Biexcitons in semiconductor microcavities
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. The...
Biexcitons in semiconductor microcavities
Borri, P.; Langbein, W.; Woggon, U.; Esser, A.; Jensen, J.R.; Hvam, Jørn Märcher
2003-01-01
microcavity, even if the vacuum Rabi splitting exceeds the biexciton binding energy. However, the presence of a longitudinal built-in electric field that results in a Stark effect slightly reducing the binding energy compared to the value measured on a reference bare quantum well is experimentally pointed out...... and compared with calculations. Additionally, the polarization decay of the transition from the crystal ground state to the biexciton is measured and is shown to be larger by approximately a factor of two compared to the value measured on the reference quantum well....
Dephasing of Quasi-2D Biexcitons
Langbein, Wolfgang; Hvam, Jørn Märcher
1999-01-01
signal at the biexcitonic resonance for negative and positive delay times, respectively. The ratio between the dephasing rates of biexcitons and excitons is found to be close to two for kBT larger than the biexciton binding energy. At lower temperatures, the ratio drops significantly. This demonstrates...
Biexcitons or bipolaritons in a semiconductor microcavity
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...
Biexciton dephasing in a semiconductor microcavity
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 ...
Localization-enhanced biexciton binding in semiconductors
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...
Binding of quasi two-dimensional biexcitons
Birkedal, Dan; Singh, J; Vadim, Lyssenko; Hvam, Jørn Märcher
Summary form only given. In this presentation we report on a determination of the biexciton binding energies in GaAs-AlGaAs quantum wells of different widths and the results of a theoretical calculation of the ratio of the biexciton binding energy to that of the exciton. We determine the binding ...
Mixed biexcitons in single quantum wells
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....
Binding-energy distribution and dephasing of localized biexcitons
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....
Langbein, W.; Hvam, Jørn Märcher
2002-01-01
We investigate the influence of excitonic localization on the corresponding biexcitonic states in GaAs quantum wells by spectrally resolved four-wave mixing. With increasing localization, the biexciton binding energy increases, while the biexciton continuum shifts to higher energies. The localiza......We investigate the influence of excitonic localization on the corresponding biexcitonic states in GaAs quantum wells by spectrally resolved four-wave mixing. With increasing localization, the biexciton binding energy increases, while the biexciton continuum shifts to higher energies. The...... localization leads to an inhomogeneous broadening of the biexciton binding energy and the biexciton continuum edge. Simultaneously, the oscillator strength of the biexciton continuum-edge is reduced. This is interpreted as a result of the different localization of biexcitonic and excitonic states by the random...
Electronic properties of exciton and biexciton in a CdTe/ZnTe nano-heterostructure
Energy eigen values and the binding energies of exciton and biexciton in a CdTe/ZnTe quantum dot are studied with the geometrical confinement effect. The single exciton binding energy and the biexciton binding energy are calculated as a function of dot radius. Overlap integral of the exciton and the biexciton is found in the CdTe/ZnTe quantum dot. The electron and hole potentials are calculated from the Poisson equations. Self-consistent method is to compute the energy eigenvalues of the exciton and the biexciton. The Hartree potential is employed to obtain the Coulomb interaction energy
Detection of a biexciton in semiconducting carbon nanotubes using nonlinear optical spectroscopy.
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
Stability and signatures of biexcitons in carbon nanotubes
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....
Biexciton emission from single isoelectronic traps formed by nitrogen-nitrogen pairs in GaAs
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.
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.
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
Biexcitonic photocurrent induced by two-photon process at a telecommunication band
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.)
Matched slow optical soliton pairs via biexciton coherence in quantum dots
We theoretically investigate the simultaneous formation and stable propagation of slow optical soliton pairs in semiconductor quantum dots with a four-level biexciton-exciton cascade configuration. Owing to the destructive interference set up by two continuous wave control fields that couple to a biexciton state, the linear as well as nonlinear dispersion can be dramatically enhanced simultaneously with the absorptions of two weak probe fields being almost suppressed. These results reveal that the detrimental distortions of the two weak-pulsed probe fields due to dispersion effects can be well balanced by the self-phase modulation effect under very low input light intensity, which leads to the slow temporal optical soliton pairs with matched group velocity and amplitude. We also show that the propagation of slow optical solitons can be strongly modified by the biexciton coherence.
Biexciton binding energy in ZnSe quantum wells and quantum wires
Wagner, Hans-Peter; Langbein, Wolfgang; Hvam, Jørn Märcher; Bacher, G.; Kümmell, T.; Forchel, Alfred
2002-01-01
The biexciton binding energy E-XX is investigated in ZnSe/ZnMgSe quantum wells and quantum wires as a function of the lateral confinement by transient four-wave mixing. In the quantum wells one observes for decreasing well width a significant increase in the relative binding energy, saturating for...... well widths less than 8 nm. In the quantum wires an increase of 30% is found in the smallest quantum wire structures compared to the corresponding quantum well value. A simple analytical model taking into account the quantum confinement in these low-dimensional systems is used to explain the...... experimentally observed dependence of the biexciton binding energies....
Biexciton formation and exciton coherent coupling in layered GaSe
Dey, P.; Paul, J.; Stevens, C. E.; Glikin, N.; Karaiskaj, D., E-mail: karaiskaj@usf.edu [Department of Physics, University of South Florida, 4202 East Fowler Ave., Tampa, Florida 33620 (United States); Moody, G. [National Institute of Standards and Technology, 325 Broadway, Boulder, Colarado 80305 (United States); Kovalyuk, Z. D.; Kudrynskyi, Z. R. [Chernivtsi Department, Frantsevich Institute of Material Sciences Problems, The National Academy of Sciences of Ukraine, 5, Iryna Vilde St., 58001 Chernivtsi (Ukraine); Romero, A. H. [Physics Department, West Virginia University, Morgantown, West Virginia 26506-6315 (United States); Cantarero, A. [Materials Science Institute, University of Valencia, P.O. Box 2205, 46071 Valencia (Spain); Hilton, D. J. [Department of Physics, University of Alabama at Birmingham, Birmingham, Alabama 35294 (United States)
2015-06-07
Nonlinear two-dimensional Fourier transform (2DFT) and linear absorption spectroscopy are used to study the electronic structure and optical properties of excitons in the layered semiconductor GaSe. At the 1s exciton resonance, two peaks are identified in the absorption spectra, which are assigned to splitting of the exciton ground state into the triplet and singlet states. 2DFT spectra acquired for co-linear polarization of the excitation pulses feature an additional peak originating from coherent energy transfer between the singlet and triplet. At cross-linear polarization of the excitation pulses, the 2DFT spectra expose a new peak likely originating from bound biexcitons. The polarization dependent 2DFT spectra are well reproduced by simulations using the optical Bloch equations for a four level system, where many-body effects are included phenomenologically. Although biexciton effects are thought to be strong in this material, only moderate contributions from bound biexciton creation can be observed. The biexciton binding energy of ∼2 meV was estimated from the separation of the peaks in the 2DFT spectra. Temperature dependent absorption and 2DFT measurements, combined with “ab initio” theoretical calculations of the phonon spectra, indicate strong interaction with the A{sub 1}{sup ′} phonon mode. Excitation density dependent 2DFT measurements reveal excitation induced dephasing and provide a lower limit for the homogeneous linewidth of the excitons in the present GaSe crystal.
Excitons, Biexcitons and Dephasing in GaAs T-shaped quantum wires
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...
Magnetoluminescence from trion and biexciton in type-II quantum dot
Okuyama Rin
2011-01-01
Full Text Available Abstract We theoretically investigate optical Aharonov-Bohm (AB effects on trion and biexciton in the type-II semiconductor quantum dots, in which holes are localized near the center of the dot, and electrons are confined in a ring structure formed around the dot. Many-particle states are calculated numerically by the exact diagonalization method. Two electrons in trion and biexciton are strongly correlated to each other, forming a Wigner molecule. Since the relative motion of electrons are frozen, the Wigner molecule behaves as a composite particle whose mass and charges are twice those of an electron. As a result, the period of AB oscillation for trion and biexciton becomes h/2e as a function of magnetic flux penetrating the ring. We find that the magnetoluminescence spectra from trion and biexciton change discontinuously as the magnetic flux increases by h/2e. PACS: 71.35.Ji, 73.21.-b, 73.21.La, 78.67.Hc
Optical instabilities and chaos due to the virtual formation of biexcitons
Optical instabilities and chaos due to virtual formation of biexcitons in optically excited semiconductors are investigated. A complete linear stability analysis of steady-state bistable solutions of nonlinear coupled differential equations describing the nonlinear dynamics of semiconductors is carried out. The dynamical solutions are studied numerically using an iterative procedure. (author). 20 refs, 3 figs
In this study, a detailed investigation of the electronic and optical properties (i.e., binding energies, absorption wavelength, overlap of the electron-hole wave functions, recombination oscillator strength, etc.) of an exciton and a biexciton in CdTe/CdSe core/shell type-II quantum dot heterostructures has been carried out in the frame of the single band effective mass approximation. In order to determine the electronic properties, we have self-consistently solved the Poisson-Schrödinger equations in the Hartree approximation. We have considered all probable Coulomb interaction effects on both energy levels and also on the corresponding wave functions for both single exciton and biexciton. In addition, we have taken into account the quantum mechanical exchange-correlation effects in the local density approximation between same kinds of particles for biexciton. Also, we have examined the effect of the ligands and dielectric mismatch on the electronic and optical properties. We have used a different approximation proposed by Sahin and Koc [Appl. Phys. Lett. 102, 183103 (2013)] for the recombination oscillator strength of the biexciton for bound and unbound cases. The results obtained have been presented comparatively as a function of the shell thicknesses and probable physical reasons in behind of the results have been discussed in a detail
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 ...
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.
Role of Strain on the Coherent Properties of GaAs Excitons and Biexcitons
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.
Phase control of optical bistability based biexciton coherence in a quantum dot nanostructure
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.
Exciton-exciton annihilation and biexciton stimulated emission in graphene nanoribbons
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.
Exciton–exciton annihilation and biexciton stimulated emission in graphene nanoribbons
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
2016-01-01
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. PMID:26984281
Hamedi, H. R.; Afshari, Hadi
2016-01-01
In this letter, the two-dimensional (2D) spatial-dependent of probe absorption based on biexciton coherence is investigated by monitoring the probe absorption spectra in a Quantum Dot (QD) Nanostructure. We find that due to the quantum interference which is set up by two control pulses that couples to a resonance of the biexciton, the 2D spatial distribution of probe absorption spectrum can be controlled via adjusting the system parameters. We study the effect of controlling parameters of the QD system on spatial distribution of the probe field absorption for two different cases in which the QD interacts with the standing-wave laser fields; first, when two laser fields which couple to a biexciton state, correspond to the two orthogonal standing-wave fields and couple the different transitions. Second, when only one of laser fields correspond to the combination of two orthogonal standing-wave fields, while the other one corresponds to a traveling-wave field. Results exhibit different interesting 2D absorption patterns.
Excitons and biexcitons in InGaN quantum dot like localization centers
Indium segregation in a narrow InGaN single quantum well creates quantum dot (QD) like exciton localization centers. Cross-section transmission electron microscopy reveals varying shapes and lateral sizes in the range ∼1–5 nm of the QD-like features, while scanning near field optical microscopy demonstrates a highly inhomogeneous spatial distribution of optically active individual localization centers. Microphotoluminescence spectroscopy confirms the spectrally inhomogeneous distribution of localization centers, in which the exciton and the biexciton related emissions from single centers of varying geometry could be identified by means of excitation power dependencies. Interestingly, the biexciton binding energy (Ebxx) was found to vary from center to center, between 3 to −22 meV, in correlation with the exciton emission energy. Negative binding energies are only justified by a three-dimensional quantum confinement, which confirms QD-like properties of the localization centers. The observed energy correlation is proposed to be understood as variations of the lateral extension of the confinement potential, which would yield smaller values of Ebxx for reduced lateral extension and higher exciton emission energy. The proposed relation between lateral extension and Ebxx is further supported by the exciton and the biexciton recombination lifetimes of a single QD, which suggest a lateral extension of merely ∼3 nm for a QD with strongly negative Ebxx = −15.5 meV. (paper)
Nonradiative Auger recombination of biexcitons in CdSe/CdS core-shell nanocrystal quantum dots
Vaxenburg, Roman; Rodina, Anna; Lifshitz, Efrat; Efros, Alexander
Semiconductor nanocrystals are known for their applicative potential as light-emitting components in lasers and LEDs, as well as light absorbers in solar cells. The performance of these nanocrystal-based devices, however, strongly depends on the dissipative nonradiative Auger recombination. The study of dynamics of the Auger processes is therefore of key importance in connection with the performance of nanocrystals devices. Here we report on a theoretical study of the Auger recombination dynamics of biexcitons in CdSe/CdS core-shell nanocrystals. Biexcitons can decay by the Auger process via negative or positive trion recombination channels. We study the dependence of the rate of each one of these channels on the angular momentum of the initial biexciton state, nanocrystal geometry, and temperature. We observe that the overall dependence of the rates of both channels is strongly oscillating with nanocrystal geometry, indicating large differences in the Auger rates in nanocrystals of similar size. We find that the rate of the negative trion channel is independent of the initial biexciton angular momentum and is generally slower than the rate of the positive trion channel, which, in contrast, is sensitive to the biexciton angular momentum. Further, we demonstrate that by variation of temperature the Auger rate can be varied across a wide range of values.
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.
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.
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)
Identification of excitons, trions and biexcitons in single-layer WS{sub 2}
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)
Vectorial nonlinear coherent response of a strongly confined exciton–biexciton system
The vectorial four-wave mixing response of an individual strongly confined exciton–biexciton system with fine-structure splitting in a GaAs/AlGaAs quantum dot is measured by dual-polarization heterodyne spectral interferometry. The results are compared with theoretical predictions based on the optical Bloch equations. The system is described by a four-level scheme, which is a model system of the nonlinear excitonic response in low-dimensional semiconductors. We measure its coherence properties and determine the underlying dephasing mechanisms. An impact of the inhomogeneous broadening by spectral wandering on the coherent response is investigated. We further discuss the different four-wave mixing pathways, polarization selection rules, the time-resolved polarization state, the vectorial response in two-dimensional four-wave mixing and ensemble properties. (paper)
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)
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
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
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 (
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
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.
The problem of excitonic and biexcitonic binding is studied in the system of parabolic coordinates for a lens-shaped quantum box. The exciton wavefunction is expanded in terms of electron-hole configurations made from electron and hole single-particle states. Configuration interaction method and perturbative calculations are used to study the competition between confinement and correlation effects. Biexcitonic binding energy is calculated in the strong confinement regime and a comparison to the case of a spherical box is made. Absorption spectra with and without correlation effects are computed for InAs/InP quantum dots. Excitonic binding energy and enhancement factor are estimated to be equal to about 20 meV and 1.5, respectively. The excitonic absorption is finally studied in the presence of a uniform vertical electric field. A weak vertical Stark effect is predicted for lens-shaped quantum box described within this model
Cornet, C. [FOTON-UMR 6082 au CNRS, INSA de Rennes, 20 Avenue des Buttes de Coesmes, CS 14315, F-34043 Rennes Cedex (France)]. E-mail: charles.cornet@ens.insa-rennes.fr; Even, J. [FOTON-UMR 6082 au CNRS, INSA de Rennes, 20 Avenue des Buttes de Coesmes, CS 14315, F-34043 Rennes Cedex (France)]. E-mail: jacky.even@insa-rennes.fr; Loualiche, S. [FOTON-UMR 6082 au CNRS, INSA de Rennes, 20 Avenue des Buttes de Coesmes, CS 14315, F-34043 Rennes Cedex (France)
2005-09-19
The problem of excitonic and biexcitonic binding is studied in the system of parabolic coordinates for a lens-shaped quantum box. The exciton wavefunction is expanded in terms of electron-hole configurations made from electron and hole single-particle states. Configuration interaction method and perturbative calculations are used to study the competition between confinement and correlation effects. Biexcitonic binding energy is calculated in the strong confinement regime and a comparison to the case of a spherical box is made. Absorption spectra with and without correlation effects are computed for InAs/InP quantum dots. Excitonic binding energy and enhancement factor are estimated to be equal to about 20 meV and 1.5, respectively. The excitonic absorption is finally studied in the presence of a uniform vertical electric field. A weak vertical Stark effect is predicted for lens-shaped quantum box described within this model.
Laser induced magneto-Raman optical gain of an exciton and a biexciton in a CdTe/ZnTe quantum dot
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.
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...
Excitons, biexcitons, and phonons in ultrathin CdSe/ZnSe quantum structures
Gindele, F.; Woggon, Ulrike; Langbein, Wolfgang Werner; Hvam, Jørn Märcher; Leonhardi, K.; Hommel, D.; Selke, H.
1999-01-01
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...
Birkedal, Dan; Shah, Jagdeep; Pfeiffer, L. N.
1999-01-01
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...
Klenovský, P.; Brehm, M.; Křápek, Vlastimil; Lausecker, E.; Munzar, D.; Hackl, F.; Steiner, H.; Fromherz, T.; Bauer, G.; Humlíček, J.
2012-01-01
Roč. 86, č. 11 (2012), "115305-1"-"115305-8". ISSN 1098-0121 Institutional research plan: CEZ:AV0Z10100521 Keywords : semiconductors nanocrystals * cyclotron resonance * uniaxial-stress * band alignment * Ge islands * germanium * wells * silicon * Si(001) * luminescence Subject RIV: BM - Solid Matter Physics ; Magnetism Impact factor: 3.767, year: 2012 http://prb.aps.org/abstract/PRB/v86/i11/e115305
Spontaneous two photon emission from a single quantum dot
Ota, Y; Kumagai, N; Arakawa, Y
2011-01-01
Spontaneous two photon emission from a solid-state single quantum emitter is observed. We investigated photoluminescence from the neutral biexciton in a single semiconductor quantum dot coupled with a high Q photonic crystal nanocavity. When the cavity is resonant to the half energy of the biexciton, the strong vacuum field in the cavity inspires the biexciton to simultaneously emit two photons into the mode, resulting in clear emission enhancement of the mode. Meanwhile, suppression was observed of other single photon emission from the biexciton, as the two photon emission process becomes faster than the others at the resonance.
Interaction and Dephasing of Excitons in ZnSe Quantum Wires
Wagner, Hans Peter; Langbein, Wolfgang; Hvam, Jørn Märcher; Bacher, G.; Kümmell, T.; Forchel, A.; Gershoni, David
1999-01-01
We study the coherent formation of biexcitons in wet-etched ZnSe quantum wires of lateral sizes down to 23 nm by transient degenerate four-wave mixing. We observe an increase of the biexciton binding energy with decreasing wire width reaching 30% energy enhancement in the smallest wire structure...
Multi-excitonic effects on optical spectra of semiconducting carbon nanotubes
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.
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.
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.
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
Interaction between excitons determines the non-linear response of nanocrystals
The non-linear response of semiconductor quantum dots is investigated using three-pulse photon echo peak shift (3PEPS) experiments and simulations. The third-order non-linear response is modeled by a three-level system, utilizing Brownian oscillators to model the line-broadening functions. Our results show that biexciton formation and exciton-exciton scattering significantly influence the non-linear response of quantum dots. The exciton to biexciton excited state absorption pathways are also investigated for quantum dots with different crystal structures. Our calculations suggest that the probability of excited state absorption to the biexcitonic state is higher for zinc-blende structured nanocrystals
Identifying multiexcitons in Mo S2 monolayers at room temperature
Lee, Hyun Seok; Kim, Min Su; Kim, Hyun; Lee, Young Hee
2016-04-01
One of the unique features of atomically thin two-dimensional materials is strong Coulomb interactions due to the reduced dielectric screening effect; this feature enables the study of many-body phenomena such as excitons, trions, and biexcitons. However, identification of biexcitons remains unresolved owing to their broad peak feature at room temperature. Here, we investigate multiexcitons in monolayer Mo S2 using both electrical and optical doping and identify the transition energies for each exciton. The binding energy of the assigned biexciton is twice that of the trion, in quantitative agreement with theoretical predictions. The biexciton population is predominant under optical doping but negligible under electrical doping. The biexciton population is quadratically proportional to the exciton population, obeying the mass-action theory. Our results illustrate the stable formation of not only trions but also biexcitons due to strong Coulomb interaction even at room temperature; therefore, these results provide a deeper understanding of the complex excitonic behaviors in two-dimensional semiconductors.
Exciton effects on dipole-allowed optical absorptions in a two-dimensional parabolic quantum dot
Yuan, Jian-Hui, E-mail: jianhui831110@163.com [The Department of Physics, Guangxi Medical University, Nanning, Guangxi 530021 (China); Zhang, Yan; Huang, Daizheng [The Department of Physics, Guangxi Medical University, Nanning, Guangxi 530021 (China); Zhang, Jianjun [School of Physics, Huazhong University of Science and Technology, Wuhan 430074 (China); Zhang, Xin [The 34th Institute of China Electronics and Technology Group Corporation, Guilin, Guangxi 541004 (China)
2013-11-15
Exciton effects on the linear and nonlinear optical absorptions (the transition from the S state (L=0) to the P state (L=1)) in two-dimensional quantum dots are theoretically studied by using the configuration-integration methods (CI) and the compact density-matrix approach. The results show that the optical absorption coefficient, which can be controlled by the confinement potential strength and the incident optical intensity, is enhanced obviously when the exciton effect is taken into account. We find that both a trapped electron–hole pair and the incident optical intensity can bleach the exciton absorption and the appearance of the new absorption may be due to biexciton. -- Highlights: • This paper investigates exciton effects on dipole-allowed optical absorptions in quantum dots. • Both a trapped electron–hole pair and the incident optical intensity can bleach the exciton absorption. • The appearance of the new biexciton absorption may be due to biexciton.
Su, Dan; Dou, Xiuming; Wu, Xuefei; Liao, Yongping; Zhou, Pengyu; Ding, Kun; Ni, Haiqiao; Niu, Zhichuan; Zhu, Haijun; Jiang, Desheng; Sun, Baoquan
2016-04-01
Exciton and biexciton emission energies as well as excitonic fine-structure splitting (FSS) in single InAs/GaAs quantum dots (QDs) have been continuously tuned in situ in an optical cryostat using a developed uniaxial stress device. With increasing tensile stress, the red shift of excitonic emission is up to 5 nm; FSS decreases firstly and then increases monotonically, reaching a minimum value of approximately 10 μeV; biexciton binding energy decreases from 460 to 106 μeV. This technique provides a simple and convenient means to tune QD structural symmetry, exciton energy and biexciton binding energy and can be used for generating entangled and indistinguishable photons.
Transient four-wave mixing in T-shaped GaAs quantum wires
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...
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.
Tuning the optical properties of dilute nitride site controlled quantum dots
We show that deterministic control of the properties of pyramidal site-controlled quantum dots (QD) could be achieved by exposing the QD layer to nitrogen precursor unsymmetrical dimethylhydrazine (UDMHy). The properties that could be tuned include an expected emission reduction in dilute nitride materials, excitonic pattern (biexciton binding energy) and improved carrier confinement potential symmetry (reduced fine-structure splitting)
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.
All-optical tailoring of single-photon spectra in a quantum-dot microcavity system
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...
Photothermal Absorption Spectroscopy of Individual Semiconductor Nanocrystals
Berciaud, Stéphane; Cognet, Laurent; Lounis, Brahim
2007-01-01
Photothermal heterodyne detection is used to record the first room-temperature absorption spectra of single CdSe/ZnS semiconductor nanocrystals. These spectra are recorded in the high cw excitation regime, and the observed bands are assigned to transitions involving biexciton and trion states. Comparison with the single nanocrystals photoluminescence spectra leads to the measurement of spectral Stokes shifts free from ensemble averaging.
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...
Collective aspects of singlet fission in molecular crystals
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
Contrastive analysis of multiple exciton generation theories
Tan, Hengyu; Chang, Qing
2015-10-01
Multiple exciton generation (MEG) is an effect that semiconductor nanocrystals (NCs) quantum dots (QDs) generate multiple excitons (electron-hole pairs) through absorbing a single high energy photon. It can translate the excess photon energy of bandgap (Eg) into new excitons instead of heat loss and improve the photovoltaic performance of solar cells. However, the theories of MEG are not uniform. The main MEG theories can be divided into three types. The first is impact ionization. It explains MEG through a conventional way that a photogenerated exciton becomes multiple excitons by Coulomb interactions between carriers. The Second is coherent superposition of excitonic states. Multiple excitons are generated by the coherent superposition of single photogenerated exciton state with enough excess momentum and the two-exciton state with the same momentum. The third is excitation via virtual excitonic states. The nanocrystals vacuum generates a virtual biexciton by coulomb coupling between two valence band electrons. The virtual biexciton absorbing a photon with an intraband optical transition is converted into a real biexciton. This paper describes the MEG influence on solar photoelectric conversion efficiency, concludes and analyzes the fundamentals of different MEG theories, the MEG experimental measure, their merits and demerits, calculation methods of generation efficiency.
Dominant factors limiting the optical gain in layered two-dimensional halide perovskite thin films.
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
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
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
All-optical tailoring of single-photon spectra in a quantum-dot microcavity system
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.
All-optical depletion of dark excitons from a semiconductor quantum dot
Semiconductor quantum dots are considered to be the leading venue for fabricating on-demand sources of single photons. However, the generation of long-lived dark excitons imposes significant limits on the efficiency of these sources. We demonstrate a technique that optically pumps the dark exciton population and converts it to a bright exciton population, using intermediate excited biexciton states. We show experimentally that our method considerably reduces the dark exciton population while doubling the triggered bright exciton emission, approaching thereby near-unit fidelity of quantum dot depletion
Time-bin Entanglement from Quantum Dots
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.
Electrically driven single photon emission from a CdSe/ZnSSe single quantum dot at 200 K
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.
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
Coherent dynamics in semiconductors
Hvam, Jørn Märcher
1998-01-01
Ultrafast nonlinear optical spectroscopy is used to study the coherent dynamics of optically excited electron-hole pairs in semiconductors. Coulomb interaction implies that the optical inter-band transitions are dominated, at least at low temperatures, by excitonic effects. They are further...... 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...... as a tool to study the coherent exciton dynamics, and the importance of performing transform limited spectroscopy is demonstrated throughout....
Coherent dynamics in semiconductors
Hvam, Jørn Märcher
1998-01-01
Ultrafast nonlinear optical spectroscopy is used to study the coherent dynamics of optically excited electron-hole pairs in semiconductors. Coulomb interaction implies that the optical inter-band transitions are dominated, at least at low temperatures, by excitonic effects. They are further...... 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...
Spectral tuning of site-selected single InAs/InP quantum dots via intermixing
Mnaymneh, K.; Dalacu, D.; Poole, P. J.; Lapointe, J.; Cheriton, R.; Williams, R. L.
2011-02-01
In this paper, we present experimental results from site-selected single quantum dots that have undergone a number of intermixing process steps via rapid thermal annealing. We show that the intermixing process blueshifts the dot's emission spectrum without affecting the linewidth as well as decreasing its biexciton binding energy and s-p shell spacing. The anisotropic exchange splitting is shown to have undergone a sign inversion implying that the splitting had gone through zero. Intermixing provides another nanoengineering tool for the design of scalable solid-state photon and entangled photon pair sources.
Entangled photons from quantum dot devices: efficiency of post-selection
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.)
2D optical photon echo spectroscopy of a self-assembled quantum dot
Fingerhut, Benjamin P.; Mukamel, Shaul [Department of Chemistry, University of California, Irvine, California, 92697-2025 (United States); Richter, Marten [Department of Chemistry, University of California, Irvine, California, 92697-2025 (United States); Institut fuer Theoretische Physik, Nichtlineare Optik und Quantenelektronik, Technische Universitaet Berlin, Hardenbergstr. 36, 10623, Berlin (Germany); Luo, Jun-Wei [National Renewable Energy Laboratory, Golden, Colorado, 80401 (United States); Zunger, Alex [University of Colorado, Boulder, Colorado, 80309 (United States)
2013-02-15
Simulations of two dimensional coherent photon echo (2D-PE) spectra of self-assembled InAs/GaAs quantum dots (QD) in different charged states are presented revealing the coupling between the individual mono-exciton X{sup q} transitions and contributions of bi-excitons XX{sup q}. The information about the XX{sup q} states is crucial for various application scenarios of QDs, like e.g. highly efficient solar cells. The simulations rely on a microscopic description of the electronic structure by high-level atomistic many-body pseudopotential calculations. It is shown that asymmetric diagonal peak shapes and double cross-peaks are the result of XX{sup q} state contributions to the PE signal by analyzing the contributions of the individual pathways excited state emission, ground state bleach and excited state absorption. The results show that from the detuned X{sup q} and XX{sup q} contributions the bi-exciton binding energies of the XX{sup q} manifold are revealed in 2D-PE signals. (copyright 2012 by WILEY-VCH Verlag GmbH and Co. KGaA, Weinheim)
Light-hole exciton mixing and dynamics in Mn-doped quantum dots
Moldoveanu, V.; Dinu, I. V.; Dragomir, R.; Tanatar, B.
2016-04-01
We investigate theoretically the spectral and dynamical effects of the short-range exchange interaction between a single manganese (Mn) atom hosted by cylindrical CdTe quantum dots and its light-hole excitons or biexcitons. Our approach is based on the Kohn-Luttinger k .p theory and configuration interaction method, the dynamics of the system in the presence of intraband relaxation being derived from the von Neumann-Lindblad equation. The complex structure of the light-hole exciton absorption spectrum reveals the exchange-induced exciton mixing and depends strongly on the Mn position. In particular, if the Mn atom is closer to the edges of the cylinder, the bright and dark light-hole excitons are mixed by the hole-Mn exchange alone. Consequently, their populations exhibit exchange-induced Rabi oscillations which can be viewed as optical signatures of light-hole spin reversal. Similar results are obtained for mixed biexcitons, in this case the exchange-induced Rabi oscillations being damped by the intraband hole relaxation processes. The effect of light-hole heavy-hole mixing is also discussed.
Effect of electron-hole separation on optical properties of individual Cd(Se,Te) quantum dots
Ściesiek, M.; Suffczyński, J.; Pacuski, W.; Parlińska-Wojtan, M.; Smoleński, T.; Kossacki, P.; Golnik, A.
2016-05-01
Cd(Se,Te) quantum dots (QDs) in a ZnSe barrier typically exhibit a very high spectral density, which precludes investigation of single dot photoluminescence. We design, grow, and study individual Cd(Se,Te)/ZnSe QDs of low spectral density of emission lines achieved by the implementation of Mn-assisted epitaxial growth. We find an unusually large variation of exciton-biexciton energy difference (3 meV≤Δ EX -X X≤26 meV) and of exciton radiative recombination rate in the statistics of QDs. We observe a strong correlation between the exciton-biexciton energy difference, exciton recombination rate, splitting between dark and bright excitons, and additionally the exciton fine-structure splitting δ1 and the Landé factor. The above results indicate that the values of the δ1 and of the Landé factor in the studied QDs are dictated primarily by the electron and hole respective spatial shift and wave functions overlap, which vary from dot to dot due to a different degree of localization of electrons and holes in, respectively, CdSe- and CdTe-rich QD regions.
Vector pulsing soliton of self-induced transparency in waveguide
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
We extend excited-state structural analysis to quantify the charge-resonance and multi-exciton character in wave functions of weakly interacting chromophores such as molecular dimers. The approach employs charge and spin cumulants which describe inter-fragment electronic correlations in molecular complexes. We introduce indexes corresponding to the weights of local, charge resonance, and biexciton (with different spin structure) configurations that can be computed for general wave functions thus allowing one to quantify the character of doubly excited states. The utility of the approach is illustrated by applications to several small dimers, e.g., He-H2, (H2)2, and (C2H4)2, using full and restricted configuration interaction schemes. In addition, we present calculations for several systems relevant to singlet fission, such as tetracene, 1,6-diphenyl-1,3,5-hexatriene, and 1,3-diphenylisobenzofuran dimers
Intramolecular vibrations and noise effects on pattern formation in a molecular helix.
Fouda, H P Ekobena; Tabi, C B; Mohamadou, A; Kofané, T C
2011-09-21
Modulational instability in a biexciton molecular chain is addressed. We show that the model can be reduced to a set of three coupled equations: two nonlinear Schrödinger equations and a Boussinesq equation. The linear stability analysis of continuous wave solutions of the coupled systems is performed and the growth rate of instability is found numerically. Simulations of the full discrete systems reveal some behaviors of modulational instability, since wave patterns are observed for the excitons and the phonon spectrum. We also take the effect of thermal fluctuations into account and we numerically study both the stability and the instability of the plane waves under 300 K. The plane wave is found to be stable under modulation, but displays a gradual increase of the wave amplitudes. Under modulation, the same behaviors are observed and wave patterns are found to resist thermal fluctuations, which is in agreement with earlier research on localized structure stability under thermal noise. PMID:21878712
Luzanov, Anatoliy V. [STC “Institute for Single Crystals,” National Academy of Sciences, Kharkov 61001 (Ukraine); Casanova, David [Kimika Fakultatea, Euskal Herriko Unibertsitatea (UPV/EHU) and Donostia International Physics Center (DIPC), P.K. 1072, 20080 Donostia (Spain); IKERBASQUE, Basque Foundation for Science, 48013 Bilbao, Euskadi (Spain); Feng, Xintian; Krylov, Anna I. [Department of Chemistry, University of Southern California, Los Angeles, California 90089-0482 (United States)
2015-06-14
We extend excited-state structural analysis to quantify the charge-resonance and multi-exciton character in wave functions of weakly interacting chromophores such as molecular dimers. The approach employs charge and spin cumulants which describe inter-fragment electronic correlations in molecular complexes. We introduce indexes corresponding to the weights of local, charge resonance, and biexciton (with different spin structure) configurations that can be computed for general wave functions thus allowing one to quantify the character of doubly excited states. The utility of the approach is illustrated by applications to several small dimers, e.g., He-H{sub 2}, (H{sub 2}){sub 2}, and (C{sub 2}H{sub 4}){sub 2}, using full and restricted configuration interaction schemes. In addition, we present calculations for several systems relevant to singlet fission, such as tetracene, 1,6-diphenyl-1,3,5-hexatriene, and 1,3-diphenylisobenzofuran dimers.
Luzanov, Anatoliy V; Casanova, David; Feng, Xintian; Krylov, Anna I
2015-06-14
We extend excited-state structural analysis to quantify the charge-resonance and multi-exciton character in wave functions of weakly interacting chromophores such as molecular dimers. The approach employs charge and spin cumulants which describe inter-fragment electronic correlations in molecular complexes. We introduce indexes corresponding to the weights of local, charge resonance, and biexciton (with different spin structure) configurations that can be computed for general wave functions thus allowing one to quantify the character of doubly excited states. The utility of the approach is illustrated by applications to several small dimers, e.g., He-H2, (H2)2, and (C2H4)2, using full and restricted configuration interaction schemes. In addition, we present calculations for several systems relevant to singlet fission, such as tetracene, 1,6-diphenyl-1,3,5-hexatriene, and 1,3-diphenylisobenzofuran dimers. PMID:26071698
Type 2 quantum dots in Ge/Si system
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
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.
Low Density Self-Assembled InAs/GaAs Quantum Dots Grown by Metal Organic Chemical Vapour Deposition
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.
Ultrafast Exciton Dynamics in CdxHg(1-x)Te alloy Quantum Dots
Leontiadou, Marina A.; Al-Otaify, Ali; Kershaw, Stephen V.; Zhovtiuk, Olga; Kalytchuk, Sergii; Mott, Derrick; Maenosono, Shinya; Rogach, Andrey L.; Binks, David J.
2016-05-01
Ultrafast transient absorption spectroscopy is used to investigate sub-nanosecond exciton dynamics in CdxHg(1-x)Te alloy colloidal quantum dots. A bleach was observed at the band gap due to state-filling, the mono-exponential decay of which had a characteristic lifetime of 91 ± 1 ps and was attributed to biexciton recombination; no evidence of surface-related trapping was observed. The rise time of the bleach, which is determined by the rate at which hot electrons cool to the band-edge, ranged between 1 and 5 ps depending on the pump photon energy. Measuring the magnitude of the bleach decay for different pump fluences and wavelengths allowed the quantum yield of multiple exciton generation to be determined, and was 115 ± 1% for pump photons with energy equivalent to 2.6 times the band gap.
Thermal annealing of selected individual quantum dots
Cathodoluminescence spectra of single InAs/GaAs quantum dots were recorded before and after consecutive thermal annealing steps. The annealing process leads to an overall blueshift of the spectra indicating In/Ga interdiffusion. Excitonic fine-structure splitting and binding energies of charged and neutral excitonic complexes were monitored. A drastic reduction of the fine-structure splitting from 170 μeV to less than 20 μeV can be observed accompanied by a change of the character of the biexciton from anti-binding to binding with respect to the exciton. Tailoring the fine-structure splitting is especially important for the use of single quantum dots in opto-electronic devices for quantum key distribution where a degeneracy of the exciton ground state (i.e. a fine-structure splitting below the homogeneous linewidth) is required for the on-demand production of entangled photon pairs
Single entangled photon pair emission from an InGaAs/GaAs quantum dot up to temperatures of 30 K
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.)
Carrier dynamics in highly quantum-confined, colloidal indium antimonide nanocrystals.
Chang, Angela Y; Liu, Wenyong; Talapin, Dmitri V; Schaller, Richard D
2014-08-26
Nanometer-sized particles of indium antimonide (InSb) offer opportunities in areas such as solar energy conversion and single photon sources. Here, we measure electron-hole pair dynamics, spectra, and absorption cross sections of strongly quantum-confined colloidal InSb nanocrystal quantum dots using femtosecond transient absorption. For all samples, we observe a bleach feature that develops on ultrafast time scales, which notably moves to lower energy during the first several picoseconds following excitation. We associate this unusual red shift, which becomes larger for larger particles and more distinct at lower sample temperatures, with hot exciton cooling through states that we suggest arise from energetically proximal conduction band levels. From controlled optical excitation intensities, we determine biexciton lifetimes, which range from 2 to 20 ps for the studied 3-6 nm diameter particle sizes. PMID:25106893
A bright triggered twin-photon source in the solid state
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 ...
Tailored quantum dots for entangled photon pair creation
Greilich, A; Bayer, M; Berstermann, T; Oulton, R F; Reuter, D; Schwab, M; Stavarache, V; Wieck, A; Yakovlev, D R
2006-01-01
We compare the asymmetry-induced exchange splitting delta_1 of the bright-exciton ground-state doublet in self-assembled (In,Ga)As/GaAs quantum dots, determined by Faraday rotation, with its homogeneous linewidth gamma, obtained from the radiative decay in time-resolved photoluminescence. Post-growth thermal annealing of the dot structures leads to a considerable increase of the homogeneous linewidth, while a strong reduction of the exchange splitting is simultaneously observed. The annealing can be tailored such that delta_1 and gamma become comparable, whereupon the carriers are still well confined. This opens the possibility to observe polarization entangled photon pairs through the biexciton decay cascade.
Micro-photoluminescence study of single self-organized InAs/InP quantum sticks
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
Vector pulsing soliton of self-induced transparency in waveguide
Adamashvili, G.T., E-mail: guram_adamashvili@ymail.com
2015-01-23
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.
Conditions for entangled photon emission from (111)B site-controlled pyramidal quantum dots
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.
Dressed excitonic states and quantum interference in a three-level quantum dot ladder system
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.
Intramolecular vibrations and noise effects on pattern formation in a molecular helix
Ekobena Fouda, H P; Tabi, C B [Laboratory of Biophysics, Department of Physics, Faculty of Science, University of Yaounde I, PO Box 812, Yaounde (Cameroon); Mohamadou, A [Condensed Matter Laboratory, Department of Physics, Faculty of Science, University of Douala, PO Box 24157, Douala (Cameroon); Kofane, T C, E-mail: hekobena@gmail.com, E-mail: contab408@hotmail.com, E-mail: mohdoufr@yahoo.fr, E-mail: tckofane@yahoo.com [Laboratory of Mechanics, Department of Physics, Faculty of Science, University of Yaoune I, PO Box 812, Yaounde (Cameroon)
2011-09-21
Modulational instability in a biexciton molecular chain is addressed. We show that the model can be reduced to a set of three coupled equations: two nonlinear Schroedinger equations and a Boussinesq equation. The linear stability analysis of continuous wave solutions of the coupled systems is performed and the growth rate of instability is found numerically. Simulations of the full discrete systems reveal some behaviors of modulational instability, since wave patterns are observed for the excitons and the phonon spectrum. We also take the effect of thermal fluctuations into account and we numerically study both the stability and the instability of the plane waves under 300 K. The plane wave is found to be stable under modulation, but displays a gradual increase of the wave amplitudes. Under modulation, the same behaviors are observed and wave patterns are found to resist thermal fluctuations, which is in agreement with earlier research on localized structure stability under thermal noise. (paper)
Theoretical studies of excitons in type II CdSe/CdTe quantum dots
We present a method for calculating exciton and bi-exciton energies in type-II colloidal quantum dots. Our methodology is based on an 8-band k · p Hamiltonian of the zinc- blend structure, which incorporates the effects of spin-orbit interaction, strain between the core and the shell and piezoelectric potentials. Exciton states are found using the configuration interaction (CI) method that explicitly includes the effects of Coulomb interaction, as well as exchange and correlation between many-electron configurations. We pay particular attention to accurate modelling of the electrostatic interaction between quasiparticles. The model includes surface polarization and self-polarization effects due to the large difference in dielectric constants at the boundary of the QD.
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
Ultrafast spectroscopy of self-assembled quantum dots
The scope of this thesis is to show the limitations of ensemble spectroscopic attempts with high excitation intensities in self-assembled Indiumarsenide-Galliumarsenide quantum dots, as well as to provide a solution to circumvent these problems through the construction of an optical spectroscopy setup that is capable of accessing individual quantum dots. Fundamental quantum optics experiments, which can be realized with quantum dots, require the application of strong coherent radiation fields. Time-resolved spectral hole burning spectroscopy is employed on a self-assembled quantum dot sample, to coherently control the excitonic ground state. The corresponding high intensity optical field results in the observation of parasitic effects. The most signicant manifestations are the emergence of a broadened absorption line and luminescence from the quantum dots at energies higher than the excitation energy. These effects are explained through a two-photon absorption mediated carrier relaxation. The carriers, generated through two-photon absorption in the Galliumarsenide host matrix, relax back into the quantum dots, where they either decay radiative (causing luminescence) or supplement resonantly created excitons and thereby shift their energies (absorption line broadening), which destructs any coherence. Another observation is the two-photon biexciton creation. Optical selection rules permit the simultaneous absorption of two photons with subsequent creation of a biexciton. This is also portrayed through the emergence of two additional spectral holes. Unlike the two-photon mediated charging, however, it does not influence the resonantly created excitons. The second part is dealing with the development and characterization of a time- and energy-resolved pump-probe setup which is capable of measuring single quantum dot absorption. This setup uses acousto-optic modulators as amplitude modulators with frequencies in the Megahertz region and spectral shapers for both, pump
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.
Suppression of auger recombination in ""giant"" core/shell nanocrystals
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.
Elastic strain engineering of quantum dot excitonic emission in nanomembranes and optical resonators
We study the effect of an external biaxial stress on the light emission of single InGaAs/GaAs(001) quantum dots (QD) embedded in a 200 nm-thick-membrane. Reversible and bi-directional spectral tuning of QD excitonic emission is demonstrated via a simple electro-mechanical device. The most intriguing finding is that biaxial strain is a reliable tool to engineer the QD electronic structure and reach color coincidence between exciton and biexciton emission, providing a vital prerequisite for the generation of polarization entangled photon pairs through a time reordering strategy. The physical origin of this new phenomenon is discussed based on the empirical pseudopotential calculations. With similar technique we study the effect of biaxial stress on single QDs embedded in microring resonators. The microrings can be reversibly stretched or squeezed, resulting in a controllable engineering of both QD emissions and optical modes. Our results open up a new tuning strategy to study cQED with semiconductor quantum dots.
Whispering gallery mode lasing from hexagonal shaped layered lead iodide crystals.
Liu, Xinfeng; Ha, Son Tung; Zhang, Qing; de la Mata, Maria; Magen, César; Arbiol, Jordi; Sum, Tze Chien; Xiong, Qihua
2015-01-27
We report on the synthesis and optical gain properties of regularly shaped lead iodide (PbI2) platelets with thickness ranging from 10-500 nm synthesized by chemical vapor deposition methods. The as-prepared single crystalline platelets exhibit a near band edge emission of ∼ 500 nm. Whispering gallery mode (WGM) lasing from individual hexagonal shaped PbI2 platelets is demonstrated in the temperature-range of 77-210 K, where the lasing modes are supported by platelets as thin as 45 nm. The finite-difference time-domain simulation and the edge-length dependent threshold confirm the planar WGM lasing mechanism in such hexagonal shaped PbI2 platelet. Through a comprehensive study of power-dependent photoluminescence (PL) and time-resolved PL spectroscopy, we ascribe the WGM lasing to be biexcitonic in nature. Moreover, for different thicknesses of platelet, the lowest lasing threshold occurs in platelets of ∼ 120 nm, which attributes to the formation of a good Fabry-Pérot resonance cavity in the vertical direction between the top and bottom platelet surfaces that enhances the reflection. Our present study demonstrates the feasibility of planar light sources based on layered semiconductor materials and that their thickness-dependent threshold characteristic is beneficial for the optimization of layered material based optoelectronic devices. PMID:25562110
Scintillation response of liquid xenon to low energy nuclear recoils
Liquid Xenon (LXe) is expected to be an excellent target and detection medium to search for dark matter in the form of Weakly Interacting Massive Particles (WIMPs). We have measured the scintillation efficiency of nuclear recoils with kinetic energy between 10.4 and 56.5 keV relative to that of 122 keV gamma rays from 57Co. The scintillation yield of 56.5 keV recoils was also measured as a function of applied electric field, and compared to that of gamma rays and alpha particles. The Xe recoils were produced by elastic scattering of 2.4 MeV neutrons in liquid xenon at a variety of scattering angles. The relative scintillation efficiency is 0.130±0.024 and 0.227±0.016 for the lowest and highest energy recoils, respectively. This is about 15% less than the value predicted by Lindhard, based on nuclear quenching. Our results are in good agreement with more recent theoretical predictions that consider the additional reduction of scintillation yield due to biexcitonic collisions in LXe
Control of single quantum dot emission characteristics and fine structure by lateral electric fields
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.)
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.
Multiple exciton generation and ultrafast exciton dynamics in HgTe colloidal quantum dots.
Al-Otaify, Ali; Kershaw, Stephen V; Gupta, Shuchi; Rogach, Andrey L; Allan, Guy; Delerue, Christophe; Binks, David J
2013-10-21
The investigation of sub-nanosecond exciton dynamics in HgTe colloidal quantum dots using ultrafast transient absorption spectroscopy is reported. The transmittance change spectrum acquired immediately after pumping is dominated by a bleach blue-shifted by ~200-300 nm from the photoluminescent emission band. Comparison with a tight-binding model of the electronic structure allows this feature to be attributed to the filling of band edge states. The form of the pump-induced transmittance transients is dependent on the excitation rate and the rate of sample stirring. For moderate pumping of stirred samples, the transmittance transients are well-described by a mono-exponential decay associated with biexciton recombination, with a lifetime of 49 ± 2 ps. For samples that are strongly-pumped or unstirred, the decay becomes bi-exponential in form, indicating that trap-related recombination has become significant. We also present a new analysis that enables fractional transmittance changes to be related to band edge occupation for samples with arbitrary optical density at the pump wavelength. This allows us to identify the occurrence of multiple exciton generation, which results in a quantum yield of 1.36 ± 0.04 for a photon energy equivalent to 3.1 times the band gap, in good agreement with the results of the model. PMID:23999734
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.
Optical control of nonlinearly dressed states in an individual quantum dot
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.
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
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
Wavelength tunable InAs/InP(1 0 0) quantum dots in 1.55-μm telecom devices
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
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.
Electrical and optical measurements on a single InAs quantum dot using ion-implanted micro-LEDs
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.)
Optical properties of charged semiconductor quantum dots
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.
Growth and characterization of InP/In0.48Ga0.52P quantum dots optimized for single-photon emission
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.
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.)
Ellis, Benjamin H; Aggarwal, Somil; Chakraborty, Arindam
2016-01-12
Multicomponent systems are defined as chemical systems that require a quantum mechanical description of two or more different types of particles. Non-Born-Oppenheimer electron-nuclear interactions in molecules, electron-hole interactions in electronically excited nanoparticles, and electron-positron interactions are examples of physical systems that require a multicomponent quantum mechanical formalism. The central challenge in the theoretical treatment of multicomponent systems is capturing the many-body correlation effects that exist not only between particles of identical types (electron-electron) but also between particles of different types (electron-nuclear and electron-hole). In this work, the development and implementation of multicomponent coupled-cluster (mcCC) theory for treating particle-particle correlation in multicomponent systems are presented. This method provides a balanced treatment of many-particle correlation effects in a general multicomponent system while maintaining a size-consistent and size-extensive formalism. The coupled-cluster ansatz presented here is an extension of the electronic structure CCSD formulation for multicomponent systems and is defined as |ΨmcCC⟩ = eT1I+T2I+T1II+T2II+T11I,II+T12I,II+T21I,II+T22I,II|0I0II⟩. The cluster amplitudes in the mcCC wave function were obtained by projecting the mcCC Schrödinger equation onto a direct product space of singly and doubly excited states of type I and II particles and then solving the resulting mcCC equations iteratively. These equations were derived using an automated application of the generalized Wick’s theorem and were implemented using a computer-assisted source code generation approach. The applicability of the mcCC method was demonstrated by calculating ground state energies of multicomponent Hooke's atom and positronium hydride systems as well as by calculating exciton and biexciton binding energies in multiexcitonic systems. For each case, the mcCC results were
Short-time dynamics of correlated quantum Coulomb systems
Bonitz, Michael
2007-03-01
Strong correlations in dense Coulomb systems are attracting increasing interest in many fields ranging from dense astrophysical plasmas, dusty plasmas and semiconductors to metal clusters and ultracold trapped ions [1]. Examples are bound states in dense plasmas (atoms, molecules, clusters) and semiconductors (excitons, trions, biexcitons) and many-particle correlations such as Coulomb and Yukawa liquids and crystals. Of particular current interest is the response of these systems to short excitations generated e.g. by femtosecond laser pulses and giving rise to ultrafast relaxation processes and build up of binary correlations. The proper theoretical tool are non-Markovian quantum kinetic equations [1,2] which can be derived from Nonequilibrium Green's Functions (NEGF) and are now successfully solved numerically for dense plasmas and semiconductors [3], correlated electrons [4] and other many-body systems with moderate correlations [5]. This method is well suited to compute the nonlinear response to strong fields selfconsistently including many-body effects [6]. Finally, we discuss recent extensions of the NEGF-computations to the dynamics of strongly correlated Coulomb systems, such as single atoms and molecules [7] and electron and exciton Wigner crystals in quantum dots [8,9]. [1] H. Haug and A.-P. Jauho, Quantum Kinetics in Transport and Optics of Semiconductors, Springer 1996; M. Bonitz Quantum Kinetic Theory, Teubner, Stuttgart/Leipzig 1998; [2] Progress in Nonequilibrium Green's Functions III, M. Bonitz and A. Filinov (Eds.), J. Phys. Conf. Ser. vol. 35 (2006); [3] M. Bonitz et al. Journal of Physics: Condensed Matter 8, 6057 (1996); R. Binder, H.S. K"ohler, and M. Bonitz, Phys. Rev. B 55, 5110 (1997); [4] N.H. Kwong, and M. Bonitz, Phys. Rev. Lett. 84, 1768 (2000); [5] Introduction to Computational Methods for Many-Body Systems, M. Bonitz and D. Semkat (eds.), Rinton Press, Princeton (2006); [6] H. Haberland, M. Bonitz, and D. Kremp, Phys. Rev. E 64
Spectroscopy and Photochemistry in Single Crystals of Uranyl Formate Monohydrate.
Cox, Jack Neal
1982-03-01
attributed to the g(,(PARLL)) component of U(V). The primary photoproduct may be a U(V)-organic radical pair, coupled by hyperfine and spin-orbit interactions. The pairs are at sites with nearly intrinsic symmetry. They may be the traps responsible for the behavior of the luminescence. A model for the primary photochemical reaction is discussed. The initial step is a biexcitonic encounter between (pi)(,g) and bound-(DELTA)(,g) excitons to form a uranyl doubly excited state that lies in the CT region of the spectrum.
Kim, Danny
This thesis presents optical spectra of single InAs quantum dots on InP with an unprecedented signal-to-noise ratio and spectral resolution that has facilitated comprehensive characterization and made a significant contribution to their understanding. InAs quantum dots on InP are the leading contenders for a variety of quantum electrooptic devices that require wavelengths in the 1.5 mum range, most notably triggered single/entangled photon sources for quantum key distribution. As of yet, spectroscopic data for InAs on InP has only provided proof of emission, but no high quality data has been available, preventing any conclusive understanding of their properties. The work presented in this thesis dramatically improves upon previous reports by key optimizations at each experimental stage: growth, processing, and optical setup. The spectra clearly resolve, for the first time, the structure within the s-shell and p-shell, with fine resolution, allowing quantitative evaluation of exciton complexes such as trions, biexcitons, and triplet states. By measuring numerous dots, the behavioral trends of these species with respect to dot geometry is deduced. Also, for the first time, magnetic-field dependent spectra are obtained for individual InAs/InP dots. A remarkable discovery was the strong relation of the exciton g-factor to dot height. This thesis also demonstrates deterministic nanometer-scale control of the quantum dot dimensions---with the goal being to exploit the structure/quantum property relation in these dots. This was accomplished by using the apex of an in-situ grown nanoscale InP pyramid as a nucleation site. The dimension of this top (001) surface on which the dot nucleates is responsive to manometer-scale changes in the pyramid base dimensions, which can be precisely controlled with lithography. The InAs grown on top of these mesas then conform to the size, where the available area can be purposely relaxed or constrained. For similar height, the resulting
Process-Dependent Properties in Colloidally Synthesized “Giant” Core/Shell Nanocrystal Quantum Dots
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
Single-dot spectroscopy is now able to resolve the energies of excitons, multiexcitons, and charging of semiconductor quantum dots with ∼<1 meV resolution. We discuss the physical content of these energies and show how they can be calculated via quantum Monte Carlo (QMC) and configuration interaction (CI) methods. The spectroscopic energies have three pieces: (i) a ''perturbative part'' reflecting carrier-carrier direct and exchange Coulomb energies obtained from fixed single-particle orbitals, (ii) a ''self-consistency correction'' when the single particle orbitals are allowed to adjust to the presence of carrier-carrier interaction, and (iii) a ''correlation correction.'' We first apply the QMC and CI methods to a model single-particle Hamiltonian: a spherical dot with a finite barrier and single-band effective mass. This allows us to test the convergence of the CI and to establish the relative importance of the three terms (i)--(iii) above. Next, we apply the CI method to a realistic single-particle Hamiltonian for a CdSe dot, including via a pseudopotential description the atomistic features, multiband coupling, spin-orbit effects, and surface passivation. We include all bound states (up to 40000 Slater determinants) in the CI expansion. Our study shows that (1) typical exciton transition energies, which are ∼1 eV, can be calculated to better than 95% by perturbation theory, with only a ∼2 meV correlation correction; (2) typical electron addition energies are ∼40 meV, of which correlation contributes very little (∼1 meV); (3) typical biexciton binding energies are positive and ∼10 meV and almost entirely due to correlation energy, and exciton addition energies are ∼30 meV with nearly all contribution due to correlation; (4) while QMC is currently limited to a single-band effective-mass Hamiltonian, CI may be used with much more realistic models, which capture the correct symmetries and electronic structure of the dots, leading to qualitatively
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.
Investigations into photo-excited state dynamics in colloidal quantum dots
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