Energy optimization of a regular macromolecular crystallography beamline for ultra‐high‐resolution crystallography

A practical method for operating existing undulator synchrotron beamlines at photon energies considerably higher than their standard operating range is described and applied at beamline 19‐ID of the Structural Biology Center at the Advanced Photon Source enabling operation at 30 keV. Adjustments to the undulator spectrum were critical to enhance the 30 keV flux while reducing the lower‐ and higher‐energy harmonic contamination. A Pd‐coated mirror and Al attenuators acted as effective low‐ and high‐bandpass filters. The resulting flux at 30 keV, although significantly lower than with X‐ray optics designed and optimized for this energy, allowed for accurate data collection on crystals of the small protein crambin to 0.38 Å resolution.     

Challenges of sulfur SAD phasing as a routine method in macromolecular crystallography

The sulfur SAD phasing method allows the determination of protein structures de novo without reference to derivatives such as Se‐methionine. The feasibility for routine automated sulfur SAD phasing using a number of current protein crystallography beamlines at several synchrotrons was examined using crystals of trimeric Achromobacter cycloclastes nitrite reductase (AcNiR), which contains a near average proportion of sulfur‐containing residues and two Cu atoms per subunit. Experiments using X‐ray wavelengths in the range 1.9–2.4 Å show that we are not yet at the level where sulfur SAD is routinely successful for automated structure solution and model building using existing beamlines and current software tools. On the other hand, experiments using the shortest X‐ray wavelengths available on existing beamlines could be routinely exploited to solve and produce unbiased structural models using the similarly weak anomalous scattering signals from the intrinsic metal atoms in proteins. The comparison of long‐wavelength phasing (the Bijvoet ratio for nine S atoms and two Cu atoms is ～1.25% at ～2 Å) and copper phasing (the Bijvoet ratio for two Cu atoms is 0.81% at ～0.75 Å) for AcNiR suggests that lower data multiplicity than is currently required for success should in general be possible for sulfur phasing if appropriate improvements to beamlines and data collection strategies can be implemented.     

基于透明陶瓷材料的激光研究进展

陶瓷激光器是一种以透明陶瓷材料作为增益介质的激光器.与单晶相比,透明陶瓷具有制备周期短和烧结温度低等优势,在激活离子高掺杂浓度下能保证良好的光学均匀性,且容易制备成各种大尺寸复合结构.近年在高功率和超短超强激光输出方面得到广泛应用,产生了一系列研究成果.回顾了陶瓷激光器的发展历程,总结了透明陶瓷在高功率、超短超强脉冲激...     

空泡机制产生betatron X射线辐射的数值模拟

针对SILEX钛宝石激光器参数,采用PIC数值模拟程序VORPAL对激光尾波场加速进行了模拟,得到了电子轨迹及能量数据,进而通过理论计算得到了空泡机制下X射线辐射特性。结果表明,空泡机制下高能电子在空泡中做betatron振荡且多数电子被加速到170 MeV左右;加速能量较低的电子（约100 MeV）, 其辐射谱为临界能量约3 keV的类同步辐射谱,发散角约为8 mrad,而能量较高的电子（约170 MeV）对应的光子临界能量约为10 keV。     

反射式GaN光电阴极表面势垒对量子效率衰减的影响

针对反射式GaN光电阴极长波段量子效率衰减较大, 短波段量子效率衰减较小的实验现象, 在考虑谷间散射的情况下, 利用玻尓兹曼分布和基于Airy函数的传递矩阵法, 计算了发射电子能量分布, 分析了表面势垒变化对量子效率衰减的影响, 理论与实验符合较好. 激活层有效偶极子数的减少使表面势垒宽度和高度增加, 引起长波光子激发产生的发射电子能量分布衰减较大, 短波光子激发产生的发射电子能量分布衰减较小, 这是量子效率在长波段衰减较大, 短波段衰减较小的根本原因.     

Fluorescence studies on R-phycoerythrin and C-phycoerythrin

Biliproteins are photosynthetic light-harvesting proteins, which transfer excitons with high efficiencies over relatively long distances until they arrive at a photosynthetic reaction center. Purified R-phycoerythrin (isolated from a red alga) and C-phycoerythrin (isolated from a cyanobacterium), each of which contains several chromophores, were studied by a combination of fluorescence emission, fluorescence excitation polarization, and absorption methods. The polarization spectra of both these biliproteins showed that there was a minimum of two spectrally distinct sensitizing chromophores, which, after absorbing photons, transfer excitons to the lowest-energy (fluorescing) chromophores. Some of these spectroscopic data were used to deconvolute the absorption spectra into the spectra of the two sensitizing and one fluorescing chromophores. It was shown that the higher-energy sensitizing chromophore could readily transfer its excitation energy to the fluorescing chromophore using the lower-energy sensitizing chromophore as an intermediary. However, there was sufficient spectral overlap between the higher-energy sensitizing chromophore and the fluorescing chromophore so that direct transfer between them could not be ruled out.     

Acoustic methods for high‐throughput protein crystal mounting at next‐generation macromolecular crystallographic beamlines

To take full advantage of advanced data collection techniques and high beam flux at next‐generation macromolecular crystallography beamlines, rapid and reliable methods will be needed to mount and align many samples per second. One approach is to use an acoustic ejector to eject crystal‐containing droplets onto a solid X‐ray transparent surface, which can then be positioned and rotated for data collection. Proof‐of‐concept experiments were conducted at the National Synchrotron Light Source on thermolysin crystals acoustically ejected onto a polyimide `conveyor belt'. Small wedges of data were collected on each crystal, and a complete dataset was assembled from a well diffracting subset of these crystals. Future developments and implementation will focus on achieving ejection and translation of single droplets at a rate of over one hundred per second.     

The materials science X‐ray beamline BL8 at the DELTA storage ring

The hard X‐ray beamline BL8 at the superconducting asymmetric wiggler at the 1.5 GeV Dortmund Electron Accelerator DELTA is described. This beamline is dedicated to X‐ray studies in the spectral range from ～1 keV to ～25 keV photon energy. The monochromator as well as the other optical components of the beamline are optimized accordingly. The endstation comprises a six‐axis diffractometer that is capable of carrying heavy loads related to non‐ambient sample environments such as, for example, ultrahigh‐vacuum systems, high‐pressure cells or liquid‐helium cryostats. X‐ray absorption spectra from several reference compounds illustrate the performance. Besides transmission measurements, fluorescence detection for dilute sample systems as well as surface‐sensitive reflection‐mode experiments have been performed. The results show that high‐quality EXAFS data can be obtained in the quick‐scanning EXAFS mode within a few seconds of acquisition time, enabling time‐resolved in situ experiments using standard beamline equipment that is permanently available. The performance of the new beamline, especially in terms of the photon flux and energy resolution, is competitive with other insertion‐device beamlines worldwide, and several sophisticated experiments including surface‐sensitive EXAFS experiments are feasible.     

Laser-produced plasma He-alpha source for pulse radiography

Through the use of time and space integrated kiloelectronvolt （keV） spectroscopy, we investigate the thermal emission of plasma, which produces strong line emission from the titanium K shell （He-a at 4.7 keV and H-α at 4.9 keV）, created by laser. In order to optimize the conversion efficiency enhancement on titanium foils, the experiment is conducted under a variety of laser-driven intensity conditions. The X-ray emission intensity at 4.7 keV is measured and compared with prediction. The experimental result demonstrates that the solid Ti target laser-produced plasma （LPP） source has X-ray emission at 4.7 keV, which are all generated from electronic transitions in Ti ions at pulse width of 2.1 ns or 30 ps, the crudely evaluated He-α X-ray intensity appears to slightly increase with laser intensity enhancement, and the pre- pulse effect increases the conversion efficiency of the He-α X-ray. In addition, a 90-μm-thick Ti foil as a filter is used to transmit He-α X-ray at near 4.7 keV, creating a quasi-monochromatic transmission and greatly reducing the lower- and higher-energy background.     

XDS: a flexible beamline for X‐ray diffraction and spectroscopy at the Brazilian synchrotron

The majority of the beamlines at the Brazilian Synchrotron Light Source Laboratory (LNLS) use radiation produced in the storage‐ring bending magnets and are therefore currently limited in the flux that can be used in the harder part of the X‐ray spectrum (above ～10 keV). A 4 T superconducting multipolar wiggler (SCW) was recently installed at LNLS in order to improve the photon flux above 10 keV and fulfill the demands set by the materials science community. A new multi‐purpose beamline was then installed at the LNLS using the SCW as a photon source. The XDS is a flexible beamline operating in the energy range between 5 and 30 keV, designed to perform experiments using absorption, diffraction and scattering techniques. Most of the work performed at the XDS beamline concentrates on X‐ray absorption spectroscopy at energies above 18 keV and high‐resolution diffraction experiments. More recently, new setups and photon‐hungry experiments such as total X‐ray scattering, X‐ray diffraction under high pressures, resonant X‐ray emission spectroscopy, among others, have started to become routine at XDS. Here, the XDS beamline characteristics, performance and a few new experimental possibilities are described.     

复合样品厚度参数同步辐射测量方法

 薄膜样品在实验研究领域要求样品的厚度测量精度非常高,但由于样品质量小,采用称重的方法,测量精度较差。在北京同步辐射装置的中能（4B7A）和低能（4B7B）束线上（光源能区为0.1～6.0 keV,能量分辨大于1 000）,采用材料对单能光子的透过率来确定样品的质量厚度,通过不同能点的测量值进行不确定度分析,提高测量精度,降低不确定度。利用该方法开展了复合样品厚度的测量方法研究,给出了有CH衬底的薄膜样品的厚度,通过不确定度分析得出,薄膜样品厚度的测量不确定度小于1％。     

Difference-frequency terahertz-wave generation from 4-dimethylamino-N-methyl-4-stilbazolium-tosylate by use of an electronically tuned Ti:sapphire laser

Among nonlinear materials, the organic ionic salt crystal 4-dimethylamino- N -methyl-4-stilbazolium-tosylate (DAST) is known for its large nonlinearity. We generated a coherent terahertz (THz) wave, using DAST, from the difference frequency between two oscillating wavelengths of an electronically tuned Ti:sapphire laser. In LiNbO(3), LiTaO(3), KTiOPO(4), and GaP crystals, THz-wave generation was not observed under the same experimental conditions. This result proves the high efficiency of DAST crystals for generation of difference-frequency THz waves.     

Enhancement of optical luminescence of solids using a capillary lens

The Advanced Photon Source (APS) at Argonne National Laboratory is a 1-km-circumference, 7-GeV, third generation synchrotron light source. It is the largest light source in the Western Hemisphere and attracts about 3,500 users every year from around the globe. The APS is currently preparing for a major upgrade, a goal of which is to focus on high brightness at photon energies of around 20 keV and higher. The APS is particularly well suited for this high photon energy range due to its higher-energy, 7-GeV electron beam, but it also needs new insertion devices with short periods and high fields, i.e., superconducting devices.     

An X‐ray Raman spectrometer for EXAFS studies on minerals: bent Laue spectrometer with 20 keV X‐rays

An X‐ray Raman spectrometer for studies of local structures in minerals is discussed. Contrary to widely adopted back‐scattering spectrometers using ≤10 keV X‐rays, a spectrometer utilizing ～20 keV X‐rays and a bent Laue analyzer is proposed. The 20 keV photons penetrate mineral samples much more deeply than 10 keV photons, so that high intensity is obtained owing to an enhancement of the scattering volume. Furthermore, a bent Laue analyzer provides a wide band‐pass and a high reflectivity, leading to a much enhanced integrated intensity. A prototype spectrometer has been constructed and performance tests carried out. The oxygen K‐edge in SiO₂ glass and crystal (α‐quartz) has been measured with energy resolutions of 4 eV (EXAFS mode) and 1.3 eV (XANES mode). Unlike methods previously adopted, it is proposed to determine the pre‐edge curve based on a theoretical Compton profile and a Monte Carlo multiple‐scattering simulation before extracting EXAFS features. It is shown that the obtained EXAFS features are reproduced fairly well by a cluster model with a minimal set of fitting parameters. The spectrometer and the data processing proposed here are readily applicable to high‐pressure studies.     

Energy dependence of site‐specific radiation damage in protein crystals

It is important to consider radiation damage to crystals caused by data collection when solving structures and critical when determining protein function, which can often depend on very subtle structural characteristics. In this study the rate of damage to specific sites in protein crystals cooled at 100 K is found to depend on the energy of the incident X‐ray beam. Several lysozyme crystals were each subjected to 3–26 MGy of cumulative X‐ray exposure by collecting multiple data sets from each crystal at either 9 keV or 14 keV. The integrated electron density surrounding each S atom in the structure was calculated for each data set and the change in electron density was evaluated as a function of dose at the two energies. The rate of electron density decrease per cubic Å per MGy was determined to be greater at 14 keV than at 9 keV for cysteine sulfurs involved in disulphide bridges; no statistically significant differences in the decay rates were found for methionine sulfurs. These preliminary results imply that it might be possible to minimize certain types of specific radiation damage by an appropriate choice of energy. Further experiments studying a variety of photolabile sites over a wider range of energies are needed to confirm this conclusion.     

The optimum conditions to collect X‐ray data from very small samples

A previous paper [Nave & Hill (2005). J. Synchrotron Rad. 12 , 299–303] examined the possibility of reduced radiation damage for small crystals (10 µm and below in size) under conditions where the photoelectrons could escape from the sample. The conclusion of this paper was that higher‐energy radiation (e.g. 40 keV) could offer an advantage as the photoelectron path length was greater and less energy would be deposited in the crystal. This paper refines these calculations further by including the effects of energy deposited owing to Compton scattering and the energy difference between the incident photon and the emitted photoelectron. An estimate is given for the optimum wavelength for collecting data from a protein crystal of a given size and composition. Another way of reducing radiation damage from a protein crystal is to collect data with a very short pulsed X‐ray source where a single image can be obtained before subsequent radiation damage occurs. A comparison of this approach compared with the use of shorter wavelengths is made.     

Interferometric autocorrelation in the ultraviolet utilizing spontaneous parametric down-conversion inside an enhancement cavity

Autocorrelation is a common method to estimate the duration of ultrashort laser pulses. In the ultraviolet (UV) regime it is challenging to employ the process of second-harmonic generation, most prominently due to absorption in nonlinear crystals at very short wavelengths. Here we show how to utilize spontaneous parametric down-conversion (SPDC) to generate an autocorrelation signal in the infrared (IR) for UV pulses. Our method utilizes the nth-order emission of the SPDC process, which occurs for low pumping powers proportional to the nth power of the UV intensity. Thus, counting 2n down-converted photons directly yields the nth-order autocorrelation. The method, now with detection of near-IR photons, is applied to the first direct measurement of ultrashort UV pulses circulating inside a UV enhancement cavity.     

Untersuchungen über den Doppel-Compton-Effekt

The differential cross section for the double Compton effect has been measured by analysing the energy of the scattered photons. The γ rays are detected by sodium iodid scintillation crystals and photomultipliers, fixed at 90° to each other and to the incident beam. For detecting low energy photons down to 7.2 keV one photomultiplier was replaced by a proportional counter. The experimental results obtained in this work are over the total range of the measured spectrum in good agreement with the theoretical predictions.     

Studying the energy dependence of intrinsic conversion efficiency of single crystal scintillators under X-ray excitation

Single crystal scintilators are used in various radiation detectors applications. The efficiency of the crystal can be determined by the Detector Optical Gain (DOG) defined as the ratio of the emitted optical photon flux over the incident radiation photons flux. A parameter affecting DOG is the intrinsic conversion efficiency (n _C ) giving the percentage of the X-ray photon power converted to optical photon power. n _C is considered a constant value for X-ray energies in the order of keV although a non-proportional behavior has been reported. In this work an analytical model, has been utilized to single crystals scintillators GSO:Ce, LSO:Ce and LYSO:Ce to examine whether the intrinsic conversion efficiency shows non proportional behavior under X-ray excitation. DOG was theoretically calculated as a function of the incident X-ray spectrum, the X-ray absorption efficiency, the energy of the produced optical photons and the light transmission efficiency. The theoretical DOG values were compared with experimental data obtained by irradiating the crystals with X-rays at tube voltages from 50 to 140 kV and by measuring the light energy flux emitted from the irradiated screen. An initial value for n _C (calculated from literature data) was assumed for the X-ray tube voltage of 50 kV. For higher X-ray tube voltages the optical photon propagation phenomena was assumed constant and any deviations between experimental and theoretical data were associated with changes in the intrinsic conversion efficiency. The experimental errors were below 7% for each experimental setup. The behavior of n _C values for LSO:Ce and LYSO:Ce were found very similar, i.e., ranging with values from 0.089 at 50 kV to 0.015 at 140 kV, while for GSO:Ce, n _C demonstrated a peak at 80 kV.