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.     

Femtosecond X-rays from relativistic electrons: new tools for probing structural dynamics

Femtosecond X-ray science is a new frontier in ultrafast research in which time-resolved measurement techniques are applied with X-ray pulses to investigate structural dynamics at the atomic scale on the fundamental time scale of an atomic vibrational period (∼100 fs). This new research area depends critically on the development of suitable femtosecond X-ray sources with the appropriate flux (ph/(s·0.1% BW)), brightness (ph/(s·mm²·mrad²·0.1% BW)), and tunability for demanding optical/X-ray pump probe experiments. In this paper we review recently demonstrated techniques for generating femtosecond X-rays via interaction between femtosecond laser pulses and relativistic electron beams. We give an overview of a novel femtosecond X-ray source that is proposed based on a linear accelerator combined with X-ray pulse compression.     

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.     

Dynamics of Self-Organized and Self-Assembled Structures,by Rashmi C. Desai and Raymond Kapral

The arrival of the first hard X-ray free electron laser facilities promises new advances in structural dynamics and nanoscale imaging that will have impact across the sciences. This introductory review is intended to cover the basic physics behind this potential and illustrate the current state-of-the-art by discussing a number of recent findings from the LCLS facility at the Stanford Linear Accelerator Centre (SLAC). We concentrate on the new science using these light sources rather than the new light source technology itself, although a brief introduction to the operation of LCLS is given. Emphasis is placed upon the new regime of high intensity X-ray matter interaction physics with ultrashort X-ray pulses. We discuss how the unique combination of X-ray parameters will open new opportunities for time resolved structural studies and how the high brightness enables a new class of coherent diffraction X-ray imaging. The potential importance of this new imaging method in the study of nanostructures and biological systems at the sub-cellular and molecular level will be outlined.     

基于光纤中脉冲压缩与受激喇曼散射的超短光脉冲产生方法

本文系统地综述了基于单模光纤中脉冲压缩与超快受激喇曼散射过程的超短光脉冲产生方法、原理及其进展,报道了我们最近的研究结果,讨论了在光纤中实现高效率超短光脉冲产生的途径.     

VUV超短脉冲的产生及其在超快动力学中的应用

真空紫外超短脉冲激光具有波长短、单光子能量高、脉宽小等特点,在飞秒化学以及超快动力学等方面具有相当广泛的应用前景.由于直接利用受激辐射获得真空紫外超短脉冲是相当困难,因此利用非线性频率转换技术,超短脉冲与惰性气体相互作用,将红外、可见或紫外光波段的超短脉冲转换到真空紫外波段是目前获得紫外超短脉冲最快捷有效的方式.围绕真空紫外超短脉冲的产生及其在超短动力学中应用展开,介绍了产生真空紫外超短脉冲的高斯谐波、空心光纤四波混频和光丝四波混频的方法,对其优缺点作了评述,并对真空紫外超短脉冲激光在超快动力学过程中的应用进行了简单的总结.     

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.     

Synthesis of periodic femtosecond pulse trains in the ultraviolet by phase-locked Raman sideband generation

We demonstrate a new technique for femtosecond-pulse generation that employs ultrafast modulation of a laser field phase by impulsively excited molecular rotational or vibrational motion with subsequent temporal compression. An ultrashort pump pulse at 800 nm performs impulsive excitation of a molecular gas in a hollow waveguide, and a weak delayed probe pulse at 400 nm is scattered on the temporal oscillations of its dielectric index. The resultant sinusoidal phase modulation of the probe pulse permits probe pulse temporal compression by use of both positively and negatively dispersive elements. The potential of this new method is demonstrated by the generation of a periodic train of 5.8-fs pulses at 400 nm with positive group-delay dispersion compensation.     

Indo‐French meeting on indus‐2 and soleil

With the availability of the first generation of X-ray free electron lasers, pump-probe measurements with femtosecond resolution and high brilliance are now possible. For condensed matter systems, a wealth of modes in the mid-infrared (MIR) and terahertz (THz) regime determine the physics such that targeted excitation with ultrashort pulses at long wavelength becomes an important tool. We will briefly discuss the methodology of pump-probe experiments at the Linac Coherent Light Source (LCLS) and then review methods of generation of intense THz and MIR pulses. This is followed with recent examples from atomic and condensed matter physics at LCLS, and we conclude with an outlook of future developments in this field.     

Spatiotemporal control of ultrashort optical pulses by refractive-diffractive-dispersive structured optical elements

Structured optical elements that control the spatial and temporal characteristics of femtosecond light pulses are analyzed and synthesized. We show that unique spatiotemporal effects can be attained based on the diffraction, refraction, and dispersive effects that appear in the femtosecond regime. We argue that the design requirements for ultrafast optics are beyond the achromatization considerations that are usually applied to incoherent illumination because of the need to consider coherent effects. Despite fundamental limitations in the space-time control of ultrashort pulses, we show the potential of this technique to improve simultaneously the spatial and the temporal resolution of a lens and to generate ultrafast pulse sequences.     

Probing nonequilibrium dynamics with white-light femtosecond pulses

Femtosecond pulsed lasers have become an invaluable tool for examining ultrafast nonequilibrium dynamics. With pulsewidths of a few hundred femtoseconds (fs) to less than 10 fs, these lasers can clearly provide unprecedented temporal resolution. By amplifying ultrashort laser pulses to sufficient levels of energy per pulse, it is possible to exploit the nonlinear optical properties of certain materials to generate extremely broadband pulses. These pulses retain the time structure of the incident pulse, but contain a spectral bandwidth extending from the infrared to as far as the ultraviolet. By generating white-light pulses, it becomes possible to probe ultrafast nonlinear processes over a large range of energies. In this paper, the process of generating white-light ultrashort pulses will be presented, along with a discussion of different probing techniques and procedures necessary for modeling the transient optical data. Finally, results from pump-probe measurements using a white-light probe on indium phosphide (InP) films will be presented as a demonstration of this technique.     

Advanced time-resolved absorption spectroscopy with an ultrashort visible/near IR laser and a multi-channel lock-in detector

Ultrashort visible-near infrared (NIR) pulse generation and its applications to ultrafast spectroscopy are discussed. Femtosecond pulses of around 800 nm from a Ti:sapphire laser are used as a pump of an optical parametric amplifier (OPA) in a non-collinear configuration to generate ultrashort visible (500–780 nm) pulses and deep-ultraviolet (DUV, 259–282 nm) pulses. The visible-NIR pulses and DUV pulses were compressed to 3.9 fs and 10.4 fs, respectively, and used to elucidate various ultrafast dynamics in condensed matter with a sub-10 fs resolution by pump-probe measurements. We have also developed a 128-channel lock-in amplifier. The combined system of the world-shortest visible pulse from the OPA and the lock-in amplifier with the world-largest channel-number can clarify the sub-10 fs-dynamics in condensed matter. This system clarified structural changes in an excited state, reaction intermediate, and a transition state. This is possible even during molecular vibration and reactions via a real-time-resolved vibronic spectrum, which provides molecular structural change information. Also, ultrafast dynamics in exotic materials like carbon nanotubes, topological insulators, and novel solar battery systems have been clarified. Furthermore, the carrier-envelope phase in the ultrashort pulse has been controlled and measured.     

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.     

The Modern Problems of Ultrafast Magnetoacoustics (Review)

Acoustical Physics - A review of modern lines of research in the field of ultrafast magnetoacoustics is presented. Effects of interaction of ultrashort (picosecond) acoustic pulses with a magnetic...     

Generation of femtosecond X-ray pulses via laser–electron beam interaction

The generation of femtosecond X-ray pulses will have important scientific applications by enabling the direct measurement of atomic motion and structural dynamics in condensed matter on the fundamental time scale of a vibrational period. Interaction of femtosecond laser pulses with relativistic electron beams is an effective approach to generating femtosecond pulses of X-rays. In this paper we present recent results from proof-of-principle experiments in which 300 fs pulses are generated from a synchrotron storage ring by using an ultrashort optical pulse to create femtosecond time structure on the stored electron bunch. A previously demonstrated approach for generating femtosecond X-rays via Thomson scattering between terawatt laser pulses and relativistic electrons is reviewed and compared with storage-ring based schemes.     

Spectral and temporal analysis of ultrashort ultraviolet pulses generated by high-intensity laser radiation in the atmosphere

We report direct spectral and temporal characterization of ultrashort ultraviolet (UV) pulses resulting from third-harmonic generation by high-intensity Ti: sapphire laser radiation in the atmosphere. The experimental technique implemented in this work enables the measurement of the pulse width and the chirp of the UV field, as well as the electron density of the plasma produced by laser pulses. The bandwidth of the third harmonic generated in our experiments by laser pulses with an initial pulse width of 45 fs supports transform-limited UV pulses as short as 30 fs.     

Progress in sub-femtosecond control of electron localization in molecules

Recent advances in controlled generation of intense, ultrashort laser pulses in the femtosecond and attosecond time-scales have pushed new avenues of research in the coherent control of ultrafast electron dynamics in atoms and molecules. We present a topical review on the phenomenon of control of electron localization in small dissociating molecules. By creating and controlling coherent superposition of the symmetric and antisymmetric electronic states, it becomes possible to confine the evolving electron cloud onto a preferred nucleus, thereby steering the molecule towards a desired dissociation route. We discuss the origin of the idea and various mechanisms to achieve electron localization in small molecules. To highlight recent experimental progress, we explain how one can employ few-cycle IR pulses and different attosecond extreme ultraviolet (EUV) pulses in various ways to successfully demonstrate the control of electronic dynamics. Future research opportunities and challenges on this topic are envisioned.     

Modeling of dynamics of a femtosecond Kerr-lens mode-locked laser by the mode decomposition of the intracavity beam

A full spatio-temporal model is used for analyzing the features of generation of femtosecond pulses in a Kerr-lens mode-locked laser. The developed algorithm involves the field decomposition in terms of Laguerre-Gaussian functions which are the modes of empty space. Polarization of the medium is calculated from the Bloch equations for the two-level transition. With allowance for the frequency-dependent diffraction, such a method allows us to describe generation of pulses with a duration of several femtoseconds. It is shown that diffraction results in a shift of the carrier frequency of sub-10-fs pulses toward shorter wavelengths. A multiple-pulse oscillation regime can be realized near zero group-velocity dispersion in the cavity. It is shown that such a regime can be realized in the absence of higher-order dispersion. Strong coupling between the spatial and temporal characteristics of the field is observed for the pulses with a duration of several femtoseconds. This leads to a complicated dependence of the beam size on its power and, therefore, to a complicated variation in power-dependent losses. Due to this feature, regimes of generation of ultrashort pulses cannot be correctly described by models in which power-dependent losses are introduced artificially.     

利用一维原子链模型研究薄膜瞬态结构变化

对于晶格结构响应的仿真与实验有助于我们理解激光激发引起的动态过程.利用一维原子链模型研究了激光加热后由于温度分布不均匀性产生的热应力对晶格的影响,该模型的计算结果与使用超快X射线衍射获得的实验结果相符合.该模型为研究光激发金属以及半导体等材料的超快晶格动力学提供了理论分析基础.     

Adaptive control of femtosecond laser ablation plasma emission

The influence of temporal pulse shaping on plasma plume generated by ultrafast laser irradiation of aluminum is investigated. Time resolved plasma emission spectroscopy is coupled with a temporal shaping procedure in a closed loop. The ionic emission is enhanced relative to the neutral one via an adaptive optimization strategy. The plasma emission efficiency in case of optimized and ultrashort temporal shapes of the laser pulses are compared, evidencing an enhancement of the ionization degree of the plasma plume. Simplified temporal shapes of the femtosecond laser pulses are extracted from the optimized shape and their corresponding effect on laser induced plasma emission is discussed.