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.     

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     

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.     

Ultrafast structural changes measured by time-resolved X-ray diffraction

Received: 17 April 1998/Accepted: 17 April 1998     

An accurate dynamical electron diffraction algorithm for reflection high-energy electron diffraction

The conventional multislice method (CMS) method, one of the most popular dynamical electron diffraction calculation procedures in transmission electron microscopy, was introduced to calculate reflection high-energy electron diffraction (RHEED) as it is well adapted to deal with the deviations from the periodicity in the direction parallel to the surface. However, in the present work, we show that the CMS method is no longer sufficiently accurate for simulating RHEED with the accelerating voltage 3–100 kV because of the high-energy approximation. An accurate multislice (AMS) method can be an alternative for more accurate RHEED calculations with reasonable computing time. A detailed comparison of the numerical calculation of the AMS method and the CMS method is carried out with respect to different accelerating voltages, surface structure models, Debye–Waller factors and glancing angles.     

Ultrafast electron microscopy in material science

Recent advances in the ultrafast transmission electron microscope(UTEM), with combined spatial and temporal resolutions, have made it possible to directly visualize the atomic, electronic, and magnetic structural dynamics of materials.In this review, we highlight the recent progress of UTEM techniques and their applications to a variety of material systems.It is emphasized that numerous significant ultrafast dynamic issues in material science can be solved by the integration of the pump–probe approach with the well-developed conventional transmission electron microscopy(TEM) techniques. For instance, UTEM diffraction experiments can be performed to investigate photoinduced atomic-scale dynamics, including the chemical reactions, non-equilibrium phase transition/melting, and lattice phonon coupling. UTEM imaging methods are invaluable for studying, in real space, the elementary processes of structural and morphological changes, as well as magnetic-domain evolution in the Lorentz TEM mode, at a high magnification. UTEM electron energy-loss spectroscopic techniques allow the examination of the ultrafast valence states and electronic structure dynamics, while photoinduced near-field electron microscopy extends the capability of the UTEM to the regime of electromagnetic-field imaging with a high real space resolution.     

Ultrafast electron interactions in metal clusters

The recent extension of time-resolved femtosecond optical techniques to the investigation of the ultrafast electron scattering processes in metal clusters offers the unique possibility to follow their evolution from a bulk to a confined metal. The size dependent results obtained in model materials, the noble metals, are presented, focusing on the impact of the confinement on energy redistribution processes (electron–electron and electron–phonon coupling). Their application to the investigation of the acoustic vibration property of cluster and to the cluster-surrounding matrix energy transfers are also discussed. To cite this article: N. Del Fatti, F. Vallée, C. R. Physique 3 (2002) 365–380.     

Ultrafast structural dynamics studied by kilohertz time-resolved x-ray diffraction

Ultrashort multi-ke V x-ray pulses are generated by electron plasma produced by the irradiation of femtosecond pulses on metals. These sub-picosecond x-ray pulses have extended the field of x-ray spectroscopy into the femtosecond time domain. However, pulse-to-pulse instability and long data acquisition time restrict the application of ultrashort x-ray systems operating at low repetition rates. Here we report on the performance of a femtosecond laser plasma-induced hard x-ray source that operates at 1-k Hz repetition rate, and provides a flux of 2.0 × 1010 photons/s of Cu Kαradiation. Using this system for time-resolved x-ray diffraction experiments, we record in real time, the transient processes and structural changes induced by the interaction of 400-nm femtosecond pulse with the surface of a 200-nm thick Au(111) single crystal.     

Ultrafast dynamics of electron thermalization in gold

Time-resolved surface second-harmonic generation (SHG) is used to probe electron relaxation processes in gold following intense laser excitation at 1.55 eV. For the first time, an electron temperature ( T(e)) dependent enhancement in the SHG signal is clearly observed at T(e) above 0.7 eV, which is shown to relate to the thermalization of nonequilibrium hot electrons. Therefore, the relaxation dynamics of the transient nonequilibrium electrons in the high T(e) regime is directly resolved by monitoring the time evolution of the SHG signal.     

Ultrafast x-ray diffraction using a streak-camera detector in averaging mode

We demonstrate an apparatus for measuring time-dependent x-ray diffraction. X-ray pulses from a synchrotron are diffracted by a pair of Si(111) crystals and detected with an x-ray streak camera that has single-shot resolution of better than 1 ps. The streak camera is driven by a photoconductive switch, which is triggered by 100-fs laser pulses at a repetition rate of 1 kHz. The laser and the streak camera are synchronized with the synchrotron pulses. In the averaging mode, trigger jitter results in 2-ps temporal resolution. We measured the duration of 5-keV pulses from the Advanced Light Source synchrotron to be 70ps.     

Surface studies by electron diffraction

The problems in the analysis of surface structures by means of electron diffraction, particularly at low energy, are reviewed. A brief introduction is given to the basic scattering and diffraction phenomena occurring at a solid surface after which the nature of the experimental diffraction data is described. The theoretical interpretation of the diffracted intensity by various kinematical and dynamical methods is outlined and the present difficulties in obtaining a complete surface structure determination are examined. The different types of ordered and disordered layers which may be formed on a surface—usually by adsorption of foreign species—are discussed and the interpretation of the corresponding diffraction patterns is illustrated by some examples.     

苯乙炔分子电子激发态超快动力学研究

采用飞秒时间分辨质谱技术结合飞秒时间分辨光电子影像技术研究了苯乙炔分子电子激发态超快非绝热弛豫动力学.用235 nm光作为泵浦光,将苯乙炔分子激发到第二激发态S2,用400 nm光探测激发态的演化过程.时间分辨的母体离子的变化曲线用指数和高斯函数卷积得到不同的两个组分,一个是超快衰减组分,时间常数为116 fs,一个是慢速组分,时间常数为106 ps.通过分析时间分辨的光电子影像得到光电子动能分布,结合时间分辨光电子能谱数据发现,时间常数为116 fs的快速组分反映了S2态向S1态的内转换过程.实验还表明S1态通过内转换被布局后向T1态的系间窜跃过程为重要的衰减通道.本工作为苯乙炔分子S2态非绝热弛豫动力学提供了较清晰的物理图像.     

超快时间分辨光电子显微镜技术及应用

光电子显微镜是一种基于光电效应的电子显微镜,利用样品不同空间位置光电子产量的差异作为图像衬度进行投影成像。其成像速度快、空间分辨率高、探测无损伤等特点和优势,在表面科学、表面等离激元学、半导体学等学科有着广泛应用。另外,结合超快光泵浦探测技术为光电子显微镜提供了高时间分辨能力,特别适用于高时空分辨的动力学过程研究。时间分辨光电子显微镜是具备多维度直观测量的技术方法,为研究人员开辟了新的道路。文章首先简要回顾电子显微成像技术的发展,然后介绍在表面等离激元学和半导体物理领域中应用光电子显微镜的最新进展,最后介绍北京大学最近建设的超快光电子显微镜系统和相关研究工作及展望。     

Isolated attosecond electron wave packet diffraction

Wave-particle duality is one of the most fundamental and mysterious natures of matters.Here,we present an interesting scheme of isolated electron wave packet diffraction with a few-cycle laser pulse and an extreme ultraviolet (XUV) pulse.The diffraction fringes are clearly present in the laser dressed XUV photoelectron spectra,strongly resembling the Airy diffraction pattern of optical waves.This phenomenon suggests a great potential of attosecond diffractometry.According to this scheme we also propose a simple method to determine the XUV pulse duration from the photoelectron spectra with a rather high resolution.     

Ultrafast coherent electron transport in semiconductor quantum cascade structures

Coherent electron transport is studied in an electrically driven quantum cascade structure. Ultrafast quantum transport from the injector into the upper laser state is investigated by midinfrared pump-probe experiments directly monitoring the femtosecond saturation and subsequent recovery of electrically induced optical gain. We demonstrate for the first time pronounced gain oscillations giving evidence for a coherent electron motion. The coexistence of a long dephasing time of quantum coherence and high Coulomb scattering rates in the injector points to the occurrence of scattering-induced coherence in electron transport.     

电子双缝衍射的计算机模拟

根据电子双缝衍射强度分布函数,利用Visual Basic编程,实现了电子双缝衍射的计算机模拟.该模拟不仅生动再现了电子衍射图像,而且通过控制电子产生的速度,能让电子逐个打到屏上,能加深电子是概率波的认识.程序语言简单易学,利于进一步开发.     

Atomic resolution three-dimensional electron diffraction microscopy

We report the development of a novel form of diffraction-based 3D microscopy to overcome resolution barriers inherent in high-resolution electron microscopy and tomography. By combining coherent electron diffraction with the oversampling phasing method, we show that the 3D structure of a nanocrystal can be determined ab initio at a resolution of 1 A from 29 simulated noisy diffraction patterns. This new form of microscopy can be used to image the 3D structures of nanocrystals and noncrystalline samples, with resolution limited only by the quality of sample diffraction.     

Medium energy electron diffraction on aluminum

Measurements of the specular beam intensity in the medium range of energy (645 eV and 980 eV) are presented for the aluminum (001) and (110) surfaces. They have been performed with a LEED goniometer allowing to achieve high accuracy in the determination of the angular parameters of the diffraction experiment. The experimental results are displayed in the form of iso-intensity maps in (θ, φ) coordinates at a constant primary beam energy. θ denotes the colatitude angle of incidence and is varied in the range 30° to 80°. φ denotes the azimuth and is varied between 0° and 360°. Sections of the maps at constant angle of incidence are known as rotation diagrams. A model calculation ignoring intra-layer multiple scattering, but incorporating inter-layer multiple scattering processes shows the prominent role of the latter, in many cases, and the non-negligible contribution of the former in other cases. Sections of the maps at constant azimuth are called incidence-profiles. They are very sensitive to the azimuth and very hard to compute. Using the preceding model calculation, average incidence profiles have been computed, using as input parameters the refractive and absorptive potentials and the surface normal relaxation parameter obtained by a pseudo-kinematic analysis of experimental average incidence profiles as explained in another paper. The peak position and width have been compared to those obtained from the pseudo-kinematic calculation. From the result, it is shown that if averaging is performed according to a specific set of restrictive rules, the pseudokinematic analysis of the data has a semi-quantitative meaning.