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.     

Potential for biomolecular imaging with femtosecond X-ray pulses

Sample damage by X-rays and other radiation limits the resolution of structural studies on non-repetitive and non-reproducible structures such as individual biomolecules or cells. Cooling can slow sample deterioration, but cannot eliminate damage-induced sample movement during the time needed for conventional measurements. Analyses of the dynamics of damage formation suggest that the conventional damage barrier (about 200 X-ray photons per A2 with X-rays of 12 keV energy or 1 A wavelength) may be extended at very high dose rates and very short exposure times. Here we have used computer simulations to investigate the structural information that can be recovered from the scattering of intense femtosecond X-ray pulses by single protein molecules and small assemblies. Estimations of radiation damage as a function of photon energy, pulse length, integrated pulse intensity and sample size show that experiments using very high X-ray dose rates and ultrashort exposures may provide useful structural information before radiation damage destroys the sample. We predict that such ultrashort, high-intensity X-ray pulses from free-electron lasers that are currently under development, in combination with container-free sample handling methods based on spraying techniques, will provide a new approach to structural determinations with X-rays.     

Direct observation of electron dynamics in the attosecond domain

Dynamical processes are commonly investigated using laser pump-probe experiments, with a pump pulse exciting the system of interest and a second probe pulse tracking its temporal evolution as a function of the delay between the pulses. Because the time resolution attainable in such experiments depends on the temporal definition of the laser pulses, pulse compression to 200 attoseconds (1 as = 10(-18) s) is a promising recent development. These ultrafast pulses have been fully characterized, and used to directly measure light waves and electronic relaxation in free atoms. But attosecond pulses can only be realized in the extreme ultraviolet and X-ray regime; in contrast, the optical laser pulses typically used for experiments on complex systems last several femtoseconds (1 fs = 10(-15) s). Here we monitor the dynamics of ultrafast electron transfer--a process important in photo- and electrochemistry and used in solid-state solar cells, molecular electronics and single-electron devices--on attosecond timescales using core-hole spectroscopy. We push the method, which uses the lifetime of a core electron hole as an internal reference clock for following dynamic processes, into the attosecond regime by focusing on short-lived holes with initial and final states in the same electronic shell. This allows us to show that electron transfer from an adsorbed sulphur atom to a ruthenium surface proceeds in about 320 as.     

Information extraction and CT reconstruction of liver images based on diffraction enhanced imaging

X-ray phase-contrast imaging (PCI) is a new emerging imaging technique that generates a high spatial resolution and high contrast of biological soft tissues compared to conventional radiography. Herein a biomedical application of diffraction enhanced imaging (DEI) is presented. As one of the PCI methods, DEI derives contrast from many different kinds of sample information, such as the sample's X-ray absorption, refraction gradient and ultra-small-angle X-ray scattering (USAXS) properties, and the sample information is expressed by three parametric images. Combined with computed tomography (CT), DEI-CT can produce 3D volumetric images of the sample and can be used for investigating micro-structures of biomedical samples. Our DEI experiments for liver samples were implemented at the topography station of Beijing Synchrotron Radiation Facility (BSRF). The results show that by using our provided information extraction method and DEI-CT reconstruction approach, the obtained parametric images clearly display the inner structures of liver tissues and the morphology of blood vessels. Furthermore, the reconstructed 3D view of the liver blood vessels exhibits the micro blood vessels whose minimum diameter is on the order of about tens of microns, much better than its conventional CT reconstruction at a millimeter resolution. In conclusion, both the information extraction method and DEI-CT have the potential for use in biomedical micro-structures analysis.     

Determination of surface topography of biological specimens at high resolution by scanning tunnelling microscopy

Although techniques are available for the determination of the three-dimensional structure of biological specimens, for example scanning electron microscopy, they all have some serious drawback, such as low resolution, the requirement for crystals or for the sample to be analysed in a high vacuum. In an attempt to develop a technique for high-resolution three-dimensional structure analysis of non-crystalline biological material, we have tested the applicability of scanning tunnelling microscopy (STM), a method that has been used successfully in the analysis of metal and semiconductor surface structures. We report here that scanning tunnelling electron microscopy can be used to determine the surface topography of biological specimens at atmospheric pressure and room temperature, giving a vertical resolution of the order of 1 A. Our results show that quantum mechanical tunnelling of electrons through biological material is possible provided that the specimen is deposited on a conducting surface.     

Probing carrier dynamics in nanostructures by picosecond cathodoluminescence

Picosecond and femtosecond spectroscopy allow the detailed study of carrier dynamics in nanostructured materials. In such experiments, a laser pulse normally excites several nanostructures at once. However, spectroscopic information may also be acquired using pulses from an electron beam in a modern electron microscope, exploiting a phenomenon called cathodoluminescence. This approach offers several advantages. The multimode imaging capabilities of the electron microscope enable the correlation of optical properties (via cathodoluminescence) with surface morphology (secondary electron mode) at the nanometre scale. The broad energy range of the electrons can excite wide-bandgap materials, such as diamond- or gallium-nitride-based structures that are not easily excited by conventional optical means. But perhaps most intriguingly, the small beam can probe a single selected nanostructure. Here we apply an original time-resolved cathodoluminescence set-up to describe carrier dynamics within single gallium-arsenide-based pyramidal nanostructures with a time resolution of 10 picoseconds and a spatial resolution of 50 nanometres. The behaviour of such charge carriers could be useful for evaluating elementary components in quantum computers, optical quantum gates or single photon sources for quantum cryptography.     

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.     

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.     

Fractal morphology, imaging and mass spectrometry of single aerosol particles in flight

The morphology of micrometre-size particulate matter is of critical importance in fields ranging from toxicology to climate science, yet these properties are surprisingly difficult to measure in the particles' native environment. Electron microscopy requires collection of particles on a substrate; visible light scattering provides insufficient resolution; and X-ray synchrotron studies have been limited to ensembles of particles. Here we demonstrate an in situ method for imaging individual sub-micrometre particles to nanometre resolution in their native environment, using intense, coherent X-ray pulses from the Linac Coherent Light Source free-electron laser. We introduced individual aerosol particles into the pulsed X-ray beam, which is sufficiently intense that diffraction from individual particles can be measured for morphological analysis. At the same time, ion fragments ejected from the beam were analysed using mass spectrometry, to determine the composition of single aerosol particles. Our results show the extent of internal dilation symmetry of individual soot particles subject to non-equilibrium aggregation, and the surprisingly large variability in their fractal dimensions. More broadly, our methods can be extended to resolve both static and dynamic morphology of general ensembles of disordered particles. Such general morphology has implications in topics such as solvent accessibilities in proteins, vibrational energy transfer by the hydrodynamic interaction of amino acids, and large-scale production of nanoscale structures by flame synthesis.     

掺杂Ce的纳米W复合粉末的制备及其表征

以钨酸盐为原料,以液氮为冷冻媒质,采用液液混合-冷冻干燥-两段还原方法获得了粒径为20～30 nm的掺杂Ce的纳米W粉末;并采用X射线衍射、扫描电镜、透射电镜对冻干粉、一次还原粉和二次还原粉的物相组成和形貌进行了分析.研究结果表明:冻干粉呈现非晶态,以絮状团聚在一起,没有明显的颗粒形貌,表面平滑;一次还原粉末也呈现非晶态,为疏松的海绵体结构,由许多杆状晶体搭桥而成,使其在装料时能够形成孔隙;最终产物是晶态的W Ce2WO6粉末,粒度分布均匀;冻干粉末具有Keggin结构;冻干粉分3个阶段失去其吸附水、结晶水和结构水.     

微波接收前端高功率微波效应实验研究

高功率微波可通过雷达、电子战装备的天线进入装备内部,这种方式耦合能力强、峰值幅度大,容易造成装备电磁干扰或损伤.因此,有必要开展高功率微波对电子设备的作用效应和防护研究.针对设备级高功率微波效应研究较少的现状,以某X波段微波接收前端为对象,采用注入法开展高功率微波损伤效应实验,获取了效应现象和数据.结果显示,无限幅器保护时,注入微波的峰值功率达到48.8 dBm,单个脉冲就能损伤微波接收前端的低噪声放大器;采用限幅器防护后,注入微波的峰值功率需增加到60.7 dBm,脉冲数增加到100个才能实现微波接收前端的损伤.实验表明,能量沉积是进行损伤的必要条件,通过高峰值功率短脉冲或长脉宽脉冲串,高功率微波都可以对电子设备中的敏感器件造成损伤,综合运用峰值功率、脉宽和脉冲数等参数可增强高功率微波作用效应.在此基础上,还分析了典型参数高功率微波武器对电子设备的作用距离、作用规律,可为武器装备高功率微波效应评估和防护设计提供参考.     

Imaging ultrafast molecular dynamics with laser-induced electron diffraction

Establishing the structure of molecules and solids has always had an essential role in physics, chemistry and biology. The methods of choice are X-ray and electron diffraction, which are routinely used to determine atomic positions with sub-?ngstr?m spatial resolution. Although both methods are currently limited to probing dynamics on timescales longer than a picosecond, the recent development of femtosecond sources of X-ray pulses and electron beams suggests that they might soon be capable of taking ultrafast snapshots of biological molecules and condensed-phase systems undergoing structural changes. The past decade has also witnessed the emergence of an alternative imaging approach based on laser-ionized bursts of coherent electron wave packets that self-interrogate the parent molecular structure. Here we show that this phenomenon can indeed be exploited for laser-induced electron diffraction (LIED), to image molecular structures with sub-?ngstr?m precision and exposure times of a few femtoseconds. We apply the method to oxygen and nitrogen molecules, which on strong-field ionization at three mid-infrared wavelengths (1.7, 2.0 and 2.3?μm) emit photoelectrons with a momentum distribution from which we extract diffraction patterns. The long wavelength is essential for achieving atomic-scale spatial resolution, and the wavelength variation is equivalent to taking snapshots at different times. We show that the method has the sensitivity to measure a 0.1?? displacement in the oxygen bond length occurring in a time interval of ～5?fs, which establishes LIED as a promising approach for the imaging of gas-phase molecules with unprecedented spatio-temporal resolution.     

Lensless imaging of magnetic nanostructures by X-ray spectro-holography

Our knowledge of the structure of matter is largely based on X-ray diffraction studies of periodic structures and the successful transformation (inversion) of the diffraction patterns into real-space atomic maps. But the determination of non-periodic nanoscale structures by X-rays is much more difficult. Inversion of the measured diffuse X-ray intensity patterns suffers from the intrinsic loss of phase information, and direct imaging methods are limited in resolution by the available X-ray optics. Here we demonstrate a versatile technique for imaging nanostructures, based on the use of resonantly tuned soft X-rays for scattering contrast and the direct Fourier inversion of a holographically formed interference pattern. Our implementation places the sample behind a lithographically manufactured mask with a micrometre-sized sample aperture and a nanometre-sized hole that defines a reference beam. As an example, we have used the resonant X-ray magnetic circular dichroism effect to image the random magnetic domain structure in a Co/Pt multilayer film with a spatial resolution of 50 nm. Our technique, which is a form of Fourier transform holography, is transferable to a wide variety of specimens, appears scalable to diffraction-limited resolution, and is well suited for ultrafast single-shot imaging with coherent X-ray free-electron laser sources.     

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.     

单相和多相Y-Ba-Cu-O超导化合物的制备

本文报导单相和多相Y-Ba-Cu-O化合物超导体的制备工艺及其超导电性.X射线分析及电子显微镜观察表明,名义配比Y:Ba:Cu=1:2:3的样品为单相,其他配比成分的样品呈多相,但在一定配比范围内均呈现超导电性.它们的零电阻温度均在90K附近.     

等规聚苯乙烯单链单晶的结构和耐辐照性能

利用电子衍射（ED）和高分辨电子显微（HREM）技术，研究等规聚苯乙烯（i－PS）单链单晶的结构．纳米级的单链单晶具有很强的耐电子辐照性能．按照i－PS的晶胞能对ED图中的衍射环和HREM像中的晶格条纹进行晶面指标化，但发现低指数衍射缺失．由于单链单晶的尺寸很小，电子辐照所产生的次级电子可以逸出晶体，使辐照损伤大大减小．另外，单链单晶存在着较少的低指数晶面，未能产生足够的衍射强度，使低指数晶面的衍射缺失．单链单晶对电子辐照稳定，在室温下，可得到高分辨晶格条纹象，这为研究高分子晶体的结构开辟了新的实验方法．     

Adaptive subwavelength control of nano-optical fields

Adaptive shaping of the phase and amplitude of femtosecond laser pulses has been developed into an efficient tool for the directed manipulation of interference phenomena, thus providing coherent control over various quantum-mechanical systems. Temporal resolution in the femtosecond or even attosecond range has been demonstrated, but spatial resolution is limited by diffraction to approximately half the wavelength of the light field (that is, several hundred nanometres). Theory has indicated that the spatial limitation to coherent control can be overcome with the illumination of nanostructures: the spatial near-field distribution was shown to depend on the linear chirp of an irradiating laser pulse. An extension of this idea to adaptive control, combining multiparameter pulse shaping with a learning algorithm, demonstrated the generation of user-specified optical near-field distributions in an optimal and flexible fashion. Shaping of the polarization of the laser pulse provides a particularly efficient and versatile nano-optical manipulation method. Here we demonstrate the feasibility of this concept experimentally, by tailoring the optical near field in the vicinity of silver nanostructures through adaptive polarization shaping of femtosecond laser pulses and then probing the lateral field distribution by two-photon photoemission electron microscopy. In this combination of adaptive control and nano-optics, we achieve subwavelength dynamic localization of electromagnetic intensity on the nanometre scale and thus overcome the spatial restrictions of conventional optics. This experimental realization of theoretical suggestions opens a number of perspectives in coherent control, nano-optics, nonlinear spectroscopy, and other research fields in which optical investigations are carried out with spatial or temporal resolution.     

结晶硅材料的单脉冲和多脉冲激光损伤研究

对半导体材料硅的单脉冲和多脉冲激光损伤现象进行研究,实验结果表明多脉冲激光辐照的损伤阈值比单脉冲的少,且多脉冲激光损伤阈值是与脉冲重复频率相关的,随脉冲重复频率增大而减少,说明损伤过程中累积效应的存在。根据实验结果和理论计算,我们指出热积累并不是损伤阈值降低的唯一原因,并对可能的损伤机理进行了讨论。     

Progress of AFM single-cell and single-molecule morphology imaging

Atomic force microscopy (AFM) can probe single living cells and single native membrane proteins in natural fluid environments with label-free high spatial resolution. It has thus become an important tool for cellular and molecular biology that significantly complements traditional biochemical and biophysical techniques such as optical and electron microscopy and X-ray crystallog-raphy. Imaging surface topography is the primary application of AFM in the life sciences. Since the early 1990s, researchers have used AFM to investigate morphological features of living cells and native membrane proteins with impressive results. Steady improvements in AFM techniques for imaging soft biological samples have greatly expanded its applications. Based on the authors’ own research in AFM imaging of living cell morphologies, a review of sample preparation procedures for single-cell and single-molecule imaging experiments is presented, along with a summary of recent progress in AFM imaging of living cells and native membrane proteins. Finally, the challenges of AFM high-resolution imaging at the single-cell and single-molecule levels are discussed.     

High resolution structure of the RNA duplex [U(U-A)6A]2

RNA is involved in many biological functions, ranging from information storage and transfer to the catalysis of reactions involving both nucleic acids and proteins. Previous crystallographic studies on RNA oligomeric chains provide only averaged structures or information limited in resolution. The oligomer [U(U-A)6A]2 was chosen for the study of protein-RNA interactions in viruses. Its size and base composition mimic portions of the genomic RNA in alfalfa mosaic virus that bind to the amino terminus of the viral subunit. The actual sequence was designed to guarantee the formation of a single species of duplex and to facilitate the production of the pure oligomer in large quantities. The molecular structure, derived from the 2.25 A resolution X-ray diffraction data, allows the most detailed analysis of an A-RNA helix reported to date. Two kinks are observed that divide the duplex into three blocks, each close to a canonical A-helical conformation. A few intermolecular hydrogen bonds involving 2'-hydroxyl groups stabilize this peculiar conformation of the RNA, which may be related to the temperature used for the crystallization (35 degrees C). The structure demonstrates both the plasticity of the RNA molecule and the role of the 2'-hydroxyl groups in intermolecular interactions.