LA声子对激子qubit纯退相干的影响

在一个抛物量子点中,以激子的真空态和基态作为量子比特(qubit),采用求密度矩阵元的方法,计算了由形变势下声学声子引发的激子量子比特纯退相干.找到了激子量子比特纯退相干因子对时间、温度和量子点受限长度的依赖关系.研究发现,激子量子比特的退相干因子在2.5ps的时间范围内随时间的增加而迅速增加,其纯退相干时间在ps量级;在温度即使为绝对温度0K时由LA声子引发的退相干依然存在,在温度大于3K后退相干因子随温度的增大而开始迅速增大;并同时发现量子点受限长度对退相干因子有重要影响,激子越受限退相干越快.研究结果表明,对激子量子比特使用适当大小量子点,且保持环境低温,并采用低能超快光学操作可以有效地抑制声子对激子量子比特纯退相干的影响. 关键词： 量子点 量子信息 量子比特     

纳米混合分子聚集体材料中弗兰克尔激子迁移的相位弛豫

在有机染料ＰＩＣ－１中引入其衍生物ａｚａＰＩＣ－Ｉ形成能量势垒，改变在混合分子聚集体中ＰＩＣ－Ｉ的Ｊ－聚集体的实体长度。用双调制外差检测的累积光子回波技术研究了相干弗兰克尔激子失相过程。观测到激子失相时间Ｔ２随ａｚａＰＩＣ－１克分子数的增大从６０ｐｓ变为２２４ｐｓ。     

叶绿素a、b分子体系激子相干迁移的时间特性

本文利用激发能传递的广义主方程理论和光谱实验结果,首次研究了相同和相异叶绿素分子体系的激子相干迁移的时间特性.Chla分子间的相干时间为350fs,Chlb分子间为160fs,Chla与Chlb分子间为200fs.主要叶绿素分子间的激子相干迁移属弛豫前转移过程.并分析了该迁移的作用及影响相干时间长短的主要因素.     

室温下CdSe胶体量子点超快自旋动力学

利用时间分辨法拉第旋转光谱技术研究了室温下CdSe胶体量子点的自旋相干特性.获得了不同磁场下的自旋退相干时间,并分析了自旋退相干的物理机理.零磁场时量子点激子自旋退相干时间为102 ps,主要受电子与核自旋之间的超精细相互作用所影响.当外加横向磁场强度为250 mT时,激子自旋退相干时间为294 ps;增大磁场强度,自旋退相干时间逐渐减小.在较强磁场环境中(≥250mT),量子点激子自旋动力学由非均匀退相干机制所主导.     

双光子共振激发Rb原子高激发态的瞬态相干效应

本文采用微微秒同步泵浦可调谐染料激光器,研究了Rb原子高激发态15d的双光子共振激发和增强效应,获得了1.065μ→4210(?)的频率上转换;给出自位相匹配与4210(?)相干辐射输出的关系.本文重点研究了高激发态的瞬态相干效应,得到了高激发态瞬态相干的失相过程;实验指明,双光子共振激发获得最大极化的时间是120ps,直到350ps,在探测光作用下仍可诱导出4212(?)相干辐射光.     

飞秒相干态相位差分光谱学

 理论上证明了测量脉冲对激发的相干态布居等价于测量单脉冲激发的感应极化,能同时获得瞬态相干光学过程的振幅与相位信息,发展了双通道飞秒脉冲对实验技术,提出了相位差分光谱实验方法。研究了半导体GaAs和稀土材料的飞秒相干态动力学过程,根据自相关曲线和样品信号的关系得到相位光谱。理论拟合得液氮温度下GaAs的激子退相时间为190fs;单晶Nd:YVO₄和粉末Nd:YAG 4f电子在室温下的退相时间为300fs。并研究了液氮温度下稀土材料原子核波包的动力学过程。     

ZnCdSe量子阱/CdSe量子点耦合结构中的激子隧穿过程

用室温光致发光谱和飞秒脉冲抽运探测方法对不同垒宽的ZnCdSe量子阱/ZnSe/CdSe 量子点新型耦合结构中激子隧穿过程进行研究，观察到激子从量子阱到量子点的快速隧穿过 程.在ZnSe垒宽为10nm, 15nm, 20nm时，测得激子隧穿时间分别为1.8ps, 4.4ps, 39ps. 关键词： ZnCdSe量子阱 CdSe量子点 激子 隧穿     

基于光场一阶关联的时域成像

与通常利用二阶强度关联测量实现时域鬼成像不同,本文利用时域热光源借助干涉仪通过一阶关联实现时域成像.基于空域光束的近轴衍射和时域窄带脉冲在色散介质中色散之间的空间-时间二象性,在时域脉冲响应函数的基础上得到了表征一阶关联时域成像的强度表达式,分析研究了光源脉冲宽度和相干时间对成像可见度和分辨率的影响.结果一方面表明基于热光场一阶关联的时域成像在不需要额外色散补偿或消除条件下可以实现时域物体信号的再现,另一方面表明当光源脉冲宽度一定时,成像可见度随光源脉冲相干时间的增加而增加,但是成像分辨率逐渐降低,其中当光源脉冲宽度约为100 ps,相干时间约为0.5 ps时,间隔为20 ps,宽度为8 ps的时域矩形波型物体的成像质量(兼顾可见度和分辨率)较好.该结果对于基于热光一阶关联的时域成像在时序信号测量中的应用具有重要意义.     

双激子和浸润层泄漏以及俄歇俘获对量子点Rabi振荡衰减的影响

研究了脉冲激光激发下半导体量子点激子Rabi振荡中多能级过程引起的退相干特性.运用多能级粒子数运动方程组，分别计算和分析了三种多能级过程(双激子、浸润层泄漏以及俄歇俘获过程)对量子点中Rabi振荡衰减的影响.分析表明，双激子的影响在激发脉冲的脉宽较长时(>5ps)可以忽略；浸润层的泄漏虽然使得激子基态上粒子数振荡的振幅随着激发场的增强而减小，但是同时也导致了振荡平均值的减小；分析和讨论了两种俄歇俘获方式对激子振荡和复合发光的影响. 关键词： Rabi振荡 半导体量子点 退相干 俄歇俘获     

从捕光天线到反应中心分子能量传递研究

利用飞秒时间分辨光谱技术研究了PSⅡ中捕光天线LHCⅡ内Chla分子和β-Car分子传递光能到反应中心的时间特性,实验测得Chla分子用了25 ps,β-Car分子用了250 ps.理论研究得出:25 ps是相邻Chl分子之间随机转移传能的时间常数,250 ps是LHCⅡ内相邻β-Car分子,通过Chla分子单步FÖrster共振传递、Dexter电子交换机制、激子转移把能量转移到反应中心的总时间.理论计算与实验结果基本符合,激子随机转移传递激发能快而有效.     

Ultrafast nonlinear optical response and high density excitation effects of the stacking fault exciton in BiI3

On the exciton states localized at a two-dimensional stacking fault interface in a layered crystal BiI₃, some nonlinear optical phenomena clearly appear reflecting large transition probability. The optical Stark shift and other high density exciton effect on the energy-shift and the spectral broadening are observed with clear separation under intense laser pumping by time-resolved measurements. The optical Stark shift is analyzed based on the dressed exciton model. The ultrafast optical response faster than 3 ps for the pump-laser field is confirmed on the Stark shift. Degenerate four-wave-mixing signals show fairly long dephasing time of 40 ps in this system. The dephasing probability depends linearly on the pump-laser intensity in the same manner as that of the spectral line-broadening reflecting the relaxation process. The dephasing mechanisms are understood by the exciton scattering at high density in parallel with the spectral changes. The blue-shift due to the high density excitons are discussed on the basis of exciton-exciton interaction in connection with a phase-space filling theory in two-dimensional systems.     

Temporal characteristics of picosecond stimulated Raman scattering in oxide crystals

The temporal characteristics of stimulated Raman scattering (SRS) under 22-ps laser excitation were studied in eight oxide crystals with a T ₂ optical-phonon dephasing time variable by up to two orders of magnitude. The measured SRS pulse width was shortened from 13.8 ps for Ba(NO₃)₂ (T ₂ = 26.5 ps) to 4 ps for the LiNbO₃ (T ₂ = 0.38 ps) crystal. The dependence of SRS pulse width on the dephasing time was analyzed in the framework of the known SRS theory.     

Decoherence of excitons in multichromophore systems: thermal line broadening and destruction of superradiant emission

We study the temperature-dependent dephasing rate of excitons in chains of chromophores, accounting for scattering on static disorder as well as acoustic phonons in the host matrix. From this we find a power-law temperature dependence of the absorption linewidth, in excellent quantitative agreement with experiments on dye aggregates. We also propose a relation between the linewidth and the exciton coherence length imposed by the phonons. The results indicate that the much debated steep rise of the fluorescence lifetime of pseudoisocyanine aggregates above 40 K results from the fact that this coherence length drops below the localization length imposed by static disorder.     

Time domain investigation of the intrachain vibrational dynamics of a prototypical light-emitting conjugated polymer

Coherent nuclear motion of the carbon backbone is monitored in real time in substituted poly(phenylene)-vinylene in both excited and ground electronic state using sub-10-fs light pulses. Characteristic features of the intrachain vibrational dynamics are obtained. We observe vibrational dephasing in the excited state within 1 ps (time constant T(2e) approximately 300 fs). These findings are in agreement with the molecular picture for photoexcitation in conjugated polymers.     

Coherent dynamics in InGaAs quantum dots and quantum dot molecules

We measure the dephasing time of the exciton ground state transition in InGaAs quantum dots (QD) and quantum dot molecules (QDM) using a sensitive four-wave mixing technique. In the QDs we find experimental evidence that the dephasing time is given only by the radiative lifetime at low temperatures. We demonstrate the tunability of the radiatively limited dephasing time from 400 ps up to 2 ns in a series of annealed QDs with increasing energy separation of 69–330 meV from the wetting layer continuum. Furthermore, the distribution of the fine-structure splitting δ₁ and of the biexciton binding energy δ_B is measured. δ₁ decreases from 96 to with increasing annealing temperature, indicating an improving circular symmetry of the in-plane confinement potential. The biexciton binding energy shows only a weak dependence on the confinement energy, which we attribute to a compensation between decreasing confinement and decreasing separation of electron and hole. In the QDM we measured the exciton dephasing as function of interdot barrier thickness in the temperature range from 5 to 60 K. At 5 K dephasing times of several hundred picoseconds are found. Moreover, a systematic dependence of the dephasing dynamics on the barrier thickness is observed, showing how the quantum mechanical coupling in the molecules affects the exciton lifetime and acoustic-phonon interaction.     

Emission of a single conjugated polymer chain isolated in its single crystal monomer matrix

The excitonic luminescence of a highly ordered single conjugated polymer chain is studied by microphotoluminescence. At T< or =10 K it consists of a single Lorentzian line. The linewidth increases linearly with T between 6 and 60 K, from 350 microeV at 6 K, indicating a pure dephasing time of approximately 2 ps. Above 10 K, other neighboring regions along the chain direction start to emit at a slightly higher (by approximately 1 meV) energy. This indicates very small inhomogeneous broadening, very long chains ( > or =10 microm), and a long range and very rapid exciton energy transfer ( >10 microm in <100 ps).     

All-ultraviolet time-resolved coherent anti-Stokes Raman scattering

We report all-UV coherent anti-Stokes Raman scattering (CARS) in calcite with 250-280 nm pump, Stokes, probe, and anti-Stokes light. UV CARS efficiency is approximately 7x higher than for comparable scattering in the visible, 480-540 nm. Time-resolved UV CARS reveals lengthening of the dephasing time of 1086 cm(-1) CO3(2-) internal vibrations from 4 to 7 ps with increasing vibrational excitation, consistent with a phonon depletion model.     

Recombination dynamics of free and bound excitons in bulk GaN

We report new data on the transient photoluminescence behaviour of free and donor bound excitons in high quality bulk GaN material grown by HVPE. With 266 nm photoexcitation the no-phonon free exciton has a short decay time, about 100 ps at 2 K, assigned to nonradiative surface recombination. The LO replicas of the free exciton have a much longer decay at 2 K, about 1.4 ns, believed to be a lower bound for the bulk radiative lifetimes of the free excitons at 2 K. The donor bound exciton no-phonon lines exhibit a rather short (about 300 ps) nonexponential decay at 2 K, which appears to be dominated by a scattering process. The corresponding LO replicas and the two-electron transitions have a much longer decay. From the latter, the lower bound of the radiative lifetime of the O- and Si-bound excitons are 1800 ps and 1100 ps, respectively.