物质动态结构的非弹性散射研究

在静态结构的基础上 ,考虑原子的振动 ,分子键的振动、转动和振—转运动的结构称为动态结构 ,它是用非弹性散射方法来测定的。本文评述研究动态结构的实验方法 :中子非弹性散射、非弹性X射线散射、核非弹性散射和Raman散射以及红外吸收谱。简单介绍了声子散射理论基础。继后 ,分三节描述了用这些方法来研究动态结构的若干结果。 1 )结晶物质 ,包括晶内、表面和界面、高纯近完整晶体中杂质引起的、多晶中、薄膜和纳米晶体中的点阵动力学研究 ;2 )非晶物质 ,包括非晶固体、高聚合物、生物大分子、准晶和液体的动态结构研究 ;3 )高温超导体的点阵动力学研究。文末给出了小结和最后评论。     

分子（H2,D2）与固体表面散射的理论研究

在含时量子计算方法的基础，利用量子散射中的角动量耦合理论等，导出了分子与固体表面非弹性散射的计算公式，对分子（Ｈ２，Ｄ２）与粗糙固体表面在较低能量下的非弹性散射做了计算，得出了模型势下的散射规律。     

Ar+N2体系在长势域上转动非弹性散射的Opacity函数

用一种新的方法研究了Ａ＋ＢＣ体系的转动非弹性散射，即对体系总Ｈａｍｉｌｔｏｎ量中的平动能部分在坐标表象中的显示式用代数方法解析求出，离心势能部分采用ｃｅｎｌｒｉｆｕｇａｌ ｓｕｄｄｅｎ（缩写为ＣＳ）近似，转动能部分采用Ｆｏｕｒｉｅｒ变换处理，并利用二阶差分（ＳＯＤ）法近似含时间的Ｓｃｈｒ?ｄｉｎｇｅｒ方程中的时间偏导，由此得到散射波函数。利用该法对Ａｒ＋Ｎ₂体系的非弹性散射ｏｐａｃｉｔｙ函数做了详细的计算，结果表明，本法比常用的波包（ｃｌｏｓｅ ｃｏｕｐｌｉｎｇ ｗａｖｅ ｐａｃｋｅｔ，缩写为ＣＣＷＰ）法更适合于计算长势域上的高Ｊ（总角动量）值散射，且计算量较后者小。 关键词：     

中子散射技术及其应用

热中子的波长和凝聚态物质的原子／分子间距具有相同的量级，而其能量又和原子／分子的热运动能量相近．因此，利用热中子的弹性和非弹性散射效应，可以从微观层次上获取物质的结构和动力学知识。目前，中子散射技术在物理、化学、化工、生物和材料科学等研究领域的应用已经获得了许多用其他方法无法得到的知识，文章介绍了中子散射的基本原理和特点，并列举了中子散射技术在相关研究领域中的典型应用     

高里德伯态氢原子与氢分子的全量子态分辨的散射动力学研究:费米模型的精确性

文章描述了高里德伯态氢原子与氘分子（D2）散射的近期研究结果。实验研究表明，在高里德伯态氢原子与D2的散射中，非弹性散射和化学反应散射都是重要的。在非弹性散射过程中，氘分子的核自旋是守恒的。反应散射结果说明，高里德伯态氢原子与氘分子的散射动力学和质子与氘分子的散射动力学是非常类似的．这一结果表明，费米的独立碰撞模型在态-态散射动力学的层次上也是正确的。     

强磁场中Rydberg NO分子的回归谱研究

利用分子的闭合轨道理论和多通道量子亏损理论,考虑核的转动影响,计算了Rydberg NO分子在外磁场中的回归谱.研究表明,复杂谱的结构可以用包含分子实散射的闭合轨道理论来解释,不管是同一通道内的弹性散射还是不同通道间的非弹性散射都起着非常重要的作用,尤其是较大标度作用量下,散射作用远大于基本轨道和重复轨道的贡献,很大程度上影响着体系的动力学性质。     

46.8MeV的p+12C非弹性散射

在Glauber多重散射理论框架下，使用跃迁密度方法和三种N湮没势，计算了46.8MeV的反质子在¹²C上的非弹性散射微分截面. 理论曲线与实验数据符合得较好. 关键词： Glauber理论 反质子 非弹性散射 湮没势 跃迁密度     

Cu(100)表面上H2/D2散射的六维态-态量子动力学研究：位点平均模型的有效性

基于由optPBE-vdW密度泛函计算的数千个数据点拟合得到的精确的神经网络势能面,本文采用含时波包方法对H₂/D₂在刚性Cu(100)表面上的态-态散射进行了六维量子动力学计算. 与以往的理论和实验比较了H₂和D₂在Cu(100)中的振转(非)弹性散射的结果. 特别是通过将六维的(非)弹性散射几率与从十五个位点加权平均四维几率的结果比较,测试了在该体系中位点平均近似模型的有效性. 具体来说,位点平均模型很好地重现了振动弹性散射几率,尽管对于高能下的振动非弹性散射结果没那么好. 结果说明在未来研究重双原子或多原子分子从金属表面的态-态散射动力学时,可以使用位点平均模型来降低全维计算过高的成本.     

高效率Be过滤探测器中子非弹性散射谱仪

在中国原子能科学研究院重水堆水平孔道旁,建立了高效率的Be过滤探测器中子非弹性散射谱仪,首次研制了具有宽的接受角(～30°)和聚焦安排的新型Be过滤器,使探测效率提高3倍以上,同时也克服了一般Be过滤谱仪在低能段相干散射的影响.本谱仪还通过具有特殊取向的Ge单色器的不同晶面的自动转向,拓宽了测量的能量范围(10—400meV),并有较好的能量分辨率(4%—9%).在此谱仪上对ZrH_1.6和PdH_0.58的光学振动模以及高Tc超导材料YBa₂ Cu₃ O_6+x的全频谱进行了测试,观察出奇异的结构峰、高频模和反常的散射强度,表明本谱仪不仅效率高而且还具有优良的物理性能,可以在中等通量水平的反应堆上开展广泛的热中子非弹性散射研究.     

中能反质子-核的弹性和非弹性散射

利用实验的PN振幅和多重散射理论 ,在冲量近似下 ,入射能量在 1 80～ 1 80 0MeV范围内我们可以得到反质子的光学势。结果发现能量在 1 30～ 1 4 0MeV范围内 ,光学势强度的虚部几乎是个常数。用能量为 1 80MeV的反质子去打击1 2 C ,1 6O ,40 Ca和2 0 8Pb发生弹性散射和用相同能量的反质子去打击1 2 C发生非弹性散射 ,在程函近似下分析这些散射数据。在绝热近似下 ,用反质子光学势讨论一声子级的集体激发。同时预测了用能量为 1 80～1 833MeV的反质子打击1 2 C ,1 6O ,40 Ca ,2 0 8Pb的弹性散射以及同样情况下打击1 2 C的非弹性散射的微分散射截面。     

A large‐solid‐angle X‐ray Raman scattering spectrometer at ID20 of the European Synchrotron Radiation Facility

An end‐station for X‐ray Raman scattering spectroscopy at beamline ID20 of the European Synchrotron Radiation Facility is described. This end‐station is dedicated to the study of shallow core electronic excitations using non‐resonant inelastic X‐ray scattering. The spectrometer has 72 spherically bent analyzer crystals arranged in six modular groups of 12 analyzer crystals each for a combined maximum flexibility and large solid angle of detection. Each of the six analyzer modules houses one pixelated area detector allowing for X‐ray Raman scattering based imaging and efficient separation of the desired signal from the sample and spurious scattering from the often used complicated sample environments. This new end‐station provides an unprecedented instrument for X‐ray Raman scattering, which is a spectroscopic tool of great interest for the study of low‐energy X‐ray absorption spectra in materials under in situ conditions, such as in operando batteries and fuel cells, in situ catalytic reactions, and extreme pressure and temperature conditions.     

High‐resolution spectroscopy on an X‐ray absorption beamline

A bent‐crystal spectrometer based on the Rowland circle geometry has been installed and tested on the BM30b/FAME beamline at the European Synchrotron Radiation Facility to improve its performances. The energy resolution of the spectrometer allows different kinds of measurements to be performed, including X‐ray absorption spectroscopy, resonant inelastic X‐ray scattering and X‐ray Raman scattering experiments. The simplicity of the experimental device makes it easily implemented on a classical X‐ray absorption beamline. This improvement in the fluorescence detection is of particular importance when the probed element is embedded in a complex and/or heavy matrix, for example in environmental sciences.     

The Raman effect in crystals

A review is given of progress in the theoretical and experimental study of the Raman effect in crystals during the past ten years. Attention is given to the theory of those properties of long-wavelength lattice vibrations in both cubic and uniaxial crystals which can be studied by Raman scattering. In particular the phenomena observed in the Raman scattering from crystals which lack a centre of inversion are related to the theory. The angular variations of the scattering by any type of lattice vibration in a crystal having any symmetry can be easily calculated using a complete tabulation of the Raman tensor. Recent measurements of first-order lattice vibration spectra are listed. A discussion of Brillouin scattering is included. The relation of second-order Raman spectra to critical points in the lattice vibration density of states is discussed, and measurements of the second-order spectra of diamond and the alkali halides are reviewed. The theory and experimental results for Raman scattering by electronic levels of ions in crystals are examined, and proposals for Raman scattering by spin waves, electronic excitations across the superconductive gap and by plasmons are collected together. Finally, the prospects for applying lasers as sources for Raman spectroscopy are discussed, and progress in the new technique of stimulated Raman scattering is reviewed.     

The Raman effect in crystals

A review is given of progress in the theoretical and experimental study of the Raman effect in crystals during the past ten years. Attention is given to the theory of those properties of long-wavelength lattice vibrations in both cubic and uniaxial crystals which can be studied by Raman scattering. In particular the phenomena observed in the Raman scattering from crystals which lack a centre of inversion are related to the theory. The angular variations of the scattering by any type of lattice vibration in a crystal having any symmetry can be easily calculated using a complete tabulation of the Raman tensor. Recent measurements of first-order lattice vibration spectra are listed. A discussion of Brillouin scattering is included. The relation of second-order Raman spectra to critical points in the lattice vibration density of states is discussed, and measurements of the second-order spectra of diamond and the alkali halides are reviewed.

The theory and experimental results for Raman scattering by electronic levels of ions in crystals are examined, and proposals for Raman scattering by spin waves, electronic excitations across the superconductive gap and by plasmons are collected together.

Finally, the prospects for applying lasers as sources for Raman spectroscopy are discussed, and progress in the new technique of stimulated Raman scattering is reviewed.     

Symmetry properties of the lattice vibrations of cadmium diarsenide crystals

The symmetry of the normal vibrations of crystals with the CdAs₂ lattice is established. Selection rules are derived for the infrared absorption and Raman scattering of light; also derived are the selection rules for the inelastic scattering of slow neutrons.     

The pH effects on the growth rate of KDP (KH2PO4) crystal by investigating Raman active lattice modes

We report on the dependence of the pH value on the growth rates of KDP single crystals. Extensive experimental work has been carried out in order to find the optimum pH ranges for growing KDP single crystals with suitable sizes and high optical quality. Different techniques including micro‐Raman back‐scattering spectroscopy, UV/vis/IR transmission spectroscopy and X‐ray diffraction have been employed for this investigation. Deuterated substituted single crystals of KDP and DKDP also have been grown for the investigation of growth rates and Raman active mode identification purposes. The molecular vibration modes of the grown crystals, including internal modes of PO₄ tetrahedrons molecular vibrations, external modes of optical phonons and hydrogen bonding modes have been determined exactly by micro‐Raman back‐scattering spectroscopy. The best pH values of the solution for the KDP crystal growth with reasonably higher growth rates from aqueous solutions that have been supersaturated ata temperature range of 30–50 °C have been found to be in the pH range of 3.2–5.4. Copyright © 2007 John Wiley & Sons, Ltd.     

Neutron Scattering and Vibrational Spectra of Molecular Crystals

Infrared and Raman spectra of a number of molecular crystals have been measured for studying molecular vibrations and the intermolecular and intramolecular force fields. The infrared absorption bands arise from interaction of the electric wave with the oscillating dipole moment of the crystal. Raman scattering covers inelastic photon scattering processes and accordingly Raman lines arise from the oscillating polarizability of the crystal. Thus, the vibrational modes observed in infrared absorption or Raman scattering spectra are k = 0 modes, for which translationally equivalent molecules vibrate in phase.     

From high resolution spectroscopy to the modeling of potential energy surfaces

Methods and recipes used to establish potential energy surfaces in condensed molecular phases are discussed. The reliability of calculations is tested by confrontation with spectroscopic measurements in crystals. Optical spectroscopy, in particular, hole burning as a line-narrowing technique, as well as high resolution inelastic neutron scattering (INS), are used to resolve tunneling level structures corresponding to large-amplitude atomic and molecular motions. Rotational tunneling of methyl groups is discussed, and new measurements by INS are presented for crystals that are proposed as suitable candidates for optical studies. Translational tunneling in benzoic acid crystals and the role of promoting modes are reviewed, and new measurements of vibrational spectra by inelastic x-ray scattering are compared with INS and Raman spectra.     

A three‐crystal spectrometer for high‐energy resolution fluorescence‐detected X‐ray absorption spectroscopy and X‐ray emission spectroscopy at SSRF

A Johann‐type spectrometer for the study of high‐energy resolution fluorescence‐detected X‐ray absorption spectroscopy, X‐ray emission spectroscopy and resonant inelastic X‐ray scattering has been developed at BL14W1 X‐ray absorption fine structure spectroscopy beamline of Shanghai Synchrotron Radiation Facility. The spectrometer consists of three crystal analyzers mounted on a vertical motion stage. The instrument is scanned vertically and covers the Bragg angle range of 71.5–88°. The energy resolution of the spectrometer ranges from sub‐eV to a few eV. The spectrometer has a solid angle of about 1.87 × 0^?3 of 4π sr, and the overall photons acquired by the detector could be 10⁵ counts per second for the standard sample. The performances of the spectrometer are illustrated by the three experiments that are difficult to perform with the conventional absorption or emission spectroscopy. Copyright © 2016 John Wiley & Sons, Ltd.     

Lattice dynamics and inelastic neutron scattering experiments on andalusite,Al2SiO5

We report coherent inelastic neutron scattering measurements of the phonon dispersion relations and lattice dynamics shell model calculations of several microscopic and macroscopic properties of andalusite, Al₂SiO₅. Andalusite has an orthorhombic structure with 32 atoms/unit cell. The inelastic neutron scattering measurements (up to energy transfers of 45 meV) were carried out using the triple axis spectrometer at Dhruva reactor, India using a single crystal of andalusite and the phonon dispersion relations along the [100] direction have been measured. The shell model calculations have been used to compute the crystal structure, elastic constants, phonon frequencies, dispersion relations, density of states and the specific heat. The calculated results are in good agreement with available experimental data. The computed one-phonon neutron scattering structure factors based on the shell model have been very useful in the planning and analysis of the inelastic neutron scattering experiments.