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.     

Resonant Rayleigh scattering from excitons in CdxZn1−xTe:ZnTe quantum wells: measurement of homogeneous linewidths

The technique of resonant Rayleigh scattering is used to determine the homogeneous linewidth across the inhomogeneously broadened exciton resonance in a Cd_0.25Zn_0.75Te/ZnTe multiple quantum well structure. An order of magnitude increase of the Rayleigh scattering signal over background is observed on tuning a narrow-band laser through the exciton resonance at low temperatures. Spectral and temporal measurements show the effect to be a true scattering process rather than luminescence. The interface and alloy fluctuations in the quantum well give rise to spatial fluctuations in the dielectric response of the system while the large exciton resonance causes strong enhancement of scattering. The homogeneous linewidth was calculated across the exciton resonance. The technique is compared with the dephasing and hole-burning techniques more commonly used in homogeneous linewidth measurements.     

Influence of acoustic phonons on dephasing of free excitons in quantum wells

A theory of the dephasing rate of quasi-2D free excitons due to acoustic phonon interaction at low exciton densities is presented. Both deformation potential and piezoelectric couplings are considered for the exciton–phonon interaction in quantum wells. Using the derived interaction Hamiltonian obtained recently by us, exciton linewidth and dephasing rate are calculated as a function of the exciton density, exciton temperature, exciton momentum and lattice temperature.     

Exciton linewidth due to scattering from free carriers in semiconducting quantum well structures

The contribution to the exciton linewidth in semiconducting quantum well structures due to the scattering of excitons by free carriers is calculated. It is found that this contribution becomes very important in limiting the exciton linewidth when a high density of free carriers is present or at low temperatures where the scattering of the excitons by optical and acoustic phonons is reduced. This contribution to the linewidth in quantum well structures is found to increase with the free carrier concentration and to extremely broaden and exciton peak at high carrier concentrations. At lower carrier concentrations, where the carriers behave as a nondegenerate gas of particles, the contribution to the exciton linewidth due to scattering by free carriers increases with temperature.     

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.     

Voltage-controlled optics of a quantum dot

We show how the optical properties of a single semiconductor quantum dot can be controlled with a small dc voltage applied to a gate electrode. We find that the transmission spectrum of the neutral exciton exhibits two narrow lines with approximately 2 mueV linewidth. The splitting into two linearly polarized components arises through an exchange interaction within the exciton. The exchange interaction can be turned off by choosing a gate voltage where the dot is occupied with an additional electron. Saturation spectroscopy demonstrates that the neutral exciton behaves as a two-level system. Our experiments show that the remaining problem for manipulating excitonic quantum states in this system is spectral fluctuation on a mueV energy scale.     

Exciton fine structure splitting of single InGaAs self-assembled quantum dots

We show how the resonant absorption of the ground state neutral exciton confined in a single InGaAs self-assembled quantum dot can be directly observed in an optical transmission experiment. A spectrum of the differential transmitted intensity is obtained by sweeping the exciton energy into resonance with laser photons exploiting the voltage induced Stark-shift. We describe the details of this experimental technique and some example results which exploit the 1 μeV spectral resolution. In addition to the fine structure splitting of the neutral exciton and an upper bound on the homogeneous linewidth at 4.2 K, we also determine the transition electric dipole moment.     

CdTe/CdZnTe多量子阱激子复合动力学性质的研究

报道了分子束外延制备的高质量CdTe/Cd_0.64Zn_0.36Te多量子阱结构的光学性质,由变温光致发光光谱讨论了随温度升高辐射线展宽和辐射复合效率降低的机理.在变密度激发的皮秒时间分辨光谱中,发现不同激发密度下发光衰减时间不同,并研究了它的机理.在高激发密度下观测到n=2的重空穴激子发光. 关键词：     

CdSe/ZnS纳晶中相干电声耦合效应的二维电子光谱研究

Coherent exciton-phonon coupling in CdSe/ZnS nanocrystals have been investigated by temperature-dependent two-dimensional electronic spectroscopy (2DES) measurements. Benefiting from the ability of 2DES to dissect assembles in nanocrystal films, we have clearly identified experimental evidences of coherent coupling between exciton and phonon in CdSe/ZnS nanocrystals. In time domain, 2DES signals of excitonic transitions beat at a frequency resonant to a longitudinal optical phonon mode; in energy domain, phonon side bands are distinct at both Stokes and anti-Stokes sides. When temperature increases, phonon-induced exciton dephasing is observed with dramatic broadening of homogeneous linewidth. The results suggest exciton-phonon coupling is essential in elucidating the quantum dynamics of excitonic transitions in semiconductor nanocrystals.     

Highly reduced fine-structure splitting in InAs/InP quantum dots offering an efficient on-demand entangled 1.55-microm photon emitter

To generate entangled photon pairs via quantum dots (QDs), the exciton fine-structure splitting (FSS) must be comparable to the exciton homogeneous linewidth. Yet in the (In,Ga)As/GaAs QD, the intrinsic FSS is about a few tens microeV. To achieve photon entanglement, it is necessary to cherry-pick a sample with extremely small FSS from a large number of samples or to apply a strong in-plane magnetic field. Using theoretical modeling of the fundamental causes of FSS in QDs, we predict that the intrinsic FSS of InAs/InP QDs is an order of magnitude smaller than that of InAs/GaAs dots, and, better yet, their excitonic gap matches the 1.55 microm fiber optic wavelength and, therefore, offers efficient on-demand entangled photon emitters for long distance quantum communication.     

Optical properties of microcavity polaritons

This work contains a theoretical analysis of the optical properties of semiconductor quantum wells embedded in planar Fabry-Perot microcavities. In particular, the properties of the system in correspondence to the excitonic transition are studied by means of the polariton formalism. The polariton states in microcavities are derived and the polar-iton dispersion is presented. Particular emphasis is put on the existence of two well distinct regimes depending on the exciton and cavity parameters: strong coupling and weak coupling regime. The main experimental results are reviewed and compared with the prediction of the theory. After the polariton states have been characterized, the optical response of the system is discussed, with particular attention to the photoluminescence measurements. The polariton formation and relaxation through phonon scattering and the effect of the exciton inhomogeneous broadening are considered and, finally, a phe-nomenological model for the polariton photoluminescence spectra is presented.     

The exciton states and the hypochromism of polypeptides

The exciton states of the α and β-helical conformations of polypeptides are studied by a new molecular exciton theory. It is found that the α-helical structure shows hypochromism while the parallel and anti-parallel β forms exhibit no remarkable changes. In the α-helical structure the band splitting and the optical rotational strength are reasonably well calculated and the migration velocities for the two exciton states are estimated.     

The effect of interchain coupling on the reverse polarization of a high-energy exciton in conjugated polymers

By using the one-dimensional extended Su–Schrieffer–Heeger model, we investigate the effect of interchain coupling on the reverse polarization of a high-energy exciton in conjugated polymers. Our results show that, without interchain coupling, the high-energy exciton is completely localized in one chain, which could be reversely polarized by an electric field. However, when taking into account interchain coupling, the high-energy exciton tends to extend between two chains. Its reverse polarization would be reduced accordingly. We also find that the interchain coupling effect is more obvious for polymers with a stronger non-degenerate confinement. Besides this, the effect of electron–electron interaction is also discussed.     

CdSe/CdZnSe超晶格的激子光学性质的研究

用分子束外延法在GaAs衬底上生长了CdSe/Cd0.65Zn0.35Se超晶格结构。利用X射线衍射（XRD）、77K下变密度激发的光致发光光谱和变温度光致发光光谱研究了CdSe/CdZnSe超晶格结构和激光复合特性，在该材料中观测到激子－激子散射发射峰，变密度激发光致发光光谱和谱温度光致发光光谱证实了这一现象，激子发射峰的线宽随着温度的升高而展宽，低温时发光峰的宽度主要是由合金组分和阱垒起伏引起的，没温时激子线宽展宽是由于激子与纵光学声子和离化的施主杂质间的散射作用引起的，光致发光的强度随着温度的升高而降低，这主要是由激子的热离化造成的，也就是说，热激发使得电子或空穴由阱中跃迁至垒上。     

ZnCdSe/ZnSe多量子阱的生长和激子光学性质的研究

用分子束外延在GaAs衬底上生长了ZnCdSe/ZnSe多量子阱结构.利用X射线衍射(XRD)、变温度PL光谱和ps发光衰减等研究了ZnCdSe/ZnSe多量子阱结构和激子复合特性.由变温PL光谱讨论了随温度升高辐射线宽展宽和辐射复合效率降低的机理.     

On the calculation of surface exciton energies in molecular crystals

In this paper a general theory is established for surface exciton states in a molecular crystal. Starting from the bulk exciton formalism the pertubation caused by the surface is taken into account by introducing a perturbation matrix. Symmetry properties of the “surface exciton bands” are derived.     

Thermal activation and thermal transfer of localized excitons in InAs self-organized quantum dots

We have investigated the temperature dependence of photoluminescence (PL) properties of a number of InAs/GaAs heterostructures with InAs layer thickness ranging from 0.5 monolayer (ML) to 3 ML. The temperature dependence of the InAs exciton energy and linewidth was found to display a significant difference when the InAs layer thickness is smaller or larger than the critical thickness around 1.7 ML, indicating spontaneous formation of quantum dots (QDs). A model, involving exciton recombination and thermal activation and transfer, is proposed to explain the experimental data. In the PL thermal quenching study, the measured thermal activation energies of different samples demonstrate that the InAs wetting layer may act as a barrier for thermionic emission of carriers in high quality InAs multilayers, while in InAs monolayers and submonolayers the carriers are required to overcome the GaAs barrier to thermally escape from the localized states.     

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.     

Temperature and density dependence of exciton lifetimes in GaAs/AlGaAs multiple quantum wells

The photoluminescence linewidths and excition lifetimes of free excitons in GaAs/AlGaAs multiple quantum wells were systematically investigated as a function of temperature, quantum well width, and carrier density. The experimental results showed that the exciton decay processes were strongly related to the linewidth of the exciton and the exciton binding energy.     

基于磁圆二向色谱的单层MoS_2激子能量和线宽温度依赖特性

以二硫化钼(MoS_2)为代表的过渡金属硫属化物属于二维层状材料,样品可以薄至单层.单层MoS_2是一种直接带隙半导体,在纳米逻辑器件、高速光电探测、纳米激光等领域具有广阔的应用前景.在实际应用中,温度是影响半导体材料能带结构和性质的主要因素之一.因此研究单层二维材料能带的温度依赖特性对理解其物理机理以及开展器件应用具有重要的意义.目前,在广泛采用的测量单层MoS_2反射谱的研究中,激子峰往往叠加在一个很强的光谱背底上,难以准确分辨激子的峰位和线宽.基于自行搭建的显微磁圆二向色谱系统,研究了单层MoS_2在65—300 K温度范围内的反射谱和磁圆二向色谱,结果表明磁圆二向色谱在研究单层材料激子能量和线宽方面具有明显的优势.通过分析变温的磁圆二向色谱,得到了不同温度下的A,B激子的跃迁能量和线宽.通过对激子能量和线宽的温度依赖关系进行拟合,进一步讨论了声子散射对激子线宽的影响.