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%。     

Image resolution and sensitivity in an environmental transmission electron microscope

An environmental transmission electron microscope provides unique means for the atomic-scale exploration of nanomaterials during the exposure to a reactive gas environment. Here we examine conditions to obtain such in situ observations in the high-resolution transmission electron microscopy (HRTEM) mode with an image resolution of 0.10nm. This HRTEM image resolution threshold is mapped out under different gas conditions, including gas types and pressures, and under different electron optical settings, including electron beam energies, doses and dose-rates. The 0.10nm resolution is retainable for H(2) at 1-10mbar. Even for N(2), the 0.10nm resolution threshold is reached up to at least 10mbar. The optimal imaging conditions are determined by the electron beam energy and the dose-rate as well as an image signal-to-noise (S/N) ratio that is consistent with Rose's criterion of S/N≥5. A discussion on the electron-gas interactions responsible for gas-induced resolution deterioration is given based on interplay with complementary electron diffraction (ED), scanning transmission electron microscopy (STEM) as well as electron energy loss spectroscopy (EELS) data.     

A low voltage time of flight electron emission microscope

This paper presents the design of a low voltage time of flight electron emission microscope (TOF-EEM), which should in principle be capable of acquiring spectral chemical information at nano-metre spatial resolution. The system will be able to operate as a photoelectron emission microscope (PEEM), an X-ray photoemission electron microscope (XPEEM), or a secondary electron emission microscope (SEEM). For each pixel in its highly magnified topographic image, the TOF-EEM column should be able to provide the emission spectrum with milli-electron-volt resolution. The system is designed to operate at secondary electron beam voltages of typically less than 100 V, and has the possibility of dynamically correcting for chromatic aberration. Provisional simulation results predict that the TOF-EEM column should be able to provide an image resolution of better than 2 nm.     

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.     

Resolution deterioration in emission electron microscopy due to object roughness

In the present paper a general analytic expression has been obtained and confirmed by a computer simulation which links the surface roughness of an object under study in an emission electron microscope and it's resolution. A quantitative derivation was made for the model case when there is a step on the object surface. It was shown that the resolution is deteriorated asymmetrically relative to the step. The effect sets a practical limit to the ultimate lateral resolution obtainable in an emission electron microscope.     

Areal density and spatial resolution of high energy electron radiography

Ultrafast imaging tools are of great importance for determining the dynamic density distribution in high energy density(HED) matter. In this work, we designed a high energy electron radiography(HEER) system based on a linear electron accelerator to evaluate its capability for imaging HED matter. 40 MeV electron beams were used to image an aluminum target to study the density resolution and spatial resolution of HEER. The results demonstrate a spatial resolution of tens of micrometers. The interaction of the beams with the target and the beam transport of the transmitted electrons are further simulated with EGS5 and PARMELA codes, with the results showing good agreement with the experimental resolution.Furthermore, the experiment can be improved by adding an aperture at the Fourier plane.     

时间分辨电子显微镜的数值模拟

对时间分辨电子显微镜进行了数值模拟。通过求解从样品透射出来的电子在静态磁场和动态电场的混合场中的运动,评价时间分辨电子显微镜的动态时空特性。根据该数值模拟,时间分辨电子显微镜能够在荧光屏上获得样品在不同时刻的6幅显微分幅图像。     

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.     

Control the revisit time of the electron wave packet

Ionization of molecules by strong laser fields launches an electron wave packet. This electron wave packet, which can be driven back by the field to recollide with the parent ion, has been widely explored to probe the ultrafast nuclear dynamics. We numerically demonstrate the precise control of the temporal characteristic of the recolliding electron wave packet (REWP) by orthogonally polarized two-color fields. Through changing the relative phase of the two fields, the revisit time of REWP can be manipulated with a resolution of less than 200 attos, thus significantly improving the resolution of the well known molecular clock. This provides an efficient method for real-time observation of the ultrafast molecular dynamics with attosecond resolution.     

Femtosecond spectroscopic imaging by time-of-flight photoemission electron microscopy

Advances in electron optics and fast-pulsed light sources have enabled the imaging of nanoscale structures with simultaneous energy and time resolutions. We present the results obtained from a time-resolved time-of-flight photoemission electron microscopy (TR-TOF-PEEM) system. This system combined the spatial resolution of conventional PEEM with the time resolution of a femtosecond-pulsed laser and the energy resolution of a TOF energy analyzer. The TOF-PEEM system consists of three electrostatic lenses in front, a drift tube for the measurement of TOF, and a delay line detector (DLD) at the end of the optics. The excitation source is femtosecond pulses from a cavity-dumped Ti:sapphire oscillator that is frequency-doubled to 400 nm using a β-barium borate (BBO) crystal. Using a pump-probe two-photon photoemission technique, we demonstrate an example of sub-100 nm space-resolved ultrafast time evolution of the electron energy spectra for the plasmon resonance of an Ag-coated Si nanostructure, which exhibited unexpectedly intense high energy photoemission signals that show different time evolution between bright and dark regions in a PEEM image.     

纳秒脉冲气体放电中逃逸电子束流的研究

经典的放电理论(Townsend和流注理论)不能很好地解释纳秒脉冲放电中的现象,近年来基于高能量电子逃逸击穿的纳秒脉冲气体放电理论研究受到广泛关注,有研究发现,高能逃逸电子是纳秒脉冲气体放电中的新特征参数,本文研制了用于测量纳秒脉冲放电中逃逸电子束流的收集器,并对脉宽3—5ns、上升沿1.2—1.6 n8激励的大气压纳秒脉冲气体放电中逃逸电子束流进行了测量,收集器采用类似法拉第杯的原理,利用金属极收集纳秒脉冲放电中的高能电子,并转换为电信号后由示波器采集,为了获得更好的逃逸电子束流波形,对逃逸电子束流收集器进行了优化设计,提高了收集器的阻抗匹配特性,基于上述的逃逸电子束流收集器,研究了纳秒脉冲气体放电中逃逸电子的特征,实验结果表明,所设计的收集器可以有效地测量到逃逸电子束流,改进设计后收集器测得的逃逸电子柬流的时间分辨率和幅值均得到提高,施加电压约80 kV时,大气压空气中的逃逸电子束流幅值可达160 mA,脉宽小于1ns,多个脉冲激励放电的结果表明逃逸电子束流收集器具有较好的可靠性,其瞬态响应与时间分辨率比较稳定。     

High resolution transmission electron microscopy to study very thin crystalline layers buried at an amorphous-crystalline interface

Structure characterisation of interfaces is a field of widespread application of high resolution transmission electron microscopy for its very high spatial resolution. Specimen thickness and electron optical condition have a deep influence on the high resolution electron transmission microscopy image contrast. Hence, in many cases, the real structure of the sample can be understood from experimental images only by comparison with the relevant simulation. Moreover, the understanding of the contrast variation of a few A at an interface is a task in which even the use of simulation could not produce an unequivocal solution of the experimental result. In this paper high resolution transmission electron microscopy image simulations show that two monolayers of crystalline material buried at an amorphous-crystalline interface can be successfully revealed and interpreted. The simulated images reproduce the experimental results as obtained from the Al/Si-As/n-GaAs (001) heterostructure.     

激光高能X射线成像中探测器表征与电子影响研究

基于激光尾场加速电子的高能X射线源具有高光子能量与小源尺寸的特点,在高空间分辨无损检测方面发挥着十分重要的作用.在X光机上测量了CsI针状闪烁屏、锗酸铋(BGO)闪烁阵列与DRZ闪烁屏的本征空间分辨率,并模拟了三类探测器对高能X射线的能量沉积响应,其中CsI针状闪烁屏的空间分辨率高达8.7 lp/mm.采用Ta转换靶产生的高能X射线开展透视照相,能够分辨最高面密度33.0 g/cm~2的两层客体结构.开展了X射线照相、X射线与电子混合照相以及电子照相三种情况的比对实验,在X射线产额不足或探测效率不够情况下采用X射线与电子混合透视照相的方案,以牺牲对比度为代价,能较大程度地提高图像信号强度.     

Inelastic electron scattering in nickel

Using a 200 keV electron spectrometer, with an energy resolution of ～0.25 eV and a momentum resolution of ～0.2 A^-1, we have measured the energy loss spectra for transmission of electrons through thin (～600 Å) Ni films. These results address the general question of the validity of momentum transfer estimates in electron loss scattering.Using low-energy electron backscattering, we have observed the dipole forbidden M₁ transition at 112 eV. For high-energy scattering, we have observed this transition only at high momentum transfer (q? 2 A^-1). These results indicates sizable contributions from high momentum transfer collisions in the low-energy experiments.     

An application of the electron mirror in the time-of-flight spectrometer

We suggest applying of the spherical electron mirror in the time-of-flight electron spectrometer with a position sensitive detector in order to increase the effective acceptance solid angle of the spectrometer. The spherical electron mirror is placed near the specimen and it focuses electrons on a position sensitive detector as a converging electron flux. The electron mirror increases the acceptance angle of the spectrometer by a factor of 20. The electron mirror of the spectrometer consists of an inner spherical electrode of the radius R and an outer spherical electrode of the radius 1.1R. The central segment of the inner electrode inside the linear angle of 80° is made of a grid. The detector plate radius is about 0.23R. The acceptance solid angle of the spectrometer with this electron mirror is about 1.1sr, the range of the polar angle of emission is 20°–90° relative to the surface normal, and the range of the azimuth angle of emission at its maximum is ±36° relative to the basic plane of the spectrometer. The design of the spectrometer allows to recover the electron trajectory for each detected electron and to calculate the energy and the emission angle of the electron. The energy resolution of the spectrometer is about 0.2 eV/ns for the electron energy of 10 eV. The energy range is from E_min0.1eU_r up to eU_r, where U_r is the retarding potential of the electron mirror. The perturbing influence of the grid of the electron mirror limits mainly the angular resolution of the spectrometer and affects relatively slightly the energy resolution. The electron spectrometer with two detectors and two electron mirrors symmetric about the spectrometer axis allows to measure electron pairs in coincidence in a wide range of emission angles and energies with k-resolutions.     

New trends in the conversion electron spectroscopy

The method of investigation of an electronic structure of chemical compounds and solids by high resolution measurement of internal conversion electron spectra for low-energy isomeric transitions is described.     

Practical spatial resolution of electron energy loss spectroscopy in aberration corrected scanning transmission electron microscopy

The resolution of electron energy loss spectroscopy (EELS) is limited by delocalization of inelastic electron scattering rather than probe size in an aberration corrected scanning transmission electron microscope (STEM). In this study, we present an experimental quantification of EELS spatial resolution using chemically modulated 2×(LaMnO(3))/2×(SrTiO(3)) and 2×(SrVO(3))/2×(SrTiO(3)) superlattices by measuring the full width at half maxima (FWHM) of integrated Ti M(2,3), Ti L(2,3), V L(2,3), Mn L(2,3), La N(4,5), La N(2,3) La M(4,5) and Sr L(3) edges over the superlattices. The EELS signals recorded using large collection angles are peaked at atomic columns. The FWHM of the EELS profile, obtained by curve-fitting, reveals a systematic trend with the energy loss for the Ti, V, and Mn edges. However, the experimental FWHM of the Sr and La edges deviates significantly from the observed experimental tendency.     

Atomic-resolution electron energy loss spectroscopy imaging in aberration corrected scanning transmission electron microscopy

The "delocalization" of inelastic scattering is an important issue for the ultimate spatial resolution of innershell spectroscopy in the electron microscope. It is demonstrated in a nonlocal model for electron energy loss spectroscopy (EELS) that delocalization of scanning transmission electron microscopy (STEM) images for single, isolated atoms is primarily determined by the width of the probe, even for light atoms. We present experimental data and theoretical simulations for Ti L-shell EELS in a [100] SrTiO3 crystal showing that, in this case, delocalization is not significantly increased by dynamical propagation. Issues relating to the use of aberration correctors in the STEM geometry are discussed.     

Lateral resolving power of a time-of-flight photoemission electron microscope

The lateral resolution of a time-of-flight photoemission electron microscope has been theoretically analyzed. It has been shown that the resolution limit can reach a few nanometers. The lateral resolution will be higher if the photoelectrons forming the image are characterized by a smaller acceptance angle obtained with the help of diaphragms in the crossover plane, a higher initial energy and a narrower interval of electron energies. The experimental results are in good agreement with the theoretical predictions. PACS 68.37.Xy     

超快电子衍射系统的时间空间分辨能力研究及其优化

超快电子衍射技术是研究物质瞬态结构变化及超快结构动力学的有效手段.研制了国内第一套同时具有超快时间分辨及超高空间分辨能力的超快电子衍射系统,并研究了在该超快电子衍射系统上实现超快时间分辨及超高空间分辨能力的技术手段及其优化方法.实验结果表明：经过优化后该系统可以具有优于500 fs的时间分辨能力,其空间分辨能力达到0.04%的衍射峰位置变化,对应的晶面变化为0.0005?.该系统可以为实时测量超快光脉冲激发的物质瞬态结构变化,特别是为研究晶体材料的超快动力学行为提供了强有力的实验工具. 关键词： 超快电子衍射 空间分辨 时间分辨