Power density and temperature dependent multi-excited states in InAs/GaAs quantum dots

Self-assembled InAs/GaAs (001) quantum dots (QDs) were grown by molecular beam epitaxy using ultra low-growth rate. A typical dot diameter of around 28 ± 2 nm and a typical height of 5 ± 1 nm are observed based on atomic force microscopy image. The photoluminescence (PL) spectra, their power and temperature dependences have been studied for ground (GS) and three excited states (1–3ES) in InAs QDs. By changing the excitation power density, we can significantly influence the distribution of excitons within the QD ensemble. The PL peak energy positions of GS and ES emissions bands depend on an excitation light power. With increasing excitation power, the GS emission energy was red-shifted, while the 1–3ES emission energies were blue-shifted. It is found that the full width at half maximum of the PL spectra has unusual relationship with increasing temperature from 9 to 300 K. The temperature dependence of QD PL spectra shown the existence of two stages of PL thermal quenching and two distinct activation energies corresponding to the temperature ranges I (9–100 K) and II (100–300 K).     

亚单层InGaAs量子点-量子阱异质结构的时间分辨光致发光谱

测定了亚单层InGaAs/GaAs量子点-量子阱异质结构在5K下的时间分辨光致发光谱.亚单层量 子点的辐射寿命在500 ps 至 800 ps之间，随量子点尺寸的增大而增大，与量子点中激子的 较小的横向限制能以及激子从小量子点向大量子点的隧穿转移有关.光致发光上升时间强烈 依赖于激发强度密度.在弱激发强度密度下，上升时间为 35 ps，纵光学声子发射为主要的 载流子俘获机理.在强激发强度密度下，上升时间随激发强度密度的增加而减小，俄歇过程 为主要的载流子俘获机理.该结果对理解亚单层量子点器件的工作特性非常有用. 关键词： 亚单层 量子点-量子阱 时间分辨光致发光谱     

Spin coherence during optical excitation of a single nitrogen-vacancy center in diamond

We examine the quantum spin state of a single nitrogen-vacancy (NV) center in diamond at room temperature as it makes a transition from the orbital ground state (GS) to the orbital excited state (ES) during nonresonant optical excitation. While the fluorescence readout of NV-center spins relies on conservation of the longitudinal spin projection during optical excitation, the question of quantum phase preservation has not been examined. Using Ramsey measurements and quantum process tomography of the optical excitation process, we measure a trace fidelity of F=0.87±0.03, which includes ES spin dephasing during measurement. Extrapolation to the moment of optical excitation yields F≈0.95. This result provides insight into the interaction between spin coherence and nonresonant optical absorption through a vibronic sideband.     

Reduced linewidth enhancement factor due to excited state transition of quantum dot lasers

The carrier induced refractive index change and linewidth enhancement factor α due to ground-state (GS) and excited-state (ES) transitions have been compared by measuring the optical gain spectra from an InAs/GaAs quantum dot (QD) laser structure. It is shown that the ES transition exhibits a reduced α-factor compared to the value due to the GS transition. This result can be explained by the α-factor due to the ES transition having a smaller increase from the non-resonant carriers in the combined state of the wetting layer and InGaAs strain reducing layer than the α-factor increase due to the GS transition, since the relaxation time for carriers from the combined state of the wetting layer and InGaAs strain reducing layer to the ES is shorter than to the GS. The result reported here shows another advantage of using ES QD lasers for optical communication, in addition to their higher modulation speed.     

Carrier scattering by Auger mechanism in a single quantum wire

We report on time-resolved microphotoluminescence experiments in a single GaAs/GaAlAs V-shaped quantum wire as a function of optical excitation intensity. At low pump power we observe that excitons are localized in quantum boxes formed by the local potential minima existing along the wire axis. As the pump power is increased, state filling of the lowest lying levels of the boxes appears. When two carriers occupy the first excited level of the box, a very efficient Auger scattering occurs, leading to a transfer of carriers from one box to another neighbouring one. The intradot Auger scattering time has been measured and is of the same order of magnitude as the LA-phonon emission rate. Received 5 February 2001     

方波激发下Er~(3+)上转换红光激发机理的研究

用方波电源驱动808 nm激光二极管(LD)激发Er3+掺杂的亚碲酸盐氟氧化物玻璃,测量4F9/2能级上转换发光的上升和衰减,根据上升的时间常数确定中间能级的寿命,从而确定4F9/2能级粒子数积累的过程。通过建立速率方程模型分析4F9/2能级的上升和衰减特性与中间能级的关系,确定808 nm LD激发下上转换红光的激发机理,同时提供了一种通过上转换发光,用光电倍增管测量红外能级寿命的方法。     

Surface-enhanced emission from single semiconductor nanocrystals

The fluorescence behavior of single CdSe(ZnS) core-shell nanocrystal (NC) quantum dots is dramatically affected by electromagnetic interactions with a rough metal film. Observed changes include a fivefold increase in the observed fluorescence intensity of single NCs, a striking reduction in their fluorescence blinking behavior, complete conversion of the emission polarization to linear, and single NC exciton lifetimes that are >10(3) times faster. The enhanced excited state decay process for NCs coupled to rough metal substrates effectively competes with the Auger relaxation process, allowing us to observe both charged and neutral exciton emission from these NC quantum dots.     

Low Density Self-Assembled InAs/GaAs Quantum Dots Grown by Metal Organic Chemical Vapour Deposition

The self-assembled InAs quantum dots （QDs） on GaAs substrates with low density （5×10^8 cm^-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 is 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.     

Excitation Wavelength Dependence of Dual Fluorescence of DMABN in Polar Solvents

Steady-state absorption, fluorescence excitation and emission spectra of 4-(N,N-dimethylamino)benzonitrile (DMABN) have been measured at room temperature in cyclohexane, 1,4-dioxane, dichloromethane, and acetonitrile solutions. The fluorescence spectra of DMABN are found to exhibit dual emission in 1,4-dioxane, dichloromethane, and acetonitrile solutions and single emission in cyclohexane solution. The effect of solvent polarity and excitation wavelength on the emission spectra has also been studied. The fluorescence excitation spectra of DMABN monitored at the emission bands are different. The presence of two different conformations of the same molecule in the ground state has lead to two close lying excited states; local excited (LE) and charge transfer (CT), and thereby results in the dual fluorescence of the compound. The experimental studies were supported by ab initio density functional theory (DFT) calculations performed at the B3LYP/6-31Gd level of theory. On the basis of the experimental results and our theoretical calculations, we suggest that there are two conformers of DMABN, which are stable in the ground state, equilibrated in solution at room temperature that give rise dual fluorescence upon excitation.     

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     

Band-dependent quasiparticle dynamics in the hole-doped Ba-122 iron pnictides

We report on band-dependent quasiparticle dynamics in the hole-doped Ba-122 pnictides measured by ultrafast pump-probe spectroscopy. In the superconducting state of the optimal and over hole-doped samples, we observe two distinct relaxation processes: a fast component whose decay rate increases linearly with excitation density and a slow component whose relaxation is independent of excitation strength. We argue that these two components reflect the recombination of quasiparticles in the two hole bands through intraband and interband processes. We also find that the thermal recombination rate of quasiparticles increases quadratically with temperature in all samples. The temperature and excitation density dependence of the decays indicates fully gapped hole bands and nodal or very anisotropic electron bands.     

Decay of cystalline order and equilibration during the solid-to-plasma transition induced by 20-fs microfocused 92-eV free-electron-laser pulses

We have studied a solid-to-plasma transition by irradiating Al foils with the FLASH free electron laser at intensities up to 10(16) W/cm(2). Intense XUV self-emission shows spectral features that are consistent with emission from regions of high density, which go beyond single inner-shell photoionization of solids. Characteristic features of intrashell transitions allowed us to identify Auger heating of the electrons in the conduction band occurring immediately after the absorption of the XUV laser energy as the dominant mechanism. A simple model of a multicharge state inverse Auger effect is proposed to explain the target emission when the conduction band at solid density becomes more atomiclike as energy is transferred from the electrons to the ions. This allows one to determine, independent of plasma simulations, the electron temperature and density just after the decay of crystalline order and to characterize the early time evolution.     

Fs-dynamics of charge-transfer excited states in anthracene–PMDA single crystals

Single crystals of the weak charge-transfer (CT) complex anthracene–PMDA have been studied by fs transient absorption spectroscopy in the temperature range between 295 and 10 K. Upon variation of the probe light polarization the complete set of transient CT-signals is identified (transient absorption of the CT-state, stimulated emission and transient bleaching), for the first time in CT single crystals. The formation of the CT-state after photoexcitation occurs faster than 150 fs without precursor, independent of temperature and excitation energy. An additional transient signal is clearly differentiated and described quantitatively by dipole-induced shifts of the ground state absorption.     

Effect of inter-level relaxation and cavity length on double-state lasing performance of quantum dot lasers

Double-state lasing phenomena are easily observed in self-assembled quantum dot (QD) lasers. The effect of inter-level relaxation rate and cavity length on the double-state lasing performance of QD lasers is investigated on the basis of a rate equation model. Calculated results show that, for a certain cavity length, the ground state (GS) lasing threshold current increases almost linearly with the inter-level relaxation lifetime. However, as the relaxation rate becomes slower, the ratio of excited state (ES) lasing threshold current over the GS one decreases, showing an evident exponential behavior. A relatively feasible method to estimate the inter-level relaxation lifetime, which is difficult to measure directly, is provided. In addition, fast inter-level relaxation is favorable for the GS single-mode lasing, and leads to lower wetting layer (WL) carrier occupation probability and higher QD GS capture efficiency and external differential quantum efficiency. Besides, the double-state lasing effect strongly depends on the cavity length.     

Effect of inter-level relaxation and cavity length on double-state lasing performance of quantum dot lasers

Double-state lasing phenomena are easily observed in self-assembled quantum dot (QD) lasers. The effect of inter-level relaxation rate and cavity length on the double-state lasing performance of QD lasers is investigated on the basis of a rate equation model. Calculated results show that, for a certain cavity length, the ground state (GS) lasing threshold current increases almost linearly with the inter-level relaxation lifetime. However, as the relaxation rate becomes slower, the ratio of excited state (ES) lasing threshold current over the GS one decreases, showing an evident exponential behavior. A relatively feasible method to estimate the inter-level relaxation lifetime, which is difficult to measure directly, is provided. In addition, fast inter-level relaxation is favorable for the GS single-mode lasing, and leads to lower wetting layer (WL) carrier occupation probability and higher QD GS capture efficiency and external differential quantum efficiency. Besides, the double-state lasing effect strongly depends on the cavity length.     

Polarization and readout of coupled single spins in diamond

We study the coupling of a single nitrogen-vacancy center in diamond to a nearby single nitrogen defect at room temperature. The magnetic dipolar coupling leads to a splitting in the electron spin resonance frequency of the nitrogen-vacancy center, allowing readout of the state of a single nitrogen electron spin. At magnetic fields where the spin splitting of the two centers is the same, we observe a strong polarization of the nitrogen electron spin. The amount of polarization can be controlled by the optical excitation power. We combine the polarization and the readout in time-resolved pump-probe measurements to determine the spin relaxation time of a single nitrogen electron spin. Finally, we discuss indications for hyperfine-induced polarization of the nitrogen nuclear spin.     

基于分子束外延生长的1.05 eV InGaAsP的超快光学特性研究

利用分子束外延方法制备了应用于四结光伏电池的1.05 eV InGaAsP薄膜, 并对其超快光学特性进行了研究. 温度和激发功率有关的发光特性表明: InGaAsP材料以自由激子发光为主. 室温下InGaAsP材料的载流子发光弛豫时间达到10.4 ns, 且随激发功率增大而增大. 发光弛豫时间随温度升高呈现S形变化, 在低于50 K时随温度升高而增大, 在50–150 K之间时减小, 而温度高于150 K时再次增大. 基于载流子弛豫动力学, 分析并解释了温度及非辐射复合中心浓度对样品材料载流子发光弛豫时间S形变化的影响.     

The participant Coster–Kronig preceded Auger transition in the resonant L2,3-M2,3V Auger electron spectrum of Ti metal

The L_2,3-M_2,3V resonant Auger electron spectroscopy (RAES) spectrum of Ti metal measured by Le Fêvre et al. [P. Le Fêvre, J. Danger, H. Magnan, D. Chandesris, J. Jupille, S. Bourgeois, M.-A. Arrio, R. Gotter, A. Verdini, A. Morgante, Phys. Rev. B69 (2004) 155421] is analyzed in the light of relaxation and decay of the resonantly excited L_2,3-hole states. The relaxation time of the resonantly excited L_2,3-hole state to the fully relaxed (screened) one is much shorter than the L_2,3-hole Auger decay time, whereas the participant Coster–Kronig (CK) decay time of the resonantly excited L₂-hole state to the fully relaxed L₃-hole state at the L₂ resonance is as short as the relaxation time of the resonantly excited L₂-hole state to the fully relaxed one. The excited electron is predominantly either rapidly decoupled from the L_2,3-hole decay or annihilated by the participant CK decay. Thus, near the L_2,3 edges the L_2,3-M_2,3V RAES spectral peak appears at constant kinetic energy. The L_2,3-M_2,3V RAES spectrum shows a normal L_2,3-M_2,3V Auger decay profile not modulated by the density of empty d states probed by the resonant excitation. Not only the relaxation time but also the participant CK decay time depends on photon energy because they depend on the density of empty d states probed by the resonant excitation. As a result, the L_2,3 X-ray absorption spectroscopy spectral line broadening depends on photon energy.     

Linear and non-linear behavior of cavity polaritons

We report on the linear and non-linear emission of cavity-polaritons under resonant excitation. At low excitation density, in addition to polariton photoluminescence, strong Rayleigh scattering is observed. At higher excitation densities, a sudden transition to a highly emissive state is observed, accompanied by spatial patterning. We attribute such phenomena to a combination of nonlinear cavity-polariton relaxation mechanism and nonlinear response of the cavity, leading to transverse pattern formation. A careful analysis of near- and far-field emission patterns with spatial filtering as well as reflectivity shows that an inhomogeneous situation develops, the center of the excited region undergoing a strong to weak coupling transition while the periphery is still in strong coupling. Despite the complex non-linear behavior we observe no signatures of Bose–Einstein condensation or Boser action.