Influence of the dark exciton state on the optical and quantum optical properties of single quantum dots

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

Electronic structure and absorption spectrum of biexciton obtained by using exciton basis

We approach the biexciton Schrödinger equation not through the free-carrier basis as usually done, but through the free-exciton basis, exciton–exciton interactions being treated according to the recently developed composite boson many-body formalism which allows an exact handling of carrier exchange between excitons, as induced by the Pauli exclusion principle. We numerically solve the resulting biexciton Schrödinger equation with the exciton levels restricted to the ground state and we derive the biexciton ground state as well as the bound and unbound excited states as a function of hole-to-electron mass ratio. The biexciton ground-state energy we find, agrees reasonably well with variational results. Next, we use the obtained biexciton wave functions to calculate optical absorption in the presence of a dilute exciton gas in quantum well. We find an asymmetric peak with a characteristic low-energy tail, identified with the biexciton ground state, and a set of Lorentzian-like peaks associated with biexciton unbound states, i.e., exciton–exciton scattering states. Last, we propose a pump–probe experiment to probe the momentum distribution of the exciton condensate.     

Using two-dimensional photon echo spectroscopy to probe the fine structure of the ground state biexciton of CdSe nanocrystals

The origin of the fine structure of the ground state single- and biexciton of CdSe nanocrystals is reviewed, along with the theoretical framework used to describe these states. Calculations were performed to determine the transition dipole moments of optically allowed transitions from the single- to biexciton fine structure states. Two-dimensional photon echo spectroscopy measurements for a sample of CdSe nanocrystals are reported. The two-dimensional electronic spectrum at a population time of 0 fs is analyzed using a simulation based on k.p theory predictions of the exciton and biexciton manifolds of states. The analysis suggests that a particular excited state absorption transition from the single- to biexciton fine structure dominates the 2D spectra. These excited state absorptions are clearly resolved in 2D spectra and the method therefore has promise for gaining clearer insights into quantum dot spectroscopy.     

Nonlinear optical properties of biexciton states in GaN quantum disks

The ground state energy of an exciton and biexciton states, in a GaN/Al_xGa_1-xN quantum disk are investigated by the variation method, within envelope function and effective mass approximations. Exciton and biexciton binding energy, and the dipole moments related to the transition between ground, exciton and biexciton states, are calculated as a function of quantum disk geometry. The optical nonlinearity via the exciton and biexciton states is studied on the basis of a three level model through the density matrix formalism. The behavior of different terms of third order susceptibility χ⁽³⁾, are studied around resonance frequencies and for different geometries of disk. The effect of values of the decay rates on χ⁽³⁾ are studied. It is found that these values have remarkable effect on the second term of, χ⁽³⁾.     

Relaxation and dephasing of multiexcitons in semiconductor quantum dots

We measure the dephasing time of ground-state excitonic transitions in InGaAs quantum dots under electrical injection in the temperature range from 10 to 70 K. Electrical injection into the barrier region results in a pure dephasing of the excitonic transitions. Once the injected carriers fill the electronic ground state, the biexciton to exciton transition is probed and a correlation of the exciton and biexciton phonon scattering mechanisms is found. Additional filling of the excited states creates multiexcitons that show a fast dephasing due to population relaxation.     

共轭聚合物中受激吸收与受激辐射的量子动力学研究

基于扩展的一维SSH紧束缚模型结合非绝热的分子动力学方法,理论研究了共轭聚合物分子(PPV)在光脉冲作用下受激吸收和受激辐射的量子动力学过程.首先,设定分子初始处于基态,讨论了受激吸收过程中不同的电子受激跃迁模式与光激发脉冲的关系.通过对终态的分析,发现分子受激后只能产生电子-空穴的束缚态,包括:激子、双激子和高能激子.计算了各种激发态的产率,特别是,给出了各种激发态产率与光激发能量的定量关系.此外,基于实验,分别讨论了光激发强度对高能激子和双激子产率的影响,并与实验结果进行了比较.最后,设定分子初始分别处于激子和双激子态,研究了分子内定域能级之间的受激辐射过程,并简单讨论了激子和双激子受激辐射与光激发能量及强度的关系.     

Phase diagram of electron-hole systems: Interplay between exciton Mott transition and quantum pair condensation

Quasi-thermal-equilibrium states of electron-hole (e-h) systems in photoexcited insulators are studied from a theoretical viewpoint, stressing the exciton Bose-Einstein condensation (BEC), the e-h BCS-type pair-condensed state, and the exciton Mott transition between an insulating exciton/biexciton gas phase and a metallic e-h plasma phase. We determine the quasi-equilibrium phase diagram of the e-h system at zero and finite temperatures with applying the dynamical mean-field theory (DMFT) to the e-h Hubbard model with both repulsive and attractive on-site interactions. Effects of inter-site interactions on the exciton Mott transition are also clarified with applying the extended DMFT to the extended e-h Hubbard model.     

Time-resolved studies of single quantum dots in magnetic fields

We present time-resolved and time-integrated spectroscopy of single InAs quantum dots grown in a GaAs matrix. We observe a number of interesting features in the spectra, including the zero field splitting of exciton and biexciton lines due to quantum dot asymmetry. By the application of an in-plane magnetic field, the normally optically active and inactive exciton states become mixed, enabling us to optically probe the normally inaccessible ‘dark’ states. Time resolved measurements on the mixed states show decay times several times longer than the exciton lifetime at zero field, which we show to be consistent with a dark exciton lifetime orders of magnitude longer than that for bright exciton.     

Theory of multi-exciton states in semiconductor nanocrystals

In this article, the fundamental physics of multi-exciton states in semiconductor nano-crystals is reviewed focusing on the mesoscopic enhancement of the excitonic radiative decay rate and the excitonic optical nonlinearity and the mechanism of their saturation with increase of the nanocrystal size. In the case of the radiative decay rate the thermal excitation of excited exciton states having small oscillator strength within the homogeneous linewidth of the exciton ground state is essential in determining the saturation behavior. The weakly correlated exciton pair states are found to cause a cancellation effect in the third-order nonlinear optical susceptibility at the exciton resonance, providing the first consistent understanding of the experimentally observed saturation of the mesoscopic enhancement of the excitonic optical nonlinearity. The presence of the weakly correlated exciton pair states is confirmed convincingly from the good correspondence between theory and experiments on the induced absorption spectra from the exciton state in CuCl nanocrystals. Furthermore, ultrafast relaxation processes of biexcitons are discussed in conjunction with the observed very fast rise of the biexciton gain in nanocrystals. In prospect of future progress in research, the theoretical formulation to calculate the triexciton states as one of the multi-exciton states beyond the biexciton is presented for the first time including the electron-hole exchange interaction.     

Vector classification, doublet splitting of exciton and biexciton subbands in crystals, and selection rules for transitions between them

The analysis of experimental data on absorption, reflection, luminescence in the region of exciton and biexciton phototransitions in CdS, including P-band structure, shows that there is doubled, contrary to known theory, number of free exciton and biexciton states. This discreapancy is removed in the vector model of these states presented in this paper. The selection rules for transitions between exciton (biexciton) states in crystals taking into consideration their L-T splitting are obtained. The spectra of stimulated FIR radiation on excitonic transitions in CdS, previously obtained experimentally, well fit to these selection rules.     

Localization-dependent photoluminescence spectrum of biexcitons in semiconductor quantum wires

We study exciton and biexciton spectra in disordered semiconductor quantum wires by means of nanophotoluminescence spectroscopy. We demonstrate a close link between the exciton localization length along the wire and the occurrence of a biexciton spectral line. The biexciton signature appears only if the corresponding exciton state extends over more than a few tens of nanometers. We also measure a nonmonotonous variation of the biexciton binding energy with decreasing exciton localization length. This behavior is quantitatively well reproduced by the solution of the single-band Schr?dinger equation of the four-particle problem in a one-dimensional confining potential.     

Inversion of the exciton fine structure splitting in quantum dots

The fine structure splitting of exciton state was measured for a large number of single InAs quantum dots in GaAs. It is shown to decrease as the exciton confinement decreases, crucially passing through zero and changing sign. Degeneracy of the exciton spin states is an important step to producing entangled photons from the biexciton cascade. Thermal annealing reduces the exciton confinement and thereby increases the number of degenerate dots in a particular sample.     

Optically induced rotation of an exciton spin in a semiconductor quantum dot

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

Electromagnetically induced transparency in bulk and microcavity semiconductors

We discuss our recent results on electromagnetically induced transparency (EIT) effects based on intrinsic free exciton and biexciton states in semiconductors. The Λ configuration obtained from the 1S and 2P yellow exciton levels of Cu₂O leads to a well-developed EIT regime, akin to the atomic case. The coherent driving of the exciton–biexciton transition in CuCl induces a tunable transparency window within the polaritonic stop-band, due to the presence of a third polariton branch in the dressed system. In a microcavity configuration, this gives rise to three reflectivity dips in the strong coupling regime.     

Eigenstate symmetry probed by biexciton transitions in a single quantum dot

The eigenstate symmetry in CdSe/ZnSe single quantum dots (SQDs) has been studied by low-temperature magnetoluminescence spectroscopy. Regarding both, the fine structure splitting and the polarization properties of the biexciton transition, the influence of exchange and Zeeman interaction on the eigenstate symmetry of the final state of recombination, the ground state of the single exciton, is investigated.     

Crossover from exciton to biexciton polaritons in semiconductor microcavities

Pump-probe measurements in a microcavity containing a quantum well show that a population of circularly polarized ( sigma(+)) excitons can completely inhibit the transition to sigma(-) one-exciton states by transferring the oscillator strength to the biexcitonic resonance. With increasing pump intensity the linear exciton-polariton doublet evolves into a triplet polariton structure and finally into a shifted biexciton-polariton doublet. A theoretical model of interacting excitons demonstrates that the crossover from exciton to biexciton polaritons is driven by three-exciton Coulomb correlation.     

Direct two-photon creation of a biexciton

The nonlinear absorption coefficient for the two-photon creation of biexciton in CuCl is calculated in the approximation of one intermediate, optically active excitonic state. The two-band model with realistic band structure at the band extrema is considered. The exciton-biexciton dipole transition momentum matrix element is expressed by the functional of the exciton and biexciton envelopes. In the numerical calculations the envelope of the Hylleraas-Ore type, modified by Brinkman et al., is used. Our calculated value of the absorption coefficient is about two orders of magnitude smaller than that estimated previously by Hanamura, and agrees better with the experimental value reported by Gale and Mysyrowicz.     

Coherent control in a single semiconductor quantum dot exhibiting excitonic and biexcitonic features

We have developed a simplified theoretical model to analyze the phenomenon of coherent control in a single semiconductor quantum dot excited by a pair of optical pulses. The first pulse populates a biexciton state by two-photon absorption while the second pulse generates population in the exciton state via deexcitation from the biexciton state. We have used density-matrix analysis for a 3-level system to calculate the time dependent biexciton and exciton state populations. The usual 9×9 matrix has been reduced to a 6×6 matrix. The time variation of the population in each state and it’s dependence on the pulse delay manifest coherent control. Numerical estimates made for In_0.5Ga_0.5As/GaAs single quantum dots qualitatively agree with the recent experimental results. PACS 78.67.Hc; 42.50.Md; 78.55.Cr     

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

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_0.905Ge_0.095/Si quantum well. It is shown that, despite the presence of an electron barrier in the Si_0.905Ge_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 _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.     

Oxygen-related band gap state in single crystal rubrene

A molecular exciton signature is established and investigated under different ambient conditions in rubrene single crystals. An oxygen-related band gap state is found to form in the ambient atmosphere. This state acts as an acceptor center and assists in the fast dissociation of excitons, resulting in a higher dark and photoconductivity of oxidized rubrene. The band gap state produces a well-defined photoluminescence band at an energy 0.25 eV below the energy of the 0-0 molecular exciton transition. Two-photon excitation spectroscopy shows that the states are concentrated near the surface of naturally oxidized rubrene.