高等植物外周捕光天线中的超快过程

利用飞秒泵浦-探测技术对高等植物LHCII中的超快光动力学过程进行了研究。实验上观察了LHCII中色素间的能量传递过程,由飞秒动力学发现,单体内Chlb到邻近的Chla之间的能量传递在200～300fs的时间尺度,Chla激子带间的能量弛豫发生在几百飞秒,不同单体Chla分子之间能量分布过程在几百个皮秒。而飞秒动力学过程中上百皮秒的慢过程归属于不同聚集体之间的能量平衡过程或分子构像变化。     

AlGaAs/GaAs多量子阱中相干控制光电流的超快弛豫

在理论和实验上对室温下AlGaAs/GaAs量子阱中的相干控制光电流的超快动力学过程进行了研究.首次由密度矩阵和电子-空穴散射弛豫模型导出相干光电流的弛豫时间为600fs,并由三波长飞秒脉冲泵浦-探测技术测量的结果得到验证.     

NaI分子在强场作用下的非绝热动力学研究

利用含时量子波包法研究了NaI分子在飞秒激光脉冲场作用下运动到势能面交叉区域的非绝热动力学以及泵浦-探测光电离动力学。根据动力学反射原理,得到了NaI分子在非绝热交叉区域的波包动力学与泵浦-探测光电子能谱之间的对应关系。研究结果给出了NaI分子在强场作用下的非绝热特性。     

超高时空和能量分辨光电子成像研究进展

测量并操控新材料和新器件中极端时空小尺度电子的超快动力学过程,是后摩尔时代柔性半导体和微纳超快响应器件研发的核心.时空和能量分辨的光发射电子显微技术将光学的泵浦-探测方案与电子显微成像技术巧妙结合,兼具飞秒-纳米极端时空和高能量分辨本领,已经成为探索纳米光子学和低维半导体器件等领域超快光物理过程的普适显微手段,推动了等离激元学、半导体材料科学及其相关交叉学科在基础和应用研究领域的革命性发展.本篇综述将重点介绍超快光电子成像技术在等离激元功能器件、高阶等离激元涡旋场、等离激元斯格明子和低维半导体材料方面的应用.最后,我们将展望超快光电子成像技术在未来基础研究和应用研究中的新机遇.     

TbFeCo薄膜激光诱导超快自旋动力学的成分比研究

采用基于磁光克尔效应的泵浦-探测技术研究不同成分比TbFeCo磁性薄膜的激光诱导超快自旋动力学过程,成功观测到具有几百飞秒的超快退磁以及几十皮秒的慢退磁的两步退磁现象.根据四温度模型,TbFeCo中的第一步超快退磁现象是由电子-自旋作用引起,第二步慢退磁现象是由晶格-FeCo自旋-Tb自旋作用引起的.不同成分比TbFeCo样品的对比实验显示,随着Tb含量增加,两步退磁程度减弱,第二步慢退磁时间增大,进一步验证四温度模型的合理性.     

紫细菌外周捕光天线LH2中的超快光物理

采用飞秒泵浦-探测技术研究了紫细菌外周捕光天线LH2中的超快光物理过程,在天然LH2中,B800到B850分子之间的能量传递时间在0.65ps左右;在B800主吸收带的兰侧激发时,观察到一个约400fs的超快弛豫过程,可归属于B800分子之间的能量分布过程;在848nm激发时观察到150fs的超快相归属于位于B850的激发能向其近邻分子的离域过程,几个皮秒的快相归属于激发能在次最低激子态和最低激子态间的分布过程.     

三态NaI分子飞秒含时光电子能谱的理论研究

利用三态模型和含时量子波包法,研究了NaI分子在飞秒泵浦—探测激光场中延时,波长,场强对光电子能谱的影响.波包在势能面上传播,受到非绝热效应的影响,传播到交叉区域时发生分裂,延时影响光电子能谱谱峰的位置和峰高.延时增加,非绝热效应对波包运动的影响越明显.泵浦波长影响光电子能谱构型,探测波长只影响谱峰位置,不影响峰高.激光场强增强,光电子谱谱峰增高.光电子能谱反映波包动力学信息.本文研究结果可以为实验上实现分子的光控制以及量子调控过程提供一定的参考,并为进一步研究NaI分子的动力学性质提供有用的信息.     

飞秒激光强场条件下碘化钠分子解离过程的理论研究

我们采用了精确的量子力学方法对飞秒激光强场条件下碘化钠分子的解离过程进行了理论研究.从计算结果中我们可以得到两个结论：第一,当泵浦-探测延迟时间超过300飞秒的时候,碘化钠分子开始光解离;第二,随着延迟时间的增加,有越来越多的处于激发态上的碘化钠分子被光解离.     

受激拉曼光谱系统的研制

拉曼光谱是一种包含丰富样品结构信息的光谱技术,但是拉曼光谱检测的缺点是检测灵敏度低和荧光干扰.本实验室研制的受激拉曼光谱系统,是将一束皮秒(10-12 s)脉宽的可见泵浦光和一束由飞秒(10-15 s)脉宽的探测白光共同作用于样品,产生受激拉曼信号.该光谱系统的拉曼泵浦光在可见和近紫外波段可连续调谐,可以同时获取受激拉曼光谱的增益和损失光谱,具有灵敏度高和抑制荧光干扰等优点.分别考察了拉曼泵浦光和拉曼探测光脉冲相对时序、拉曼泵浦光强度对受激拉曼光谱的影响,受激拉曼信号强度在拉曼泵浦和拉曼探测脉冲时间上完全重合时达到最大.在拉曼泵浦光强较小时,受激拉曼谱峰强度随泵浦光强度增大而增大;当拉曼泵浦光强度较大时,损失谱峰强度会趋于饱和,在研究的光强范围内增益谱峰会持续增长,未达到饱和.     

飞秒时间分辨荧光凹陷技术及其在振动驰豫…

发展出飞秒时间分辨受激发泵浦荧光凹陷探测技术，提高了飞秒时间分辨检测的灵敏度，其时间分辨能力理论上可达到激光脉冲宽度的极限。利用该方法研究了一些染料分子电子激发态的振动驰豫。     

Optical nonlinearity and ultrafast dynamics of ion exchanged silver nanoparticles embedded in soda-lime silicate glass

Ag nanoparticles embedded in soda-lime silicate glass were fabricated by ion-exchange and subse-quently annealing method. Z-scan technique, femtosecond time-resolved optical Kerr effect （OKE） technique and femtosecond pump-probe experiment were used to investigate the effects of laser wavelength and laser pulse duration as well as annealing temperature on the third-order optical nonlinearity and ultrafast dynamics of the composites. It was found that the third-order susceptibility of Ag nanoparticles composite glass measured by 400 nm pulse source is larger than that measured by 800 nm pulse source due to an enhancement effect of local field near surface plasmon resonance of Ag nanoparticles in silicate glass. The third-order optical nonlinearity measured by ns laser source is about two orders of magnitude larger than that measured from fs pulse. The annealing temperature has an important effect on the third-order optical nonlinearity and ultrafast dynamics of the composites. Third-order nonlinear susceptibility up to 10^-l0 esu and fast relaxation process up to 0.2 ps have been obtained in Ag nanoparticles doped glass.     

Direct observation of attosecond light bunching

Temporal probing of a number of fundamental dynamical processes requires intense pulses at femtosecond or even attosecond (1 as = 10(-18) s) timescales. A frequency 'comb' of extreme-ultraviolet odd harmonics can easily be generated in the interaction of subpicosecond laser pulses with rare gases: if the spectral components within this comb possess an appropriate phase relationship to one another, their Fourier synthesis results in an attosecond pulse train. Laser pulses spanning many optical cycles have been used for the production of such light bunching, but in the limit of few-cycle pulses the same process produces isolated attosecond bursts. If these bursts are intense enough to induce a nonlinear process in a target system, they can be used for subfemtosecond pump-probe studies of ultrafast processes. To date, all methods for the quantitative investigation of attosecond light localization and ultrafast dynamics rely on modelling of the cross-correlation process between the extreme-ultraviolet pulses and the fundamental laser field used in their generation. Here we report the direct determination of the temporal characteristics of pulses in the subfemtosecond regime, by measuring the second-order autocorrelation trace of a train of attosecond pulses. The method exhibits distinct capabilities for the characterization and utilization of attosecond pulses for a host of applications in attoscience.     

Cu薄膜的瞬态反射率及退火处理的影响

为了研究激光辐照金属薄膜后的超快热化动力学过程,利用磁控溅射技术在玻璃衬底上制备了Cu薄膜样品,同时取部分样品进行不同温度的退火处理.运用飞秒激光泵浦-探测技术观测了薄膜表面的反射率变化,研究了薄膜退火处理对反射率的影响.结果表明:飞秒激光作用下,Cu薄膜的瞬态反射率曲线分为稳定、快速上升、衰减和恢复4个阶段；退火处理对反射率曲线的峰值和衰减阶段的时间有影响,退火温度越高,反射率变化的峰值越小,衰减阶段所用的时间越长,即电子的冷却速率越慢；基于双温模型预测的电子温度与试验结果大致吻合,但是预测的电子冷却时间比试验要长.     

Femtosecond time-delay X-ray holography

Extremely intense and ultrafast X-ray pulses from free-electron lasers offer unique opportunities to study fundamental aspects of complex transient phenomena in materials. Ultrafast time-resolved methods usually require highly synchronized pulses to initiate a transition and then probe it after a precisely defined time delay. In the X-ray regime, these methods are challenging because they require complex optical systems and diagnostics. Here we propose and apply a simple holographic measurement scheme, inspired by Newton's 'dusty mirror' experiment, to monitor the X-ray-induced explosion of microscopic objects. The sample is placed near an X-ray mirror; after the pulse traverses the sample, triggering the reaction, it is reflected back onto the sample by the mirror to probe this reaction. The delay is encoded in the resulting diffraction pattern to an accuracy of one femtosecond, and the structural change is holographically recorded with high resolution. We apply the technique to monitor the dynamics of polystyrene spheres in intense free-electron-laser pulses, and observe an explosion occurring well after the initial pulse. Our results support the notion that X-ray flash imaging can be used to achieve high resolution, beyond radiation damage limits for biological samples. With upcoming ultrafast X-ray sources we will be able to explore the three-dimensional dynamics of materials at the timescale of atomic motion.     

The effect of hydrogen-bond in alcoholic solvent on the solvation ultrafast dynamics of oxazine 750 dye

The ultrafast dynamics of oxazine 750 dye was studied in methanol, ethanol, 1-propanol, 1-butanol solvents using the femtosecond time-resolved stimulated emission pumping fluorescence depletion （FS TR SEP FD） technique. The faster decays on the hundreds of femtosecond time scale and the slower decays on the order of picosecond were found. The intramolecular vibrational redistribution （IVR） and the solute-solvent intermolecular photoinduced electron transfer （ET） should account for the faster decay, while the slower decay is attributable to the diffusive solvent relaxation. The results show that the intermolecular hydrogen-bonding network will hinder the rearrangement of the alcoholic molecules in the solvaUon process and the time constants of the slower diffusive solvent relaxation decays are found to increase with the hydrogen-bonding energy in alcoholic solvents.     

Excited-state dynamics in light-harvesting complex of Rhodobacter sphaeroides

Photodynamics of peripheral antenna complexes,light-harvesting complex (LH2) of Rhodobacter (Rb) Sphaeroides 601,was studied using femtosecond pump-probe technique at different laser wavelengths. The obtained results reveal dramatic dynamical evolutions within B800 and B850 absorption bands of antenna complexes LH2. At excitation wavelength around 835 nm,a sharp photobleaching signal was observed which was assigned to the contribution of the two-exciton state,which was further confirmed by the power dependence measurement. Rate equations with eight-level scheme were used to calculate the population evolution in LH2 and the transient dynamics under femtosecond pulse excitation. The research results prove that not only the transition from ground state to one-exciton state but also that from one-exciton state to two-exciton state contribute to the photodynamics of B850.     

飞秒激光辐照CuZr非晶合金损伤动力学研究

采用考虑了电子压强梯度的双温分子动力学方法,研究了纳米CuZr非晶合金薄膜在脉宽为100 fs,能量密度为0.08～0.16 J/cm~2的飞秒激光辐照下的烧蚀动力学过程.结果表明,低能量密度下,电子压强梯度对靶材的结构损伤过程影响很小.高能量密度下,电子压强梯度对靶材内部的电子温度和晶格温度演化场产生了显著的影响,CuZr非晶合金薄膜的结构存在皮秒量级的由电子压强梯度诱导的非热烧蚀过程,并且随着能流密度的增大,这一超快的非热烧蚀过程在时间尺度上会得到提前.