神光Ⅲ原型上扩展X射线吸收精细结构谱实验研究

介绍了在大型激光装置上进行扩展X射线吸收精细结构(EXAFS)谱压缩物态参数测量的基本原理,以及为获得高质量EXAFS谱在神光Ⅲ原型装置上进行的实验研究。实验采用玻璃靶球、CH靶丸和金球作为EXAFS谱测量的背光源,通过多发次叠加、光子数累积的方法获得了信噪比良好的金属Ti在常温常压下的EXAFS谱,数据处理结果表明,实验测得的金属Ti EXAFS谱拟合结果与同步辐射实验拟合结果相吻合,表明实验设计的正确性与可靠性。对实验结果的分析表明,影响EXAFS谱质量的因素主要是光子计数、测量系统谱分辨率、噪声以及实验器件上的瑕疵。     

激光EXAFS谱仪简介

 同步辐射光源是目前世界上最好的光源,用它测量EXAFS谱自然效果极好.然而由于它设备庞大而昂贵,无法普及到一般实验室.转靶X光机比同步辐射装置要简单和便宜得多,但这种光源的性能不如同步辐射,每次实验所需时间也长得多.本文要介绍的激光EXAFS谱仪是用激光打到金属靶上所产生的X射线脉冲作为光源,并用拍照的方法记录EXAFS谱.其设备更加简单和便宜,而且测得EXAFS谱所需时间极短.当然这种方法也有它的局限性和缺点,例如一般只适用于测量较轻元素的EXAFS谱.激光EXAFS谱仪的结构如图所示.     

神光Ⅱ黑腔等离子体时间分辨的电子温度诊断

在神光Ⅱ强激光装置上,用条纹晶体谱仪对埋点于黑腔靶内壁上的双示踪Ti和Cr材料的激光等离子体高离化态离子发射的X射线谱线进行实验测量,获得超高时间分辨的X射线细致结构谱线。用碰撞辐射模型计算了非局域热动平衡的等离子体布居数,组态平均速率系数由一级微扰理论计算,电子波函数由Hartree-Fock Slater自洽场方法计算,给出了Ti和Cr激光等离子体在电子密度为1019~1022cm-3范围内的He-α线强比与电子温度的关系曲线。采用等电子X射线谱线法,获得了黑腔靶激光等离子体冕区的电子温度随激光脉冲加热从低温到高温、然后缓慢下降的演化过程,其峰值达到2.05 keV。     

超强激光超热电子激发的Kα X射线发射研究

建立了无色散型X射线谱仪. 利用SILEX-I激光装置的超强激光辐照固体物质，分别在靶前、后定量测量了Cu和Mo物质在不同激光功率密度时的X射线谱和Kα光子产额，推导了不同激光强度时的Kα X射线光子转换效率. 实验发现，打靶激光能量越高，靶后出射的Kα产额越高，100μm Mo靶可获得10^-5量级转换效率.     

超强激光超热电子激发的KαX射线发射研究

建立了无色散型X射线谱仪.利用SILEX-I激光装置的超强激光辐照固体物质,分别在靶前、后定量测量了Cu和Mo物质在不同激光功率密度时的X射线谱和Kα光子产额,推导了不同激光强度时的Kα X射线光子转换效率.实验发现,打靶激光能量越高,靶后出射的Kα产额越高,100μm Mo靶可获得10-5量级转换效率.     

双盘靶X光辐射的实验研究

在“星光Ⅱ”激光装置上,利用三倍频激光辐照双盘靶,采用两台软X光谱仪分别对初级和次级辐射的X光谱进行测量,研究X光谱在次级得到改造的特性,并对实验结果进行简单的物理分析,实验表明,次级辐射X光谱与初级的X光谱相比得到了软化,采用X光条纹相机测量双盘靶等离子体喷射的时空扫描图像,结果说明,由于双盘距离较近,初、次级喷射的等离子的体发生了碰撞。     

聚龙一号丝阵负载Z箍缩硬X射线能谱测量

为获取聚龙一号实验装置负载放电产生硬X射线的能谱分布,设计了一套7通道硬X射线能谱仪。介绍了这套多通道硬X射线能谱仪的测谱原理、主要参数及根据测量结果回推光源辐射能谱的解谱算法。在聚龙一号装置丝阵负载物理实验中对测量系统进行考核,获得了信噪比较高的测量波形。利用最大熵方法进行解谱,获得了丝阵负载产生的硬X射线能谱分布,辐射能段主要集中在200~500 keV附近,且1 MeV以上光子份额较低。     

过渡金属二硼化物的金属K边XAS研究

结合X射线衍射实验(XRD)和金属K边的X射线吸收谱(XAS)研究了过渡金属二硼化物(TiB₂,VB₂和CrB₂).在近边吸收区,除了主吸收峰之外,还观察到了3个弱的边前峰,它们是由于金属吸收原子的3d轨道在D6h配位场下分裂,分裂后的3个d轨道与高层金属原子4p轨道发生杂化而引起的.此外,还根据XRD实验得到的晶格参数初步拟合了金属K边EXAFS谱,得到了一些有意义的结果.     

基于光子筛的软X光谱仪

 介绍了采用新型软X光谱学光子筛作为分光元件的软X光谱仪的原理和结构参数设计。新谱仪理论测量范围为100 eV~2 keV,光谱分辨力达0.35 nm。应用该谱仪在SILEX-Ⅰ装置上测量了飞秒激光与固体铜靶相互作用产生的X射线发射谱。实验结果表明,该谱仪主要性能指标达到设计要求,适合于激光与等离子体相互作用产生的软X射线研究。     

Arai实测谱分布数据的应用

对Arai的靶原级谱分布数据 ,通过插值、拟合处理 ,获得适用于数值积分的Δλ =0 0 0 2nm的谱分布数据 ,建立了新的谱分布数据文件 ,应用于FPM程序中。并对耐热钢GH131进行实验研究。理论强度与测量强度的相关性良好 ;基本参数法与理论影响系数法分析结果与确认值一致 ,对Cr,Ni分析的相对误差 <1 0 %。结果表明 :经处理的Arai的靶原级谱分布数据应用于FPM程序 ,提高了分析准确性 ,并扩大了基本参数法与理论影响系数法的应用范围。     

Development of pressure-modulated EXAFS method

Many modulation techniques have been widely applied to improve the quality of conventional spectra. Here a pressure-modulated EXAFS method is proposed to detect the small changes of local structure induced by the modulation of high pressure. In the experiment a dynamic diamond anvil cell was used to put a periodic load on the sample and lock-in amplifier to measure the modulated EXAFS signals. We have applied this technique to ZnSe and revealed a sensitivity to atomic displacement of 0.1 pm that is about ten times better than that of traditional EXAFS.     

The effect of self‐consistent potentials on EXAFS analysis

A theory program intended for use with extended X‐ray‐absorption fine structure (EXAFS) spectroscopy and based on the popular FEFF8 is presented. It provides an application programming interface designed to make it easy to integrate high‐quality theory into EXAFS analysis software. This new code is then used to examine the impact of self‐consistent scattering potentials on EXAFS data analysis by methodical testing of theoretical fitting standards against a curated suite of measured EXAFS data. For each data set, the results of a fit are compared using a well characterized structural model and theoretical fitting standards computed both with and without self‐consistent potentials. It is demonstrated that the use of self‐consistent potentials has scant impact on the results of the EXAFS analysis.     

Pressure effects in Debye-Waller factors and in EXAFS

Anharmonic correlated Einstein model (ACEM) and statistical moment method (SMM) have been developed to derive analytical expressions for pressure dependence of the lattice bond length, effective spring constant, correlated Einstein frequency and temperature, Debye-Waller factors (DWF) or second cumulant, first and third cumulants in Extended X-ray Absorption Fine Structure (EXAFS) at a given temperature. Numerical results for pressure-dependent DWF of Kr and Cu agree well with experiment and other theoretical values. Simulated EXAFS of Cu and its Fourier transform magnitude using our calculated pressure-induced change in the 1st shell are found to be in a reasonable agreement with those using X-ray diffraction (XRD) experimental results.     

Icosahedral order in Cu-Zr amorphous alloys studied by means of X-ray absorption fine structure and molecular dynamics simulations

We have used the X-ray absorption fine structure method and molecular dynamics (MD) simulations to characterize atomic order in Cu-Zr metallic glasses (MGs). The microstructure of these MGs is described in terms of interconnected icosahedral-like clusters (superclusters) which are basic building units reproducing the stoichiometry of the system. The equilibrium MD configurations are used as an input for ab initio calculations of the extended X-ray absorption fine structure (EXAFS) and X-ray absorption near-edge structure (XANES) spectra. The theoretical EXAFS and XANES spectra are compared with those measured for rapidly quenched glassy Cu-Zr alloys. We demonstrate that the experimental results are well reproduced by EXAFS modeling of the population of the superclusters derived from the MD configuration. The average local structural motif can be approximated by Cu-centered icosahedral-like cluster satisfying the condition of maximal local packing efficiency and approximating the system stoichiometry. The simulated XANES exhibits good agreement with experiment, indicating that the atomic order of the MD configuration is consistent with that of the real alloy structure over distances of about 1?nm.     

谐波对EXAFS振幅的影响

本文讨论了晶体单色器高次衍射形成的谐波对EXAFS振幅的影响。给出了一般计算表达式和计算实例。这种影响是使EXAFS振幅减小,它与谐波和基波强度之比、样品厚度及吸收系数等因素有关。分别测量了不同厚度的铜箔样品有谐波与无谐波时的K吸收EXAFS谱,得出的单配位层EXAFS振幅的变化测量值与计算值相符。从而提供了对谐波影响进行修正的方法。 关键词：     

能量分辨率对EXAFS的影响

测量EXAFS谱时,系统的能量分辨率是影响其结果的重要因素。本文提出了分辨率影响结构参数的计算方法,以Ge,Ni样品为例,测量及计算了不同分辨率下的结构参数的差异。测量结果与计算结果符合得很好,讨论了分辨率如何影响EXAFS谱及结构参数,给出了修正方法。 关键词：     

Beam‐size‐related phenomena and effective normalization in energy‐dispersive EXAFS for the study of heterogeneous catalysts,powder materials and the processes they mediate: observations and (some) solutions

The effects of focal spot size and the nature of powder samples (such as heterogeneous catalysts) on the quality of data obtainable from a dispersive EXAFS experiment are characterized at ID24 of the ESRF. Using examples of supported Pd catalysts, it is shown that, for a given photon flux, massive improvements in data quality can be achieved by increasing the size of the dispersive beam in the vertical, whilst concurrently applying a methodology to account for scattering effects emanating from the samples under study. These improvements are demonstrated using progressively practical and demanding examples. Questions regarding optimal beam dimensions for the study of such materials, how to counter undesirable effects that arise from the coherence of the source, how to obtain similar results consistently across the 5–30 keV bandwidth of ID24, and whether a methodology for simultaneous normalization in dispersive EXAFS is of significant utility in such circumstances are discussed.     

Fluorescence detection of exafs: Sensitivity enhancement for dilute species and thin films

The fluorescence intensity is used to measure the X-ray absorption cross-section and is found to yield essentially the same results as a more conventional transmission experiment. However, the fluorescence method is shown to extend the sensitivity of the EXAFS technique by two or more orders of magnitude, and thus nake feasible the study of extremely dilute species.     

Lift‐off protocols for thin films for use in EXAFS experiments

Lift‐off protocols for thin films for improved extended X‐ray absorption fine structure (EXAFS) measurements are presented. Using wet chemical etching of the substrate or the interlayer between the thin film and the substrate, stand‐alone high‐quality micrometer‐thin films are obtained. Protocols for the single‐crystalline semiconductors GeSi, InGaAs, InGaP, InP and GaAs, the amorphous semiconductors GaAs, GeSi and InP and the dielectric materials SiO₂ and Si₃N₄ are presented. The removal of the substrate and the ability to stack the thin films yield benefits for EXAFS experiments in transmission as well as in fluorescence mode. Several cases are presented where this improved sample preparation procedure results in higher‐quality EXAFS data compared with conventional sample preparation methods. This lift‐off procedure can also be advantageous for other experimental techniques (e.g. small‐angle X‐ray scattering) that benefit from removing undesired contributions from the substrate.