WorldWideScience

Sample records for biexcitons

  1. Biexcitons in semiconductor microcavities

    DEFF Research Database (Denmark)

    Borri, P.; Langbein, W.; Woggon, U.

    2003-01-01

    In this paper, the present status of the experimental study of the optical properties of biexcitons in semiconductor microcavities is reviewed. In particular, a detailed investigation of a polariton-biexciton transition in a high-quality single quantum well GaAs/AlGaAs microcavity is reported...

  2. Binding energy of two-dimensional biexcitons

    DEFF Research Database (Denmark)

    Singh, Jai; Birkedal, Dan; Vadim, Lyssenko;

    1996-01-01

    Using a model structure for a two-dimensional (2D) biexciton confined in a quantum well, it is shown that the form of the Hamiltonian of the 2D biexciton reduces into that of an exciton. The binding energies and Bohr radii of a 2D biexciton in its various internal energy states are derived...... analytically using the fractional dimension approach. The ratio of the binding energy of a 2D biexciton to that of a 2D exciton is found to be 0.228, which agrees very well with the recent experimental value. The results of our approach are compared with those of earlier theories....

  3. Mixed biexcitons in single quantum wells

    DEFF Research Database (Denmark)

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

    1999-01-01

    Biexcitonic complexes in a ZnSe single quantum well are investigated by spectrally resolved four-wave mixing (FWM). The formation of heavy-heavy-hole XXh and of mixed heavy-light-hole XXm biexcitons showing binding energies of Delta(h) = 4.8 meV and Delta(m)= 2.8 meV is identified by polarization...

  4. Biexciton dephasing in a semiconductor microcavity

    DEFF Research Database (Denmark)

    Borri, P.; Langbein, W.; Woggon, U.

    2001-01-01

    The experimental observation of biexcitons in microcavities has been addressed recently. A well-resolved polariton-biexciton transition was observed in a high-quality GaAs single quantum well (QW) /spl lambda/-microcavity of 25 nm well width using a pump-probe experiment. In this microcavity the ...

  5. Biexcitons or bipolaritons in a semiconductor microcavity

    DEFF Research Database (Denmark)

    Borri, Paola; Langbein, Wolfgang Werner; Woggon, U

    2000-01-01

    A well-resolved nonlinear optical transition associated with biexcitons is observed in a high-quality microcavity with a Rabi splitting exceeding the binding energy of biexcitons in the embedded quantum well. This transition is identified as an induced absorption from the lower polariton to the b...

  6. Localization-enhanced biexciton binding in semiconductors

    DEFF Research Database (Denmark)

    Langbein, Wolfgang Werner; Hvam, Jørn Märcher

    1999-01-01

    The influence of excitonic localization on the binding energy of biexcitons is investigated for quasi-three-dimensional and quasi-two-dimensional AlxGa1-xAs structures. An increase of the biexciton binding energy is observed for localization energies comparable to or larger than the free biexcito...

  7. Coherent dynamics of biexcitons in a semiconductor microcavity

    DEFF Research Database (Denmark)

    Borri, P.; Langbein, W.; Woggon, U.

    2002-01-01

    The dephasing time of biexcitons in a semiconductor quantum well microcavity is measured at low temperature using transient four-wave mixing spectroscopy. The homogeneous linewidth corresponding to the dephasing of the transition from the crystal ground state to the biexciton is found to be appro......The dephasing time of biexcitons in a semiconductor quantum well microcavity is measured at low temperature using transient four-wave mixing spectroscopy. The homogeneous linewidth corresponding to the dephasing of the transition from the crystal ground state to the biexciton is found...

  8. Composition dependent dynamics of biexciton localization in AlxGa1-xN mixed crystals

    OpenAIRE

    2009-01-01

    We report the localization-dependent dynamics of biexcitons in AlxGa1−xN mixed crystals under exciton resonant excitation at low temperatures. After intense laser excitation, biexcitons rapidly localize into the band-tail states. The formation time of localized biexcitons becomes shorter with increasing Al composition. Both the inhomogeneous linewidth and the binding energy of biexcitons increase with the inhomogeneous linewidth of excitons. The biexciton binding energy is enhanced by the res...

  9. Charged Frenkel biexcitons in organic molecular crystals

    CERN Document Server

    Agranovich, V M; Kamchatnov, A M

    2001-01-01

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

  10. Second Bound State of Biexcitons in Quantum Dots

    Institute of Scientific and Technical Information of China (English)

    XIE Wen-Eang

    2003-01-01

    The second bound state of the biexcitons in a quantum dot, with orbital angular momentum L = 1, is reported. By using the method of few-body physics, the binding energy spectra of the second bound state of a biexciton in a GaAs quantum dot with a parabolic confinement have been calculated as a function of the electron-to-hole mass ratio and the quantum dot size. The fact that the biexcitons have a second bound state may aid in the better understanding of their binding mechanism.

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

    DEFF Research Database (Denmark)

    Langbein, Wolfgang Werner; Hvam, Jørn Märcher

    2000-01-01

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

  12. Exciton and Biexciton Binding Energies in Rectangular Quantum Dots

    Institute of Scientific and Technical Information of China (English)

    LIU Yong-Hui; KONG Xiao-Jun

    2005-01-01

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

  13. 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...... the experimentally observed dependence of the biexciton binding energies....

  14. 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....

  15. Excitons and biexcitons in CuCl nanocrystallites

    Energy Technology Data Exchange (ETDEWEB)

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

    1995-06-01

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

  16. Biexciton emission and crystalline quality of ZnO nano-objects

    Energy Technology Data Exchange (ETDEWEB)

    Corfdir, Pierre; Abid, Mohamed; Papa, Elisa; Ansermet, Jean-Philippe; Ganiere, Jean-Daniel; Deveaud-Pledran, BenoIt [Institute of Condensed Matter Physics, Ecole Polytechnique Federale de Lausanne (EPFL), 1015 Lausanne (Switzerland); Mouti, Anas; Stadelmann, Pierre A, E-mail: pierre.corfdir@epfl.ch [Centre Interdisciplinaire de Microscopie Electronique, Ecole Polytechnique Federale de Lausanne (EPFL), 1015 Lausanne (Switzerland)

    2011-07-15

    The design of cost-effective standards for the quality of nano-objects is currently a key issue toward their massive use for optoelectronic applications. The observation by photoluminescence of narrow excitonic and biexcitonic emission lines in semiconductor nanowires is usually accepted as evidence for high structural quality. Here, we perform time-resolved cathodoluminescence experiments on isolated ZnO nanobelts grown by chemical vapor deposition. We observe narrow emission lines at low temperature, together with a clear biexciton line. Still, drastic alterations in both the CL intensity and lifetime are observed locally along the nano-object. We attribute these to non-radiative recombinations at edge dislocations, closing basal plane stacking faults, inhomogeneously distributed along the NB length. This leads us to the conclusion that the observation of narrow excitonic and biexcitonic emission lines is far from sufficient to grade the quality of a nano-object.

  17. Binding energy and dephasing of biexcitons in In0.18Ga0.82As/GaAs single quantum wells

    DEFF Research Database (Denmark)

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

    1999-01-01

    Biexciton binding energies and biexciton dephasing in In0.18Ga0.82As/GaAs single quantum wells have been measured by time-integrated and spectrally resolved four-wave mixing. The biexciton binding energy increases from 1.5 to 2.6 meV for well widths increasing from 1 to 4 nm. The ratio between...... exciton and biexciton binding energy changes from 0.23 to 0.3 with increasing inhomogeneous broadening, corresponding to increasing well width. From the temperature dependence of the exciton and biexciton four-wave mixing signal decay, we have deduced the acoustic-phonon scattering of the exciton...

  18. Binding Energy of Biexcitons in GaAs Quantum-Well Wires

    Institute of Scientific and Technical Information of China (English)

    LIU Jian-Jun; CHEN Xiao-Fang; LI Shu-Shen

    2004-01-01

    @@ The binding energy of a biexciton in GaAs quantum-well wires is calculated variationally by use ofa two-parameter trial wavefunction and a one-dimensional equivalent potential model. There is no artificial parameter added in our calculation. Our results agree fairly well with the previous results. It is found that the binding energies are closely correlative to the size of wire. The binding energy of biexcitons is smaller than that of neutral bound excitons in GaAs quantum-well wires when the dopant is located at the centre of the wires.

  19. Fabrication of CuCl quantum dots and the size dependence of the biexciton binding energy

    CERN Document Server

    Park, S T; Kim, H Y; Kim, I G

    2000-01-01

    We fabricated CuCl quantum dots (QDs) in an aluminoborosilicate glass matrix. The photoluminescence of the CuCl QDs was surveyed by using the band-to-band excitation and the site selective luminescence methods. The excitation density dependence of the exciton and the biexciton luminescence was measured, and the saturation effects of the luminescence intensities were observed. The biexciton binding energies measured using the site selective luminescence method increased with decreasing QD size. The data were well fitted by a function resulting from the numerical matrix-diagonalization method.

  20. Electronic and optical properties of single excitons and biexcitons in type-II quantum dot nanocrystals

    Energy Technology Data Exchange (ETDEWEB)

    Koc, Fatih, E-mail: fatih.koc@msn.com [Department of Physics, Faculty of Sciences, Selcuk University, 42075 Konya (Turkey); Sahin, Mehmet, E-mail: mehmet.sahin@agu.edu.tr, E-mail: mehsahin@gmail.com [Department of Physics, Faculty of Sciences, Selcuk University, 42075 Konya (Turkey); Department of Material Science and Nanotechnology Engineering, Abdullah Gül University, Kayseri (Turkey)

    2014-05-21

    In this study, a detailed investigation of the electronic and optical properties (i.e., binding energies, absorption wavelength, overlap of the electron-hole wave functions, recombination oscillator strength, etc.) of an exciton and a biexciton in CdTe/CdSe core/shell type-II quantum dot heterostructures has been carried out in the frame of the single band effective mass approximation. In order to determine the electronic properties, we have self-consistently solved the Poisson-Schrödinger equations in the Hartree approximation. We have considered all probable Coulomb interaction effects on both energy levels and also on the corresponding wave functions for both single exciton and biexciton. In addition, we have taken into account the quantum mechanical exchange-correlation effects in the local density approximation between same kinds of particles for biexciton. Also, we have examined the effect of the ligands and dielectric mismatch on the electronic and optical properties. We have used a different approximation proposed by Sahin and Koc [Appl. Phys. Lett. 102, 183103 (2013)] for the recombination oscillator strength of the biexciton for bound and unbound cases. The results obtained have been presented comparatively as a function of the shell thicknesses and probable physical reasons in behind of the results have been discussed in a detail.

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

    Science.gov (United States)

    Koinov, Z. G.

    1999-04-01

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

  2. 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...

  3. Biexciton formation and exciton coherent coupling in layered GaSe

    Energy Technology Data Exchange (ETDEWEB)

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

    2015-06-07

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

  4. Cooperative biexciton generation and destructive interference in coupled quantum dots using adiabatic rapid passage

    NARCIS (Netherlands)

    Renaud, N.; Grozema, F.C.

    2014-01-01

    We report numerical simulations of biexciton generation in coupled quantum dots (CQDs) placed in a static electric field and excited by a chirped laser pulse. Our simulations explicitly account for exciton-phonon interactions at finite temperature using a non-Markovian quantum jump approach to solve

  5. 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.

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

    CERN Document Server

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

    2016-01-01

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

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

    Science.gov (United States)

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

    2016-08-01

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

  8. Binding energies of trions and biexcitons in two-dimensional semiconductors from diffusion quantum Monte Carlo calculations

    Science.gov (United States)

    Szyniszewski, M.; Mostaani, E.; Drummond, N. D.; Fal'ko, V. I.

    2017-02-01

    Excitonic effects play a particularly important role in the optoelectronic behavior of two-dimensional (2D) semiconductors. To facilitate the interpretation of experimental photoabsorption and photoluminescence spectra we provide statistically exact diffusion quantum Monte Carlo binding-energy data for Mott-Wannier models of excitons, trions, and biexcitons in 2D semiconductors. We also provide contact pair densities to allow a description of contact (exchange) interactions between charge carriers using first-order perturbation theory. Our data indicate that the binding energy of a trion is generally larger than that of a biexciton in 2D semiconductors. We provide interpolation formulas giving the binding energy and contact density of 2D semiconductors as functions of the electron and hole effective masses and the in-plane polarizability.

  9. Gradient CdSe/CdS Quantum Dots with Room Temperature Biexciton Unity Quantum Yield.

    Science.gov (United States)

    Nasilowski, Michel; Spinicelli, Piernicola; Patriarche, Gilles; Dubertret, Benoît

    2015-06-10

    Auger recombination is a major limitation for the fluorescent emission of quantum dots (QDs). It is the main source of QDs fluorescence blinking at the single-particle level. At high-power excitation, when several charge carriers are formed inside a QD, Auger becomes more efficient and severely decreases the quantum yield (QY) of multiexcitons. This limits the efficiency and the use of colloidal QDs in applications where intense light output is required. Here, we present a new generation of thick-shell CdSe/CdS QDs with dimensions >40 nm and a composition gradient between the core and the shell that exhibits 100% QY for the emission of both the monoexciton and the biexciton in air and at room temperature for all the QDs we have observed. The fluorescence emission of these QDs is perfectly Poissonian at the single-particle level at different excitation levels and temperatures, from 30 to 300 K. In these QDs, the emission of high-order (>2) multiexcitons is quite efficient, and we observe white light emission at the single-QD level when high excitation power is used. These gradient thick shell QDs confirm the suppression of Auger recombination in gradient core/shell structures and help further establish the colloidal QDs with a gradient shell as a very stable source of light even under high excitation.

  10. Phase control of Goos-Hänchen shift via biexciton coherence in a multiple quantum well

    Science.gov (United States)

    Asadpour, Seyyed Hossein; Nasehi, Rajab; Soleimani, H. Rahimpour; Mahmoudi, M.

    2015-09-01

    The behavior of the Goos-Hänchen (GH) shifts of the reflected and transmitted probe and signal pulses through a cavity containing four-level GaAs/AlGaAs multiple quantum wells with 15 periods of 17.5 nm GaAs wells and 15-nm Al0.3Ga0.7As barriers is theoretically discussed. The biexciton coherence set up by two coupling fields can induce the destructive interference to control the absorption and gain properties of probe field under appropriate conditions. It is realized that for the specific values of the intensities and the relative phase of applied fields, the simultaneous negative or positive GH shift in the transmitted and reflected light beam can be obtained via amplification in a probe light. It is found that by adjusting the controllable parameters, the GH shifts can be switched between the large positive and negative values in the medium. Moreover, the effect of exciton spin relaxation on the GH shift has also been discussed. We find that the exciton spin relaxation can manipulate the behavior of GH shift in the reflected and transmitted probe beam through the cavity. We show that by controlling the incident angles of probe beam and under certain conditions, the GH shifts in the reflected and transmitted probe beams can become either negative or positive corresponding to the superluminal or subluminal light propagation. Our proposed model may supply a new prospect in technological applications for the light amplification in optical sensors working on quantum coherence impacts in solid-state systems.

  11. Strong plasmonic enhancement of biexciton emission: controlled coupling of a single quantum dot to a gold nanocone antenna

    CERN Document Server

    Matsuzaki, Korenobu; Liu, Hsuan-Wei; Dutschke, Anke; Hoffmann, Björn; Chen, Xuewen; Christiansen, Silke; Buck, Matthew R; Hollingsworth, Jennifer A; Götzinger, Stephan; Sandoghdar, Vahid

    2016-01-01

    Multiexcitonic transitions and emission of several photons per excitation comprise a very attractive feature of semiconductor quantum dots for optoelectronics applications. However, these higher-order radiative processes are usually quenched in colloidal quantum dots by Auger and other non-radiative decay channels. To increase the multiexcitonic quantum efficiency, several groups have explored plasmonic enhancement, so far with moderate results. By controlled positioning of individual quantum dots in the near field of gold nanocone antennas, we enhance the radiative decay rates of monoexcitons and biexcitons by 109 and 100 folds at quantum efficiencies of 60% and 70%, respectively, in very good agreement with the outcome of numerical calculations. We discuss the implications of our work for future fundamental and applied research in nano-optics.

  12. Strong plasmonic enhancement of biexciton emission: controlled coupling of a single quantum dot to a gold nanocone antenna

    Science.gov (United States)

    Matsuzaki, Korenobu; Vassant, Simon; Liu, Hsuan-Wei; Dutschke, Anke; Hoffmann, Björn; Chen, Xuewen; Christiansen, Silke; Buck, Matthew R.; Hollingsworth, Jennifer A.; Götzinger, Stephan; Sandoghdar, Vahid

    2017-01-01

    Multiexcitonic transitions and emission of several photons per excitation comprise a very attractive feature of semiconductor quantum dots for optoelectronics applications. However, these higher-order radiative processes are usually quenched in colloidal quantum dots by Auger and other nonradiative decay channels. To increase the multiexcitonic quantum efficiency, several groups have explored plasmonic enhancement, so far with moderate results. By controlled positioning of individual quantum dots in the near field of gold nanocone antennas, we enhance the radiative decay rates of monoexcitons and biexcitons by 109 and 100 folds at quantum efficiencies of 60 and 70%, respectively, in very good agreement with the outcome of numerical calculations. We discuss the implications of our work for future fundamental and applied research in nano-optics. PMID:28195140

  13. Strong plasmonic enhancement of biexciton emission: controlled coupling of a single quantum dot to a gold nanocone antenna

    Science.gov (United States)

    Matsuzaki, Korenobu; Vassant, Simon; Liu, Hsuan-Wei; Dutschke, Anke; Hoffmann, Björn; Chen, Xuewen; Christiansen, Silke; Buck, Matthew R.; Hollingsworth, Jennifer A.; Götzinger, Stephan; Sandoghdar, Vahid

    2017-02-01

    Multiexcitonic transitions and emission of several photons per excitation comprise a very attractive feature of semiconductor quantum dots for optoelectronics applications. However, these higher-order radiative processes are usually quenched in colloidal quantum dots by Auger and other nonradiative decay channels. To increase the multiexcitonic quantum efficiency, several groups have explored plasmonic enhancement, so far with moderate results. By controlled positioning of individual quantum dots in the near field of gold nanocone antennas, we enhance the radiative decay rates of monoexcitons and biexcitons by 109 and 100 folds at quantum efficiencies of 60 and 70%, respectively, in very good agreement with the outcome of numerical calculations. We discuss the implications of our work for future fundamental and applied research in nano-optics.

  14. Non-polar In x Ga1-x N/GaN quantum dots: impact of dot size and shape anisotropies on excitonic and biexcitonic properties

    Science.gov (United States)

    Kanta Patra, Saroj; Schulz, Stefan

    2017-01-01

    In this work, we present a theoretical analysis of the built-in potential, the excitonic and biexcitonic properties of non-polar InGaN/GaN quantum dots by means of self-consistent Hartree calculations using \\mathbf{k}\\centerdot \\mathbf{p} theory. Special attention is paid to the impact of dot size and shape anisotropies on the results. Our calculations reveal that even though non-polar InGaN/GaN quantum dots exhibit strongly reduced built-in fields when compared to c-plane dots, the excitonic and biexcitonic properties are significantly affected by these residual fields. Furthermore, changes in the built-in field when the geometrical dot features are modified, result in an unusual variation of the exciton binding energy. All these findings highlight that the dot geometry significantly affects electronic and optical properties of non-polar InGaN/GaN systems. This is further supported by comparing our theoretical data with experimental literature results. Here, we analyze also trends in exciton and biexciton binding energies and discuss the potential use of non-polar InGaN/GaN dots for entangled photon emission via the time reordering scheme.

  15. 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

  16. 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...

  17. Controlling of Goos-Hänchen shift via biexciton coherence in a quantum dot

    Science.gov (United States)

    Asadpour, S. H.; Nasehi, R.; Mahmoudi, M.; Soleimani, H. R.

    2015-04-01

    Controlling of the Goos-Hänchen (GH) shifts of the reflected and transmitted probe pulses through a cavity containing four-level GaAs/AlGaAs quantum dot with 15 periods of 17.5 nm GaAs wells and 25-nm Al0.3Ga0.7As barriers is investigated. Under appropriate conditions, the probe absorption can be converted to the probe gain, therefore, the controlling of negative and positive GH shift in the both reflected and transmitted probe beams can be occurred simultaneously. Our obtained results show that the group index of the probe beams could be negative or positive in both reflected and transmitted pulses. Therefore, simultaneous subluminal or superluminal light propagation in reflected and transmitted pulses can be achieved.

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

    DEFF Research Database (Denmark)

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

    1999-01-01

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

  19. Energy transfer and biexciton decay in Cs2UO2Cl4 crystals

    NARCIS (Netherlands)

    Krol, D.M.

    1980-01-01

    We have investigated the influence of energy transfer on luminescence properties of Cs2UO2Cl4 crystals at low temperatures. Time-resolved emission spectra and luminescence decay times were measured between 1.5 and 15 K with the use of selective excitation techniques. The luminescence of Cs2UO2Cl4 de

  20. 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

    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...

  1. Positive binding energy of a biexciton confined in a localization center formed in a single InxGa1-xN/GaN quantum disk

    OpenAIRE

    Bardoux, R.; Kaneta, A.; Funato, M.; Kawakami, Y.; Kikuchi, A; Kishino, K.

    2009-01-01

    We report microphotoluminescence spectroscopy performed on individual and ensemble InGaN/GaN quantum disks (Q-disks). The typical spectrum of a single Q-disk exhibited the contribution of localization centers (LCs) formed in the InGaN active layer of the Q-disks, characterized by sharp lines appearing on the low energy side of the spectra. In addition, a broader emission peak identified as the luminescence of the quasi-two-dimensional (2D) InGaN active layer surrounding the LCs appears system...

  2. Dynamic control of the optical emission from GaN/InGaN nanowire quantum dots by surface acoustic waves

    Energy Technology Data Exchange (ETDEWEB)

    Lazić, S., E-mail: lazic.snezana@uam.es; Chernysheva, E.; Meulen, H. P. van der; Calleja Pardo, J. M. [Departamento de Física de Materiales, Instituto “Nicolás Cabrera” and Instituto de Física de Materia Condensada (IFIMAC), Universidad Autónoma de Madrid, 28049 Madrid (Spain); Gačević, Ž.; Calleja, E. [ISOM-DIE, Universidad Politécnica de Madrid, 28040 Madrid (Spain)

    2015-09-15

    The optical emission of InGaN quantum dots embedded in GaN nanowires is dynamically controlled by a surface acoustic wave (SAW). The emission energy of both the exciton and biexciton lines is modulated over a 1.5 meV range at ∼330 MHz. A small but systematic difference in the exciton and biexciton spectral modulation reveals a linear change of the biexciton binding energy with the SAW amplitude. The present results are relevant for the dynamic control of individual single photon emitters based on nitride semiconductors.

  3. Dynamic control of the optical emission from GaN/InGaN nanowire quantum dots by surface acoustic waves

    Science.gov (United States)

    Lazić, S.; Chernysheva, E.; Gačević, Ž.; van der Meulen, H. P.; Calleja, E.; Calleja Pardo, J. M.

    2015-09-01

    The optical emission of InGaN quantum dots embedded in GaN nanowires is dynamically controlled by a surface acoustic wave (SAW). The emission energy of both the exciton and biexciton lines is modulated over a 1.5 meV range at ˜330 MHz. A small but systematic difference in the exciton and biexciton spectral modulation reveals a linear change of the biexciton binding energy with the SAW amplitude. The present results are relevant for the dynamic control of individual single photon emitters based on nitride semiconductors.

  4. Dynamic control of the optical emission from GaN/InGaN nanowire quantum dots by surface acoustic waves

    Directory of Open Access Journals (Sweden)

    S. Lazić

    2015-09-01

    Full Text Available The optical emission of InGaN quantum dots embedded in GaN nanowires is dynamically controlled by a surface acoustic wave (SAW. The emission energy of both the exciton and biexciton lines is modulated over a 1.5 meV range at ∼330 MHz. A small but systematic difference in the exciton and biexciton spectral modulation reveals a linear change of the biexciton binding energy with the SAW amplitude. The present results are relevant for the dynamic control of individual single photon emitters based on nitride semiconductors.

  5. Identifying multiexcitons in Mo S2 monolayers at room temperature

    Science.gov (United States)

    Lee, Hyun Seok; Kim, Min Su; Kim, Hyun; Lee, Young Hee

    2016-04-01

    One of the unique features of atomically thin two-dimensional materials is strong Coulomb interactions due to the reduced dielectric screening effect; this feature enables the study of many-body phenomena such as excitons, trions, and biexcitons. However, identification of biexcitons remains unresolved owing to their broad peak feature at room temperature. Here, we investigate multiexcitons in monolayer Mo S2 using both electrical and optical doping and identify the transition energies for each exciton. The binding energy of the assigned biexciton is twice that of the trion, in quantitative agreement with theoretical predictions. The biexciton population is predominant under optical doping but negligible under electrical doping. The biexciton population is quadratically proportional to the exciton population, obeying the mass-action theory. Our results illustrate the stable formation of not only trions but also biexcitons due to strong Coulomb interaction even at room temperature; therefore, these results provide a deeper understanding of the complex excitonic behaviors in two-dimensional semiconductors.

  6. Optically induced rotation of a quantum dot exciton spin

    CERN Document Server

    Poem, E; Kodriano, Y; Benny, Y; Khatsevich, S; Avron, J E; Gershoni, D

    2011-01-01

    We demonstrate control over the spin state of a semiconductor quantum dot exciton using a polarized picosecond laser pulse slightly detuned from a biexciton resonance. The control pulse follows an earlier pulse, which generates an exciton and initializes its spin state as a coherent superposition of its two non-degenerate eigenstates. The control pulse preferentially couples one component of the exciton state to the biexciton state, thereby rotating the exciton's spin direction. We detect the rotation by measuring the polarization of the exciton spectral line as a function of the time-difference between the two pulses. We show experimentally and theoretically how the angle of rotation depends on the detuning of the second pulse from the biexciton resonance.

  7. Two-photon- photoluminescence excitation spectroscopy of single quantum-dots

    CERN Document Server

    Benny, Y; Poem, E; Khatsevitch, S; Gershoni, D; Petroff, P M

    2011-01-01

    We present experimental and theoretical study of single semiconductor quantum dots excited by two non-degenerate, resonantly tuned variably polarized lasers. The first laser is tuned to excitonic resonances. Depending on its polarization it photogenerates a coherent single exciton state. The second laser is tuned to biexciton resonances. By scanning the energy of the second laser for various polarizations of the two lasers, while monitoring the emission from the biexciton and exciton spectral lines, we map the biexciton photoluminescence excitation spectra. The resonances rich spectra of the second photon absorption are analyzed and fully understood in terms of a many carrier theoretical model which takes into account the direct and exchange Coulomb interactions between the quantum confined carriers.

  8. Backward Charge Transfer in Conjugated Polymers

    Institute of Scientific and Technical Information of China (English)

    CHENG Meng-Xing; LI Guang-Qi; Thomas F. George; SUN Xin

    2005-01-01

    It has been known that the static polarizability of a polymer chain with a biexciton is negative. In order to understand this peculiar fact, this paper studies the dynamical process of the charge transfer in the polymer chain induced by an external electric field E during forming the biexciton. The time dependence of the charge distribution in the chain reveals that the charge transfer is backward: the positive charge shifts in the opposite direction of the external electric field. Such a backward charge transfer (BCT) produces an opposite dipole, which makes the polarization negative. The effect of electron interaction on the BCT is illustrated.

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

    Energy Technology Data Exchange (ETDEWEB)

    Gallardo, E; Nowak, A K; Sanvitto, D; Meulen, H P van der; Calleja, J M [Departamento de Fisica de Materiales, Universidad Autonoma de Madrid, E-28049 Madrid (Spain); MartInez, L J; Prieto, I; Alija, A R; Granados, D; Taboada, A G; GarcIa, J M; Postigo, P A [Instituto de Microelectronica de Madrid, Centro Nacional de MicrotecnologIa, CSIC, Isaac Newton 8, PTM Tres Cantos, E-28760 Madrid (Spain); Sarkar, D, E-mail: eva.gallardo@uam.e [Department of Physics and Astronomy, University of Sheffield, S3 7RH (United Kingdom)

    2010-02-01

    Different InAs/GaAs quantum rings embedded in a photonic crystal microcavity are studied by quantum correlation measurements. Single photon emission, with g{sup (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.

  10. TURNING-OVER OF THE ELECTRIC DIPOLE IN A POLYMER

    Institute of Scientific and Technical Information of China (English)

    Guang-qi Li; Xin Suna; Sheng Li

    2001-01-01

    The transition from the biexciton to the exciton can turn over the direction of the electric dipole of a polymeric molecule. This turning-over action combined with the photoinduced polarization reversion can be used as a switch. The switching speed is governed by the relaxation time of the turning-over process, which can be determined by a dynamical simulation.

  11. Theoretical Predictions of the Electronic and Optical Properties of Single and Coupled (In,GA)As/GaAs Quantum Dots

    Energy Technology Data Exchange (ETDEWEB)

    Narvaez, G. A.; He, L.; Bester, G.; Zunger, A.

    2006-05-01

    We show how an atomistic pseudopotential plus many-body configuration interaction theory can address the main spectroscopic features of self-assembled dots including, excitons, trions, biexcitons, fine-structure, charging spectra as well as electric-field dependence of entanglement in dot molecules.

  12. Dynamics of Intraband and Interband Auger Processes in Colloidal Core-Shell Qauntum Dots

    NARCIS (Netherlands)

    Rabouw, F.T.; Vaxenburg, R.; Bakulin, A.A.; van Dijk-Moes, R.J.A.; Bakker, H.J.; Rodina, A.; Lifshitz, E.; Efros, A.L.; Koenderink, A.F.; Vanmaekelbergh, D.

    2015-01-01

    Conventional colloidal quantum dots (QDs) suffer from rapid energy losses by nonradiative (Auger) processes, leading to sub-ns lifetimes in all excited states but the lowest-energy single exciton. Suppression of interband Auger decay, such as biexciton Auger recombination, has been achieved with the

  13. Tuning the Exciton Binding Energies in Single Self-Assembled InGaAs/GaAs Quantum Dots by Piezoelectric-Induced Biaxial Stress

    NARCIS (Netherlands)

    Ding, F.; Singh, R.; Plumhof, J.D.; Zander, T.; Křápek, V.; Chen, Y.H.; Benyoucef, M.; Zwiller, V.; Dörr, K.; Bester, G.; Rastelli, A.; Schmidt, O.G.

    2010-01-01

    We study the effect of an external biaxial stress on the light emission of single InGaAs/GaAs(001) quantum dots placed onto piezoelectric actuators. With increasing compression, the emission blueshifts and the binding energies of the positive trion (X+) and biexciton (XX) relative to the neutral exc

  14. Telecom-wavelength (1.5 μm) single-photon emission from InP-based quantum dots

    Science.gov (United States)

    Benyoucef, M.; Yacob, M.; Reithmaier, J. P.; Kettler, J.; Michler, P.

    2013-10-01

    We demonstrate pronounced single-photon emission from InAs/AlGaInAs/InP quantum dots (QDs) at wavelengths above 1.5 μm that are compatible with standard long-distance fiber communication. The QDs are grown by molecular beam epitaxy on distributed Bragg reflectors. A low QD density of about 5 × 108 cm-2 was obtained using optimized growth conditions. Low-temperature micro-photoluminescence spectroscopy exhibits sharp excitonic emission lines from single QDs without the necessity of further processing steps. The combination of excitation power-dependent and polarization-resolved photoluminescence measurements reveal a characteristic exciton-biexciton behavior with biexciton binding energies that range from 3.5 to 4 meV and fine-structure splitting values down to 20 μeV.

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

    CERN Document Server

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

    2010-01-01

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

  16. Quantum confinement in MOVPE-grown structures with self-assembled InAs/GaAs quantum dots

    Energy Technology Data Exchange (ETDEWEB)

    Kuldova, K; Vyborny, Z; Pangrac, J; Oswald, J [Institute of Physics of the AS CR, v. v. i., Cukrovarnicka 10, CZ-162 00 Praha 6 (Czech Republic); Molas, M; Borysiuk, J; Babinski, A, E-mail: kuldova@fzu.c [Institute of Experimental Physics, University of Warsaw, Ho z-dot a 69, PL-00-681 Warszawa (Poland)

    2010-09-01

    In this communication we report on low-temperature, micro-photoluminescence study of quantum confinement in MOVPE-grown structures with InAs/GaAs quantum dots (QDs) with GaAs and/or strain reducing InGaAs/GaAs capping. We focus our attention on sharp emission lines, which appear in both structures at energies up to 80 meV below the wetting line emission. Power-dependent measurements confirmed their attribution to single excitons as well as biexcitons. Negative binding energy of biexcitons with systematic dependence on their energy was observed. It has been proposed that the investigated emission lines result from radiative recombination in flat non-fully developed QDs in the investigated structure. The attribution is confirmed by transmission electron microscopic analysis of investigated structures.

  17. Ultrafast room temperature single-photon source from nanowire-quantum dots.

    Science.gov (United States)

    Bounouar, S; Elouneg-Jamroz, M; Hertog, M den; Morchutt, C; Bellet-Amalric, E; André, R; Bougerol, C; Genuist, Y; Poizat, J-Ph; Tatarenko, S; Kheng, K

    2012-06-13

    Epitaxial semiconductor quantum dots are particularly promising as realistic single-photon sources for their compatibility with manufacturing techniques and possibility to be implemented in compact devices. Here, we demonstrate for the first time single-photon emission up to room temperature from an epitaxial quantum dot inserted in a nanowire, namely a CdSe slice in a ZnSe nanowire. The exciton and biexciton lines can still be resolved at room temperature and the biexciton turns out to be the most appropriate transition for single-photon emission due to a large nonradiative decay of the bright exciton to dark exciton states. With an intrinsically short radiative decay time (≈300 ps) this system is the fastest room temperature single-photon emitter, allowing potentially gigahertz repetition rates.

  18. Entangled photon pairs from a quantum dot cascade decay: the effect of time-reordering

    OpenAIRE

    F. Troiani; Tejedor, C.

    2008-01-01

    Coulomb interactions between confined carriers remove degeneracies in the excitation spectra of quantum dots. This provides a which path information in the cascade decay of biexcitons, thus spoiling the energy-polarization entanglement of the emitted photon pairs. We theoretically analyze a strategy of color coincidence across generation (AG), recently proposed as an alternative to the previous, within generation (WG) approach. We simulate the system dynamics and compute the correlation funct...

  19. Multiexciton complex from extrinsic centers in AlGaAs epilayers on Ge and Si substrates

    Energy Technology Data Exchange (ETDEWEB)

    Sarti, F.; Muñoz Matutano, G.; Bauer, D.; Dotti, N.; Vinattieri, A.; Gurioli, M., E-mail: gurioli@lens.unifi.it [Dipartimento di Fisica e Astronomia, LENS and CNISM, Università di Firenze, Via Sansone 1, I-50019 Firenze (Italy); Bietti, S.; Sanguinetti, S. [Dipartimento di Scienza dei Materiali and L-NESS, Università di Milano Bicocca, Via Cozzi 53, I-20125 Milano (Italy); Isella, G. [Dipartimento di Fisica and L-NESS, Politecnico di Milano, Via Anzani 42, 22100 Como (Italy)

    2013-12-14

    The multiexciton properties of extrinsic centers from AlGaAs layers on Ge and Si substrates are addressed. The two photon cascade is found both in steady state and in time resolved experiments. Polarization analysis of the photoluminescence provides clearcut attribution to neutral biexciton complexes. Our findings demonstrate the prospect of exploiting extrinsic centers for generating entangled photon pairs on a Si based device.

  20. Trapping photon-dressed Dirac electrons in a quantum dot studied by coherent two dimensional photon echo spectroscopy

    Science.gov (United States)

    Roslyak, O.; Gumbs, Godfrey; Mukamel, S.

    2012-05-01

    We study the localization of dressed Dirac electrons in a cylindrical quantum dot (QD) formed on monolayer and bilayer graphene by spatially different potential profiles. Short lived excitonic states which are too broad to be resolved in linear spectroscopy are revealed by cross peaks in the photon-echo nonlinear technique. Signatures of the dynamic gap in the two-dimensional spectra are discussed. The effect of the Coulomb induced exciton-exciton scattering and the formation of biexciton molecules are demonstrated.

  1. Single-Photon Emission from a Single InAs Quantum Dot

    Institute of Scientific and Technical Information of China (English)

    DOU Xiu-Ming; SUN Bao-Quan; HUANG She-Song; NI Hai-Qiao; NIU Zhi-Chuan

    2008-01-01

    Excitation power-dependent micro-photoluminescence spectra and photon-correlation measurement are used to study the optical properties and photon statistics of single InAs quantum dots.Exciton and biexciton emissions,whose photoluminescence intensities have linear and quadratic excitation power dependences,respectively,are identified.Under pulsed laser excitation,the zero time delay peak of second order correlation function corresponding to exciton emission is well suppressed,which is a clear evidence of single photon emission.

  2. Reverse polarization in conjugated heterocycle polythiophene

    Institute of Scientific and Technical Information of China (English)

    王鹿霞; 刘德胜; 张大成; 解士杰; 韩圣浩; 梅良模

    2005-01-01

    Reverse polarization in polythiophene under an applied electric field has been studied in the framework of the tightbinding model. It is found that the applied electronic field has a great influence on the excited states of polythiophene.The effect of the heteroatoms on the polarization has been calculated and analysed carefully. It is indicated that a reverse polarization of biexcitons in polythiophene will be observed more easily. The heteroatoms increase this reversed polarization strength apparently.

  3. Ultralow-threshold multiphoton-pumped lasing from colloidal nanoplatelets in solution

    OpenAIRE

    Li, Mingjie; Zhi, Min; Zhu, Hai; Wu, Wen-Ya; Xu, Qing-Hua; Jhon, Mark Hyunpong; Chan, Yinthai

    2015-01-01

    Although multiphoton-pumped lasing from a solution of chromophores is important in the emerging fields of nonlinear optofluidics and bio-photonics, conventionally used organic dyes are often rendered unsuitable because of relatively small multiphoton absorption cross-sections and low photostability. Here, we demonstrate highly photostable, ultralow-threshold multiphoton-pumped biexcitonic lasing from a solution of colloidal CdSe/CdS nanoplatelets within a cuvette-based Fabry–Pérot optical res...

  4. Reverse polarization in conjugated heterocycle polythiophene

    Science.gov (United States)

    Wang, Lu-Xia; Liu, De-Sheng; Zhang, Da-Cheng; Xie, Shi-Jie; Han, Sheng-Hao; Mei, Liang-Mo

    2005-01-01

    Reverse polarization in polythiophene under an applied electric field has been studied in the framework of the tight-binding model. It is found that the applied electronic field has a great influence on the excited states of polythiophene. The effect of the heteroatoms on the polarization has been calculated and analysed carefully. It is indicated that a reverse polarization of biexcitons in polythiophene will be observed more easily. The heteroatoms increase this reversed polarization strength apparently.

  5. Collective aspects of singlet fission in molecular crystals

    Energy Technology Data Exchange (ETDEWEB)

    Teichen, Paul E.; Eaves, Joel D., E-mail: joel.eaves@colorado.edu [Department of Chemistry and Biochemistry, The University of Colorado at Boulder, Boulder, Colorado 80309 (United States)

    2015-07-28

    We present a model to describe collective features of singlet fission in molecular crystals and analyze it using many-body theory. The model we develop allows excitonic states to delocalize over several chromophores which is consistent with the character of the excited states in many molecular crystals, such as the acenes, where singlet fission occurs. As singlet states become more delocalized and triplet states more localized, the rate of singlet fission increases. We also determine the conditions under which the two triplets resulting from fission are correlated. Using the Bethe Ansatz and an entanglement measure for indistinguishable bipartite systems, we calculate the triplet-triplet entanglement as a function of the biexciton interaction strength. The biexciton interaction can produce bound biexciton states and provides a source of entanglement between the two triplets even when the triplets are spatially well separated. Significant entanglement between the triplet pair occurs well below the threshold for bound pair formation. Our results paint a dynamical picture that helps to explain why fission has been observed to be more efficient in molecular crystals than in their covalent dimer analogues and have consequences for photovoltaic efficiency models that assume that the two triplets can be extracted independently.

  6. Time-resolved spectroscopy of excitons and carriers in GaN and InGaN

    CERN Document Server

    Kyhm, K

    2001-01-01

    delocalised electron-hole pairs from the lowest confined level are responsible for the gain in our sample. The polarization dependence of biexcitonic signals and quantum beats between A-excitons (X sub A) and A-biexcitons (X sub A X sub A) in a high-quality GaN epilayer are measured by spectrally-resolved and time-integrated four-wave mixing measurements. We also measured the polarization dependent B-biexciton (X sub B X sub B) signal. The emission mechanisms in GaN and ln sub x Ga sub 1 sub - sub x N is systematically studied to investigate carrier and exciton dynamics. Reflectance, time-integrated luminescence, and time-resolved reflectance spectroscopy are used to study exciton transitions in GaN, and the saturation of the exciton resonances with increasing carrier density has been measured in the case of resonant and non-resonant excitations. The coincidence between the density for the onset of the stimulated emission and the Mott density leads us to the conclusion that the stimulated emission mechanism i...

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

    Science.gov (United States)

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

    2017-03-01

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

  8. Resonance effects of excitons and electrons. Basics and applications

    Energy Technology Data Exchange (ETDEWEB)

    Geru, Ion [Moldovan Academy of Sciences, Chisinau (Moldova, Republic of). Inst. of Chemistry; Suter, Dieter [Technische Univ. Dortmund (Germany). Fakultaet Physik

    2013-08-01

    Represents the first book on non-traditional resonance effects of excitons in semiconductors. Explains resonance phenomena of excitons and electrons in solids. Presents the Knight shift at the Bose-Einstein condensation of excitons. This book presents the various types of resonance effects on excitons, biexcitons and the local electronic centers (LEC) in solids, such as paramagnetic and paraelectric resonances on excitons, exciton acoustic resonance at intra- and interband transitions, radio-optical double resonance on excitons, hole-nuclear double resonance on localized biexcitons, ENDOR and acoustic ENDOR on LEC. The criteria for the generation of coherent photons, phonons and magnons by excitons are explained. The interactions of excitons and biexcitons with paramagnetic centers and nuclear spins, the indirect interaction between the PC through a field of excitons as well as the quasienergy spectrum of excitons and spin systems are discussed. It is proved that the interaction of paramagnetic centers with excitons increases the spin relaxation rate of paramagnetic centers in comparison with the case of their interaction with free carriers. The giant magneto-optical effects in semi-magnetic semiconductors are theoretically interpreted. In recent years, a new perspective has been added to these systems and their interactions: they can be used for storing and processing information in the form of quantum bits (qubits), the building blocks of quantum computers. The basics of this emerging technology are explained and examples of demonstration-type quantum computers based on localized spins in solids are discussed.

  9. Instabilities in the optical response of a semiconductor quantum dot—metal nanoparticle heterodimer: self-oscillations and chaos

    Science.gov (United States)

    Nugroho, Bintoro S.; Iskandar, Alexander A.; Malyshev, Victor A.; Knoester, Jasper

    2017-01-01

    We theoretically investigate the nonlinear optical response of a heterodimer comprising a semiconductor quantum dot strongly coupled to a metal nanoparticle. The quantum dot is considered as a three-level ladder system with ground, one-exciton, and bi-exction states. As compared to the case of a two-level quantum dot model, adding the third (bi-exciton) state produces fascinating effects in the optical response of the hybrid system. Specifically, we demonstrate that the system may exhibit picosecond and sub-picosecond self-oscillations and quasi-chaotic behaviour under single-frequency continuous wave excitation. An isolated semiconductor quantum dot does not show such features. The effects originate from competing one-exciton and bi-exciton transitions in the semiconductor quantum dot, triggered by the self-action of the quantum dot via the metal nanoparticle. The key parameter that governs the phenomena mentioned is the ratio of the self-action strength and the bi-exciton shift. The self-oscillation regime can be achieved in practice, in particular, in a heterodimer comprised of a closely spaced ZnS/ZnSe core-shell quantum dot and a spherical silver nanoparticle. The results may have applications in nanodevices for generating trains of ultrashort optical pulses.

  10. 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

  11. Single-photon emission from InAsP quantum dots embedded in density-controlled InP nanowires

    Science.gov (United States)

    Yanase, Shougo; Sasakura, Hirotaka; Hara, Shinjiro; Motohisa, Junichi

    2017-04-01

    We attempted to control the density and size of InP-based nanowires (NWs) and nanowire quantum dots (NW-QDs) during selective-area metalorganic vapor phase epitaxy. InP nanowire arrays with a 5 µm pitch and an average NW diameter d of 67 nm were successfully grown by optimization of growth conditions. InAsP quantum dots were embedded in these density-controlled InP NW arrays, and clear single-photon emission and exciton-biexciton cascaded emission were confirmed by excitation-dependent photoluminescence and photon correlation measurements.

  12. All-optical tailoring of single-photon spectra in a quantum-dot microcavity system

    CERN Document Server

    Breddermann, Dominik; Binder, Rolf; Zrenner, Artur; Schumacher, Stefan

    2016-01-01

    Semiconductor quantum-dot cavity systems are promising sources for solid-state based on-demand generation of single photons for quantum communication. Commonly, the spectral characteristics of the emitted single photon are fixed by system properties such as electronic transition energies and spectral properties of the cavity. In the present work we study single-photon generation from the quantum-dot biexciton through a partly stimulated non-degenerate two-photon emission. We show that frequency and linewidth of the single photon can be fully controlled by the stimulating laser pulse, ultimately allowing for efficient all-optical spectral shaping of the single photon.

  13. Time-bin Entanglement from Quantum Dots

    CERN Document Server

    Weihs, Gregor; Predojević, Ana

    2016-01-01

    The desire to have a source of single entangled photon pairs can be satisfied using single quantum dots as emitters. However, we are not bound to pursue only polarization entanglement, but can also exploit other degrees of freedom. In this chapter we focus on the time degree of freedom, to achieve so-called time-bin entanglement. This requires that we prepare the quantum dot coherently into the biexciton state and also build special interferometers for analysis. Finally this technique can be extended to achieve time-bin and polarization hyper-entanglement from a suitable quantum dot.

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

    CERN Document Server

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

    2010-01-01

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

  15. Entangled Photons from Radiative Cascades in Semiconductor Quantum Dots

    CERN Document Server

    Akopian, N; Poem, E; Berlatzky, Y; Avron, J; Gershoni, D; Gerardot, B D; Petroff, P M

    2005-01-01

    We show, for the first time, that polarization-entangled photon pairs can be produced from the biexciton radiative cascade in a semiconductor quantum dot. We select an energy window that erases the ``which path'' information contained in the colors of the emitted photons, and use tomographic analysis to demonstrate that the photon pair violate Bell's inequality and satisfy Peres criterion for entanglement by more than 3 standard deviations of the experimental uncertainty. Our quantitative analysis show that semiconductor quantum dots can be used as sources for ``event-ready'' entangled photons.

  16. 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

  17. Low-Lying States of the A+B-A+B- Coulomb Systems in Two-Dimensional Quantum Dots

    Institute of Scientific and Technical Information of China (English)

    XIE Wen-Fang

    2001-01-01

    The features of the low-lying spectra of four-body A+B-A+B- systems have been deduced based on symmetry. Using the method of few-body physics, we calculate the energy spectra of A + B- A + B- systems in a harmonic quantum dot. We find that the biexciton in a two-dimensional quantum dot may have other bound excited states and the quantum mechanical symmetry plays a crucialrole in determining the energy levels and structures of the low-lying states.

  18. Coherent dynamics in semiconductors

    DEFF Research Database (Denmark)

    Hvam, Jørn Märcher

    1998-01-01

    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...

  19. Deterministic Photon Pairs and Coherent Optical Control of a Single Quantum Dot

    Science.gov (United States)

    Jayakumar, Harishankar; Predojević, Ana; Huber, Tobias; Kauten, Thomas; Solomon, Glenn S.; Weihs, Gregor

    2013-03-01

    The strong confinement of semiconductor excitons in a quantum dot gives rise to atomlike behavior. The full benefit of such a structure is best observed in resonant excitation where the excited state can be deterministically populated and coherently manipulated. Because of the large refractive index and device geometry it remains challenging to observe resonantly excited emission that is free from laser scattering in III/V self-assembled quantum dots. Here we exploit the biexciton binding energy to create an extremely clean single photon source via two-photon resonant excitation of an InAs/GaAs quantum dot. We observe complete suppression of the excitation laser and multiphoton emissions. Additionally, we perform full coherent control of the ground-biexciton state qubit and observe an extended coherence time using an all-optical echo technique. The deterministic coherent photon pair creation makes this system suitable for the generation of time-bin entanglement and experiments on the interaction of photons from dissimilar sources.

  20. Comparison of carrier multiplication yields in PbS and PbSe nanocrystals: The role of competing energy-loss processes

    Energy Technology Data Exchange (ETDEWEB)

    Stewart, John T.; Padilha, Lazaro A.; Qazilbash, M. M.; Pietryga, Jeffrey M.; Midgett, Aaron G; Luther, Joseph M; Beard, Matthew C; Nozik, Arthur J; Klimov, Victor I.

    2012-02-08

    Infrared band gap semiconductor nanocrystals are promising materials for exploring generation III photovoltaic concepts that rely on carrier multiplication or multiple exciton generation, the process in which a single high-energy photon generates more than one electron–hole pair. In this work, we present measurements of carrier multiplication yields and biexciton lifetimes for a large selection of PbS nanocrystals and compare these results to the well-studied PbSe nanocrystals. The similar bulk properties of PbS and PbSe make this an important comparison for discerning the pertinent properties that determine efficient carrier multiplication. We observe that PbS and PbSe have very similar biexciton lifetimes as a function of confinement energy. Together with the similar bulk properties, this suggests that the rates of multiexciton generation, which is the inverse of Auger recombination, are also similar. The carrier multiplication yields in PbS nanocrystals, however, are strikingly lower than those observed for PbSe nanocrystals. We suggest that this implies the rate of competing processes, such as phonon emission, is higher in PbS nanocrystals than in PbSe nanocrystals. Indeed, our estimations for phonon emission mediated by the polar Fröhlich-type interaction indicate that the corresponding energy-loss rate is approximately twice as large in PbS than in PbSe.

  1. Multiple population-period transient spectroscopy (MUPPETS) of CdSe/ZnS nanoparticles. II. Effects of high fluence and solvent heating.

    Science.gov (United States)

    Wu, Haorui; Sahu, Kalyanasis; Berg, Mark A

    2013-12-12

    Multiple population-period transient spectroscopy (MUPPETS) is a six-pulse experiment with two time dimensions that is capable of adding information about systems with complicated kinetics. The core theory for MUPPETS focuses on the χ(5) response of the chromophores. This theory was used to analyze the dynamics of excitons and biexcitons in CdSe/ZnS core-shell nanoparticles in part I of this paper [J. Phys. Chem. B 2013, DOI:10.1021/jp405785a]. In real experiments, the potential role of additional processes must also be considered, in particular, the χ(7), "saturation" of the MUPPETS signal and nonresonant signals from heating of the solvent. A pathway method for calculating fluence effects in MUPPETS is developed. The fluence dependence of the biexciton signal and its sign reversal, as found in part I, are explained without invoking higher excitons or unexpected species. A method is presented for quantitatively predicting the magnitude of signals from solvent heating using an external standard. Thermal effects in this system are found to be too small to affect the conclusions in part I. Their small size, combined with small, systematic errors in the data, also makes it difficult to measure the yield of solvent heat in these experiments.

  2. Electrostatic Control of Single IndiumArsenic Quantum Dots using IndiumPhosphorus Nanotemplates

    Science.gov (United States)

    Cheriton, Ross

    This thesis focuses on pioneering a scalable route to fabricate quantum information devices based upon single InAs/InP quantum dots emitting in the telecommunications wavelength band around lambda = 1550 nm. Using metallic gates in combination with nanotemplate, site-selective epitaxy techniques, arrays of single quantum dots are produced and electrostatically tuned with a high degree of control over the electrical and optical properties of each individual quantum dot. Using metallic gates to apply local electric fields, the number of electrons within each quantum dot can be tuned and the nature of the optical recombination process controlled. Four electrostatic gates mounted along the sides of a square-based, pyramidal nanotemplate in combination with a flat metallic gate on the back of the InP substrate allow the application of electric fields in any direction across a single quantum dot. Using lateral fields provided by the metallic gates on the sidewalls of the pyramid and a vertical electric field able to control the charge state of the quantum dot, the exchange splitting of the exciton, trion and biexciton are measured as a function of gate voltage. A quadrupole electric field configuration is predicted to symmetrize the product of electron and hole wavefunctions within the dot, producing two degenerate exciton states from the two possible optical decay pathways of the biexciton. Building upon these capabilities, the anisotropic exchange splitting between the exciton states within the biexciton cascade is shown to be reversibly tuned through zero for the first time. We show direct control over the electron and hole wavefunction symmetry, thus enabling the entanglement of emitted photon pairs in asymmetric quantum dots. Optical spectroscopy of single InAs/InP quantum dots atop pyramidal nanotemplates in magnetic fields up to 28T is used to examine the dispersion of the s, p and d shell states. The g-factor and diamagnetic shift of the exciton and charged

  3. Type 2 quantum dots in Ge/Si system

    CERN Document Server

    Dvurechenskij, A V

    2001-01-01

    The results on the electronic structure of spatially indirect excitons, multiparticle excitonic complexes, and negative interband photoconductivity in arrays of Ge/Si type 2 quantum dots are presented. These data have been compared with the well known results for type 2 A sup I sup I sup I B sup V and A sup I sup I B sup V sup I -based heterostructures with quantum dots. Fundamental physical phenomena are found to be the result of an increase in the binding energy of excitons in quantum dots as compared with that of free excitons in bulk homogeneous materials; the shortwave shift of exciton transition energy at multiparticle complexes production (charges excitons, biexcitons), as well as the trapping of equilibrium carrier by localized states induced by the charged quantum dot electric field

  4. Conditions for entangled photon emission from (111)B site-controlled pyramidal quantum dots

    Energy Technology Data Exchange (ETDEWEB)

    Juska, G., E-mail: gediminas.juska@tyndall.ie; Murray, E.; Dimastrodonato, V.; Chung, T. H.; Moroni, S. T.; Gocalinska, A.; Pelucchi, E. [Tyndall National Institute, University College Cork, Lee Maltings, Cork (Ireland)

    2015-04-07

    A study of highly symmetric site-controlled pyramidal In{sub 0.25}Ga{sub 0.75}As quantum dots (QDs) is presented. It is discussed that polarization-entangled photons can be also obtained from pyramidal QDs of different designs from the one already reported in Juska et al. [Nat. Photonics 7, 527 (2013)]. Moreover, some of the limitations for a higher density of entangled photon emitters are addressed. Among these issues are (1) a remaining small fine-structure splitting and (2) an effective QD charging under non-resonant excitation conditions, which strongly reduce the number of useful biexciton-exciton recombination events. A possible solution of the charging problem is investigated exploiting a dual-wavelength excitation technique, which allows a gradual QD charge tuning from strongly negative to positive and, eventually, efficient detection of entangled photons from QDs, which would be otherwise ineffective under a single-wavelength (non-resonant) excitation.

  5. Correlated Photon Emission from a Single II-VI Quantum Dot

    CERN Document Server

    Couteau, C; Tinjod, F; Gérard, J M; Kheng, K; Mariette, H; Gaj, J A; Romestain, R; Poizat, J P

    2004-01-01

    We report correlation and cross-correlation measurements of photons emitted under continuous wave excitation by a single II-VI quantum dot (QD) grown by molecular-beam epitaxy. A standard technique of microphotoluminescence combined with an ultrafast photon correlation set-up allowed us to see an antibunching effect on photons emitted by excitons recombining in a single CdTe/ZnTe QD, as well as cross-correlation within the biexciton ($X_{2}$)-exciton ($X$) radiative cascade from the same dot. Fast microchannel plate photomultipliers and a time-correlated single photon module gave us an overall temporal resolution of 140 ps better than the typical exciton lifetime in II-VI QDs of about 250ps.

  6. Telecom wavelength emitting single quantum dots coupled to InP-based photonic crystal microcavities

    Science.gov (United States)

    Kors, A.; Fuchs, K.; Yacob, M.; Reithmaier, J. P.; Benyoucef, M.

    2017-01-01

    Here we report on the fabrication and optical characterization of InP-based L3 photonic crystal (PhC) microcavities embedded with a medium density InAs/InP quantum dots (QDs) emitting at telecom wavelengths. The QDs are grown by solid source molecular beam epitaxy using a ripening technique. Micro-photoluminescence (μ-PL) measurements of PhC samples reveal sharp cavity modes with quality factors exceeding 8500. QDs emit highly linear-polarized light at telecom wavelengths with resolution-limited spectral linewidth below 50 μeV. Enhanced PL intensity of QDs in PhC is observed in comparison to the PL intensity of QDs in bulk semiconductors. The combination of excitation power-dependent and polarization-resolved μ-PL measurements reveal the existence of an exciton-biexciton system with a small fine-structure splitting.

  7. A bright triggered twin-photon source in the solid state

    CERN Document Server

    Thoma, Alexander; Schlehahn, Alexander; Gschrey, Manuel; Schnauber, Peter; Schulze, Jan-Hindrik; Strittmatter, André; Rodt, Sven; Carmele, Alexander; Knorr, Andreas; Reitzenstein, Stephan

    2016-01-01

    A non-classical light source emitting pairs of identical photons represents a versatile resource of interdisciplinary importance with applications in quantum optics and quantum biology. Emerging research fields, which benefit from such type of quantum light source, include quantum-optical spectroscopy or experiments on photoreceptor cells sensitive to photon statistics. To date, photon twins have mostly been generated using parametric downconversion sources, relying on Poissonian number distributions, or atoms, exhibiting low emission rates. Here, we propose and experimentally demonstrate the efficient, triggered generation of photon twins using the energy-degenerate biexciton-exciton radiative cascade of a single semiconductor quantum dot. Deterministically integrated within a microlens, this nanostructure emits highly-correlated photon pairs, degenerate in energy and polarization, at a rate of up to (2.8 $\\pm$ 0.4) MHz. Two-photon interference experiments reveal a significant degree of indistinguishability ...

  8. Photoluminescence of a single InAs/AlAs quantum dot

    Energy Technology Data Exchange (ETDEWEB)

    Shamirzaev, T.S.; Zhuravlev, K.S. [Institute of Semiconductor Physics, Novosibirsk (Russian Federation); Larsson, M.; Holtz, P.O. [Department of Physics and Measurement Technology, Linkoeping University (Sweden)

    2008-07-01

    Micro-photoluminescence ({mu}-PL) of a simple InAs/AlAs quantum dot (QD) has been studied. It has been found that the {mu}-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 {mu}-PL spectra at high excitation power densities. A red shift of the {mu}-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.)

  9. Multiple exciton generation in nano-crystals revisited: Consistent calculation of the yield based on pump-probe spectroscopy

    CERN Document Server

    Karki, Khadga J; Zheng, Kaibo; Zidek, Karel; Mousa, Abdelrazek; Abdellah, Mohamed A; Messing, Maria; Wallenberg, L Reine; Yartsev, Arkadi; Pullerits, Tonu

    2013-01-01

    Multiple exciton generation (MEG) is a process in which more than one exciton is generated upon the absorption of a high energy photon, typically higher than two times the band gap, in semiconductor nanocrystals. It can be observed experimentally using time resolved spectroscopy such as the transient absorption measurements. Quantification of the MEG yield is usu- ally done by assuming that the bi-exciton signal is twice the signal from a single exciton. Herein we show that this assumption is not always justified and may lead to significant errors in the estimated MEG yields. We develop a methodology to determine proper scaling factors to the signals from the transient absorption experiments. Using the methodology we find modest MEG yields in lead chalcogenide nanocrystals including the nanorods.

  10. Low Density Self-Assembled InAs/GaAs Quantum Dots Grown by Metal Organic Chemical Vapour Deposition

    Institute of Scientific and Technical Information of China (English)

    LI Lin; LIU Guo-Jun; WANG Xiao-Hua; LI Mei; LI Zhan-Guo; WAN Chun-Ming

    2008-01-01

    The serf-assembled InAs quantum dots (QDs) on GaAs substrates with low density (5×108cm-2) are achieved using relatively higher growth temperature and low InAs coverage by low-pressure metal-organic chemical vapour deposition.The macro-PL spectra exhibit three emission peaks at 1361,1280 and 1204nm,corresponding to the ground level (GS),the first excited state (ES1) and the second excited state (ES2) of the QDs,respectively,which are obtained when the GaAs capping layer/s grown using triethylgallium and tertiallybutylarsine.As a result of micro-PL,only a few peaks from individual dots have been observed.The exciton-biexciton behaviour was clearly observed at low temperature.

  11. Optical probing of spin-dependent interactions in II-VI semiconductor structures

    Energy Technology Data Exchange (ETDEWEB)

    Gaj, J.A.; Golnik, A.; Goryca, M.; Kossacki, P.; Kowalik, K.; Kudelski, A.; Maslana, W.; Nawrocki, M.; Pacuski, W.; Plochocka, P.; Senellart, P. [Institute of Experimental Physics, Warsaw University, Hoza 69, 00-681 Warszawa (Poland); Cibert, J.; Ferrand, D.; Tatarenko, S. [CNRS-CEA-UJF Joint Group ' ' Nanophysique et semiconducteurs' ' , Laboratoire de Spectrometrie Physique, BP 87, 38402 Saint Martin d' Heres Cedex (France); Karczewski, G.; Kossut, J.; Kutrowski, M. [Institute of Physics, Polish Academy of Sciences, al. Lotnikow 32/46, 02-668 Warszawa (Poland); Krebs, O.; Lemaitre, A.; Voisin, P. [Laboratoire de Photonique et Nanostructures, CNRS, Route de Nozay, 91460 Marcoussis (France); Wojtowicz, T.

    2006-03-15

    We present a selection of optical experiments, providing information on several spin-dependent interactions in II-VI semiconductor structures. Exciton-exciton and exciton-carrier interactions were studied by time-resolved picosecond pump-probe measurements. Several examples of recent studies involving ion-carrier exchange interaction in quantum wells and layers are discussed, concerning the quest for room temperature ferromagnetic semiconductors, spin temperature of Mn ions in (Cd,Mn)Te quantum wells, and spin relaxation in such wells under pulsed magnetic field. Finally, anisotropic electron-hole exchange in semiconductor quantum dots is discussed in the context of efforts to obtain generation of entangled photon pairs in a biexciton-exciton cascade in a semiconductor quantum dot. (copyright 2006 WILEY-VCH Verlag GmbH and Co. KGaA, Weinheim) (orig.)

  12. 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

  13. Quantum Yield Heterogeneity among Single Nonblinking Quantum Dots Revealed by Atomic Structure-Quantum Optics Correlation.

    Science.gov (United States)

    Orfield, Noah J; McBride, James R; Wang, Feng; Buck, Matthew R; Keene, Joseph D; Reid, Kemar R; Htoon, Han; Hollingsworth, Jennifer A; Rosenthal, Sandra J

    2016-02-23

    Physical variations in colloidal nanostructures give rise to heterogeneity in expressed optical behavior. This correlation between nanoscale structure and function demands interrogation of both atomic structure and photophysics at the level of single nanostructures to be fully understood. Herein, by conducting detailed analyses of fine atomic structure, chemical composition, and time-resolved single-photon photoluminescence data for the same individual nanocrystals, we reveal inhomogeneity in the quantum yields of single nonblinking "giant" CdSe/CdS core/shell quantum dots (g-QDs). We find that each g-QD possesses distinctive single exciton and biexciton quantum yields that result mainly from variations in the degree of charging, rather than from volume or structure inhomogeneity. We further establish that there is a very limited nonemissive "dark" fraction (<2%) among the studied g-QDs and present direct evidence that the g-QD core must lack inorganic passivation for the g-QD to be "dark". Therefore, in contrast to conventional QDs, ensemble photoluminescence quantum yield is principally defined by charging processes rather than the existence of dark g-QDs.

  14. Valence band offset, strain and shape effects on confined states in self-assembled InAs/InP and InAs/GaAs quantum dots

    Science.gov (United States)

    >M Zieliński,

    2013-11-01

    I present a systematic study of self-assembled InAs/InP and InAs/GaAs quantum dot single-particle and many-body properties as a function of the quantum dot-surrounding matrix valence band offset. I use an atomistic, empirical tight-binding approach and perform numerically demanding calculations for half-million-atom nanosystems. I demonstrate that the overall confinement in quantum dots is a non-trivial interplay of two key factors: strain effects and the valence band offset. I show that strain effects determine both the peculiar structure of confined hole states of lens type InAs/GaAs quantum dots and the characteristic ‘shell-like’ structure of confined hole states in the commonly considered ‘low-strain’ lens type InAs/InP quantum dot. I also demonstrate that strain leads to single-band-like behavior of hole states of disk type (‘indium flushed’) InAs/GaAs and InAs/InP quantum dots. I show how strain and valence band offset affect quantum dot many-body properties: the excitonic fine structure, an important factor for efficient entangled photon pair generation, and the biexciton and charged exciton binding energies.

  15. Suppression of auger recombination in ""giant"" core/shell nanocrystals

    Energy Technology Data Exchange (ETDEWEB)

    Garcia Santamaria, Florencio [Los Alamos National Laboratory; Vela, Javier [Los Alamos National Laboratory; Schaller, Richard D [Los Alamos National Laboratory; Hollingsworth, Jennifer A [Los Alamos National Laboratory; Klimov, Victor I [Los Alamos National Laboratory; Chen, Yongfen [NON LANL

    2009-01-01

    Many potential applications of semiconductor nanocrystals are hindered by nonradiative Auger recombination wherein the electron-hole (exciton) recombination energy is transferred to a third charge carrier. This process severely limits the lifetime and bandwidth of optical gain, leads to large nonradiative losses in light emitting diodes and photovoltaic cells, and is believed to be responsible for intermittency ('blinking') of emission from single nanocrystals. The development of nanostructures in which Auger recombination is suppressed has been a longstanding goal in colloidal nanocrystal research. Here, we demonstrate that such suppression is possible using so-called 'giant' nanocrystals that consist of a small CdSe core and a thick CdS shell. These nanostructures exhibit a very long biexciton lifetime ({approx}10 ns) that is likely dominated by radiative decay instead of non-radiative Auger recombination. As a result of suppressed Auger recombination, even high-order multiexcitons exhibit high emission efficiencies, which allows us to demonstrate optical amplification with an extraordinarily large bandwidth (>500 me V) and record low excitation thresholds.

  16. Engineered semiconductor nanocrystals with enhanced carrier multiplication yields

    Science.gov (United States)

    Klimov, Victor

    2014-03-01

    Carrier multiplication (CM) is a process whereby absorption of a single photon results in multiple electron-hole pairs (excitons). This process could benefit a number of solar-energy conversion technologies, most notably photocatalysis and photovoltaics. This presentation overviews recent progress in understanding the CM process in semiconductor nanocrystals, motivated by an outstanding challenge in this field - the lack of capability to predict the CM performance of nanocrystals based on their known photophysical properties or documented parameters of parental bulk solids. Here, we present a possible solution to this problem by showing that, using biexciton Auger lifetimes and intraband relaxation rates inferred from ultrafast spectroscopic studies, we can rationalize relative changes in CM yields as a function of nanocrystal composition, size and shape. Further, guided by this model, we demonstrate a two-fold enhancement in multiexciton yields in PbSe nanorods vs. quantum dots attributed to enhanced Coulomb interactions. We also explore the control of competing intra-band cooling for increasing multiexciton production. Specifically, we design a new type of hetero-structured PbSe/CdSe quantum dots with reduced rates of intra-band relaxation and demonstrate a four-fold boost in the multiexciton yield. These studies provide useful guidelines for future efforts to achieve the ultimate, energy-conservation-defined CM efficiencies.

  17. 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.

  18. 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.

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

    Science.gov (United States)

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

    2016-09-01

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

  20. Multi-excitonic (N=1,2 and 3) quantum dots in magnetic field: Analytical mapping of correlations (exchange) by multipole expansion

    Science.gov (United States)

    Singh, Sunny; Kaur, Harsimran; Sharma, Shivalika; Aggarwal, Priyanka; Hazra, Ram Kuntal

    2017-04-01

    The understanding of the physics of exciton, bi-exciton, tri-exciton and the subsequent insight into controlling the properties of mesoscopic systems holds the key to various exotic optical, electrical and magnetic phenomena like superconductivity, Mott insulation, Quantum Hall effect etc. Many of exciton properties are similar to atomic hydrogen that attracts researchers to explore electronic structure of exciton in quantum dots, but nontriviality arises due to coulombic interactions among electrons and holes. We propose an exact integral of coulomb (exchange) correlation in terms of finitely summed Lauricella functions to examine 3-D exciton of harmonic dots confined in zero and non-zero arbitrary magnetic field. The highlight of our work is the use of exact variational solution for coloumbic interaction between the hole and the electron and evaluation of the cross terms arising out of the coupling among centre-of-mass and relative coordinates. We also have extended the size of the system to generalized N-body problem with N=3,4 for tri-exciton (e-e-h/e-h-h)

  1. Elucidation of two giants: challenges to thick-shell synthesis in CdSe/ZnSe and ZnSe/CdS core/shell quantum dots.

    Science.gov (United States)

    Acharya, Krishna P; Nguyen, Hue M; Paulite, Melissa; Piryatinski, Andrei; Zhang, Jun; Casson, Joanna L; Xu, Hongwu; Htoon, Han; Hollingsworth, Jennifer A

    2015-03-25

    Core/thick-shell giant quantum dots (gQDs) possessing type II electronic structures exhibit suppressed blinking and diminished nonradiative Auger recombination. We investigate CdSe/ZnSe and ZnSe/CdS as potential new gQDs. We show theoretically and experimentally that both can exhibit partial or complete spatial separation of an excited-state electron-hole pair (i.e., type II behavior). However, we reveal that thick-shell growth is challenged by competing processes: alloying and cation exchange. We demonstrate that these can be largely avoided by choice of shelling conditions (e.g., time, temperature, and QD core identity). The resulting CdSe/ZnSe gQDs exhibit unusual single-QD properties, principally emitting from dim gray states but having high two-exciton (biexciton) emission efficiencies, whereas ZnSe/CdS gQDs show characteristic gQD blinking suppression, though only if shelling is accompanied by partial cation exchange.

  2. 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.)

  3. Low light adaptation: energy transfer processes in different types of light harvesting complexes from Rhodopseudomonas palustris.

    Science.gov (United States)

    Moulisová, Vladimíra; Luer, Larry; Hoseinkhani, Sajjad; Brotosudarmo, Tatas H P; Collins, Aaron M; Lanzani, Guglielmo; Blankenship, Robert E; Cogdell, Richard J

    2009-12-01

    Energy transfer processes in photosynthetic light harvesting 2 (LH2) complexes isolated from purple bacterium Rhodopseudomonas palustris grown at different light intensities were studied by ground state and transient absorption spectroscopy. The decomposition of ground state absorption spectra shows contributions from B800 and B850 bacteriochlorophyll (BChl) a rings, the latter component splitting into a low energy and a high energy band in samples grown under low light (LL) conditions. A spectral analysis reveals strong inhomogeneity of the B850 excitons in the LL samples that is well reproduced by an exponential-type distribution. Transient spectra show a bleach of both the low energy and high energy bands, together with the respective blue-shifted exciton-to-biexciton transitions. The different spectral evolutions were analyzed by a global fitting procedure. Energy transfer from B800 to B850 occurs in a mono-exponential process and the rate of this process is only slightly reduced in LL compared to high light samples. In LL samples, spectral relaxation of the B850 exciton follows strongly nonexponential kinetics that can be described by a reduction of the bleach of the high energy excitonic component and a red-shift of the low energetic one. We explain these spectral changes by picosecond exciton relaxation caused by a small coupling parameter of the excitonic splitting of the BChl a molecules to the surrounding bath. The splitting of exciton energy into two excitonic bands in LL complex is most probably caused by heterogenous composition of LH2 apoproteins that gives some of the BChls in the B850 ring B820-like site energies, and causes a disorder in LH2 structure.

  4. 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.

  5. Low light adaptation: Energy transfer processes in different types of light harvesting complexes from Rhodopseudomonas palustris

    Energy Technology Data Exchange (ETDEWEB)

    Moulisova, Vladimira; Luer, Larry; Hoseinkhani, Sajjad; Brotosudarmo, Tatas H.P.; Collins, Aaron M.; Lanzani, Guglielmo; Blankenship, R. E.; Cogdell, Richard J

    Energy transfer processes in photosynthetic light harvesting 2 (LH2) complexes isolated from purple bacterium Rhodopseudomonas palustris grown at different light intensities were studied by ground state and transient absorption spectroscopy. The decomposition of ground state absorption spectra shows contributions from B800 and B850 bacteriochlorophyll (BChl) a rings, the latter component splitting into a low energy and a high energy band in samples grown under low light (LL) conditions. A spectral analysis reveals strong inhomogeneity of the B850 excitons in the LL samples that is well reproduced by an exponential-type distribution. Transient spectra show a bleach of both the low energy and high energy bands, together with the respective blue-shifted exciton-to-biexciton transitions. The different spectral evolutions were analyzed by a global fitting procedure. Energy transfer from B800 to B850 occurs in a mono-exponential process and the rate of this process is only slightly reduced in LL compared to high light samples. In LL samples, spectral relaxation of the B850 exciton follows strongly nonexponential kinetics that can be described by a reduction of the bleach of the high energy excitonic component and a red-shift of the low energetic one. We explain these spectral changes by picosecond exciton relaxation caused by a small coupling parameter of the excitonic splitting of the BChl a molecules to the surrounding bath. The splitting of exciton energy into two excitonic bands in LL complex is most probably caused by heterogenous composition of LH2 apoproteins that gives some of the BChls in the B850 ring B820-like site energies, and causes a disorder in LH2 structure.

  6. Tunable Optical Phenomena and Carrier Recombination Dynamics in III-V Semiconductor Nanostructures

    Science.gov (United States)

    Kumar Thota, Venkata Ramana

    Semiconductor nanostructures such as quantum dots, quantum wires and quantum wells have gained significant attention in the scientific community due to their peculiar properties, which arise from the quantum confinement of charge carriers. In such systems, confinement plays key role and governs the emission spectra. With the advancements in growth techniques, which enable the fabrication of these nanostructured devices with great precision down to the atomic scale, it is intriguing to study and observe quantum mechanical effects through light-matter interactions and new physics governed by the confinement, size, shape and alloy composition. The goal is to reduce the size of semiconductor bulk material to few nanometers, which in turn localizes the charge carriers inside these structures such that the spin associated with them is used to carry and process information within ultra-short time scales. The main focus of this dissertation is the optical studies of quantum dot molecule (QDM) systems. A system where the electrons can tunnel between the two dots leading to observable tunneling effects. The emission spectra of such system has been demonstrated to have both intradot transitions (electron-hole pair residing in the same dot) and interdot transitions (electron-hole pair participating in the recombination origin from different dots). In such a system, it is possible to apply electric field such that the wavefunction associated with the charge carriers can be tuned to an extent of delocalizing between the two dots. This forms the first project of this dissertation, which addresses the origin of the fine structure splitting in the exciton-biexciton cascade. Moreover, we also show how this fine structure can be tuned in the quantum dot molecule system with the application of electric field along the growth direction. This is demonstrated through high resolution polarization dependent photoluminescence spectroscopy on a single QDM, which was described in great detail

  7. Coulomb crystallization in classical and quantum systems

    Science.gov (United States)

    Bonitz, Michael

    2007-11-01

    Coulomb crystallization occurs in one-component plasmas when the average interaction energy exceeds the kinetic energy by about two orders of magnitude. A simple road to reach such strong coupling consists in using external confinement potentials the strength of which controls the density. This has been succsessfully realized with ions in traps and storage rings and also in dusty plasma. Recently a three-dimensional spherical confinement could be created [1] which allows to produce spherical dust crystals containing concentric shells. I will give an overview on our recent results for these ``Yukawa balls'' and compare them to experiments. The shell structure of these systems can be very well explained by using an isotropic statically screened pair interaction. Further, the thermodynamic properties of these systems, such as the radial density distribution are discussed based on an analytical theory [3]. I then will discuss Coulomb crystallization in trapped quantum systems, such as mesoscopic electron and electron hole plasmas in coupled layers [4,5]. These systems show a very rich correlation behavior, including liquid and solid like states and bound states (excitons, biexcitons) and their crystals. On the other hand, also collective quantum and spin effects are observed, including Bose-Einstein condensation and superfluidity of bound electron-hole pairs [4]. Finally, I consider Coulomb crystallization in two-component neutral plasmas in three dimensions. I discuss the necessary conditions for crystals of heavy charges to exist in the presence of a light component which typically is in the Fermi gas or liquid state. It can be shown that their exists a critical ratio of the masses of the species of the order of 80 [5] which is confirmed by Quantum Monte Carlo simulations [6]. Familiar examples are crystals of nuclei in the core of White dwarf stars, but the results also suggest the existence of other crystals, including proton or α-particle crystals in dense matter

  8. Fundamental studies of interfacial excited-state charge transfer in molecularly tethered semiconductor nanoassemblies

    Science.gov (United States)

    Youker, Diane Greer

    The research presented in this dissertation focuses on elucidating the parameters affecting dynamics and yield of electron transfer reactions in semiconducting nanoparticle assemblies through the use of time-resolved spectroscopy. In particular, the dissertation focuses on photoinduced electron injection in assemblies of CdSe, CdS, or PbS quantum dots covalently bound to either metal oxide films or each other through the use of bifunctional molecular linkers. Chapter 2 elucidates the influence of electronic coupling on excited-state electron transfer from CdS quantum dots to TiO2 nanoparticles via molecular linkers with phenylene bridges. We establish that the efficiency of electron injection from CdS quantum dots to TiO2 nanoparticle varies dramatically with electronic coupling, which can be controlled by tuning the properties of molecular linkers. Chapter 3 presents the role of excitation energy on interfacial electron transfer in tethered assemblies of CdSe quantum dots and TiO2 nanoparticles. Through this work, we determined that injection efficiency from band-edge states is independent of excitation energy. However, the efficiency of injection from trap-states decreases at lower-energy excitation. We attribute the decrease to a lower energy distribution of emissive trap-states from which injection is less efficient. Chapter 4 presents the observation of multiphasic electron injection dynamics from photoexcited PbS quantum dots to TiO2 nanoparticles. In this collaborative study with Dr. Masumoto from the University of Tsukuba we observed electron injection on multiple timescales. We determined that electron injection occurred in this system through two different mechanisms. The first involved injection from thermalized PbS excited states and the second through injection of hot electrons through Auger recombination of biexcitons that creates high lying excitonic states. Chapter 5 investigates charge transfer in covalently bound quantum dot assemblies. We utilize

  9. Process-Dependent Properties in Colloidally Synthesized “Giant” Core/Shell Nanocrystal Quantum Dots

    Energy Technology Data Exchange (ETDEWEB)

    Hollingsworth, Jennifer A. [Los Alamos National Laboratory; Ghosh, Yagnaseni [Los Alamos National Laboratory; Dennis, Allison M. [Los Alamos National Laboratory; Mangum, Benjamin D. [Los Alamos National Laboratory; Park, Young-Shin [Los Alamos National Laboratory; Kundu, Janardan [Los Alamos National Laboratory; Htoon, Han [Los Alamos National Laboratory

    2012-06-07

    Due to their characteristic bright and stable photoluminescence, semiconductor nanocrystal quantum dots (NQDs) have attracted much interest as efficient light emitters for applications from single-particle tracking to solid-state lighting. Despite their numerous enabling traits, however, NQD optical properties are frustratingly sensitive to their chemical environment, exhibit fluorescence intermittency ('blinking'), and are susceptible to Auger recombination, an efficient nonradiative decay process. Previously, we showed for the first time that colloidal CdSe/CdS core/shell nanocrystal quantum dots (NQDs) comprising ultrathick shells (number of shell monolayers, n, > 10) grown by protracted successive ionic layer adsorption and reaction (SILAR) leads to remarkable photostability and significantly suppressed blinking behavior as a function of increasing shell thickness. We have also shown that these so-called 'giant' NQDs (g-NQDs) afford nearly complete suppression of non-radiative Auger recombination, revealed in our studies as long biexciton lifetimes and efficient multiexciton emission. The unique behavior of this core/shell system prompted us to assess correlations between specific physicochemical properties - beyond shell thickness - and functionality. Here, we demonstrate the ability of particle shape/faceting, crystalline phase, and core size to determine ensemble and single-particle optical properties (quantum yield/brightness, blinking, radiative lifetimes). Significantly, we show how reaction process parameters (surface-stabilizing ligands, ligand:NQD ratio, choice of 'inert' solvent, and modifications to the SILAR method itself) can be tuned to modify these function-dictating NQD physical properties, ultimately leading to an optimized synthetic approach that results in the complete suppression of blinking. We find that the resulting 'guiding principles' can be applied to other NQD compositions, allowing us to

  10. 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.

  11. 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

  12. Proprietes optiques des heterostructures contraintes de type II Ga(x)In(1-x)P/InP

    Science.gov (United States)

    Chennouf, Abderrahim

    recombinaison des excitons localises dans une queue de bande generee par les fluctuations locales du potentiel. Nous avons reproduit les spectres de photoluminescence a basse temperature a l'aide d'un modele bien adapte tenant compte de ces fluctuations de potentiel. Nous avons egalement identifie une transition, qui apparai t sur le flanc basse energie de la raie associee a la recombinaison des excitons libres aux intensites d'excitation relativement fortes, que nous avons associee a la recombinaison de biexcitons. Nous avons montre que la largeur des barrieres joue un role particulierement important puisque dans le cas des puits quantiques multiples, les resultats obtenus sont differents. En effet, nous avons montre que la transition basse energie des spectres de photoluminescence de ces heterostructures est de nature intrinseque. L'analyse des resultats obtenus laisse supposer que cette transition pourrait etre associee a un condensat excitonique de type liquide electron-trou ou condensat de Bose, phenomene predit theoriquement dans les systemes de type II. Nous avons rejete cette hypothese principalement a cause de son apparition a basse intensite d'excitation. Une autre hypothese est de lui assigner la meme origine que dans le cas des super-reseaux, qui est la recombinaison des excitons localises dans une queue de bande. La valeur de l'energie de localisation estimee experimentalement reste toutefois encore a expliquer.

  13. 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

  14. Dynamic Processes

    Science.gov (United States)

    Klingshirn, C.

    . Phys. Lett. 92:211105, 2008). For this point, recall Figs. 6.16 and 6.33. Since the polarisation amplitude is gone in any case after the recombination process, there is an upper limit for T 2 given by T 2 ≤ 2 T1. The factor of two comes from the fact that T 2 describes the decay of an amplitude and T 1 the decay of a population, which is proportional to the amplitude squared. Sometimes T 2 is subdivided in a term due to recombination described by T 1 and another called 'pure dephasing' called T 2 ∗ with the relation 1 / T 2 = 1 / 2 T 1 + 1 / T2 ∗. The quantity T 2 ∗ can considerably exceed 2 T 1. In the part on relaxation processes that is on processes contributing to T 3, we give also examples for the capture of excitons into bound, localized, or deep states. For more details on dynamics in semiconductors in general see for example, the (text-) books [Klingshirn, Semiconductor Optics, 3rd edn. (Springer, Berlin, 2006); Haug and Koch, Quantum Theory of the Optical and Electronic Properties of Semiconductors, 4th edn. (World Scientific, Singapore, 2004); Haug and Jauho, Quantum Kinetics in Transport and Optics of Semiconductors, Springer Series in Solid State Sciences vol. 123 (Springer, Berlin, 1996); J. Shah, Ultrafast Spectroscopy of Semiconductors and of Semiconductor Nanostructures, Springer Series in Solid State Sciences vol. 115 (Springer, Berlin, 1996); Schafer and Wegener, Semiconductor Optics and Transport Phenomena (Springer, Berlin, 2002)]. We present selected data for free, bound and localized excitons, biexcitons and electron-hole pairs in an EHP and examples for bulk materials, epilayers, quantum wells, nano rods and nano crystals with the restriction that - to the knowledge of the author - data are not available for all these systems, density ranges and temperatures. Therefore, we subdivide the topic below only according to the three time constants T 2, T 3 and T 1.