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.     

三重简并拓扑半金属磷化钼的时间分辨超快动力学

拓扑半金属磷化钼(MoP)同时具有三重和二重简并费米子.为了研究其费米面以上的激发态超快动力学特性,对其进行了时间分辨超快泵浦-探测实验.获得了MoP的准粒子动力学,包含来源于电子-声子散射的快分量,寿命为0.3 ps,以及来源于声子-声子散射的慢分量,寿命为150 ps.温度依赖的研究表明,快分量和慢分量的弛豫寿命均随着温度的增加产生微小增大.同时还激发并探测到一支相干态声学支声子,其由热应力引起,频率为0.033 THz且不随温度而改变.对于MoP激发态准粒子超快动力学以及相干态声子的研究为理解该体系总体的激发态超快动力学特性以及电子-声子相互作用对温度的依赖提供了有益的实验依据.     

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.     

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     

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%。     

半导体超晶格声子激光器的研究进展

太赫兹频率的相干声子在纳米尺度器件的探测和操控领域具有重要的应用价值。半导体超晶格声子激光器是实现太赫兹频率相干声子源稳定输出的重要途径。本文首先回顾了GHz到THz频率范围声学放大的多种方法,然后详细阐述了超晶格声子放大、超晶格声学布拉格镜的工作原理与设计方法以及声子激光器的阈值条件,同时总结了电抽运和光抽运结构器件的研究现状,最后简要讨论了亚太赫兹声子激光器在声-电子领域的应用。分析表明,这种能够产生强相干太赫兹声子的半导体超晶格声子激光器在纳米尺度器件的探测与成像等方面具有广阔的发展前景。     

超快电子衍射研究分子动力学

随着超快激光、超快X射线和超快电子束技术在近年的快速发展,通过泵浦探测的方法在超快的尺度观察原子运动正逐步成为可能. 本综述将讨论如何利用超快电子衍射技术探测激光激发的分子动力学过程. 此技术以电子束为探针,能以飞秒量级的时间分辨率和埃量级的空间分辨率追踪激光触发的原子运动. 阐述超快电子衍射技术的基本原理和最新进展,同时介绍其在研究分子动力学方面的代表性工作. 这项“桌面级”的技术和X射线自由电子激光大科学装置互补,预期将在化学反应动力学领域发挥重要作用.     

超快电子衍射研究分子动力学（英文）

随着超快激光、超快X射线和超快电子束技术在近年的快速发展,通过泵浦探测的方法在超快的尺度观察原子运动正逐步成为可能.本综述将讨论如何利用超快电子衍射技术探测激光激发的分子动力学过程.此技术以电子束为探针,能以飞秒量级的时间分辨率和埃量级的空间分辨率追踪激光触发的原子运动.阐述超快电子衍射技术的基本原理和最新进展,同时介绍其在研究分子动力学方面的代表性工作.这项"桌面级"的技术和X射线自由电子激光大科学装置互补,预期将在化学反应动力学领域发挥重要作用.     

相干光学声子的操控以及对能量输运过程的影响

利用脉冲整形器生成双脉冲泵浦光,通过调整双脉冲的间隔时间,在不改变泵浦光能量密度的前提下,实现了相干光学声子的增强和完全消除,进而研究了相干光学声子对半导体能量输运过程的影响。实验直接验证了光学声子在超快能量输运过程的重要作用。相干光学声子增强时测量得到的热电子冷却以及晶格加热的特征时间均减小,因此激发相干光学声子可提高超快能量输运效率。当电子与晶格处于热平衡状态时,相干光学声子增强和消除前后反射信号的下降趋势相同,因此光学声子对热量输运没有显著影响。     

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 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.     

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.     

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.     

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.     

Design of an ultrafast electron diffractometer with multiple operation modes

Directly resolving structural changes in material on the atomic scales of time and space is desired in studies of many disciplines. Ultrafast electron diffraction(UED), which combines the temporal resolution of femtosecond-pulse laser and the spatial sensitivity of electron diffraction, is an advancing methodology serving such a goal. Here we present the design of a UED apparatus with multiple operation modes for observation of collective atomic motions in solid material of various morphologies. This multi-mode UED employs a pulsed electron beam with propagation trajectory of parallel and convergent incidences, and diffraction configurations of transmission and reflection, as well utilities of preparation and characterization of cleaned surface and adsorbates. We recorded the process of electron–phonon coupling in single crystal molybdenum ditelluride following excitation of femtosecond laser pulses, and diffraction patterns of polycrystalline graphite thin film under different settings of electron optics, to demonstrate the temporal characteristics and tunable probe spot of the built UED apparatus, respectively.     

Generation mechanism for coherent LO phonons in surface-space-charge fields of III-V-compounds

We report on details of coherent LO phonon generation in surface-space-charge regions of III-V-compounds by optical injection of free carriers with laser pulses of 50 fs duration at 2 eV. Both the dynamics of the transient surface field, as well as the coherent lattice vibration, are measured via electro-optic sampling techniques under different experimental conditions. The driving force for the coherent phonon vibration is the sudden depolarization of the crystal lattice due to ultrafast screening of the intrinsic electrical surface field by photoexcited free carriers.     

Discrete solitons and soliton-induced dislocations in partially coherent photonic lattices

We investigate both experimentally and theoretically the interaction between a light beam and a photonic lattice optically induced with partially coherent light. We demonstrate a clear transition from two-dimensional discrete diffraction to discrete solitons in such a partially coherent lattice and show that the nonlinear interaction process is associated with a host of new phenomena including lattice dislocation, lattice deformation, and creation of structures akin to optical polarons.     

化学反应飞秒相干动力学与激光相干控制——1999年诺贝尔化学奖介绍

文章主要介绍了１９９９ 年诺贝尔化学奖得主艾哈默德·泽维尔（Ａｈｍｅｄ．Ｈ．Ｚｅｗａｉｌ） 教授的获奖工作———用飞秒技术和飞秒光谱的方法研究化学反应飞秒相干动力学,叙述了它们的原理、方法和应用,并简要介绍了其获奖背景、重要意义、相关研究及应用展望．