WS_2与WSe_2单层膜中的A激子及其自旋动力学特性研究

单层过渡金属硫化物由于其特有的激子效应以及强自旋-谷耦合性质,在光电子学及谷电子学等方面有着很广阔的应用前景.利用超快时间分辨光谱,本文系统地比较了两类钨基单层硫化物(WS_2和WSe_2)的A-激子动力学和谷自旋弛豫特性.实验结果表明, WS_2单层膜的A-激子弛豫表现为双指数过程,而对于WSe_2,其A-激子衰减表现为三指数过程,且激子的寿命远长于前者. WS_2谷自旋极化弛豫表现为单指数衰减,其寿命约0.35 ps,主要由电子-空穴交换作用所主导.而对于WSe_2,谷自旋弛豫表现出双指数弛豫特性:一个寿命为0.5 ps的快过程和一个寿命为28 ps的慢过程.快过程的弛豫来源于电子-空穴交换作用,而慢过程则由于自旋晶格散射形成暗激子的过程.通过调谐抽运光波长,进一步证实WSe_2较WS_2更容易形成暗激子.     

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.     

Screening of the electron-hole interaction in quantum well structures

Recent optical non-linearities in GaAs/Ga_1?xAl_xAs quantum well structures have been attributed to the screening of the electron-hole interaction in such structures by the free carriers created. We here present the results of a variational calculation of the ground state energy of an electron-hole pair confined to move in two dimensions when screening of the Coulomb interaction between the electron-hole pair by the free carriers present is taken into account by using the screened potential obtained by Stern and Howard for hydrogenic impurities in semiconducting inversion layers. It is found that the binding energy of the 2D exciton decreases less rapidly with the screening parameter than is the case for a 3D exciton and that the 2D exciton remains bound even for large values of the screening parameter. This is in contrast to the case in bulk semiconductors where the electron-hole pair no longer bind into an exciton when the screening length of the free carriers becomes less than the Bohr radius of the exciton.     

Series Solution for Localization and Entanglement of an Exciton in a Quantum Dot Molecule by an ac Electric Field

The Schrödinger equation involving the phenomenon of the localization and entanglement for an exciton in a quantum dot molecule by an ac electric field is analytically investigated. New exact series solutions for the Schrödinger equation have been obtained for the first time. The analytical expressions can further describe the dynamical behaviors of an interacting electron-hole pair in a double coupled quantum dot molecule under an ac electric field accurately.     

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.     

Excitonic versus plasma screening in highly excited gallium arsenide

We report band edge absorption spectra of GaAs under conditions of high electron-hole pair excitation in the range of 10¹³-10¹⁷ cm^-3 achieved with picosecond light pulses tuned (i) to the 1s exciton energy and (ii) to the continuum (ω#62;E_g), where critical densities for bleaching of the exciton absorption lines are much lower. A substantial blue shift of the 2s absorption line relative to the 1s exciton was found, the latter remained constant in energy up to complete bleaching.     

Spin relaxation of Mn ions in (CdMn)Te/(CdMg)Te quantum wells under picosecond optical pumping

Spin relaxation of Mn ions in a Cd_0.97Mn_0.03Te/Cd_0.75Mg_0.25Te quantum well with photogenerated quasi-two-dimensional electron-hole plasma at liquid helium temperatures in an external magnetic field has been investigated. Heating of Mn ions by photogenerated carriers due to spin and energy exchange between the hot electron-hole plasma and Mn ions through direct sd-interaction between electron and Mn spins has been detected. This process has a short characteristic time of about 4 ns, which leads to appreciable heating of the Mn spin subsystem in about 0.5 ns. Even under uniform excitation of a dense electron-hole plasma, the Mn heating is spatially nonuniform, and leads to formation of spin domains in the quantum well magnetic subsystem. The relaxation time of spin domains after pulsed excitation is measured to be about 70 ns. Energy relaxation of excitons in the random exchange potential due to spin domains results from exciton diffusion in magnetic field B=14 T with a characteristic time of 1 to 4 ns. The relaxation time decreases with decreasing optical pump power, which indicates smaller dimensions of spin domains. In weak magnetic fields (_B=2 T) a slow down in the exciton diffusion to 15 ns has been detected. This slow down is due to exciton binding to neutral donors (formation of bound excitons) and smaller spin domain amplitudes in low magnetic fields. The optically determined spin-lattice relaxation time of Mn ions in a magnetic field of 14 T is 270±10 and 16±7 ns for Mn concentrations of 3% and 12%, respectively. Zh. éksp. Teor. Fiz. 112, 1440–1463 (October 1997)     

熔石英中过氧缺陷及中性氧空位缺陷的几何结构、电子结构和吸收光谱的准粒子计算

本文使用密度泛函理论研究了熔石英中peroxy linkage(POL)缺陷和中性氧空位(NOV)缺陷的几何结构,电子结构以及光学性质.采用自洽的准粒子GW计算结合求解Bathe-Salpeter方程的多体理论,研究了缺陷引起的电子结构和光学吸收谱的变化.首先研究了无缺陷非晶结构的电子结构与吸收谱,得到的结果与实验值非常接近.对POL的计算表明,其在基态下的局部结构与过氧化氢分子类似.采用多体理论计算得到的吸收谱表明其最低吸收峰位于6.3 eV处.这一结果不支持实验认为的位于3.8 eV处的吸收峰是由POL缺陷导致的说法.对于NOV缺陷,计算表明其基态的Si—Si键长为2.51?而三重态下的值则为3.56?.相应的GW+BSE计算表明中性氧空位缺陷导致了位于7.4 eV处的吸收峰,与实验测量结果一致.     

神经网络法研究多溴代二苯胺热力学性质

通过时间分辨光谱技术详细地研究了ZnCuInS/ZnSe/ZnS量子点的激子弛豫动力学. 基于速率分布模型,波长依赖的发射动力学表明本征激子、界面缺陷态中的激子、给-受体对态中的激子都会参与量子点的发光过程,整个发光过程主要依赖于给-受体对态发射. 瞬态吸收数据表明激发后本征激子和界面缺陷物种可能会同时出现,在高激发光强下,光强依赖的俄歇复合过程也存在于量子点中     

Multiplication of anion and cation electronic excitations in luminescent wide-gap ionic crystals

The spectra of intrinsic luminescence excitation by synchrotron radiation (6–32 eV) at 8 K have been analyzed for NaCl, KCl, RbCl, KBr, RbBr, CsBr, MgO, CaO and YalO₃ crystals. In all crystalsv (except MgO and CaO) the process of multiplication of electronic excitations (MEE) causes a sharp increase of the intensity of self-trapped exciton emission, but leads (in KBr and NaCl) to the decrease of intra-band luminescence efficiency. The analysis of the intensity ratio spectra for two components of exciton emission allows us to separate the process of secondary exciton creation by hot photolectrons (NaCl, KBr, YAlO₃). The threshold energies of excitonic and electron-hole mechanisms of MEE are compared for a number of alkali halides.     

Transient interband light absorption by quantum dots: Degenerate pump-probe spectroscopy

The optical pump-probe method, which makes it possible to determine the energy relaxation rate for excited electron-hole pairs and excitons in semiconductor quantum dots (QDs), is theoretically described. A scheme in which the carrier frequencies of optical pump and probe pulses are close to resonance with the same interband transition in the QD electron subsystem (degenerate case) is considered. The pump-induced probe energy absorption is analyzed as a function of the delay time between the pump and probe pulses. It is shown that under certain conditions this dependence is reduced to monoexponential, whose exponent is proportional to the energy relaxation rate for the considered state of electron-hole pairs and excitons. The size dependence of the energy relaxation rate of the electron-hole pair states is modeled by the example of PbSe-based QDs, whose electron subsystem is in the strong-confinement regime.     

Pattern formation as a signature of quantum degeneracy in a cold exciton system

The development of a Turing instability to a spatially modulated state in a photoexcited electron-hole system is proposed as a novel signature of exciton Bose statistics. We show that such an instability, driven by kinetics of exciton formation, can result from stimulated processes that build up near quantum degeneracy. The stability of an electron-hole interface which describes recently observed exciton rings is analyzed. Interface instability occurs below a critical temperature, with a periodic 1D pattern developing via a continuous (type II) transition, in a qualitative agreement with observations.     

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.     

Dynamical process of photoinduced polarization reversion in polymers

In polymeric molecules, the self-trapping associated with the photoinduced polarization reversion (PPR) produces bond distortion and creates gap states. The relaxation processes of the bond distortion and the gap states are revealed by studying the dynamics of the photoexcitation. The switching speed associated with the PPR can be determined from the relaxation process.     

CdSeS合金结构量子点的多激子俄歇复合过程

多激子效应通常是指吸收单个光子产生多个激子的过程,该效应不仅可以为研究基于量子点的太阳能电池开拓新思路,还可以为提高太阳能电池的光电转换效率提供新方法.但是,超快多激子产生和复合机制尚不明确.这里以CdSeS合金结构量子点为研究对象,研究了其多激子生成和复合动力学.稳态吸收光谱显示, 510, 468和430 nm附近的稳态吸收峰,分别对应1S_(3/2)(h)-1S(e)(或1S), 2S_(3/2)(h)-1S(e)(或2S)和1P_P(3/2)(h)-1P(e)(或1P)激子的吸收带.通过飞秒时间分辨瞬态吸收光谱和纳秒时间分辨荧光光谱两种时间分辨光谱技术对CdSeS合金结构量子点的超快动力学进行了探究,结果显示, 1S激子的双激子复合时间大概是80 ps,这一时间比传统量子点的双激子复合时间(小于50 ps)延长了近一倍,结合最近发展的超快界面电荷分离技术,在激子湮灭之前将其利用起来,这一时间的延长将有很大的应用前景;其中,在2S和1P激子中除上述双激子复合外,还存在一个通过声子耦合路径的空穴弛豫过程,时间大概是5—6 ps.最后,利用纳秒时间分辨荧光光谱得到该样品体系单激子复合的时间约为200 ns.     

Observation of bound exciton and distant pair resonances in amorphous phosphorus

For the first time in an amorphous semiconductor magnetic resonance of a bound exciton is reported. ODMR investigations of amorphous phosphorous show that the luminescence consists of two bands, a low energy emission which is consistent with triple exciton recombination at IVAPs and a high energy emission due to electron-hole recombination at distant IVAPs. The triplet exciton has g = 2.13 ± 0.05, and the distant pair resonance occurs at g = 2.0 ± 0.02.     

Ground state energy of the electron-hole liquid in type-II (GaAs)m/(AlAs)m quantum wells

The ground state energy of quasi-two-dimensional electron-hole liquid (EHL) at zero temperature is calculated for type-II (GaAs)_m/(AlAs)_m (5≤m≤10) quantum wells (QWs). The correlation effects of Coulomb interaction are taken into account by a random phase approximation of Hubbard. Our EHL ground state energy per electron-hole pair is lower than the exciton energy calculated recently for superlattices, so we expected that EHL is more stable state than excitons at high excitation density. It is also demonstrated that the equilibrium density of EHL in type-II GaAs/AlAs QWs is of one order of magnitude larger than that in type-I GaAs/AlAs QWs.     

Spin-dependent electron-hole capture kinetics in luminescent conjugated polymers

The recombination of electron-hole pairs injected in extended conjugated systems is modeled as a multistep interconversion relaxation in monoexcited electronic state space, mediated by electron-phonon coupling. The computed ratio of triplet-to-singlet exciton formation times r=tau(T)/tau(S) increases from 0.9 for a model dimer to 2.5 for a 32-unit chain, in good agreement with recent experiments. We rationalize the conjugation-length dependence of r in terms of spin-specific energetics and mutual vibronic coupling of the excited states.     

Influence of the Wavefunction Distribution on Exciton Dissociation in Electric Field

We show that the dissociation threshold of an exciton, a bound electron-hole pair, by an electric field is mainly determined by its energy: as expected, the dissociation voltage decreases with increasing exciton energy. However, within the multiplet of states belonging to a particular principal quantum number n, the dissociation voltage rises with increasing state energy, in contrast to the expectations based on energy arguments. This behavior is demonstrated for the yellow exciton states of Cu₂O and is attributed to the distribution of the wavefunction in the potential landscape, where the lower (higher) lying state in the multiplet is shifted away (towards) the tunnel barrier.     

Terahertz emission with a time-dependent amplitude in asymmetric triple quantum wells

In this work, we have numerically integrated in space and time the effective-mass Schrödinger equation for an exciton in a GaAs/GaAlAs triple quantum well heterostructure. Considering a Coulomb interaction between the electron-hole pair in a triple quantum well, we have obtained a time-varying dipole moment in the system whose amplitude is also oscillating with time. In this way, we have shown the possibility of having a new kind of terahertz electromagnetic radiation emerging from a semiconductor device after an optical excitation of the system.