Energy Technology Data Exchange (ETDEWEB)

Baer, N.

2006-06-15

In the present thesis, the electronic and optical properties of such nanostructures have been investigated for the well established III-V and the new group-III nitride material system. The influence of Coulomb correlations on the optical spectra of InGaAs QDs are studied using a full configuration interaction approach. The resulting multi-exciton spectra for up to twelve excitons are investigated in detail. Characteristic features of the spectra are explained using simplified Hamiltonians that are derived taking into account the relative importance of various interaction contributions. Additionally, we study the electronic and optical properties of self-assembled InN/GaN quantum dots. The existence of an exactly degenerate p-shell is discussed in detail. Dipole and Coulomb matrix elements are calculated from these one-particle wave functions and serve as an input for configuration interaction calculations. We present multi-exciton emission spectra and investigate how Coulomb correlations and oscillator strengths are altered by the built-in electrostatic fields present in these structures. From our results, we predict vanishing exciton and biexciton ground state emission for small lens-shaped dots, which is explained by a careful analysis of the underlying symmetry group. To study the photoluminescence dynamics of an initially excited QD system, we employ a microscopic semiconductor theory. Carrier-carrier correlations beyond the Hartee-Fock level are included within a cluster expansion truncation scheme up to the singlet-doublet level. The influence of these correlations on the spectrum and the photoluminescence dynamics is investigated for the emission into free space as well as for QDs embedded in an optical microcavity. (orig.)

Optical and electronic properties of InGaAs and nitride quantum dots

International Nuclear Information System (INIS)

Baer, N.

2006-06-01

In the present thesis, the electronic and optical properties of such nanostructures have been investigated for the well established III-V and the new group-III nitride material system. The influence of Coulomb correlations on the optical spectra of InGaAs QDs are studied using a full configuration interaction approach. The resulting multi-exciton spectra for up to twelve excitons are investigated in detail. Characteristic features of the spectra are explained using simplified Hamiltonians that are derived taking into account the relative importance of various interaction contributions. Additionally, we study the electronic and optical properties of self-assembled InN/GaN quantum dots. The existence of an exactly degenerate p-shell is discussed in detail. Dipole and Coulomb matrix elements are calculated from these one-particle wave functions and serve as an input for configuration interaction calculations. We present multi-exciton emission spectra and investigate how Coulomb correlations and oscillator strengths are altered by the built-in electrostatic fields present in these structures. From our results, we predict vanishing exciton and biexciton ground state emission for small lens-shaped dots, which is explained by a careful analysis of the underlying symmetry group. To study the photoluminescence dynamics of an initially excited QD system, we employ a microscopic semiconductor theory. Carrier-carrier correlations beyond the Hartee-Fock level are included within a cluster expansion truncation scheme up to the singlet-doublet level. The influence of these correlations on the spectrum and the photoluminescence dynamics is investigated for the emission into free space as well as for QDs embedded in an optical microcavity. (orig.)

Wavelength tunable InAs/InP(1 0 0) quantum dots in 1.55-{mu}m telecom devices

Energy Technology Data Exchange (ETDEWEB)

Anantathanasarn, S. [eiTT/COBRA Inter-University Research Institute on Communication Technology, Eindhoven University of Technology, 5600 MB Eindhoven (Netherlands)], E-mail: S.Anantathanasarn@tue.nl; Barbarin, Y. [eiTT/COBRA Inter-University Research Institute on Communication Technology, Eindhoven University of Technology, 5600 MB Eindhoven (Netherlands); Cade, N.I. [NTT Basic Research Laboratories, NTT Corporation, Atsugi 243-0198 (Japan); Veldhoven, P.J. van; Bente, E.A.J.M.; Oei, Y.S. [eiTT/COBRA Inter-University Research Institute on Communication Technology, Eindhoven University of Technology, 5600 MB Eindhoven (Netherlands); Kamada, H. [NTT Basic Research Laboratories, NTT Corporation, Atsugi 243-0198 (Japan); Smit, M.K.; Noetzel, R. [eiTT/COBRA Inter-University Research Institute on Communication Technology, Eindhoven University of Technology, 5600 MB Eindhoven (Netherlands)

2008-02-15

This paper reviews the growth, characterization and device applications of self-assembled InAs/InP(1 0 0) quantum dots (QDs) formed by MOVPE. The problematic As/P exchange reaction during QD growth is suppressed by the insertion of a GaAs interlayer together with optimum growth conditions. This produces QDs with continuously tunable emission over the 1.55-{mu}m wavelength region for fiber-based telecom applications. Device quality of these QDs is proven by continuous wave lasing at room temperature from the as-cleaved facets of Fabry-Perot narrow ridge-waveguide lasers implementing widely stacked QDs as gain medium. The low transparency current density of 6 A/cm{sup 2} per QD layer and low loss of 4.2 cm{sup -1} are accompanied by a 80-nm wide gain spectrum. The deeply etched QD lasers possess similar threshold current densities as the shallowly etched ones and do not deteriorate with time, revealing that device performance does not suffer from sidewall recombination. This allows the fabrication of mono-mode and more compact devices with small bending radii, as demonstrated by the operation of a QD ring laser with 40-GHz free spectral range. Unpolarized emission from the cleaved side, important for the realization of polarization insensitive semiconductor optical amplifiers, is obtained by close stacking of QDs due to vertical electronic coupling. Sharp exciton-biexciton emission from a single QD around 1.55 {mu}m is observed with clearly resolvable peaks above 70 K, which is required for single photon sources working at liquid nitrogen temperature for fiber-based quantum cryptography systems.

Energy transfer mechanisms in layered 2D perovskites.

Science.gov (United States)

Williams, Olivia F; Guo, Zhenkun; Hu, Jun; Yan, Liang; You, Wei; Moran, Andrew M

2018-04-07

Two-dimensional (2D) perovskite quantum wells are generating broad scientific interest because of their potential for use in optoelectronic devices. Recently, it has been shown that layers of 2D perovskites can be grown in which the average thicknesses of the quantum wells increase from the back to the front of the film. This geometry carries implications for light harvesting applications because the bandgap of a quantum well decreases as its thickness increases. The general structural formula for the 2D perovskite systems under investigation in this work is (PEA) 2 (MA) n-1 [Pb n I 3n+1 ] (PEA = phenethyl ammonium, MA = methyl ammonium). Here, we examine two layered 2D perovskites with different distributions of quantum well thicknesses. Spectroscopic measurements and model calculations suggest that both systems funnel electronic excitations from the back to the front of the film through energy transfer mechanisms on the time scales of 100's of ps (i.e., energy transfer from thinner to thicker quantum wells). In addition, the model calculations demonstrate that the transient absorption spectra are composed of a progression of single exciton and biexciton resonances associated with the individual quantum wells. We find that exciton dissociation and/or charge transport dynamics make only minor contributions to the transient absorption spectra within the first 1 ns after photo-excitation. An analysis of the energy transfer kinetics indicates that the transitions occur primarily between quantum wells with values of n that differ by 1 because of the spectral overlap factor that governs the energy transfer rate. Two-dimensional transient absorption spectra reveal a pattern of resonances consistent with the dominance of sequential energy transfer dynamics.

Energy transfer mechanisms in layered 2D perovskites

Science.gov (United States)

Williams, Olivia F.; Guo, Zhenkun; Hu, Jun; Yan, Liang; You, Wei; Moran, Andrew M.

2018-04-01

Two-dimensional (2D) perovskite quantum wells are generating broad scientific interest because of their potential for use in optoelectronic devices. Recently, it has been shown that layers of 2D perovskites can be grown in which the average thicknesses of the quantum wells increase from the back to the front of the film. This geometry carries implications for light harvesting applications because the bandgap of a quantum well decreases as its thickness increases. The general structural formula for the 2D perovskite systems under investigation in this work is (PEA)2(MA)n-1[PbnI3n+1] (PEA = phenethyl ammonium, MA = methyl ammonium). Here, we examine two layered 2D perovskites with different distributions of quantum well thicknesses. Spectroscopic measurements and model calculations suggest that both systems funnel electronic excitations from the back to the front of the film through energy transfer mechanisms on the time scales of 100's of ps (i.e., energy transfer from thinner to thicker quantum wells). In addition, the model calculations demonstrate that the transient absorption spectra are composed of a progression of single exciton and biexciton resonances associated with the individual quantum wells. We find that exciton dissociation and/or charge transport dynamics make only minor contributions to the transient absorption spectra within the first 1 ns after photo-excitation. An analysis of the energy transfer kinetics indicates that the transitions occur primarily between quantum wells with values of n that differ by 1 because of the spectral overlap factor that governs the energy transfer rate. Two-dimensional transient absorption spectra reveal a pattern of resonances consistent with the dominance of sequential energy transfer dynamics.

Growth and characterization of InP/In{sub 0.48}Ga{sub 0.52}P quantum dots optimized for single-photon emission

Energy Technology Data Exchange (ETDEWEB)

Ugur, Asli

2012-08-28

In this work the growth of self-assembled InP/InGaP quantum dots, as well as their optical and structural properties are presented and discussed. The QDs were grown on In{sub 0.48}Ga{sub 0.52}P, lattice matched to GaAs. Self-assembled InP quantum dots are grown using gas-source molecular beam epitaxy over a wide range of InP deposition rates, using an ultra-low growth rate of about 0.01 atomic monolayers/s, a quantum-dot density of 1 dot/μm{sup 2} is realized. The resulting isolated InP quantum dots are individually characterized without the need for lithographical patterning and masks on the substrate. Both excitonic and biexcitonic emissions are observed from single dots, appearing as doublets with a fine-structure splitting of 320 μeV. Hanbury Brown-Twiss correlation measurements for the excitonic emission under cw excitation show anti-bunching behavior with an autocorrelation value of g{sup (2)}(0)=0.2. This system is applicable as a single-photon source for applications such as quantum cryptography. The formation of well-ordered chains of InP quantum dots on GaAs (001) substrates by using self-organized In{sub 0.48}Ga{sub 0.52}P surface undulations as a template is also demonstrated. The ordering requires neither stacked layers of quantum dots nor substrate misorientation. The structures are investigated by polarization-dependent photoluminescence together with transmission electron microscopy. Luminescence from the In{sub 0.48}Ga{sub 0.52}P matrix is polarized in one crystallographic direction due to anisotropic strain arising from a lateral compositional modulation. The photoluminescence measurements show enhanced linear polarization in the alignment direction of quantum dots. A polarization degree of 66% is observed. The optical anisotropy is achieved with a straightforward heterostructure, requiring only a single layer of QDs.

Electrical and optical measurements on a single InAs quantum dot using ion-implanted micro-LEDs; Elektrische und optische Untersuchungen an einem einzelnen InAs-Quantenpunkt mit Hilfe ionenstrahlimplantierter Mikro-LEDs

Energy Technology Data Exchange (ETDEWEB)

Schmidt, R.F.

2006-10-19

The goal of this present thesis was to electrically and optically address a single InAs quantum dot. Therefore micro-structured quantum-dot-LEDs with an emission area smaller than 1 {mu}m{sup 2} were developed. One major part of this work was contributed to optimizing several steps of the micro-LED fabrication process. To be able to compare the electrical conductivity obtained from Hall-measurements to the expected values, the implantation profile was investigated both theoretically and experimentally. As the thermal annealing step had to be performed in the growth chamber of the MBE-system several annealing parameters had to be modified to achieve optimum electrical conductivity and quantum dot growth. For one of the Be-implanted pin-samples the principle of the single-quantum-dot-LEDs could be proved. The smallest device of this sample, with nominal stripe widths of 150 nm (FIB-stripe) and 400 nm (top-stripe), showed typical features of a single quantum dot. In the high-resolution EL-spectra of this device three extremely sharp emission lines were observed which clearly could be assigned to the electron-hole recombination from a single quantum dot. To further identify the origin of these lines their optical intensities were plotted against the injection current. From this plot it could be deduced, that the first evolving line clearly belongs to the simple exciton 1X. The following lines could be assigned to the decay of the biexciton 2X and the triexciton 3X{sub s}, respectively. With increasing bias all three lines show a pronounced red-shift due to the quantum confined Stark effect (QCSE). To identify the charge state of the observed excitonic lines, additional high-resolution IV curves were taken. (orig.)

CdZnTe quantum dots study: energy and phase relaxation process

International Nuclear Information System (INIS)

Viale, Yannick

2004-01-01

We present a study of the electron-hole pair energy and phase relaxation processes in a CdTe/ZnTe heterostructure, in which quantum dots are embedded. CdZnTe quantum wells with a high Zinc concentration, separated by ZnTe barriers, contain islands with a high cadmium concentration. In photoluminescence excitation spectroscopy experiments, we evidence two types of electron hole pair relaxation processes. After being excited in the CdZnTe quantum well, the pairs relax their energy by emitting a cascade of longitudinal optical phonons until they are trapped in the quantum dots. Before their radiative recombination follows an intra-dot relaxation, which is attributed to a lattice polarization mechanism of the quantum dots. It is related to the coupling between the electronic and the vibrational states. Both relaxation mechanisms are reinforced by the strong polar character of the chemical bond in II-VI compounds. Time resolved measurements of transmission variations in a pump-probe configuration allowed us to investigate the population dynamics of the electron-hole pairs during the relaxation process. We observe a relaxation time of about 2 ps for the longitudinal phonon emission cascade in the quantum well before a saturation of the quantum dot transition. We also measured an intra-box relaxation time of 25 ps. The comparison of various cascades allows us to estimate the emission time of a longitudinal optical phonon in the quantum well to be about 100 fs. In four waves mixing experiments, we observe oscillations that we attribute to quantum beats between excitonic and bi-excitonic transitions. The dephasing times that we measure as function of the density of photons shows that excitons are strongly localized in the quantum dots. The excitonic dephasing time is much shorter than the radiative lifetime and is thus controlled by the intra-dot relaxation time. (author) [fr

Growth and characterization of InP/In0.48Ga0.52P quantum dots optimized for single-photon emission

International Nuclear Information System (INIS)

Ugur, Asli

2012-01-01

In this work the growth of self-assembled InP/InGaP quantum dots, as well as their optical and structural properties are presented and discussed. The QDs were grown on In 0.48 Ga 0.52 P, lattice matched to GaAs. Self-assembled InP quantum dots are grown using gas-source molecular beam epitaxy over a wide range of InP deposition rates, using an ultra-low growth rate of about 0.01 atomic monolayers/s, a quantum-dot density of 1 dot/μm 2 is realized. The resulting isolated InP quantum dots are individually characterized without the need for lithographical patterning and masks on the substrate. Both excitonic and biexcitonic emissions are observed from single dots, appearing as doublets with a fine-structure splitting of 320 μeV. Hanbury Brown-Twiss correlation measurements for the excitonic emission under cw excitation show anti-bunching behavior with an autocorrelation value of g (2) (0)=0.2. This system is applicable as a single-photon source for applications such as quantum cryptography. The formation of well-ordered chains of InP quantum dots on GaAs (001) substrates by using self-organized In 0.48 Ga 0.52 P surface undulations as a template is also demonstrated. The ordering requires neither stacked layers of quantum dots nor substrate misorientation. The structures are investigated by polarization-dependent photoluminescence together with transmission electron microscopy. Luminescence from the In 0.48 Ga 0.52 P matrix is polarized in one crystallographic direction due to anisotropic strain arising from a lateral compositional modulation. The photoluminescence measurements show enhanced linear polarization in the alignment direction of quantum dots. A polarization degree of 66% is observed. The optical anisotropy is achieved with a straightforward heterostructure, requiring only a single layer of QDs.

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.

Dynamics of the phase transitions in the system of nonequilibrium charge carriers in quantum-dimensional Si{sub 1−x}Ge{sub x}/Si structures

Energy Technology Data Exchange (ETDEWEB)

Bagaev, V. S.; Krivobok, V. S., E-mail: krivobok@lebedev.ru; Nikolaev, S. N.; Onishchenko, E. E.; Pruchkina, A. A.; Aminev, D. F.; Skorikov, M. L. [Russian Academy of Sciences, Lebedev Physical Institute (Russian Federation); Lobanov, D. N.; Novikov, A. V. [Russian Academy of Sciences, Institute for Physics of Microstructures (Russian Federation)

2013-11-15

The dynamics of the phase transition from an electron-hole plasma to an exciton gas is studied during pulsed excitation of heterostructures with Si{sub 1−x}Ge{sub x}/Si quantum wells. The scenario of the phase transition is shown to depend radically on the germanium content in the Si{sub 1−x}Ge{sub x} layer. The electron-hole system decomposes into a rarefied exciton and a dense plasma phases for quantum wells with a germanium content x = 3.5% in the time range 100–500 ns after an excitation pulse. In this case, the electron-hole plasma existing in quantum wells has all signs of an electron-hole liquid. A qualitatively different picture of the phase transition is observed for quantum wells with x = 9.5%, where no separation into phases with different electronic spectra is detected. The carrier recombination in the electron-hole plasma leads a gradual weakening of screening and the appearance of exciton states. For a germanium content of 5–7%, the scenario of the phase transition is complex: 20–250 ns after an excitation pulse, the properties of the electron-hole system are described in terms of a homogeneous electron-hole plasma, whereas its separation into an electron-hole liquid and an exciton gas is detected after 350 ns. It is shown that, for the electron-hole liquid to exist in quantum wells with x = 5–7% Ge, the exciton gas should have a substantially higher density than in quantum wells with x = 3.5% Ge. This finding agrees with a decrease in the depth of the local minimum of the electron-hole plasma energy with increasing germanium concentration in the SiGe layer. An increase in the density of the exciton gas coexisting with the electron-hole liquid is shown to enhance the role of multiparticle states, which are likely to be represented by trions T{sup +} and biexcitons, in the exciton gas.

Photophysical Properties of Novel Organic, Inorganic, and Hybrid Semiconductor Materials

Science.gov (United States)

Chang, Angela Yenchi

For the past 200 years, novel materials have driven technological progress, and going forward these advanced materials will continue to deeply impact virtually all major industrial sectors. Therefore, it is vital to perform basic and applied research on novel materials in order to develop new technologies for the future. This dissertation describes the results of photophysical studies on three novel materials with electronic and optoelectronic applications, namely organic small molecules DTDCTB with C60 and C70, colloidal indium antimonide (InSb) nanocrystals, and an organic-inorganic hybrid perovskite with the composition CH3NH3PbI 3-xClx, using transient absorption (TA) and photoluminescence (PL) spectroscopy. In chapter 2, we characterize the timescale and efficiency of charge separation and recombination in thin film blends comprising DTDCTB, a narrow-band gap electron donor, and either C60 or C70 as an electron acceptor. TA and time-resolved PL studies show correlated, sub-picosecond charge separation times and multiple timescales of charge recombination. Our results indicate that some donors fail to charge separate in donor-acceptor mixed films, which suggests material manipulations may improve device efficiency. Chapter 3 describes electron-hole pair dynamics in strongly quantum-confined, colloidal InSb nanocrystal quantum dots. For all samples, TA shows a bleach feature that, for several picoseconds, dramatically red-shifts prior to reaching a time-independent position. We suggest this unusual red-shift relates transient population flow through two energetically comparable conduction band states. From pump-power-dependent measurements, we also determine biexciton lifetimes. In chapter 4, we examine carrier dynamics in polycrystalline methylammonium lead mixed halide perovskite (CH3NH3PbI3-xCl x) thin films as functions of temperature and photoexcitation wavelength. At room temperature, the long-lived TA signals stand in contrast to PL dynamics, where the

Preface

Science.gov (United States)

2003-10-01

polariton branch to allow much of the new physics in semiconductor microcavities. Non-linear effects in semiconductor microcavities, which include stimulated polariton scattering, parametric oscillation, spin dynamics, and the possibilities of a polariton condensate, are discussed by Baumberg et al. The suppression of the relaxation bottleneck on the lower polariton branch and the stimulation of the emission in II-VI based microcavities is demonstrated by Dang and collaborators, who also probe the coherent dynamics along the lower polariton branch by means of angle-resolved four wave mixing experiments. The possibility to observe parametric polariton amplification at room temperature is discussed by Deveaud's team, who demonstrate that this could be achieved in cavities, in which quantum wells with a large exciton binding energy are embedded, such as in GaN-based cavities. The effects induced by a two-dimensional electron gas on the interaction between the electromagnetic field and the excitons in a semiconductor microcavity are discussed by Cohen et al, who show that the presence of the electron gas is responsible for an efficient interaction between electrons and polaritons. The modification of the optical mode spectrum in microcavities, by introducing lateral photon confinement, is demonstrated by Bayer and collaborators, who show the possibility of tailoring elastic polariton pair-scattering and a suppression of the spontaneous emission for quantum dots embedded in such cavities. The optical properties of biexcitons in microcavities are reviewed by Langbein et al, who perform a detailed investigation of the polariton-biexciton transition and study the biexciton binding energy and dephasing in a microcavity at low temperature. A detailed experimental study of linear and circular polarization dynamics in secondary emission of microcavities in the strong coupling regime is presented by Amand's group, who show that it is possible to manipulate the polariton spin and

Photophysical Properties of II-VI Semiconductor Nanocrystals

Science.gov (United States)

Gong, Ke

implementation of QDs in commercial devices. Chapter 3 will elucidate the mechanism of static thermal quenching, in which the reduction of QYs does not affect the PL decay kinetics, on CdSe, CdTe and CdSe/ZnSe QDs as a function of particle sizes/shapes, surface composition and surface ligands. Through systematic experiments, this part of the dissertation discusses several possible mechanisms (e.g. structural, activated excited state, and electronic charging) and examines which the dominant cause for loss of QY at high temperature is. The more practical step is to develop the synthetic method of highly luminescent and stable core/shell QDs with minimum thermal quenching, which greatly enhance the energy efficiency of light emitting and photovoltaic devices. As the nonradiative Auger processed are induced by surface charging described in chapter 3, static and time-resolved fluorescence and high and low power transient absorption results on CdSe/CdS and CdSe/ZnSe core/shell particles are presented in chapter 4. Two CdS shell thicknesses were examined and all of the particles had either octadecylamine (ODA) and tributylphosphine (TBP) or just ODA ligands. The results can be understood in terms of a mechanism in which there is a thermal equilibrium between electrons being in the valence band or in chalcogenide localized surface states. Thermal promotion of a valence band electron to a surface state leaves the particle core positively charged. Photon absorption when the particle is in this state results in a positive trion, which undergoes a fast Auger recombination, making the particle nonluminescent. A lack of TBP ligands results in more empty surface orbitals and therefore shifts the equilibrium toward surface trapped electrons and hence trion formation. Low- and high-power transient absorption measurements give the trion and biexciton lifetimes and the ratio of the trion to biexciton Auger lifetimes are examined and compared to the degeneracies of Auger pathways. We also study the