Femtosecond time-delay X-ray holography

Extremely intense and ultrafast X-ray pulses from free-electron lasers offer unique opportunities to study fundamental aspects of complex transient phenomena in materials. Ultrafast time-resolved methods usually require highly synchronized pulses to initiate a transition and then probe it after a precisely defined time delay. In the X-ray regime, these methods are challenging because they require complex optical systems and diagnostics. Here we propose and apply a simple holographic measurement scheme, inspired by Newton's 'dusty mirror' experiment, to monitor the X-ray-induced explosion of microscopic objects. The sample is placed near an X-ray mirror; after the pulse traverses the sample, triggering the reaction, it is reflected back onto the sample by the mirror to probe this reaction. The delay is encoded in the resulting diffraction pattern to an accuracy of one femtosecond, and the structural change is holographically recorded with high resolution. We apply the technique to monitor the dynamics of polystyrene spheres in intense free-electron-laser pulses, and observe an explosion occurring well after the initial pulse. Our results support the notion that X-ray flash imaging can be used to achieve high resolution, beyond radiation damage limits for biological samples. With upcoming ultrafast X-ray sources we will be able to explore the three-dimensional dynamics of materials at the timescale of atomic motion.     

全反射相干自相关法测量飞秒脉冲的特性分析

 全反射相干自相关法在测量紫外-X光波段的超短脉冲和宽频带脉冲方面具有优势。借助数值模拟,比较了全反射相干自相关和传统相干自相关方法测量不同相位结构脉冲时信号特征的异同。利用自建的组合式自相关装置测量了钛宝石激光器输出的飞秒脉冲及经由40 mm厚BK7玻璃块展宽而成的啁啾脉冲。理论分析和实验结果表明,同一脉冲的两种自相关曲线是基本相似的,因而在传统自相关方法不适用或操作不便的情况下,可以用全反射相干自相关法来替代。     

Single mimivirus particles intercepted and imaged with an X-ray laser

X-ray lasers offer new capabilities in understanding the structure of biological systems, complex materials and matter under extreme conditions. Very short and extremely bright, coherent X-ray pulses can be used to outrun key damage processes and obtain a single diffraction pattern from a large macromolecule, a virus or a cell before the sample explodes and turns into plasma. The continuous diffraction pattern of non-crystalline objects permits oversampling and direct phase retrieval. Here we show that high-quality diffraction data can be obtained with a single X-ray pulse from a non-crystalline biological sample, a single mimivirus particle, which was injected into the pulsed beam of a hard-X-ray free-electron laser, the Linac Coherent Light Source. Calculations indicate that the energy deposited into the virus by the pulse heated the particle to over 100,000?K after the pulse had left the sample. The reconstructed exit wavefront (image) yielded 32-nm full-period resolution in a single exposure and showed no measurable damage. The reconstruction indicates inhomogeneous arrangement of dense material inside the virion. We expect that significantly higher resolutions will be achieved in such experiments with shorter and brighter photon pulses focused to a smaller area. The resolution in such experiments can be further extended for samples available in multiple identical copies.     

超短脉冲的能量与载波相位的关系

以高斯、双曲正割、洛伦兹3种脉冲为例,研究了载波相位与超短脉冲携带的能量之间的关系,给出了3种脉冲携带的能量与载波相位的解析表达式．研究结果表明,当脉冲包络的宽度短于1个光学振荡周期时,载波相位对超短脉冲携带的能量开始有较显著的影响．     

Ways to produce and measure atto- and femtosecond soft X-ray pulses

The ways to produce and measure atto-and femtosecond soft X-ray pulses are reported. The laser phase relation of high-order harmonic generation(HHG) shows two different radiation energy distribu-tions in time(or laser phase) domain. These energy-phase relations are helpful for realizing the dy-namic processes of HHG. Two presented parameterized formulas can be used to calculate the durations of the energy distributions with a bandwidth of the pulse. These formulas are useful in calculating and simulating pulses transports and interactions with mediums. The time structures of atto-and femto-second soft X-ray pulses can be directly measured with photoelectron spectrum transfer equations and the related laser phase determination methods without any previous pulse shape and the instantane-ous frequency assumptions. These equations and methods can be used to evaluate and improve the technical parameters of the ultra-short X-ray sources. They have wide measurement ranges and high time resolutions,which may enable ultra-fast measurements to reach metrological precisions,and lead to a new tide of scientific researches in physics,chemistry,biochemistry,etc. The application of atto-and femtosecond X-rays as well as the theoretical and technical problems in measurements are briefly discussed.     

光纤中基于交叉相位调制的基孤子压缩

提出了一种在单模光纤负群速度色散区由基孤子产生超短光脉冲的新方法，即当波长位于光纤负色散区的基孤子信号脉冲和波长位于光纤正色散区的泵浦脉冲在光纤中共同传输，光纤零色散波长位于基孤子波长与泵浦脉冲波长中间附近时，交叉相位调制能使基孤子压缩．数值计算表明，入射泵浦脉冲越强，由基孤子信号脉冲产生的光脉冲的宽度越窄，峰值功率越高，而且所需的光纤长度越短，但是压缩质量减小．当泵浦脉冲的阶数不变、泵浦脉冲脉宽减小时，信号脉冲的压缩因子增大．     

Coherent control of pulsed X-ray beams.

Synchrotrons produce continuous trains of closely spaced X-ray pulses. Application of such sources to the study of atomic-scale motion requires efficient modulation of these beams on timescales ranging from nanoseconds to femtoseconds. However, ultrafast X-ray modulators are not generally available. Here we report efficient subnanosecond coherent switching of synchrotron beams by using acoustic pulses in a crystal to modulate the anomalous low-loss transmission of X-ray pulses. The acoustic excitation transfers energy between two X-ray beams in a time shorter than the synchrotron pulse width of about 100 ps. Gigahertz modulation of the diffracted X-rays is also observed. We report different geometric arrangements, such as a switch based on the collision of two counter-propagating acoustic pulses: this doubles the X-ray modulation frequency, and also provides a means of observing a localized transient strain inside an opaque material. We expect that these techniques could be scaled to produce subpicosecond pulses, through laser-generated coherent optical phonon modulation of X-ray diffraction in crystals. Such ultrafast capabilities have been demonstrated thus far only in laser-generated X-ray sources, or through the use of X-ray streak cameras.     

Femtosecond X-ray protein nanocrystallography

X-ray crystallography provides the vast majority of macromolecular structures, but the success of the method relies on growing crystals of sufficient size. In conventional measurements, the necessary increase in X-ray dose to record data from crystals that are too small leads to extensive damage before a diffraction signal can be recorded. It is particularly challenging to obtain large, well-diffracting crystals of membrane proteins, for which fewer than 300 unique structures have been determined despite their importance in all living cells. Here we present a method for structure determination where single-crystal X-ray diffraction 'snapshots' are collected from a fully hydrated stream of nanocrystals using femtosecond pulses from a hard-X-ray free-electron laser, the Linac Coherent Light Source. We prove this concept with nanocrystals of photosystem I, one of the largest membrane protein complexes. More than 3,000,000 diffraction patterns were collected in this study, and a three-dimensional data set was assembled from individual photosystem I nanocrystals (～200?nm to 2?μm in size). We mitigate the problem of radiation damage in crystallography by using pulses briefer than the timescale of most damage processes. This offers a new approach to structure determination of macromolecules that do not yield crystals of sufficient size for studies using conventional radiation sources or are particularly sensitive to radiation damage.     

Atomic inner-shell X-ray laser at 1.46 nanometres pumped by an X-ray free-electron laser

Since the invention of the laser more than 50 years ago, scientists have striven to achieve amplification on atomic transitions of increasingly shorter wavelength. The introduction of X-ray free-electron lasers makes it possible to pump new atomic X-ray lasers with ultrashort pulse duration, extreme spectral brightness and full temporal coherence. Here we describe the implementation of an X-ray laser in the kiloelectronvolt energy regime, based on atomic population inversion and driven by rapid K-shell photo-ionization using pulses from an X-ray free-electron laser. We established a population inversion of the Kα transition in singly ionized neon at 1.46 nanometres (corresponding to a photon energy of 849 electronvolts) in an elongated plasma column created by irradiation of a gas medium. We observed strong amplified spontaneous emission from the end of the excited plasma. This resulted in femtosecond-duration, high-intensity X-ray pulses of much shorter wavelength and greater brilliance than achieved with previous atomic X-ray lasers. Moreover, this scheme provides greatly increased wavelength stability, monochromaticity and improved temporal coherence by comparison with present-day X-ray free-electron lasers. The atomic X-ray lasers realized here may be useful for high-resolution spectroscopy and nonlinear X-ray studies.     

Quantum coherent control of ultrashort laser pulses

The effective photonic control is one of the key issues in photo-physics. Significant advancement in photonic crystals, quantum optics, ultrafast optics as well as micro-nano-optics gives rise to new op-portunities to manipulate the emission and propagation in optical fields, leading to a number of new and interesting discoveries, e.g., ultrashort light pulse storage and efficient energy conversion. This paper reviews the latest research progress in storage, release and energy conversion for ultrashort laser pulses in periodical arrays of absorbing medium. Techniques to fabricate such devices are also presented.     

Nonlinear optics in the extreme ultraviolet

Nonlinear responses to an optical field are universal in nature but have been difficult to observe in the extreme ultraviolet (XUV) and soft X-ray regions owing to a lack of coherent intense light sources. High harmonic generation is a well-known nonlinear optical phenomenon and is now drawing much attention in attosecond pulse generation. For the application of high harmonics to nonlinear optics in the XUV and soft X-ray regime, optical pulses should have both large pulse energy and short pulse duration to achieve a high optical electric field. Here we show the generation of intense isolated pulses from a single harmonic (photon energy 27.9 eV) by using a sub-10-femtosecond blue laser pulse, producing a large dipole moment at the relatively low (ninth) harmonic order nonadiabatically. The XUV pulses with pulse durations of 950 attoseconds and 1.3 femtoseconds were characterized by an autocorrelation technique, based on two-photon above-threshold ionization of helium atoms. Because of the small cross-section for above-threshold ionization, such an autocorrelation measurement of XUV pulses with photon energy larger than the ionization energy of helium has not hitherto been demonstrated. The technique can be extended to the characterization of higher harmonics at shorter wavelengths.     

测量飞秒光参量产生器输出光脉冲脉宽的自相关仪的设计

设计出一台只用一块非线性晶体就能够测量宽波长范围的飞秒激光脉冲脉宽的单次脉冲自相关仪,适用于测量由光参量产生获得的可调谐飞秒激光脉冲的脉宽.     

Editor’s note

The past two decades have witnessed great progress in development of ultrashort laser pulse in laser science, often at an unexpected speed. It has found various applications, both theoretical and practical, in the frontiers of science.     

超短脉冲激光及其应用

评述了国际上超短脉冲激光技术的最新研究进展以及超短脉冲激光在超高速光通讯、海量信息存储、光合作用研究、化学反应过程研究等领域广泛的应用状况     

初始啁啾对飞秒光脉冲传输的影响

超短光脉冲在光纤中传输时将受到多种类型的扰动,而初始啁啾对超短光脉冲传输的影响也越来越得到重视.本文以广义非线性薛定谔方程为理论基础,采用对称分步傅立叶方法作为数值模拟的方法,分析了初始啁啾对飞秒光脉冲在光纤中传输的影响,数值计算表明:啁啾的临界值有不同程度的减小,相对较小的啁啾也会大大影响飞秒光脉冲的传输,引起很大的能量损耗.为保证通信系统性能,必须消除或尽可能减小初始啁啾.     

A high-intensity highly coherent soft X-ray femtosecond laser seeded by a high harmonic beam

Synchrotrons have for decades provided invaluable sources of soft X-rays, the application of which has led to significant progress in many areas of science and technology. But future applications of soft X-rays--in structural biology, for example--anticipate the need for pulses with much shorter duration (femtoseconds) and much higher energy (millijoules) than those delivered by synchrotrons. Soft X-ray free-electron lasers should fulfil these requirements but will be limited in number; the pressure on beamtime is therefore likely to be considerable. Laser-driven soft X-ray sources offer a comparatively inexpensive and widely available alternative, but have encountered practical bottlenecks in the quest for high intensities. Here we establish and characterize a soft X-ray laser chain that shows how these bottlenecks can in principle be overcome. By combining the high optical quality available from high-harmonic laser sources (as a seed beam) with a highly energetic soft X-ray laser plasma amplifier, we produce a tabletop soft X-ray femtosecond laser operating at 10 Hz and exhibiting full saturation, high energy, high coherence and full polarization. This technique should be readily applicable on all existing laser-driven soft X-ray facilities.     

超短激光双脉冲在硝基苯胺分子介质中传播的动力学过程

通过数值求解麦克斯韦-布洛赫方程，研究了2个相干超短激光脉冲在硝基苯胺分子（pNA分子）介质中的非线性传播过程．量化计算表明该分子在低能级区域内只有1个电荷转移态，因此可把该分子看作二能级体系．当3竹共振脉冲与4π非共振脉冲先后入射到硝基苯胺分子介质中进行传播时，3π脉冲的能量将转移给后面的4竹脉冲，前者面积逐渐变为2π，激发分子能级占有率发生一次完整的拉比振荡；后者在介质中仍保持非共振传播，只能激发分子能级占有率发生不完整的拉比振荡．脉冲的频谱发生展宽，并在共振频率附近振荡剧烈．通过引入固有偶极矩为零的赝分子作为比较对象，发现硝基苯胺分子的固有偶极矩导致非线性传播过程更为复杂．     

Radiation properties of high-order harmonic generation for the measurements of femto- and attosecond X-ray pulses

Radiation properties of high-order harmonic generation （HHG） are calculated for atoms in a strong laser field. The laser-duration dependence and the carrier-envelope-phase （CEP） dependence of HHG radiation properties are presented. The CEP dependence of the pure single distribution pulse of HHG radiation properties shows interesting 180° periodic structures. The quantum enhancement of the laser-assisted photo-ionization by femtosecond （1 fs=10^-15 s） and attosecond （1 as=10^-18 s） X-ray pulses and the interference patterns of photo-electron energy spectra are theoretically investigated. Transfer equations are presented for pulse reconstructions. The theoretical root-mean-square time （energy） differences of attosecond pulse reconstructions with different durations are less than 2 as （0,8 eV）. These methods may be developed as basic techniques to access ultra-fast measurements and molecular movie.     

超短余弦-高斯脉冲的能量分析

研究了超短余弦-高斯脉冲的能量与绝对相位以及余弦函数的参数之间的关系,给出了余弦-高斯脉冲能量的解析表达式.研究结果表明,当脉冲宽度较小时,绝对相位对脉冲能量有很大影响;余弦函数的参数Ω在一定取值范围内对脉冲能量也有很大影响,它会导致脉冲宽度大于一个光学振荡周期的几周期余弦-高斯脉冲能量有较大的变化.     

基于单模光纤的超短光脉冲产生方法（Ⅰ）──脉冲压缩方法

本文系统地介绍了光纤—光栅对光学脉冲压缩和孤子效应光学脉冲压缩的原理及其进展，报道了我们最近的研究结果，讨论了在光纤中实现高效率孤子效应光学脉冲压缩的途径。