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     

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.     

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.     

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.     

Ultrafast Electron Diffraction with Spatiotemporal Resolution of Atomic Motion

Ultrafast electron diffraction （UED） is a rapidly advancing technique capable of recording the atomic-detail structural dynamics in real time. We report the establishment of the first UED system in China. Employing this UED apparatus, both the coherent and the concurrent thermal lattice motions in an aluminium thin-film, trigged by ultrafast laser heating, have been observed. These results demonstrate its ability to directly measure a sub-milli-angstrom lattice spacing change on a sub-picosecond time scale.     

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.     

飞秒电子衍射系统的设计

研发的超快电子衍射系统由超快电子枪、样品室、超快读出系统、电源系统,以及真空系统等组成,该超快电子衍射系统具有较高的时间分辩能力和较强的探测能力.光电阴极是蒸镀于MgFB2窗上的35 nm的银膜,该阴极对266 nm的紫外光比较敏感,有较高的量子效率,又具有很好的化学稳定性.用短磁聚焦系统来实现对光电子的聚焦,有两对偏转板,其中的一对在测量时间脉宽时用作扫描板.用双MCP探测器来增强电子图像的强度,其增益在104以上,具有单电子探测能力.系统的总时间脉宽设计为358 fs.     

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.     

超紧凑型飞秒电子衍射仪的设计

由于空间电荷效应的限制,产生百飞秒的极短电子脉冲是超快电子衍射技术的一大难点.同时,电子的穿透深度随着电子能量的增加而增加,而电子的散射几率却具有相反的规律.因而,除了时间分辨的提升,还需要可宽范围调节的电子能量以优化不同厚度样品对其的需求.基于此,提出并设计了一种新型超紧凑电子枪,结合均匀场阴极和可移动阳极的配置,可在10-125 kV加速电压范围内实现100 fs量级时间分辨率.通过优化设计高压电极轮廓,使得其轴上和整个阴极面的场增强因子在不同阴阳极间距下均小于约4%,从而保证了不同加速电压下最大轴上场强均可达10 MV/m量级,有效地抑制了电子脉冲的展宽效应;进一步将阳极小孔设计成可放置致密电镜载网的阶梯孔,一方面可将载网支撑的样品紧贴小孔后方放置,最大程度上缩短了电子从阴极到样品的时间弥散,同时也可以有效地减弱阳极孔对电子束的散焦效应,提升电子束的横向聚焦性能.     

Design of an MeV ultra-fast electron diffraction experiment at Tsinghua university

Time-resolved MeV ultra-fast electron diffraction (UED) is a powerful tool for structure dynamics studies. In this paper, we present a design of a MeV UED facility based on a photocathode RF gun at Tsinghua University. Electron beam qualities are optimized with numerical simulations, indicating that resolutions of 250 fs and 0.01 , and bunch charge exceeding 105 electrons are expected with technically achievable machine parameters. Status of experiment preparation is also presented.     

Photo-triggered pulsed cavity compressor for bright electron bunches in ultrafast electron diffraction

Temporally resolved observation of microscopic structural dynamics of solids with ultrafast electron diffraction (UED) requires extremely short pulsed, highly charged, monoenergetic electron beams with sufficient transverse coherence length of several unit cells of the investigated samples. However, Coulomb repulsion defeats these parameters in free propagation of an electron pulse initially bright on the photo cathode. We demonstrate a new electron pulse compressor design based on a simple and compact RF structure incorporating a pair of gallium arsenide photoconductive semiconductor switches that are triggered by femtosecond laser pulses, thereby providing a longitudinal voltage gradient of up to 20?V/ps. Our proof of principle experiment achieved compression of bunches containing 26,000 electrons to a duration of below 750?fs and a beam diameter of 300???m in the temporal and spatial focus of the device while maintaining the good beam collimation required for time resolved electron diffraction experiments. The simplicity of the compressor provides a strong incentive for its further development toward practical implementation in sub-relativistic UED experiments requiring the highest possible source brightness.     

室温下金属中电子格林艾森常数的测量

在室温条件下用自己研制的超快电子衍射实验设备精确测量了金属铝的电子格林艾森常数(γ_e).当飞秒脉冲激光瞬间加热铝膜时,电子和晶格对固体热膨胀的作用在时间域上是不同步的,借助于超快电子衍射实验设备的高时间分辨能力,可以摆脱以往测量非磁性金属材料时低温的限制,在室温条件下,实验通过直接观测瞬间加热的铝膜中电子和晶格对热膨胀的不同贡献得到电子的格林艾森常数. 关键词： 格林艾森常数 超快电子衍射 晶格热运动 电子热运动     

Ultrafast electron diffraction

Ultrafast electron diffraction(UED) technique has proven to be an innovative tool for providing new insights in lattice dynamics with unprecedented temporal and spatial sensitivities. In this article, we give a brief introduction of this technique using the proposed UED station in the Synergetic Extreme Condition User Facility(SECUF) as a prototype. We briefly discussed UED's functionality, working principle, design consideration, and main components. We also briefly reviewed several pioneer works with UED to study structure-function correlations in several research areas. With these efforts,we endeavor to raise the awareness of this tool among those researchers, who may not yet have realized the emerging opportunities offered by this technique.     

A proposal for fs-electron microscopy experiments on high-energy excitations in solids

Recent advances in ultrafast technology enable both the study and the control of materials properties thanks to the ability to record high temporal resolution movies of their transformations, or the ability to generate new states of matter by selecting ad hoc an excitation to drive the system out of equilibrium. The holy grail of this type of experiments is to combine a high tuneability of the excitation with a wide observation window. For example, this is achieved in multidimensional optical spectroscopy where the response to several excitation energies is monitored in a broad energy range by a large bandwidth optical pulse. In this article, the possibility to combine the chemical sensitivity of intense tuneable X-rays pulses from a free electron laser, with the wide range of observables available in an ultrafast transmission electron microscope is discussed. The requirements for such experiments are quantified via estimates based on state of the art experiments and simulations, and it is proposed that ultrafast electron imaging, diffraction and spectroscopy experiments can be performed in combination with a chemically selective X-ray excitation of materials.     

超快电子衍射装置的束流能量反馈控制

上海交通大学的超快电子衍射(UED)装置由一台电子直线加速器作为驱动,电子枪为一台光阴极微波电子枪。加速器在运行中电子枪会偶尔打火,腔体失谐,造成束流损失,束流能量产生变化,束流需要很长时间才能恢复到初始状态,影响了用户的使用。为此,对低电平控制器(LLRF)的幅度相位控制环路进行了改进,增加了能量反馈,代替了幅度反馈,通过对束流的中心位置进行实时的反馈以控制低电平控制器输出信号的幅度,保证了电子束流的能量稳定和电子枪加速场强的稳定。长时间的稳定性测试表明,电子枪在打火产生时,束流能量可以很快恢复,能量抖动由4.2933×10^-4(RMS)提高到2.8557×10^-4(RMS),实现了束流能量的长期稳定。     

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%。     

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.     

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     

A method for determining foil thicknesses in TEM by using convergent beam electron diffraction under weak beam conditions

In the present work, convergent beam electron diffraction was studied in zirconium (a material of intermediate atomic number) at 300 keV, under weak beam diffraction conditions. For a particular thickness, the details in an observed low order disc were matched to those calculated using the multibeam dynamical theory. This presents the possibility of determining foil thickness over a wide range, with an estimated experimental accuracy of ≈7% or less. In contrast to other convergent beam techniques, the present method, which uses weak beam conditions, can employ commonly-occurring low order reflections to extract thicknesses.

A simple equation based on the two beam approximation, is derived to determine foil thickness (to within ≈ 10%) without resorting to detailed image matching. This equation can be used for a rough estimate of foil thickness while carrying out TEM observations.