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. Dephasing of Quasi-2D Biexcitons

    DEFF Research Database (Denmark)

    Langbein, Wolfgang; Hvam, Jørn Märcher

    1999-01-01

    The temperature dependent dephasing of the biexcitonic resonance in a homogeneously broadened single quantum well is studied by transient four-wave mixing. Using cross-linear excitation polarization, we deduce the biexcitonic and excitonic dephasing rates from the delay-time dependence of the FWM...... that biexcitonic dephasing at high temperature is connected to thermal dissociation, and that the intrinsic low-temperature dephasing time of biexcitons can be longer than that of excitons....

  3. 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...

  4. 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...

  5. Binding of Quasi-Two-Dimensional Biexcitons

    DEFF Research Database (Denmark)

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

    1996-01-01

    Biexciton binding in GaAs quantum wells has been investigated for a range of well thicknesses (80-160 Angstrom) with spectrally resolved photoluminescence and transient degenerate four-wave mixing. Both light and heavy hole biexcitons are observed. The ratio of the binding energy of the heavy hole...

  6. 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 ...

  7. 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...... selection rules. The coherent dynamics of the FWM response and the observed FWM intensity ratio between the XXh and XXm biexciton-induced nonlinear signals are in agreement with the solution of an extended optical Bloch equation....

  8. Binding-energy distribution and dephasing of localized biexcitons

    DEFF Research Database (Denmark)

    Langbein, Wolfgang Werner; Hvam, Jørn Märcher; Umlauff, M.;

    1997-01-01

    We report on the binding energy and dephasing of localized biexciton states in narrow ZnSe multiple quantum wells. The measured binding-energy distribution of the localized biexcitons shows a width of 2.2 meV centered at 8.5 meV, and is fairly independent of the exciton localization energy. In four......-wave mixing, the biexciton photon echo decays fast and nonexponentially. This behavior results from the inhomogeneous broadening of the biexciton binding energy, as we show by a comparison with an analytical model calculation. The fast decay is thus not related to a fast microscopic biexciton dephasing....

  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. Detection of a biexciton in semiconducting carbon nanotubes using nonlinear optical spectroscopy.

    Science.gov (United States)

    Colombier, L; Selles, J; Rousseau, E; Lauret, J S; Vialla, F; Voisin, C; Cassabois, G

    2012-11-01

    We report the observation of the biexciton in semiconducting single-wall carbon nanotubes by means of nonlinear optical spectroscopy. Our measurements reveal the universal asymmetric line shape of the Fano resonance intrinsic to the biexciton transition. For nanotubes of the (9,7) chirality, we find a biexciton binding energy of 106 meV. From the calculation of the χ((3)) nonlinear response, we provide a quantitative interpretation of our measurements, leading to an estimation of the characteristic Fano factor q of 7 ± 3. This value allows us to extract the first experimental information on the biexciton stability and we obtain a biexciton annihilation rate comparable to the exciton-exciton annihilation one. PMID:23215424

  13. 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....

  14. Biexciton emission from single isoelectronic traps formed by nitrogen-nitrogen pairs in GaAs

    Energy Technology Data Exchange (ETDEWEB)

    Takamiya, Kengo; Fukushima, Toshiyuki; Yagi, Shuhei; Hijikata, Yasuto; Yaguchi, Hiroyuki [Graduate School of Science and Engineering, Saitama University, 255 Shimo-Okubo, Sakura-ku , Saitama 338-8570 (Japan); Mochizuki, Toshimitsu; Yoshita, Masahiro; Akiyama, Hidefumi [Institute for Solid State Physics, The University of Tokyo, 5-1-5 Kashiwanoha, Kashiwa, Chiba 277-8581 (Japan); Kuboya, Shigeyuki; Onabe, Kentaro [Department of Advanced Materials Science, The University of Tokyo, 5-1-5 Kashiwanoha, Kashiwa, Chiba 277-8581 (Japan); Katayama, Ryuji [Institute for Materials Research, Tohoku University, 2-1-1 Katahira, Aoba-ku, Sendai 980-8577 (Japan)

    2013-12-04

    We have studied photoluminescence (PL) from individual isoelectronic traps formed by nitrogen-nitrogen (NN) pairs in GaAs. Sharp emission lines due to exciton and biexciton were observed from individual isoelectronic traps in nitrogen atomic-layer doped (ALD) GaAs. The binding energy of biexciton bound to individual isoelectronic traps was approximately 8 meV. Both the exciton and biexciton luminescence lines show completely random polarization and no fine-structure splitting. These results are desirable to the application to the quantum cryptography used in the field of quantum information technology.

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

    Energy Technology Data Exchange (ETDEWEB)

    Gotoh, Hideki, E-mail: gotoh.hideki@lab.ntt.co.jp; Sanada, Haruki; Yamaguchi, Hiroshi; Sogawa, Tetsuomi [NTT Basic Research Laboratories, NTT Corporation, 3-1 Morinosato-Wakamiya, Atsugi-shi, Kanagawa 243-0198 (Japan)

    2014-10-15

    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.

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

    International Nuclear Information System (INIS)

    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

  17. Biexcitonic photocurrent induced by two-photon process at a telecommunication band

    International Nuclear Information System (INIS)

    We report on photocurrent (PC) measurements of biexciton in a single self-assembled InAs quantum dot (QD) at a telecommunication wavelength of 1.3μm. We use shadow mask technique on an n-i Schottky photodiode structure with QDs to excite a single QD resonantly. Coherent pulse excitation is realized in two types of setups utilizing (i) an optical parametric oscillator and (ii) a stable semiconductor laser diode. In both setups we observe the biexcitonic PC peaks induced by a coherent two-photon process. Especially in the latter setups, the narrower pulse linewidth in energy provides a clearer biexcitonic PC peak because of reduced unwanted excitation. We estimate the binding energy ΔEB of our telecom-band biexciton to be 0.9 meV from the splitting between excitonic and biexcitonic resonances. The result suggests our telecom-band exciton-biexciton system is a good candidate for the building block of fiber-based controlled-rotation quantum logic operation. (copyright 2009 WILEY-VCH Verlag GmbH and Co. KGaA, Weinheim) (orig.)

  18. Efficient Biexciton Interaction in Perovskite Quantum Dots Under Weak and Strong Confinement.

    Science.gov (United States)

    Castañeda, Juan A; Nagamine, Gabriel; Yassitepe, Emre; Bonato, Luiz G; Voznyy, Oleksandr; Hoogland, Sjoerd; Nogueira, Ana F; Sargent, Edward H; Cruz, Carlos H Brito; Padilha, Lazaro A

    2016-09-27

    Cesium lead halide perovskite quantum dots (PQDs) have emerged as a promising new platform for lighting applications. However, to date, light emitting diodes (LED) based on these materials exhibit limited efficiencies. One hypothesized limiting factor is fast nonradiative multiexciton Auger recombination. Using ultrafast spectroscopic techniques, we investigate multicarrier interaction and recombination mechanisms in cesium lead halide PQDs. By mapping the dependence of the biexciton Auger lifetime and the biexciton binding energy on nanomaterial size and composition, we find unusually strong Coulomb interactions among multiexcitons in PQDs. This results in weakly emissive biexcitons and trions, and accounts for low light emission efficiencies. We observe that, for strong confinement, the biexciton lifetime depends linearly on the PQD volume. This dependence becomes sublinear in the weak confinement regime as the PQD size increases beyond the Bohr radius. We demonstrate that Auger recombination is faster in PQDs compared to CdSe nanoparticles having the same volume, suggesting a stronger Coulombic interaction in the PQDs. We confirm this by demonstrating an increased biexciton binding energy, which reaches a maximum of about 100 meV, fully three times larger than in CdSe quantum dots. The biexciton shift can lead to low-threshold optical gain in these materials. These findings also suggest that materials engineering to reduce Coulombic interaction in cesium lead halide PQDs could improve prospects for high efficiency optoelectronic devices. Core-shell structures, in particular type-II nanostructures, which are known to reduce the bandedge Coulomb interaction in CdSe/CdS, could beneficially be applied to PQDs with the goal of increasing their potential in lighting applications. PMID:27574807

  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. 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.

  1. Excitons, Biexcitons and Dephasing in GaAs T-shaped quantum wires

    DEFF Research Database (Denmark)

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

    2000-01-01

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

  2. 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...

  3. 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

  4. Impact of biexcitons on the relaxation mechanisms of polaritons in III-nitride based multiple quantum well microcavities

    OpenAIRE

    Corfdir, P.; Levrat, J.; Rossbach, G; Butte, R.; Feltin, E.; Carlin, J.-F.; Christmann, G.; Lefebvre, P.; Ganiere, J. -D.; Grandjean, N.; Deveaud-Pledran, B.

    2012-01-01

    We report on the direct observation of biexcitons in a III-nitride based multiple quantum well microcavity operating in the strong light-matter coupling regime by means of nonresonant continuous wave and time-resolved photoluminescence at low temperature. First, the biexciton dynamics is investigated for the bare active medium (multiple quantum wells alone) evidencing localization on potential fluctuations due to alloy disorder and thermalization between both localized and free excitonic and ...

  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

    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.

  7. Phase control of optical bistability based biexciton coherence in a quantum dot nanostructure

    International Nuclear Information System (INIS)

    In this paper, phase control of optical bistability and multistability based biexciton coherence is investigated in GaAs/AlxGal−xAs semiconductor structure with 15 periods of 17.5 nm GaAs layer and 25-nm Al0.3Ga0.7 barriers, grown by molecular beam epitaxy, four-level quantum dot nanostructure. By two control fields that couple to a biexciton state, the destructive interference can be obtained. In this case, the optical bistability (OB) and optical multistability (OM) can be dramatically altered with adjusting the absorption of two weak probe and signal fields. The results show that the OB and OM behavior of the medium are different for two-weak-pulsed probe fields due to effect of exciton spin relaxation, intensity of coupling fields and relative phase between applied fields.

  8. Exciton-exciton annihilation and biexciton stimulated emission in graphene nanoribbons

    Science.gov (United States)

    Soavi, Giancarlo; Dal Conte, Stefano; Manzoni, Cristian; Viola, Daniele; Narita, Akimitsu; Hu, Yunbin; Feng, Xinliang; Hohenester, Ulrich; Molinari, Elisa; Prezzi, Deborah; Müllen, Klaus; Cerullo, Giulio

    2016-03-01

    Graphene nanoribbons display extraordinary optical properties due to one-dimensional quantum-confinement, such as width-dependent bandgap and strong electron-hole interactions, responsible for the formation of excitons with extremely high binding energies. Here we use femtosecond transient absorption spectroscopy to explore the ultrafast optical properties of ultranarrow, structurally well-defined graphene nanoribbons as a function of the excitation fluence, and the impact of enhanced Coulomb interaction on their excited states dynamics. We show that in the high-excitation regime biexcitons are formed by nonlinear exciton-exciton annihilation, and that they radiatively recombine via stimulated emission. We obtain a biexciton binding energy of ~250 meV, in very good agreement with theoretical results from quantum Monte Carlo simulations. These observations pave the way for the application of graphene nanoribbons in photonics and optoelectronics.

  9. 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.

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

    Science.gov (United States)

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

    2002-05-01

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

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

    DEFF Research Database (Denmark)

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

    1999-01-01

    The coherent dynamics of both exciton and biexciton resonances have been investigated in In0.18Ga0.82As/GaAs single quantum wells with thicknesses ranging from 1 to 4 nm, using time-integrated and spectrally-resolved transient four-wave mixing. From the temperature dependence of the exciton...... dephasing time we obtain linewidth broadening coefficients for acoustic and optical phonons. Biexciton binding energies are extracted from the four-wave mixing response in the spectral domain, and are found to be between 1.5 and 2.6 meV. The temperature dempendence of the dephasing of the exciton...

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

    Science.gov (United States)

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

    1999-10-01

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

  13. 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

    -space filling nonlinearity, excitation-induced dephasing (EID) and biexciton formation (BIF) are important. EID leads to a strong dependence of the signal on the angle between the linear input polarizations. We find that EID persists in inhomogeneous systems, showing that the mutual density-dependent dephasing......-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...

  14. Efficiency of the coherent biexciton admixture mechanism for multiple exciton generation in InAs nanocrystals

    International Nuclear Information System (INIS)

    We study the coherent mixing between two-particle (single exciton) and four-particle (biexciton) states of a semiconductor nanocrystal resulting from the Coulomb coupling between states with different numbers of electron-hole pairs. Using a simple model of the nanocrystal wave functions and an envelope function approach, we estimate the efficiency of the multiple exciton generation (MEG) process resulting from such coherent admixture mechanism, including all the relevant states in a very broad energy interval. We show that in a typical ensemble of nanocrystals with an average radius of 3nm, the onset of the MEG process appears about 1 eV above the lower edge of the biexciton density of states. This is due to the angular momentum conservation that imposes selection rules and limits the available MEG pathways, thus taking over the role of momentum conservation that hinders this process in bulk. The efficiency of the MEG process reaches 50% for photon energies around 5 eV. The MEG onset shifts to lower energies and therefore the efficiency increases in a certain energy range as the radius grows. The energy dependence of the MEG efficiency differs considerably between ensembles with small and large inhomogeneity of nanocrystal sizes. (paper)

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2015-08-15

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

  16. Phonon impacts on entangled photon pair generation from the biexciton cascade in a quantum dot: phonon coherent state representation

    International Nuclear Information System (INIS)

    A full quantum microscopic theory is developed to analyze a biexciton radiative cascade coupled to bulk acoustic phonons in a quantum dot. By considering the phonon sub-system in coherent state representation a new approach is proposed for investigating the phonon effects. Via this approach it is possible to obtain an exact analytical result for the phonon kernel in this system. This approach is introduced in the context of an example: the process of generating polarization-entangled photon pairs from the biexciton cascade in a quantum dot. We calculate the exact density matrix (using quantum state tomography) of photons and their concurrence. We show that the exchange interaction and temperature have remarkable effects on the degree of entanglement of the emitted photons. The approach introduced provides an exact analytical result for finite discrete electron states interacting with phonons. (paper)

  17. An experimental and theoretical mechanistic study of biexciton quantum yield enhancement in single quantum dots near gold nanoparticles

    Science.gov (United States)

    Dey, Swayandipta; Zhou, Yadong; Tian, Xiangdong; Jenkins, Julie A.; Chen, Ou; Zou, Shengli; Zhao, Jing

    2015-04-01

    In this work, we systematically investigated the plasmonic effect on blinking, photon antibunching behavior and biexciton emission of single CdSe/CdS core/shell quantum dots (QDs) near gold nanoparticles (NPs) with a silica shell (Au@SiO2). In order to obtain a strong interaction between the plasmons and excitons, the Au@SiO2 NPs and CdSe/CdS QDs of appropriate sizes were chosen so that the plasmon resonance overlaps with the absorption and emission of the QDs. We observed that in the regime of a low excitation power, the photon antibunching and blinking properties of single QDs were modified significantly when the QDs were on the Au@SiO2 substrates compared to those on glass. Most significantly, second-order photon intensity correlation data show that the presence of plasmons increases the ratio of the biexciton quantum yield over the exciton quantum yield (QYBX/QYX). An electrodynamics model was developed to quantify the effect of plasmons on the lifetime, quantum yield, and emission intensity of the biexcitons for the QDs. Good agreement was obtained between the experimentally measured and calculated changes in QYBX/QYX due to Au@SiO2 NPs, showing the validity of the developed model. The theoretical studies also indicated that the relative position of the QDs to the Au NPs and the orientation of the electric field are important factors that regulate the emission properties of the excitons and biexcitons of QDs. The study suggests that the multiexciton emission efficiency in QD systems can be manipulated by employing properly designed plasmonic structures.In this work, we systematically investigated the plasmonic effect on blinking, photon antibunching behavior and biexciton emission of single CdSe/CdS core/shell quantum dots (QDs) near gold nanoparticles (NPs) with a silica shell (Au@SiO2). In order to obtain a strong interaction between the plasmons and excitons, the Au@SiO2 NPs and CdSe/CdS QDs of appropriate sizes were chosen so that the plasmon resonance

  18. 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.

  19. Quantitative characterization of highly efficient correlated photon-pair source using biexciton resonance.

    Science.gov (United States)

    Yamamoto, Yasuo; Oohata, Goro; Mizoguchi, Kohji

    2016-03-21

    A high efficiency method for the generation of correlated photon pairs accompanied by reliable means to characterize the efficiency of that process is needed in the study of entangled states, which have important potential applications in quantum information and quantum communication. In this study, we report the first characterization of the efficiency of generation of correlated photon pairs emitted from a CuCl single crystal using the biexciton-resonance hyper-parametric scattering (RHPS) method which is the highly efficient method of generation of correlated photon pairs. In order to characterize the generation efficiency and signal-to-noise ratio of correlated photon pairs using this method, we investigated the pump power dependence on the photon counting rate and coincidence counting rate under resonant excitation. The pump power dependence shows that the power characteristic of the photon counting rates changes from linear to quadratic dependence of the pump power. This behavior represents a superposition of contributions from correlated photon pairs and non-correlated photons. The analysis of the pump power dependence shows that one photon-pair is produced by a pump pulse with 2 x 106 photons. Moreover, the generation efficiency of this method obtained by calculating the number of generated photon pairs per pump power is comparable to that of several methods based on the χ(3) parametric process. PMID:27136797

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

    DEFF Research Database (Denmark)

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

    1999-01-01

    The optical properties of CdSe nanostructures grown by migration-enhanced epitaxy of CdSe on ZnSe are studied by time-, energy-, and temperature-dependent photoluminescence and excitation spectroscopy, as well as by polarization-dependent four-wave mixing and two-photon absorption experiments....... The nanostructures consist of a coherently strained Zn1-xCdxSe/ZnSe quantum well with embedded islands of higher Cd content with sizes of a few nanometer due to strain-induced CdSe accumulation. The local increase in CdSe concentration results in a strong localization of the excitonic wave function, in an increase...... in radiative lifetime, and a decrease of the dephasing rate. Local LO-phonon modes caused by the strong modulation of the Cd concentration profile are found in phonon-assisted relaxation processes. Confined biexcitons with large binding energies between 20 and 24 meV are observed, indicating the important role...

  1. Ultrafast Supercontinuum Spectroscopy of Carrier Multiplication and Biexcitonic Effects in Excited States of PbS Quantum Dots

    Energy Technology Data Exchange (ETDEWEB)

    Sfeir M. Y.; Gesuele, F.; Koh, W.-K.; Murray, C.B.; Heinz, T.F.; Wong, C.W.

    2012-06-01

    We examine the population dynamics of multiple excitons in PbS quantum dots using spectrally resolved ultrafast supercontinuum transient absorption (SC-TA) measurements. We simultaneously probe the first three excitonic transitions. The transient spectra show the presence of bleaching of absorption for the 1S{sub h}-1S{sub e} transition, as well as transients associated with the 1P{sub h}-1P{sub e} transition. We examine signatures of carrier multiplication (multiple excitons arising from a single absorbed photon) from analysis of the bleaching features in the limit of low absorbed photon numbers (biexciton population is red shifted with respect to the single exciton feature, which is in accordance with a positive binding energy for the biexciton.

  2. On the possibility of the biexciton semiconductor state excitence in the intermediate valence system of the SmB6 and golden SmS types

    International Nuclear Information System (INIS)

    A possibility of biexciton semiconductor state existence in the intermediate valence systems of the SmB6 and ''gold'' SmS types is shown. It leads to nonmetallic behaviour. A model, describing f-c interactions with regard to Coulomb repulsion of f-holes at different units, promoting to their ordering into a Wigner crystal, is considered

  3. 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.

  4. Laser induced magneto-Raman optical gain of an exciton and a biexciton in a CdTe/ZnTe quantum dot

    Science.gov (United States)

    Sujanah, P.; John Peter, A.; Lee, Chang Woo

    2016-06-01

    Magnetic field and laser field amplitude dependent electronic and optical properties of exciton and biexciton in a CdTe/ZnTe quantum dot nanostructure are brought out taking into account the spatial confinement effect. Binding energies of exciton and biexciton as functions of laser field amplitude and magnetic field strength are computed in a CdTe/ZnTe quantum dot for the constant dot radius 30 Å. Oscillator strength, resonant absorption coefficients and resonant optical Raman intensity of the exciton and biexciton as a function of laser field amplitude are obtained in the presence of magnetic field strength in a CdTe/ZnTe quantum dot. The laser field induced magneto-Raman gain is studied for a constant dot radii. The Coulomb interaction energy which is involved in Hartree potential is obtained numerically. The result shows that the applications of magnetic field strength and the laser field amplitude alter the electronic and optical properties considerably in the CdTe/ZnTe quantum dot.

  5. Photon echo studies of biexcitons and coherences in colloidal CdSe quantum dots

    Science.gov (United States)

    Colonna, Anne E.; Yang, Xiujuan; Scholes, Gregory D.

    2005-04-01

    The cover picture shows the size-dependent photoluminescence from CdSe colloidal quantum dots that were investigated in the work [1]. Ultrafast photon echo experiments were undertaken in conjunction with simulations based on a realistic many-body theory, shown in the picture, to ascertain the significance of many-body contributions to the third-order nonlinear response.The first author Anne E. Colonna undertook this research during a summer internship in the Department of Chemistry, University of Toronto. She is currently pursuing graduate studies at École Polytechnique, Saclay, in the Laboratoire d'Optique et Biosciences.The author Gregory D. Scholes is an Assistant Professor in the Department of Chemistry, University of Toronto. His research interests include synthesis and shape control of quantum dots, as well as the application of ultrafast laser spectroscopy to investigate the electronic structure of inorganic and organic semiconductors.

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

    DEFF Research Database (Denmark)

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

    1999-01-01

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

  7. 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...

  8. Multi-excitonic effects on optical spectra of semiconducting carbon nanotubes

    Energy Technology Data Exchange (ETDEWEB)

    Watanabe, Kouta; Asano, Kenichi; Ogawa, Tetsuo, E-mail: watanabe@acty.phys.sci.osaka-u.ac.j [Department of Physics, Osaka University, 1-1 Machikaneyama, Toyonaka, Osaka 560-0043 (Japan)

    2009-02-01

    We calculated the wavefunction and the binding energy of the biexciton in semiconducting carbon nanotubes and studied the spectral weights of the photoluminescence spectra and the biexciton contribution to the two-photon absorption spectra. The wavefunction and the binding energy are calculated by means of the the Lanczos method.

  9. Multiparticle states and the factors that complicate an experimental observation of the quantum coherence in the exciton gas of SiGe/Si quantum wells

    Energy Technology Data Exchange (ETDEWEB)

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

    2015-12-15

    The measured stationary and time-resolved photoluminescence is used to study the properties of the exciton gas in a second-order 5-nm-thick Si{sub 0.905}Ge{sub 0.095}/Si quantum well. It is shown that, despite the presence of an electron barrier in the Si{sub 0.905}Ge{sub 0.095} layer, a spatially indirect biexciton is the most favorable energy state of the electron–hole system at low temperatures. This biexciton is characterized by a lifetime of 1100 ns and a binding energy of 2.0–2.5 meV and consists of two holes localized in the SiGe layer and two electrons mainly localized in silicon. The formation of biexcitons is shown to cause low-temperature (5 K) luminescence spectra over a wide excitation density range and to suppress the formation of an exciton gas, in which quantum statistics effects are significant. The Bose statistics can only be experimentally observed for a biexciton gas at a temperature of 1 K or below because of the high degree of degeneracy of biexciton states (28) and a comparatively large effective mass (about 1.3m{sub e}). The heat energy at such temperatures is much lower than the measured energy of localization at potential fluctuations (about 1 meV). This feature leads to biexciton localization and fundamentally limits the possibility of observation of quantum coherence in the biexciton gas.

  10. 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.

  11. 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.

  12. Influence of the Dark Exciton State on the Optical and Quantum Optical Properties of Single Quantum Dots

    Science.gov (United States)

    Reischle, M.; Beirne, G. J.; Roßbach, R.; Jetter, M.; Michler, P.

    2008-10-01

    The dark exciton state strongly affects the optical and quantum optical properties of flat InP/GaInP quantum dots. The exciton intensity drops sharply compared to the biexciton with rising pulsed laser excitation power while the opposite is true with temperature. Also, the decay rate is faster for the exciton than the biexciton and the dark-to-bright state spin flip is enhanced with temperature. Furthermore, long-lived dark state related memory effects are observed in second-order cross-correlation measurements between the exciton and biexciton and have been simulated using a rate-equation model.

  13. Binding energies of exciton complexes in transition metal dichalcogenide monolayers and effect of dielectric environment

    Science.gov (United States)

    Kylänpää, Ilkka; Komsa, Hannu-Pekka

    2015-11-01

    Excitons, trions, biexcitons, and exciton-trion complexes in two-dimensional transition metal dichalcogenide sheets of MoS2, MoSe2, MoTe2, WS2, and WSe2 are studied by means of density functional theory and path-integral Monte Carlo method in order to accurately account for the particle-particle correlations. In addition, the effect of dielectric environment on the properties of these exciton complexes is studied by modifying the effective interaction potential between particles. Calculated exciton and trion binding energies are consistent with previous experimental and computational studies, and larger systems such as biexciton and exciton-trion complex are found highly stable. Binding energies of biexcitons are similar to or higher than those of trions, but the binding energy of the trion depends significantly stronger on the dielectric environment than that of biexciton. Therefore, as a function of an increasing dielectric constant of the environment the exciton-trion complex "dissociates" to a biexciton rather than to an exciton and a trion.

  14. 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.

  15. 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.

  16. Coherent dynamics in semiconductors

    DEFF Research Database (Denmark)

    Hvam, Jørn Märcher

    1998-01-01

    enhanced in quantum confined lower-dimensional systems, where exciton and biexciton effects dominate the spectra even at room temperature. The coherent dynamics of excitons are at modest densities well described by the optical Bloch equations and a number of the dynamical effects known from atomic...... 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...

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

    DEFF Research Database (Denmark)

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

    1999-01-01

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

  18. Configuration space method for calculating binding energies of exciton complexes in quasi-1D/2D semiconductors

    Science.gov (United States)

    Bondarev, Igor

    A configuration space method, pioneered by Landau and Herring in studies of molecular binding and magnetism, is developed to obtain universal asymptotic relations for lowest energy exciton complexes (trion, biexciton) in confined semiconductor nanostructures such as nanowires and nanotubes, as well as coupled quantum wells. Trions are shown to be more stable (have greater binding energy) than biexcitons in strongly confined quasi-1D structures with small reduced electron-hole masses. Biexcitons are more stable in less confined quasi-1D structures with large reduced electron-hole masses. The theory predicts a crossover behavior, whereby trions become less stable than biexcitons as the transverse size of the quasi-1D nanostructure increases, which might be observed on semiconducting carbon nanotubes of increasing diameters. This method is also efficient in calculating binding energies for trion-type electron-hole complexes formed by indirect excitons in double coupled quantum wells, quasi-2D nanostructures that show new interesting electroabsorption/refraction phenomena. Supported by DOE-DE-SC0007117.

  19. 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.

  20. Metal-organic vapor-phase epitaxy-grown ultra-low density InGaAs/GaAs quantum dots exhibiting cascaded single-photon emission at 1.3 μm

    Energy Technology Data Exchange (ETDEWEB)

    Paul, Matthias, E-mail: m.paul@ihfg.uni-stuttgart.de; Kettler, Jan; Zeuner, Katharina; Clausen, Caterina; Jetter, Michael; Michler, Peter [Institut für Halbleiteroptik und Funktionelle Grenzflächen, University of Stuttgart, Allmandring 3, 70569 Stuttgart (Germany)

    2015-03-23

    By metal-organic vapor-phase epitaxy, we have fabricated InGaAs quantum dots on GaAs substrate with an ultra-low lateral density (<10{sup 7} cm{sup −2}). The photoluminescence emission from the quantum dots is shifted to the telecom O-band at 1.31 μm by an InGaAs strain reducing layer. In time-resolved measurements, we find fast decay times for exciton (∼600 ps) and biexciton (∼300 ps). We demonstrate triggered single-photon emission (g{sup (2)}(0)=0.08) as well as cascaded emission from the biexciton decay. Our results suggest that these quantum dots can compete with their counterparts grown by state-of-the-art molecular beam epitaxy.

  1. 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.

  2. 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.

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

    OpenAIRE

    Breddermann, Dominik; Heinze, Dirk; 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 frequen...

  4. 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.

  5. Effects of photo-neutralization on the emission properties of quantum dots

    Science.gov (United States)

    Huber, Tobias; Predojević, Ana; Solomon, Glenn S.; Weihs, Gregor

    2016-09-01

    In this paper we investigate the coherence properties of a quantum dot under two-photon resonant excitation in combination with an additional photo-neutralization laser. The photo-neutralization increases the efficiency of the excitation process and thus, the brightness of the source, by a factor of approximately 1.5 for biexciton-exciton pairs. This enhancement does not degrade the relevant coherences in the system; neither the single photon coherence time, nor the coherence of the excitation process.

  6. A quantum dot single-photon source with on-the-fly all-optical polarization control and timed emission

    OpenAIRE

    Heinze, Dirk; Breddermann, Dominik; Zrenner, Artur; Schumacher, Stefan

    2015-01-01

    Sources of single photons are key elements in the study of basic quantum optical concepts and applications in quantum information science. Among the different sources available, semiconductor quantum dots excel with their straight forward integrability in semiconductor based on-chip solutions and the potential that photon emission can be triggered on demand. Usually, the photon emission event is part of a cascaded biexciton-exciton emission scheme. Important properties of the emitted photon s...

  7. 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.

  8. Génération électrique de lumière intriquée destinée au transfert optique d'information quantique

    OpenAIRE

    Nilsson, Jonas

    2013-01-01

    Semiconductor quantum dots offer an attractive route towards efficient and high-quality photon sources for optical quantum information applications, with potential for miniaturization and integration on chip. Here, entangled photon pairs are generated in the biexcitonic radiative cascade resulting from electrical excitation of InAs self-assembled quantum dots placed in a p-i-n diode. In a first set of experiments the non-classical polarisation correlations and the ability to interfere the pho...

  9. Binding energies of exciton complexes in transition metal dichalcogenides and effect of dielectric environment

    OpenAIRE

    Kylänpää, Ilkka; Komsa, Hannu-Pekka

    2015-01-01

    Excitons, trions, biexcitons, and exciton-trion complexes in two-dimensional transition metal dichalcogenide sheets of MoS$_2$, MoSe$_2$, MoTe$_2$, WS$_2$ and WSe$_2$ are studied by means of density functional theory and path integral Monte Carlo method in order to accurately account for the particle-particle correlations. In addition, the effect of dielectric environment on the properties of these exciton complexes is studied by modifying the effective interaction potential between particles...

  10. Dominant factors limiting the optical gain in layered two-dimensional halide perovskite thin films.

    Science.gov (United States)

    Chong, Wee Kiang; Thirumal, Krishnamoorthy; Giovanni, David; Goh, Teck Wee; Liu, Xinfeng; Mathews, Nripan; Mhaisalkar, Subodh; Sum, Tze Chien

    2016-05-25

    Semiconductors are ubiquitous gain media for coherent light sources. Solution-processed three-dimensional (3D) halide perovskites (e.g., CH3NH3PbI3) with their outstanding room temperature optical gain properties are the latest members of this family. Their two-dimensional (2D) layered perovskite counterparts with natural multiple quantum well structures exhibit strong light-matter interactions and intense excitonic luminescence. However, despite such promising traits, there have been no reports on room temperature optical gain in 2D layered perovskites. Herein, we reveal the challenges towards achieving amplified spontaneous emission (ASE) in the archetypal (C6H5C2H4NH3)2PbI4 (or PEPI) system. Temperature-dependent transient spectroscopy uncovers the dominant free exciton trapping and bound biexciton formation pathways that compete effectively with biexcitonic gain. Phenomenological rate equation modeling predicts a large biexciton ASE threshold of ∼1.4 mJ cm(-2), which is beyond the damage threshold of these materials. Importantly, these findings would rationalize the difficulties in achieving optical gain in 2D perovskites and provide new insights and suggestions for overcoming these challenges.

  11. 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.

  12. Collective aspects of singlet fission in molecular crystals

    International Nuclear Information System (INIS)

    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

  13. Dominant factors limiting the optical gain in layered two-dimensional halide perovskite thin films.

    Science.gov (United States)

    Chong, Wee Kiang; Thirumal, Krishnamoorthy; Giovanni, David; Goh, Teck Wee; Liu, Xinfeng; Mathews, Nripan; Mhaisalkar, Subodh; Sum, Tze Chien

    2016-05-25

    Semiconductors are ubiquitous gain media for coherent light sources. Solution-processed three-dimensional (3D) halide perovskites (e.g., CH3NH3PbI3) with their outstanding room temperature optical gain properties are the latest members of this family. Their two-dimensional (2D) layered perovskite counterparts with natural multiple quantum well structures exhibit strong light-matter interactions and intense excitonic luminescence. However, despite such promising traits, there have been no reports on room temperature optical gain in 2D layered perovskites. Herein, we reveal the challenges towards achieving amplified spontaneous emission (ASE) in the archetypal (C6H5C2H4NH3)2PbI4 (or PEPI) system. Temperature-dependent transient spectroscopy uncovers the dominant free exciton trapping and bound biexciton formation pathways that compete effectively with biexcitonic gain. Phenomenological rate equation modeling predicts a large biexciton ASE threshold of ∼1.4 mJ cm(-2), which is beyond the damage threshold of these materials. Importantly, these findings would rationalize the difficulties in achieving optical gain in 2D perovskites and provide new insights and suggestions for overcoming these challenges. PMID:27184073

  14. 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.

  15. 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

  16. 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.

  17. 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

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

    DEFF Research Database (Denmark)

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

    1998-01-01

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

  19. 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.

  20. 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.

  1. Entangled Photon Pairs Produced by a Quantum Dot Strongly Coupled to a Microcavity

    Science.gov (United States)

    Johne, R.; Gippius, N. A.; Pavlovic, G.; Solnyshkov, D. D.; Shelykh, I. A.; Malpuech, G.

    2008-06-01

    We show theoretically that entangled photon pairs can be produced on demand through the biexciton decay of a quantum dot strongly coupled to the modes of a photonic crystal. The strong coupling allows us to tune the energy of the mixed exciton-photon (polariton) eigenmodes and to overcome the natural splitting existing between the exciton states coupled with different linear polarizations of light. Polariton states are moreover well protected against dephasing due to their lifetime of ten to a hundred times shorter than that of a bare exciton. Our analysis shows that the scheme proposed is achievable with the present technology.

  2. Electrically driven single photon emission from a CdSe/ZnSSe single quantum dot at 200 K

    Energy Technology Data Exchange (ETDEWEB)

    Quitsch, Wolf; Kümmell, Tilmar; Bacher, Gerd [Werkstoffe der Elektrotechnik and CENIDE, Universität Duisburg-Essen, Bismarckstraße 81, 47057 Duisburg (Germany); Gust, Arne; Kruse, Carsten; Hommel, Detlef [Institut für Festkörperphysik, Universität Bremen, Otto-Hahn-Allee 1, 28334 Bremen (Germany)

    2014-09-01

    High temperature operation of an electrically driven single photon emitter based on a single epitaxial quantum dot is reported. CdSe/ZnSSe/MgS quantum dots are embedded into a p-i-n diode architecture providing almost background free excitonic and biexcitonic electroluminescence from individual quantum dots through apertures in the top contacts. Clear antibunching with g{sup 2}(τ = 0) = 0.28 ± 0.20 can be tracked up to T = 200 K, representing the highest temperature for electrically triggered single photon emission from a single quantum dot device.

  3. 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.

  4. Quantum Light Emission of Two Lateral Tunnel-Coupled (In,Ga)As/GaAs Quantum Dots Controlled by a Tunable Static Electric Field

    Science.gov (United States)

    Beirne, G. J.; Hermannstädter, C.; Wang, L.; Rastelli, A.; Schmidt, O. G.; Michler, P.

    2006-04-01

    Lateral quantum coupling between two self-assembled (In,Ga)As quantum dots has been observed. Photon statistics measurements between the various excitonic and biexcitonic transitions of these lateral quantum dot molecules display strong antibunching confirming the presence of coupling. Furthermore, we observe an anomalous exciton Stark shift with respect to static electric field. A simple model indicates that the lateral coupling is due to electron tunneling between the dots when the ground states are in resonance. The electron probability can then be shifted to either dot and the system can be used to create a wavelength-tunable single-photon emitter by simply applying a voltage.

  5. Entangled photons from quantum dot devices: efficiency of post-selection

    Energy Technology Data Exchange (ETDEWEB)

    Seliger, Marek; Hohenester, Ulrich [Institut fuer Physik, Karl-Franzens-Universitaet Graz (Austria); Pfanner, Gernot [Max-Planck-Institut fuer Eisenforschung, Duesseldorf (Germany)

    2009-02-15

    We theoretically investigate the production of polarization-entangled photons through the biexciton cascade decay in a single semiconductor quantum dot. A biexciton radiatively decays through two intermediate exciton states, where polarization-entangled photons are emitted if the two decay paths differ in polarization but are indistinguishable otherwise. This ideal performance is usually spoiled by the electron-hole exchange interaction splitting the intermediate exciton states by a small amount and consequently attaching a which-path information to the photon frequencies. We discuss post-selection schemes to mask this which-path information to an outside observer. We show how spectral filtering and time shifts at a single photon level affect the photon state. Here the solid state environment plays a crucial role in the effective measurement of intermediate exciton states. Evaluating our analytical results with realistic quantum dot parameters we quantify the applicability of suggested protocols for solid-state based quantum cryptography. Our results indicate, that a high degree of entanglement is only reached by spectral alignment of the exciton states. (copyright 2009 WILEY-VCH Verlag GmbH and Co. KGaA, Weinheim) (orig.)

  6. 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 ...

  7. Vector pulsing soliton of self-induced transparency in waveguide

    International Nuclear Information System (INIS)

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

  8. 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

  9. 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.

  10. 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.

  11. Single entangled photon pair emission from an InGaAs/GaAs quantum dot up to temperatures of 30 K

    Energy Technology Data Exchange (ETDEWEB)

    Hafenbrak, R.; Ulrich, S.M.; Michler, P. [Institut fuer Halbleiteroptik und Funktionelle Grenzflaechen, Universitaet Stuttgart (Germany); Wang, L. [Max-Planck-Institut fuer Festkoerperforschung, Stuttgart (Germany); Rastelli, A.; Schmidt, O.G. [Institut fuer Integrative Nanowissenschaften, IFW Dresden (Germany)

    2009-02-15

    Photon pairs emitted from the biexciton-exciton cascade of a single self-assembled InGaAs/GaAs quantum dot can be polarization-entangled. The degree of entanglement is reduced by the fine structure splitting of the involved exciton level. We measure this splitting in high resolution using a scanning Fabry-Perot interferometer. By quantum state tomography we can determine the two-photon polarization state.We are able to verify the conditions of entangled or classically correlated photon pairs in full consistence with the observed fine structure splittings. The entanglement remains relatively unaffected for elevated sample temperatures where we observe reliable entanglement up to 30 K. (copyright 2009 WILEY-VCH Verlag GmbH and Co. KGaA, Weinheim) (orig.)

  12. 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.

  13. 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.)

  14. A dimer PT -symmetric model simulated in GaAs/AlGaAs quantum wells

    Science.gov (United States)

    Meng, Li-Chen; Zhang, Wen-Jing; Liu, Jibing; Xie, Xiao-Tao

    2016-05-01

    We perform the possibility to generate a dimer PT -symmetric model based on a double lambda four-level system in GaAs/AlGaAs quantum wells with biexcitonic transitions. By presenting the detuning management and modulating the Rabi frequencies of the two strong coupling laser fields, we show that the PT -symmetric model can be realized by the spatial evolution of the weak probe laser and four-wave mixing (FWM)-generated field along the propagation direction. The two weak fields in our model may be used to simulate two laser propagating in two PT -symmetric parallel waveguides. The diffraction effect also can be studied in some conditions. Our scheme offers two advantages: the complex refractive index is controlled by the strong coupling fields; the symmetry energy exchange between a dimer PT -symmetric structure is guaranteed by the four-wave mixing process. The present investigation may provide research opportunities in optical experiments.

  15. Dressed excitonic states and quantum interference in a three-level quantum dot ladder system

    Energy Technology Data Exchange (ETDEWEB)

    Gerardot, B D; Brunner, D; Dalgarno, P A; Warburton, R J [School of Engineering and Physical Sciences, Heriot-Watt University, Edinburgh EH14 4AS (United Kingdom); Karrai, K [Center for NanoScience and Department fuer Physik der LMU, Geschwister-Scholl-Platz 1, 80539 Munich (Germany); Badolato, A [Institute of Quantum Electronics, ETH Zurich, 8093 Zurich (Switzerland); Petroff, P M [Materials Department, University of California, Santa Barbara, CA 93106 (United States)], E-mail: b.d.gerardot@hw.ac.uk

    2009-01-15

    We observe dressed states and quantum interference effects in a strongly driven three-level quantum dot ladder system. The effect of a strong coupling field on one dipole transition is measured by a weak probe field on the second dipole transition using differential reflection. When the coupling energy is much larger than both the homogeneous and inhomogeneous linewidths an Autler-Townes splitting is observed. Significant differences are observed when the transitions resonant with the strong and weak fields are swapped, particularly when the coupling energy is nearly equal to the measured linewidth. This result is attributed to quantum interference: destructive or constructive interference with modest visibility is observed depending on the pump/probe geometry. The data demonstrate that coherence of both the bi-exciton and the exciton is maintained in this solid-state system, even under intense illumination, which is crucial for prospects in quantum information processing and nonlinear optical devices.

  16. 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.)

  17. Micro-photoluminescence study of single self-organized InAs/InP quantum sticks

    International Nuclear Information System (INIS)

    Micro-photoluminescence spectroscopy (μ-PL) as a function of excitation power density and temperature, is used to study single self-organized InAs/InP quantum sticks (QSs) suitable for optoelectronic applications around 1.55 μm. The micro-photoluminescence experiments performed on sub-micron mesas at low temperature and low excitation power show several peaks associated to the exciton, biexciton and excited states of single QS, but which present large linewidths in the 0.8-2.5 meV range. The experiments performed through sub-micron apertures on the same bare sample show peaks with narrower linewidths close to 300 μeV. This difference in the linewidth value is thought to be due to a coulomb charge effect induced by the non-intentional doping of the InP barrier layers

  18. Time-Resolved Optical Spectroscopy of Tunnel Coupled Lateral Quantum Dot Molecules

    Science.gov (United States)

    Hermannstädter, C.; Beirne, G. J.; Wang, L.; Rastelli, A.; Schmidt, O. G.; Michler, P.

    2007-04-01

    The two laterally coupled quantum dots, also referred to as lateral quantum dot molecules, exhibit a characteristic photoluminescence spectrum consisting of six dominant emission lines that are due to neutral and charged excitonic as well as biexcitonic recombination. All of these lines are found to originate from the same single quantum emitter following photon statistics measurements. Using a parallel electric field we are able to control the quantum coupling between the dots. This control manifests itself as an ability to reversibly switch the relative intensities of the two neutral excitonic transitions, which results in a possible application of the molecules as tunable single-photon emitters. To further investigate the exact origin of the photoluminescence lines we have also investigated the decay times of the molecule emission.

  19. Polarization fine structure and enhanced single-photon emission of self-assembled lateral InGaAs quantum dot molecules embedded in a planar microcavity

    Science.gov (United States)

    Hermannstädter, C.; Witzany, M.; Beirne, G. J.; Schulz, W.-M.; Eichfelder, M.; Rossbach, R.; Jetter, M.; Michler, P.; Wang, L.; Rastelli, A.; Schmidt, O. G.

    2009-06-01

    Single lateral InGaAs quantum dot molecules have been embedded in a planar microcavity in order to increase the luminescence extraction efficiency. Using a combination of metal-organic vapor phase and molecular beam epitaxy samples could be produced that exhibit a 30 times enhanced single-photon emission rate. We also show that the single-photon emission is fully switchable between two different molecular excitonic recombination energies by applying a lateral electric field. Furthermore, the presence of a polarization fine structure splitting of the molecular neutral excitonic states is reported which leads to two polarization split classically correlated biexciton-exciton cascades. The fine structure splitting is found to be on the order of 10 μeV.

  20. Tunable lateral tunnel coupling between two self-assembled InGaAs quantum dots

    Science.gov (United States)

    Beirne, Gareth J.; Hermannstädter, Claus; Wang, Lijuan; Rastelli, Armando; Müller, Elisabeth; Schmidt, Oliver G.; Michler, Peter

    2007-02-01

    We demonstrate direct control over the level of lateral quantum coupling between two self-assembled InGaAs/GaAs quantum dots. This coupled system, which we also refer to as a lateral quantum dot molecule, was produced using a unique technique which combines molecular beam epitaxy and in-situ atomic layer etching. Atomic force microscopy measurements show that each molecule consists of two structurally distinct dots, which are aligned along the [1-10] direction. Each molecule exhibits a characteristic photoluminescence spectrum primarily consisting of two neutral excitonic and two biexcitonic transitions. The various transitions have been investigated using micro-photoluminescence measurements as a function of excitation power density, time, and applied electric field. Photon statistics experiments between the excitonic emission lines display strong antibunching in the second-order cross-correlation function which confirms that the two dots are quantum coupled. Cascaded emission between corresponding biexcitonic and excitonic emission has also been observed. Using a parallel electric field we can control the quantum coupling between the dots. This control manifests itself as an ability to reversibly switch the relative intensities of the two neutral excitonic transitions. Furthermore, detailed studies of the emission energies of the two neutral excitonic transitions as a function of parallel lateral electric field show a clear anomalous Stark shift which further demonstrates the presence of quantum coupling between the dots. In addition, this shift allows for a reasonable estimate of the coupling energy. Finally, a simple one-dimensional model, which assumes that the coupling is due to electron tunneling, is used to qualitatively describe the observed effects.

  1. 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

  2. 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.

  3. Highly-reduced Fine-structure splitting in InAs/InP quantum dots offering efficient on-demand 1.55 μm entangled photon emitter

    Science.gov (United States)

    He, Lixin; Gong, M.; Li, C.-F.; Guo, G.-C.; Zunger, A.

    2009-03-01

    There has been intense recent interest in finding efficient entangled photon sources, including the demonstration of generation of ``event-ready'' entangled photon pairs via a biexciton cascade process using an (In,Ga)As/GaAs quantum dot(QD). However, a genuine finite energy difference between photons with different polarizations, known as the fine structure splitting (FSS), can destroy the entanglement of the photon pairs. To achieve entanglement from (In,Ga)As/GaAs QD, it was, indeed, necessary to Cherry-pick a sample with extremely small FSS from a large number of samples, or to apply strong in-plane magnetic field. Furthermore, the emission wavelength of (In,Ga)As/GaAs QD (880 - 950 nm) is mismatched with the 1.55 μm needed for communications using the optical fibers. Using theoretical modeling of the fundamental causes of FSS in QDs, we predict that the intrinsic FSS of InAs/InP QDs is an order of magnitude smaller than that of InAs/GaAs dots, and better yet, their excitonic gap matches the 1.55 μm fiber optic wavelength,therefore offer efficient on-demand entangled photon emitters for long distance quantum communication.

  4. Control of single quantum dot emission characteristics and fine structure by lateral electric fields

    Energy Technology Data Exchange (ETDEWEB)

    Ulrich, S.M.; Hafenbrak, R.; Michler, P. [Institut fuer Halbleiteroptik und Funktionelle Grenzflaechen, Universiaet Stuttgart (Germany); Vogel, M.M. [Institut fuer Halbleiteroptik und Funktionelle Grenzflaechen, Universiaet Stuttgart (Germany); Institut fuer Strahlwerkzeuge, Universitaet Stuttgart (Germany); Wang, L. [Max-Planck-Institut fuer Festkoerperforschung, Stuttgart (Germany); Rastelli, A.; Schmidt, O.G. [Insitute for Integrative Nanosciences, IFW Dresden (Germany)

    2009-02-15

    The spontaneous emission characteristics of individual self-assembled (In,Ga)As/GaAs quantum dots have been investigated under the application of a tunable electric field in the lateral growth plane. For the neutral excitonic and bi-excitonic as well as a singly-charged (trionic) QD carrier configuration, similar quantum-confined Stark effects could be observed, thus enabling a direct and comparative determination of corresponding polarizability values {alpha}. In addition we have applied a refined detection technique of high-resolution Fabry-Perot interferometry on single QDs to investigate the anisotropy-induced excitonic fine structure and to monitor its tunability under a lateral electric field. Whereas most quantum dots reveal an oscillatory-type modulation and partial reduction in fine structure under the applied field, we also demonstrate the case of a selected QD where the initial fine structure could even be reversibly tuned down to zero. This fine structure tunability of single QDs represents an essential prerequisite for the realization of individually controlled entangled photon sources in the future. (copyright 2009 WILEY-VCH Verlag GmbH and Co. KGaA, Weinheim) (orig.)

  5. Polymer fluorescence: Even-parity states, alternation, and heteroatoms

    Energy Technology Data Exchange (ETDEWEB)

    Soos, Z.G. [Princeton Univ., NJ (United States). Dept. of Chemistry; Galvao, D.S. [Bell Communications Research, Red Bank, NJ (United States)]|[Univ. Estadual de Campinas, Sao Paulo (Brazil). Dept. de Fisica Aplicada; Etemad, S. [Bell Communications Research, Red Bank, NJ (United States)

    1994-12-31

    Polymer fluorescence indicates a lowest singlet excitation S{sub 1} of odd parity, while an even-parity S{sub 1} favors radiationless decay. The optical gap E{sub g} defines the lowest odd-parity singlet, 1{sup 1}B{sub u}, and the two-photon gap E{sub a} fixes the 2{sup 1}A{sub g} state. The 1B/2A ordering of conjugated polymers reflects different single-particle gaps, 4t{delta} for alternating chains, at nearly constant correlations. The authors discuss topological and heteroatom contributions to the effective alternation of poly-p-phenylenevinylenes and polythiophenes, respectively, and analyze polymer spectra in term of molecular {pi}-electron theory. Even-parity states at E{sub a} and biexcitons derived from two-electron excitation across E{sub g} indicate intermediate correlations and alternations, thereby limiting the accuracy of band, strong-correlation, and large-{delta} descriptions. Correlated states in the dimer limit illustrate the 2A/1B crossover of Hubbard or excitonic systems.

  6. 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.

  7. Effect of Auger Recombination on Lasing in Heterostructured Quantum Dots with Engineered Core/Shell Interfaces.

    Science.gov (United States)

    Park, Young-Shin; Bae, Wan Ki; Baker, Thomas; Lim, Jaehoon; Klimov, Victor I

    2015-11-11

    Nanocrystal quantum dots (QDs) are attractive materials for applications as laser media because of their bright, size-tunable emission and the flexibility afforded by colloidal synthesis. Nonradiative Auger recombination, however, hampers optical amplification in QDs by rapidly depleting the population of gain-active multiexciton states. In order to elucidate the role of Auger recombination in QD lasing and isolate its influence from other factors that might affect optical gain, we study two types of CdSe/CdS core/shell QDs with the same core radii and the same total sizes but different properties of the core/shell interface ("sharp" vs "smooth"). These samples exhibit distinctly different biexciton Auger lifetimes but are otherwise virtually identical. The suppression of Auger recombination in the sample with a smooth (alloyed) interface results in a notable improvement in the optical gain performance manifested in the reduction of the threshold for amplified spontaneous emission and the ability to produce dual-color lasing involving both the band-edge (1S) and the higher-energy (1P) electronic states. We develop a model, which explicitly accounts for the multiexciton nature of optical gain in QDs, and use it to analyze the competition between stimulated emission from multiexcitons and their decay via Auger recombination. These studies re-emphasize the importance of Auger recombination control for the realization of real-life QD-based lasing technologies and offer practical strategies for suppression of Auger recombination via "interface engineering" in core/shell structures. PMID:26397312

  8. Optical control of nonlinearly dressed states in an individual quantum dot

    Science.gov (United States)

    Ardelt, P.-L.; Koller, M.; Simmet, T.; Hanschke, L.; Bechtold, A.; Regler, A.; Wierzbowski, J.; Riedl, H.; Finley, J. J.; Müller, K.

    2016-04-01

    We report nonlinear resonance fluorescence of an individual semiconductor quantum dot. By driving a single semiconductor quantum dot via a two-photon transition, we probe the linewidth of two-photon excitation processes and show that, similar to their single-photon counterparts, they are close to being Fourier limited at low temperatures. The evolution of the population of excitonic states with increasing Rabi energy exhibits a clear S-shaped behavior, indicative of the nonlinear response via the two-photon excitation process. Numerical calculations of the nonlinear response using a four-level atomic system representing the manifold of excitonic and biexcitonic states in the quantum dot are in excellent agreement with our experiments and reveal the effect of interactions with LA phonons in the solid-state environment. Finally, we demonstrate the formation of dressed states emerging from a nonlinear two-photon interaction between the quantum dot and the optical excitation field. The nonlinear optical dressing induces a mixing of all four excitonic states that allows direct optical tuning of the polarization selection rules and energies of the dressed states in the artificial atom. We expect our results to play a pivotal role for the generation of nonclassical photon pairs desired for applications in quantum communication and fundamental experiments on quantum optical properties of photons.

  9. Comparison of magneto-optical properties of various excitonic complexes in CdTe and CdSe self-assembled quantum dots.

    Science.gov (United States)

    Kobak, J; Smoleński, T; Goryca, M; Rousset, J-G; Pacuski, W; Bogucki, A; Oreszczuk, K; Kossacki, P; Nawrocki, M; Golnik, A; Płachta, J; Wojnar, P; Kruse, C; Hommel, D; Potemski, M; Kazimierczuk, T

    2016-07-01

    We present a comparative study of two self-assembled quantum dot (QD) systems based on II-VI compounds: CdTe/ZnTe and CdSe/ZnSe. Using magneto-optical techniques we investigated a large population of individual QDs. The systematic photoluminescence studies of emission lines related to the recombination of neutral exciton X, biexciton XX, and singly charged excitons (X(+), X(-)) allowed us to determine average parameters describing CdTe QDs (CdSe QDs): X-XX transition energy difference 12 meV (24 meV); fine-structure splitting δ1=0.14 meV (δ1=0.47 meV); g-factor g  =  2.12 (g  =  1.71); diamagnetic shift γ=2.5 μeV T(-2) (γ =1.3 μeV T(-2)). We find also statistically significant correlations between various parameters describing internal structure of excitonic complexes. PMID:27173643

  10. 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.

  11. Coupling Single Giant Nanocrystal Quantum Dots to the Fundamental Mode of Patch Nanoantennas through Fringe Field

    Science.gov (United States)

    Wang, Feng; Karan, Niladri S.; Minh Nguyen, Hue; Ghosh, Yagnaseni; Hollingsworth, Jennifer A.; Htoon, Han

    2015-09-01

    Through single dot spectroscopy and numerical simulation studies, we demonstrate that the fundamental mode of gold patch nanoantennas have fringe-field resonance capable of enhancing the nano-emitters coupled around the edge of the patch antenna. This fringe-field coupling is used to enhance the radiative rates of core/thick-shell nanocrystal quantum dots (g-NQDs) that cannot be embedded into the ultra-thin dielectric gap of patch nanoantennas due to their large sizes. We attain 14 and 3 times enhancements in single exciton radiative decay rate and bi-exciton emission efficiencies of g-NQDs respectively, with no detectable metal quenching. Our numerical studies confirmed our experimental results and further reveal that patch nanoantennas can provide strong emission enhancement for dipoles lying not only in radial direction of the circular patches but also in the direction normal to the antennas surface. This provides a distinct advantage over the parallel gap-bar antennas that can provide enhancement only for the dipoles oriented across the gap.

  12. 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.

  13. Comparison of magneto-optical properties of various excitonic complexes in CdTe and CdSe self-assembled quantum dots

    Science.gov (United States)

    Kobak, J.; Smoleński, T.; Goryca, M.; Rousset, J.-G.; Pacuski, W.; Bogucki, A.; Oreszczuk, K.; Kossacki, P.; Nawrocki, M.; Golnik, A.; Płachta, J.; Wojnar, P.; Kruse, C.; Hommel, D.; Potemski, M.; Kazimierczuk, T.

    2016-07-01

    We present a comparative study of two self-assembled quantum dot (QD) systems based on II–VI compounds: CdTe/ZnTe and CdSe/ZnSe. Using magneto-optical techniques we investigated a large population of individual QDs. The systematic photoluminescence studies of emission lines related to the recombination of neutral exciton X, biexciton XX, and singly charged excitons (X+, X‑) allowed us to determine average parameters describing CdTe QDs (CdSe QDs): X–XX transition energy difference 12 meV (24 meV); fine-structure splitting δ1=0.14 meV (δ1=0.47 meV); g-factor g  =  2.12 (g  =  1.71) diamagnetic shift γ=2.5 μeV T‑2 (γ =1.3 μeV T‑2). We find also statistically significant correlations between various parameters describing internal structure of excitonic complexes.

  14. Time-resolved optical spectroscopy of lateral InGaAs quantum dot molecules

    Energy Technology Data Exchange (ETDEWEB)

    Hermannstaedter, Claus; Beirne, Gareth; Michler, Peter [Institut fuer Strahlenphysik, Universitaet Stuttgart, Allmandring 3, 70569 Stuttgart (Germany); Wang, Lijuan; Rastelli, Armando; Schmidt, Oliver [Max-Planck- Institut fuer Festkoerperforschung, Heisenbergstr. 1, 70569 Stuttgart (Germany)

    2007-07-01

    We demonstrate direct control over the level of lateral quantum coupling between two self-assembled InGaAs/GaAs quantum dots. These coupled systems which we refer to as lateral quantum dot molecules are, due to their unique growth technique, all aligned along the [1-10] crystal direction. Electrodes on the sample surface allow for the application of a lateral electric field. By applying an electric field parallel to the coupling-axis the degree of coupling can be manipulated as manifested by the shift of the emission energies and relative intensities of the characteristic photoluminescence lines. Time-correlated singlephoton counting experiments performed on single molecules provide access to both the rise and decay characteristics of the molecule emission lines. Typical decay times for the excitonic recombination are on the order of 1 ns, about half the latter value for biexcitonic recombination, and intermediate for charged excitonic recombination. An analysis of the exciton rise behavior strongly indicates that electron tunneling is the predominant coupling mechanism in the molecules.

  15. Suppression of the blinking of single QDs by using an N-typ e semiconductor nanomaterial%利用N型半导体纳米材料抑制单量子点的荧光闪烁特性∗

    Institute of Scientific and Technical Information of China (English)

    王早; 张国峰; 李斌; 陈瑞云; 秦成兵; 肖连团; 贾锁堂

    2015-01-01

    Single quantum dots (QDs) always exhibit strong blinking in fluorescence intensity when they are on some inert substrates. The blinking activity is attributed to the photoinduced charging of QDs by electron transfer (ET) to trap states in QDs and the surrounding matrix, which has been considered as an undesirable property in many applications. Here, we use N-doped indium tin oxide (ITO) semiconductor nanoparticles to suppress fluorescence blinking activity of single CdSe/ZnS core/shell QDs. The fluorescence characteristics of single QDs in ITO and on SiO2 cover glass are measured by a laser scanning confocal fluorescence microscopy, respectively. It is found that the on- and off-state probability densities of QDs on different substrates both can be fit by a truncated power law. Blinking rates for single QDs on glass and in ITO are also calculated. By contrast, single QDs doped in ITO show that their blinking rate and fluorescence lifetime both decrease. The on-state probability density of single QDs in ITO is approximately two orders of magnitude higher than that of QDs on SiO2 cover glass. It means that single QDs doped in ITO have a longer time to be on-state. Because the Fermi level in QDs is lower than in ITO, when they are in contact, electrons in ITO will transfer to QDs. As a result, the equilibration of their Fermi levels leads to the formation of negatively charged QDs. These electrons fill in the holes of QDs shell and enhance the on-state probability of QDs. Fluorescence decays of single QDs on glass and in ITO are measured by TAC/MCA, and they can be fit by biexponential function. The two lifetime values correspond to the single exciton lifetime and biexciton lifetime of QDs, respectively. It is worth noting that the distribution of the amplitude weighted average lifetime for single QDs in ITO is approximately 41% of that for single QDs on SiO2 cover glass and its full width at half maximum (FWHM) is changed to 50%. For the conduction band potential of

  16. Wavelength tunable InAs/InP(1 0 0) quantum dots in 1.55-μm telecom devices

    International Nuclear Information System (INIS)

    This paper reviews the growth, characterization and device applications of self-assembled InAs/InP(1 0 0) quantum dots (QDs) formed by MOVPE. The problematic As/P exchange reaction during QD growth is suppressed by the insertion of a GaAs interlayer together with optimum growth conditions. This produces QDs with continuously tunable emission over the 1.55-μm wavelength region for fiber-based telecom applications. Device quality of these QDs is proven by continuous wave lasing at room temperature from the as-cleaved facets of Fabry-Perot narrow ridge-waveguide lasers implementing widely stacked QDs as gain medium. The low transparency current density of 6 A/cm2 per QD layer and low loss of 4.2 cm-1 are accompanied by a 80-nm wide gain spectrum. The deeply etched QD lasers possess similar threshold current densities as the shallowly etched ones and do not deteriorate with time, revealing that device performance does not suffer from sidewall recombination. This allows the fabrication of mono-mode and more compact devices with small bending radii, as demonstrated by the operation of a QD ring laser with 40-GHz free spectral range. Unpolarized emission from the cleaved side, important for the realization of polarization insensitive semiconductor optical amplifiers, is obtained by close stacking of QDs due to vertical electronic coupling. Sharp exciton-biexciton emission from a single QD around 1.55 μm is observed with clearly resolvable peaks above 70 K, which is required for single photon sources working at liquid nitrogen temperature for fiber-based quantum cryptography systems

  17. 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.)

  18. Electrical and optical measurements on a single InAs quantum dot using ion-implanted micro-LEDs

    International Nuclear Information System (INIS)

    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 μm2 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 3Xs, 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.)

  19. Optical properties of charged semiconductor quantum dots

    Science.gov (United States)

    Jha, Praket P.

    The effect of n-type doping on the luminescence properties of II-VI quantum dots is studied. The addition of two shells of CdS on CdSe quantum dots prevents the creation of surface traps and makes the system stable under reducing environment. The injection of electrons into films of quantum dots leads to lower photoluminescence (PL) efficiency, with the extent of quenching dependent on both the number and the quantum states of the spectator charges in the nanocrystal. It is found that a 1Pe electron is an eightfold better PL quencher than the 1Se electron. Reduced threshold for stimulated emission is also observed in doped CdSe/CdS films. Time resolved photoluminescence measurements are used to extract the recombination rates of a charged exciton, called trion. It is observed that the negative trion has a radiative rate ˜2.2 +/- 0.4x faster than a neutral exciton, while its non-radiative recombination rate is slower than the biexciton non-radiative recombination rate by a factor of 7.5 +/- 1.7. The knowledge of the recombination rates of the trion enables us to calculate the quantum yield of a negative trion to be ˜10% for the nanocrystals investigated in our work. This is larger than the off state quantum yield from a single quantum dot photoluminescence trajectory and eliminates the formation of negative trion as the possible reason for the PL blinking of single quantum dots. Single quantum dot electrochemistry has also been achieved. It is shown that by varying the Fermi level of the system electrons can be reversibly injected into and extracted out of single CdSe/CdS and CdSe/ZnS nanoparticles to modulate the photoluminescence.

  20. 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.

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

    International Nuclear Information System (INIS)

    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 In0.48Ga0.52P, 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/μm2 is realized. The resulting isolated InP quantum dots are individually characterized without the need for lithographical patterning and masks on the substrate. Both excitonic and biexcitonic emissions are observed from single dots, appearing as doublets with a fine-structure splitting of 320 μeV. Hanbury Brown-Twiss correlation measurements for the excitonic emission under cw excitation show anti-bunching behavior with an autocorrelation value of g(2)(0)=0.2. This system is applicable as a single-photon source for applications such as quantum cryptography. The formation of well-ordered chains of InP quantum dots on GaAs (001) substrates by using self-organized In0.48Ga0.52P 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 In0.48Ga0.52P 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.

  2. 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.

  3. 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

  4. 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.

  5. Investigations into photo-excited state dynamics in colloidal quantum dots

    Science.gov (United States)

    Singh, Gaurav

    Colloidal Quantum dots (QDs) have garnered considerable scientific and technological interest as a promising material for next generation solar cells, photo-detectors, lasers, bright light-emitting diodes (LEDs), and reliable biomarkers. However, for practical realization of these applications, it is crucial to understand the complex photo-physics of QDs that are very sensitive to surface chemistry and chemical surroundings. Depending on the excitation density, QDs can support single or multiple excitations. The first part of this talk addresses evolution of QD excited state dynamics in the regime of low excitation intensity. We use temperature-resolved time-resolved fluorescence spectroscopy to study exciton dynamics from picoseconds to microseconds and use kinetic modeling based on classical electron transfer to show the effect of surface trap states on dynamics of ground-state exciton manifold in core-shell CdSe/CdS QDs. We show that the thickness of CdS shell plays an important role in interaction of CdSe core exciton states with nanocrystal environment, and find that a thicker shell can minimize the mixing of QD exciton states with surface trap states. I will then present an investigation into the dynamics of multiply-excited states in QDs. One of the key challenges in QD spectroscopy is to reliably distinguish multi- from single-excited states that have similar lifetime components and spectroscopic signatures. I will describe the development of a novel multi-pulse fluorescence technique to selectively probe multi-excited states in ensemble QD samples and determine the nature of the multi-excited state contributing to the total fluorescence even in the limit of low fluorescent yields. We find that in our sample of CdSe/CdS core/shell QDs the multi-excited emission is dominated by emissive trion states rather than biexcitons. Next, I will discuss the application of this technique to probe exciton-plasmon coupling in layered hybrid films of QD/gold nanoparticles