用超快电子衍射技术研究Al薄膜的超快动力学行为

超快电子衍射（UED）技术因其同时具有亚皮秒的时间分辨和亚毫埃的空间分辨能力,成为研究物质瞬态结构变化,特别是研究晶格材料超快动力学的有力工具.应用国内首台自行研制的UED系统,我们实时测量了超快激光脉冲激发下,20 nm金属Al多晶薄膜产生的相干声子和晶格热运动.实验结果显示,在晶格热运动加剧的同时,热应力的作用使晶格产生了相干振荡,并最终膨胀达到新的平衡位置.实验中测得的振荡周期以及晶格上升的温度与理论计算的结果符合较好,展示了UED技术在超快晶格动力学研究方面的广阔应用前景 关键词： 超快电子衍射 相干声子 晶格热运动     

飞秒电子衍射系统的静态特性研究

超快电子衍射系统是认识超快物理、化学及生物过程的重要工具之一.介绍了自主研制的一套飞秒电子衍射系统，调试并测量了该系统的电子束斑特性、X-Y偏转板的偏转灵敏度等.在该系统上进行了金膜的静态电子衍射图像的测量. 关键词： 飞秒电子衍射 偏转灵敏度 时间分辨 空间分辨     

超快电子衍射技术及其应用

时间和空间上实时观测原子运动对于自然科学研究有着非常重大的意义, 而超快电子衍射(UED)技术同时具备飞秒激光脉冲的高时间分辨特性和电子衍射技术的高空间特性, 可以为实时观测原子级分辨尺度物质的结构变化提供一种有效工具. 本文综述了超快电子衍射技术的发展历史、实验方法以及相关应用, 并且展望了超快电子衍射技术未来的发展.     

超快电子衍射仪理论及实验研究

研制一套同时具有时间分辨及空间分辨能力的超快电子衍射(UED)系统,理论时间分辨能力达到300 fs,空间分辨能力160 lp/mm,并对该系统进行了静态性能分析。实验表明,优化后系统电子束直径约为300 m,电子打靶角度约为0.09,同时对x和y偏转板的灵敏度、电子束斑尺寸及位置稳定性进行定量分析,利用该系统进行多晶铝膜电子衍射实验,分析衍射图样表明系统最小可以分辨单个晶格间距的0.36%。     

长寿命吸收过程对超快动力学过程测量的影响

使用飞秒时间分辨抽运-探测透射光谱技术,实验研究了GaAs体材料中光激发载流子的超快弛豫动力学的波长依赖.在相同的光激发载流子浓度和抽运/探测比时,发现760 nm和780 nm两中心波长处的瞬态透射变化延迟扫描信号出现负的和振荡的信号.与模拟计算结果对比,判定该实验瞬态信号是错误的.分析探测器输出波形,发现是由于反相波形导致的,而引起反相波形的原因在于样品中存在长寿命的吸收过程.指出通过提高探测器上的抽运/探测比能够矫正反相波形,从而获得正确的瞬态透射变化动力学.提高探测器上的抽运/探测比与目前的应尽量减小抽运光对探测器的散射贡献的观点是对立的.文章的研究结果对应用抽运-探测时间分辨光谱技术正确地测量超快瞬态动力学过程具有重要的参考价值. 关键词： 时间分辨抽运-探测透射光谱 饱和吸收 吸收增强 GaAs体材料     

高相干超快电子源研究进展

以原子级时空分辨监测物质的动力学行为并从最根本层面理解自然界中的微观基本过程一直是飞秒物理、飞秒化学以及飞秒生物学研究的目标.时间分辨电子衍射巧妙地结合了抽运-探测技术和电子衍射技术,可实现直接"观察"和"冻结"类似的超快过程.然而,目前常用的超快电子探针的横向相干性仍受到电子源的初始尺寸、有效温度、能量弥散以及电子间固有库仑排斥的限制,还很难分辨化学和生物相关的复杂有机分子.近年来大量研究工作都集中在发展高相干的超短电子源,其不仅对时间分辨电子衍射研究起到推动作用,也将极大地促进超快电子显微镜、相干衍射成像以及叠层成像等的发展.本综述以相干性为主线,介绍了几种常用平面阴极光电发射源的研究进展,并从产生机理、独有特性和实验成果方面讨论了尖端发射源和冷原子电子源这两类新型的高相干超快电子源,最后对衍射技术的相干性发展和未来应用进行了展望.     

基于瞬态光克尔效应的超快光学快门技术

系统介绍了几种基于瞬态光克尔效应的超快光学快门技术,包括传统的光克尔双折射快门技术,瞬态光栅快门技术,以及利用瞬态克尔透镜效应的光学快门技术。这些技术都是在泵浦-探测的实验配置基础上,利用门控光对克尔介质折射率的瞬态调制导致的信号光的相位（偏振态）、传播方向或光束发散角等光学特性的改变实现对信号光的超快时间分辨测量。对比讨论了这些超快快门技术的工作原理和实验配置,结果表明瞬态光束偏折快门技术相比其他快门技术具有无偏振配置要求、无相位匹配条件、超宽带光谱响应范围的特点,在光与物质相互作用的超快动力学研究中具有更为广阔的应用前景。     

时间分辨偏振红外光谱及其应用

时间分辨偏振红外光谱已被广泛应用于研究光化学过程中的分子结构动力学. 通过测定瞬态物质跃迁偶极矩之间的角度等结构信息,可以提供光化学过程中伴随的电荷分布、分子结构和构象变化等动态信息. 包括简要介绍时间分辨偏振红外光谱技术的原理和应用：(i) 时间分辨偏振红外光谱概述;(ii) 时间分辨偏振红外光谱的原理及其优势;(iii) 利用时间分辨偏振红外光谱探测多种化学动力学过程,例如蛋白质构象动力学、激发态的电子局域化和光致异构化等;(iv) 时间分辨偏振红外光谱的局限和发展前景.     

飞秒时间分辨的能谱分析光电子显微镜：异质结超快载流子动力学测量

本文成功搭建了一套集成了能谱分析功能的时间分辨光电子显微镜系统(TR-PEEM),能够对电子密度分布进行时间分辨和能量分辨的成像.这套4D显微镜在空间、时间、能量多维度获取电子动力学信息提供了前所未有的手段.本文使用184 fs的时间分辨、150 meV的能量分辨和优于150 nm的空间分辨对半导体进行了测量,在Si(111)表面的Pb岛上获得了微区光电子能谱和能量分辨的TR-PEEM图像.实验结果表明,这套系统是进行异质结载流子动力学观察的有力工具,有助于在亚微米/纳米空间尺度和超快时间尺度上加深对半导体性质的理解.     

超快电子枪发射系统的优化设计

改进了超快电子衍射系统发射部分的数值计算模型和处理方法,使得计算结果更加接近于实际发射情形.研究了阴极表面面型对超快电子衍射系统时间分辨率的影响,提出了改进超快电子衍射系统时间分辨率的一个思路,该思路对于超快电子枪的设计及提高系统时间分辨率具有一定的作用.     

Compressing ultrafast electron pulse by radio frequency cavity

An ultrafast electron diffraction technique with both high temporal and spatial resolution has been shown to be a powerful tool to observe the material transient structural change on an atomic scale.The space charge forces in a multi-electron bunch will greatly broaden the electron pulse width,and therefore limit the temporal resolution of the high brightness electron pulse.Here in this work,we design an ultrafast electron diffraction system,and utilize a radio frequency cavity to realize the ultrafast electron pulse compression.We experimentally demonstrate that the stretched electron pulse width of14.98 ps with an electron energy of 40 keV and the electron number of 1.0 ×10~5 can be maximally compressed to about0.61 ps for single-pulse measurement and 2.48 ps for multi-pulse measurement by using a 3.2-GHz radiofrequency cavity.We also theoretically and experimentally analyze the parameters influencing the electron pulse compression efficiency for single-and multi-pulse measurements by considering radiofrequency field time jitter,electron pulse time jitter and their relative time jitter.We suggest that increasing the electron energy or shortening the distance between the compression cavity and the streak cavity can further improve the electron pulse compression efficiency.These experimental and theoretical results are very helpful for designing the ultrafast electron diffraction experiment equipment and compressing the ultrafast electron pulse width in a future study.     

Bunch evolution study in optimization of MeV ultrafast electron diffraction

Megaelectronvolt ultrafast electron diffraction (UED) is a promising detection tool for ultrafast processes. The quality of diffraction image is determined by the transverse evolution of the probe bunch. In this paper, we study the contributing terms of the emittance and space charge effects to the bunch evolution in the MeV UED scheme, employing a mean-field model with an ellipsoidal distribution as well as particle tracking simulation. The small transverse dimension of the drive laser is found to be critical to improve the reciprocal resolution, exploiting both smaller emittance and larger transverse bunch size before the solenoid. The degradation of the reciprocal spatial resolution caused by the space charge effects should be carefully controlled.     

Bunch evolution study in optimization of Me V ultrafast electron diffraction

Megaelectronvolt ultrafast electron diffraction（UED） is a promising detection tool for ultrafast processes.The quality of diffraction image is determined by the transverse evolution of the probe bunch. In this paper, we study the contributing terms of the emittance and space charge effects to the bunch evolution in the MeV UED scheme, employing a mean-field model with an ellipsoidal distribution as well as particle tracking simulation. The small transverse dimension of the drive laser is found to be critical to improve the reciprocal resolution, exploiting both smaller emittance and larger transverse bunch size before the solenoid. The degradation of the reciprocal spatial resolution caused by the space charge effects should be carefully controlled.     

Ultrafast structural dynamics with table top femtosecond hard X-ray and electron diffraction setups

The following tutorial review is directed to graduate students willing to be part of the emerging field of ultrafast structural dynamics. It provides them with an introduction to the field and all the very basic assumptions and experimental tricks involved in femtosecond (fs) diffraction techniques. The concept of stroboscopic photography and its implication in ultrafast science are introduced. Special attention is paid to the generation of ultrashort electron and hard X-ray pulses in table top setups, and a direct comparison in terms of brightness and temporal resolution between current table top and facility-based methodologies is given for proper calibration. This review is focused on ultrafast X-ray and electron diffraction techniques. The progress in the development of fs-structural probes during the last twenty years has been tremendous. Current ultrafast structural probes provide us with the temporal and spatial resolutions required to observe atoms in motion. Different compression approaches have made it possible the generation of ultrashort and ultrabright electron pulses with an effective brightness close to that of fs-hard X-ray pulses produced by free electron lasers. We now have in hand a variety of ultrafast structural cameras ready to be applied for the study of an endless list of dynamical phenomena at the atomic level of inspection.     

Influence of Time-of-Flight Chromatic Aberration on the Dynamics of Propagation of Pulsed Electron Beam in Ultrafast Electron Microscopy: A New Strategy for Better Temporal Resolution

Journal of Experimental and Theoretical Physics - A common strategy aimed at achieving a high temporal resolution in ultrafast electron microscopy and diffraction is based on the use of strong...     

How to realize an ultrafast electron diffraction experiment with a terahertz pump: A theoretical study

To integrate a terahertz pump into an ultrafast electron diffraction (UED) experiment has attracted much attention due to its potential to initiate and detect the structural dynamics both directly. However, the deflection of the electron probe by the electromagnetic field of the terahertz pump alters the incident angle of the electron probe on the sample, impeding it from recording structural information afterwards. In this article, we studied this issue by a theoretical simulation of the terahertz-induced deflection effect on the electron probe, and came up with several possible schemes to reduce such effect. As a result, a terahertz-pump-electron-probe UED experiment with a temporal resolution comparable to the terahertz period is realized. We also found that MeV UED was more suitable for such terahertz pump experiment.     

Accurate retrieval of structural information from laser-induced photoelectron and high-order harmonic spectra by few-cycle laser pulses

By analyzing accurate theoretical results from solving the time-dependent Schr?dinger equation of atoms in few-cycle laser pulses, we established the general conclusion that laser-generated high-energy electron momentum spectra and high-order harmonic spectra can be used to extract accurate differential elastic scattering and photo-recombination cross sections of the target ion with free electrons, respectively. Since both electron scattering and photoionization (the inverse of photo-recombination) are the conventional means for interrogating the structure of atoms and molecules, this result implies that existing few-cycle infrared lasers can be implemented for ultrafast imaging of transient molecules with temporal resolution of a few femtoseconds.