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.     

Near-field optical mapping of exciton wave functions in a GaAs quantum dot

Near-field photoluminescence imaging spectroscopy of naturally occurring GaAs quantum dots (QDs) is presented. We successfully mapped out center-of -mass wave functions of an exciton confined in a GaAs QD in real space due to the enhancement of spatial resolution up to 30 nm. As a consequence, we discovered that the spatial profile of the exciton emission, which reflects the shape of a monolayer-high island, differs from that of biexciton emission, due to different distributions of the polarization field for the exciton and biexciton recombinations. This novel technique can be extensively applied to wave function engineering in the design and the fabrication of quantum devices.     

高分子中激子和双激子的极化率(解析计算)

高分子的电致发光是载流子在电场中的输运和复合,为了阐明它的机理,需要研究高分子中激子的极化性质,首先求得了激子和双激子的解析解,然后用线性响应的Green函数方法计 算了两者的极化率,解析地证明了一个重要的结论：激子的极化率为正,双激子的极化率为负.从激子跃迁至双激子,高分子的电偶极矩要反转方向. 关键词： 激子 双激子 解析解 负极化率     

Photoluminescence due to exciton–exciton scattering in a GaAs/AlAs multiple quantum well

We have investigated photoluminescence (PL) properties of a GaAs (20 nm)/AlAs (20 nm) multiple quantum well at 10 K under intense excitation conditions. It has been found that a PL band due to exciton–exciton scattering, the so-called P emission, is observed in addition to the biexciton PL under an excitation energy higher than the fundamental heavy-hole exciton by the energy of the longitudinal optical phonon. On the other hand, the P band could never be observed at an excitation energy much higher than the exciton energy, where a band-filling phenomenon appears in the PL spectrum. Furthermore, we confirmed the existence of optical gain leading to stimulated emission in the energy region of the P band using a variable-stripe-length method.     

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.     

Biexcitons in Si

We observe a new peak in the photoluminescence spectrum of intrinsic Si which we attribute to the recombination of an electron-hole pair in a biexciton leaving behind a free exciton. A calculation of the emission line shape based on a simple model is found to be in good agreement with experiment. From this theoretical fit we deduce a binding energy of 1.2 meV and a ‘radius’ of 100 Å for the biexciton.     

Correlated photons from multi-carrier complexes in GaAs quantum dots

We have studied micro-photoluminescence spectra of a self-assembled single GaAs quantum dot under 8 K. With strong pulsed excitation, the micro-photoluminescence spectrum shows bright emission lines originated from an exciton, a positively charged exciton, and a biexciton, together with weak lower energy emissions reflecting multi-excitonic structures with more carriers. We have identified the origins of these weak emission lines, and showed the existence of charged biexciton states, through single photon correlation measurements and excitation power dependence of the photoluminescence intensity. In addition, investigating the radiative recombination process of the charged biexciton, we have determined the electron–hole exchange energy in the GaAs quantum dot.     

InAs 单量子点中级联辐射光子的关联测量

利用分子束外延生长InAs单量子点样品,温度为5 K时,测量了单量子点中单、双激子自发辐射的荧光(PL)光谱.研究了单、双激子发光强度随激发功率的变化及对应发光峰的偏振特性和精细结构劈裂.基于Hanbury-Brown Twiss(HBT) 实验,测量了单、双激子间发光光谱的关联函数,证实了其发光过程为级联发射过程. 关键词： InAs 单量子点 单、双激子 荧光光谱 级联辐射     

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.     

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.     

Coherence of an entangled exciton-photon state

We study the effect of the exciton fine-structure splitting on the polarization entanglement of photon pairs produced by the biexciton cascade in a quantum dot. Entanglement persists despite separations between the intermediate energy levels of up to 4 microeV. Measurements show that entanglement of the photon pair is robust to the dephasing of the intermediate exciton state responsible for the first-order coherence time of either single photon. We present a theoretical framework incorporating the effects of spin scattering, background light, and dephasing. We distinguish between the first-order coherence time, and a parameter which we measure for the first time and define as the cross-coherence time.     

Excitation spectroscopy on the M-band of red HgI2

The luminescence of red HgI₂ is investigated as a function of excitation intensity and -wavelength. At low excitation, emission is due to free and bound exciton recombination, at high levels a “M-band” is dominating. This M-band is partially ascribed to biexciton decay, this assumption being supported by resonances found in the excitation spectra. The biexciton binding energy is determined to be 6±1 meV.     

Signatures of stimulated bosonic exciton-scattering in semiconductor luminescence

We observe signatures of stimulated bosonic scattering of excitons, a precursor of Bose-Einstein-Condensation (BEC), in the photoluminescence of semiconductor quantum wells. The optical decay of a spinless molecule of two excitons (biexciton) into an exciton and a photon with opposite angular momenta is subject to bosonic enhancement in the presence of other excitons. In a gas of biexcitons and spin polarized excitons the bosonic enhancement breaks the symmetry of two equivalent biexciton decay channels leading to circularly polarized luminescence of the biexciton with the sign opposite to the circularly polarized exciton luminescence. Comparison of experiment and many body theory clearly indicates the existence of stimulated exciton-scattering, but excludes the presence of a fully condensed BEC-like state.     

Effect of interchain coupling on a biexciton in organic polymers

The effect of interchain coupling on the formation and the stability of a biexciton is studied in poly (p-phenylene vinylene) chains in the framework of the tight-binding approach. We obtain an intrachain exciton and biexciton as well as an interchain exciton and biexciton through a double-photon excitation. It is found that a biexciton is energetically favourable to two single excitons even when there exists an interchain coupling. There is a turnover value t_⊥C of the interchain coupling for the formation of a biexciton, beyond which two excitons are combined into one biexciton. The binding energy of a biexciton is calculated to decrease with the increase of interchain coupling, which indicates that a biexciton is relatively stable in polymers with a weak interchain coupling. The conclusion is consistent with the experimental observations. In addition, a suggestion about how to improve the yielding efficiency or the formation of biexcitons in actual applications is given.     

Identifying multi‐excitons in quantum dots: the subtle connection between electric dipole moments and emission linewidths

The emission linewidths of excitonic complexes confined in quantum dots (QDs) mirror their interaction with a defect‐induced, fluctuating charge environment, a phenomenon known as spectral diffusion. Interestingly, extended excitonic complexes that comprise several interacting excitons exhibit significantly smaller emission linewidths if compared to the optical fingerprint of their building block, a sole exciton. Hence, it is not the absolute, but the relative electric dipole moment that governs the directly accessible emission linewidths. Exemplarily we investigate this matter based on differing exciton and biexciton emission linewidths of single GaN QDs with varying emission energies, i.e. QD dimensions. Our results establish the full width at half maximum (FWHM) or any other linewidths criterion for the identification of excitonic complexes, a technique that can directly be applied to polar but even non‐polar QD materials. Additionally, we find an emission energy dependent trend for the FWHM ratios of the biexciton and the exciton (XX_FWHM/X_FWHM) in perfect agreement with their relative dipole moment ratios as derived from our 8‐band‐ k · p based treatment of the Coulomb and exchange interaction within these multi‐particle complexes. (© 2015 WILEY‐VCH Verlag GmbH &Co. KGaA, Weinheim)     

Impact of shell thickness on exciton and biexciton binding energies of a ZnSe/ZnS core–shell quantum dot

Impact of shell structure on the exciton and biexciton binding energies has been studied in a ZnSe/ZnS core–shell quantum dot using Wentzel–Kramers–Brillouin (WKB) approximation. For excitons, the binding is caused by the Coulombic as well as the confinement potentials while biexciton binding energy is determined by taking into account the exchange and correlation effects. The exciton binding energy was found to increase initially with increasing shell thickness which reaches saturation at larger shell thickness. On the other hand, the biexciton binding energy exhibits a crossover from the bonding to antibonding state with increasing shell thickness for smaller core radius of the quantum dot.     

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

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

高分子中双激子态对外电场的线性响应

在外电场中,非简并基态共轭高分子中的双激子具有反向极化的奇异特性.利用响应函数求得高分子链的双激子态在任意频率下的动态极化率χ(ω),并通过求ω→0极限,给出双激子态的静态极化率χ,证实了χ确实为负值.并与激子态和基态作了比较,分析了分子负极化率的起因.考察了响应函数在低频时的行为,指出激子和双激子的激发浓度增大会导致材料折射率n(ω)向不同方向变化. 关键词：     

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.     

Time-resolved photoluminescence on the stimulated emission in polycrystalline ZnO nanoparticles

The detailed room temperature stimulated emission including its optical characteristics from ZnO nanoparticles, which were prepared by a homogenous precipitation method, has been investigated by the time-resolved spectroscopy. The light emission originates from a free exciton recombination at a lower excitation level; the amplified spontaneous emission appears at a moderate excitation level, in which the threshold excitation intensity is 0.65 GW cm⁻². The resonant stimulated emission was observed in ZnO nanoparticles at a higher excitation intensity. Also, the emission lifetime is drastically reduced. Compared to the fluorescence decay curves, the time-resolved spectrum of the stimulated emission suggests the Gaussian-like decay time with only a few of picoseconds. The dynamic processes of lasing behavior and the characteristics of lasing emission in ZnO nanoparticles could provide the information on the crystal quality, the exciton and the lasing action in the particles.