电子衍射径向分布函数测定稀土顺1,4聚丁二烯的原子间距分布

本文用电子衍射径向分布函数测定了稀土顺1,4聚丁二烯的原子间距分布。从电子衍射实验强度曲线的傅里叶变换得到的RDF曲线上,具有二个分子内峰和三个分子间峰。说明在熔点以上,处于非晶态的顺1,4聚丁二烯中不同程度的存在分子链间的局部有序性。     

分子动力学模拟无定形BCN体系结构特征

为研究无定形BCN材料的原子结构特征, 采用分子动力学方法模拟了高温下无定形BCN体系的动力学行为, 计算并分析了引入C原子对体系的径向分布函数(RDF)和配位数的影响. 模拟结果表明, C原子对BCN体系的RDF曲线的峰位置及形状影响很小, 但使其偏径向分布函数(PRDF)的一些峰向右偏移; 引入的C原子部分占据了原来N原子的位置, 使得B-N的配位数降低. 在模拟条件下, 未观察到BN相与C相分离.     

Prepeak in the structural factor. Inhomogeneous packings of Lennard-Jones atoms

This work reports on the effects of structural inhomogeneities within the models of spherical atomic packings on the radial distribution function (RDF) and the structural factor (SF). Models of inhomogeneous packings were constructed by removing some atoms from homogeneous packing according to a predetermined template. Thus various additional voids, leading to specific structural correlations of atoms on a middle scale (several atomic sizes), are introduced in the model. A dense noncrystalline packing of 27,000 Lennard-Jones atoms serves as the initial system. Three various templates were used, and models containing different fractions of additional voids were constructed with each of these templates. It is demonstrated that RDF is only slightly sensitive to such inhomogeneities; in contrast, the SF has additional peaks at small q, these peaks being notable even after removal of a small fraction of atoms. Some models yield a single narrow prepeak, which is akin to that observed in diffraction experiment for some glasses.     

RDF法对非晶态聚醚砜共聚物的近程有序结构研究

用径向分布函数(RDF)研究了聚醚砜共聚物(PES)在r=1.5 nm范围内的近程结构, 结果表明, 分子链间存在近程有序结构, 有序周期约为0.5 nm; 聚醚砜共聚物经退火处理后, 由g(r)图可以看出, 第一个峰变高、变窄; 由G(r)图可以看出, 分子链间第一个有序区内, 分子链间贡献大于链内贡献; 于200 ℃退火处理后有序畴尺寸(rs)略有增大, 原子平均位移(σ)变小, 使得分子链内原子间距分布更加均匀, 相邻分子链间距(rv)变小. 同时透射电镜(TEM)的形态结构分析表明, 经退火处理后, 其聚集态确实形成了某种局部有序的结构.     

Monte Carlo Simulation of the Local Ordering of Water Molecules. II. Spatial Correlations and Hydrogen Bonds

The Monte Carlo method is used to calculate spatial distribution functions of oxygen and hydrogen atoms within a large-size water model (33666 SPC/E water molecules) under atmospheric pressure at room temperature. The work focuses on structural interpretation of local densities of water at the distances of about 3–5 Å from its molecules. The distribution of the distances between water molecules connected by chains of two or more hydrogen bonds indicates that the molecules between the first and second peaks of the radial distribution function (RDF) are mainly second and, to a lesser extent, third neighbors along the chain of bonds.     

Hydration water and bulk water in proteins have distinct properties in radial distributions calculated from 105 atomic resolution crystal structures

Water plays a critical role in the structure and function of proteins, although the experimental properties of water around protein structures are not well understood. The water can be classified by the separation from the protein surface into bulk water and hydration water. Hydration water interacts closely with the protein and contributes to protein folding, stability, and dynamics, as well as interacting with the bulk water. Water potential functions are often parametrized to fit bulk water properties because of the limited experimental data for hydration water. Therefore, the structural and energetic properties of the hydration water were assessed for 105 atomic resolution (相似文献   

熔融LiCl系中微观空间的确定和分布

分子动力学计算机模拟计算表明在熔融碱金属卤化物中存在微观空洞.本文报道计算微观空洞和描述微观空洞分布的方法. 根据模拟所求相轨道,考虑到周期性边界条件,若在中心元胞的某处能加入一个至少跟组分粒子尺寸相当的“虚粒子”且又不跟任何其它粒子(包括组分粒子和已加入的虚粒子)相交,则称在该处存在一个微观空洞,可容纳最大虚粒子的孔洞的半径即微观空洞半径. 为嵌入虚粒子,须对已存在的粒子进行搜索.以四个粒子为一组,在中心元胞中依次选择一个粒子为母粒子,在其周围的一定范围内再另任选三个粒子,构成一个四粒子组.设法     

Deriving the 3D structure of organic molecules from their infrared spectra

The representation of the 3D structure of a molecule by a radial distribution function (RDF) code is described. The use of the RDF code for the simulation of an infrared spectrum by a counterpropagation (CPG) neural network is shown. Furthermore, a CPG network can also be operated in reverse mode: on input of an infrared spectrum an RDF code is obtained for which a 3D structure can be searched in a database. An empirical modelling process is used to refine this 3D structure to obtain a three-dimensional model of the molecular structure that corresponds to the infrared spectrum.     

Pair correlation function of soft-sphere fluids

A closed-form analytic formula for the radial distribution function (RDF) or g(r) of inverse power fluids is proposed. The RDF is expressed as a sum of separate component functions, one monotonic and a series of exponentially damped oscillatory functions. Unlike previous treatments in the literature, this formula does not rely on patching different functional forms at arbitrary crossover distances. This expression, which we refer to as g(M)(r), yields the expected asymptotic behavior at large distance and reproduces the main features of the RDF generated by molecular dynamics (MD) simulations. The g(M) is applied to the soft n = 4 inverse power fluid, and it is shown that in this case seven or fewer terms are sufficient to represent accurately the MD-generated RDF over the entire fluid domain. The relative contributions of the separate terms of the g(M) as a function of density are analyzed and discussed. The key role played by the monotonic component function and two oscillatory terms is demonstrated. The origin of the crossover from the oscillatory to the monotonic behavior is shown to be the same as that recently proposed by Evans and Henderson [R. Evans and J. R. Henderson, J. Phys.: Condens. Matter 21, 474220 (2009)] for the dispersion interactions.     

Theoretical Study on the Hydration Structure of Divalent Radium Ion Using Fragment Molecular Orbital–Molecular Dynamics (FMO–MD) Simulation

Using fragment molecular orbital–molecular dynamics (FMO–MD) simulation at the FMO3-HF/6-31G(d,p) level, the hydration of a Ra²⁺ ion was theoretically investigated. The first peaks of the radial distribution function (RDF) for Ra–O and Ra–H lengths were predicted to be 2.85 and 3.45 Å with broad envelopes in the ranges of 2.5–3.5 and 2.8–4.3 Å, respectively. The broad peaks shows that the first hydration shell of Ra²⁺ is much more flexible than those in the other hydrated divalent alkaline earth metal ions, i.e., Ra²⁺ is a structure-breaking ion. The hydration number of Ra²⁺ was predicted to be 8.1. From the angular distribution function (ADF), it was clarified that the octa hydrated Ra²⁺ ion has a flexible square antiprism structure at room temperature.     

Surface tension correlation for pure polar fluids by a new molecular model and SRK equation of state

In this work, a new model based on molecular thermodynamic was presented to correlate the surface tension of pure polar liquids. This model was developed based on the Davis theory. According to this theory, the surface tension is defined as a function of radial distribution function (RDF) and potential function (PF) as well. The proposed model includes three additive terms; hard sphere, dispersion and polar interactions. The RDF of Kolafa equation of state and Dirac delta function as a PF were used for hard sphere interaction. The RDF expression of Xu and Hu was considered for both dispersion and polar interactions. The presented model has two adjustable parameters, size and energy, which were obtained by optimization of an objective function for each pure fluid. This proposed approach was used for 19 pure polar fluids divided into 6 groups; organic acids, alcohols, ketones, ethers, aldehydes, and water. The average absolute deviation percent (AAD%) obtained for 19 fluids are 0.74. Also the surface tension of these 19 fluids was calculated by the use of SRK EOS and Sugden empirical formula in two cases. In case 1, Sugden's Parachor was calculated from Hugill and van Welsenes correlation and in case 2, it was obtained by optimization of an objective function for each component. The values of AAD% are 43.544 and 2.281 for cases 1 and 2, respectively. These results show the new model, which includes two adjustable parameters, can correlate the surface tension of the pure polar liquids with a high accuracy.     

高斯多峰拟合在径向分布函数中的应用

利用同步辐射X射线散射法测定了盐水摩尔比分别为1:30和1:14的Rb2SO4和Cs2SO4的水溶液结构. 通过对散射数据的处理, 获得了两种溶液的径向分布函数. 采用多峰拟合中的Gaussian法对径向分布函数中金属离子第一水合层附近的叠加峰进行了处理, 多峰拟合结果与实验结果吻合得很好. 通过将拟合数据与已报道的溶液结构和晶体结构对比分析, 确定了每个拟合峰的归属.多峰拟合结果分析表明, Rb+和Cs+第一水合层配位数为6, 为变形的八面体构型. 两种溶液中都存在着金属离子和硫酸根离子接触离子对: Rb—S 和Cs—S 的特征距离分别为0.407和0.427 nm. 研究证实, 多峰拟合有助于阐述溶液中离子的水合结构.     

Structural features and molecular assembly of amorphous phosphazenic materials in the bulk--combined theoretical and experimental techniques: Tris-(2,2'-dioxy-1,1'-binaphthyl)cyclotriphosphazen

The structure and the assembly of tris-(2,2'-dioxy-binaphthyl)cyclotriphosphazene [(+)-[NP3(O2C20H12)3], DBNP, in the solid amorphous state was studied using molecular dynamics (MD) including ad hoc quantum mechanically derived force field (FF) parameters, in combination with the energy dispersive X-ray diffraction (EDXD) technique. The atom-atom radial distribution function (RDF) curve obtained through the EDXD experiment revealed low intensity peaks not attributable to the intramolecular distances of the single molecule, but clearly featuring a low energy state of long-distance three-dimensional assembly. The radial distribution functions (RDF) were calculated for various models of DBNP submitted to theoretical MD simulations. Based on the comparison of theoretically calculated RDFs and those obtained from the EDXD experiment, the predominant structural motif of the material in the bulk was found to have DBNP molecules laid one upon the other to form tubular nanostructures. These contain eight DBNP units each (length ca. 46 A) with two and three of these units aligned in parallel and held together. The material can be represented as a bulk of tubular snake-like chains undergoing distortions with a step of eight DBNP units. The bending angles, that vary randomly, attain limited values sufficient to induce disorder and thus nonperiodic structure. The present application of MD simulations combined with EDXD data appear to be a general approach to solve for the first time otherwise intractable issues concerning structural features and assembly of molecular materials in the bulk.     

Rietveld法在半结晶聚酯二相共存结构分析中的应用

用Rietveld法对试样的BaF2的实测X射线衍射全谱图(XDWP)数据进行精修，获得正确的结晶相结构参数，重点讨论了如何正确选择衍射峰型函数和评价精修结构参数的可靠性；特别指出，当把Rietveld法和Fourier过滤技术及径向分布函数(radial distribution function，RDF)联用来研究半结晶聚酯(PET)的两相结构参数时，除需用R因子判断结晶相之精修结构参数的可靠性外，还要判断由非品相散射强度数据计算的RDF是否合理；如果忽视后一判据，则有可能导致错误的计算结果。     

新型含磷无机离子交换剂研究(Ⅵ)——非晶态交换剂六偏磷酸锡的结构分析

通过大角度X射线散射分析,求出了新型无机离子交换剂六偏磷酸锡的径向分布函数,推断其化学结构。应用此结构较好地解释了交换剂的离子交换性质。     

垃圾衍生燃料等温快速热解和燃烧反应特性

利用热天平和管式炉对RDF(Refuse Derived Fuel)等温快速热解和燃烧反应特性进行了研究。实验发现，在等温快速升温的条件下，RDF热解和燃烧的反应速率都非常快，从受热开始到反应结束需60 s～80 s;从开始失重到完成反应为20 s。RDF热解和燃烧热重反应曲线非常类似，都只有一个反应失重区;RDF组成对其燃烧和热解反应性有重要影响，含有橡胶的RDF的热解和燃烧反应速率较小。在650 ℃～800 ℃RDF快速热解产物中气、液产物的产率可达80%～90%，而固体产物的产率只有10%～20%，热解气体的热值为20kJ/m3，RDF较适合进行热解处理。     

The sound velocities in dense fluids from distribution functions

The sound velocities and adiabatic compressibilities in dense fluids have been evaluated using three known analytical expressions for radial distribution functions (RDFs). Using such approach not only tests the power of distribution functions theory in predicting the sound velocities and adiabatic compressibilities, but also specifies better expressions in determining these properties. To calculate these quantities, the variation of RDF with density and temperature is required. Therefore, we should have analytical expressions which explicitly present RDF as a function of temperature, density and interparticle distance. It is shown that if an expression is used which properly presents RDFs as a function of interparticle distance, density and temperature, it is possible to calculate sound velocities and adiabatic compressibilities from distribution function theory.     

Radial distribution function of a hard-sphere fluid for the nearest neighbor surroundings

An expression for RDF as a function of two variables, the distance r and the packing factor η, was obtained by approximating the results of Monte Carlo simulation of a hard-sphere fluid. The mean square accuracy of the expressions presented is about ±0.0002 (1 ≤ r ≤ 1.5, 0 ≤ η ≤ 0.5). A continuous extension of RDF to the region of r < 1 is proposed, which provides the continuity of the first and second derivatives of RDF at the point r = 1. Analysis of the problem of determining the hard sphere diameter in WCA theory of simple liquids shows that the proposed expression makes it possible to directly calculate the hard sphere diameter without any simplifying approximations.     

Investigation on spontaneous ignition of two kinds of organic material with water

A systematic investigation was performed to elucidate the cause of spontaneous ignition of Refuse Derived Fuel (RDF) and Meat Bone Meal (MBM). Heat generation in both RDF and MBM with addition of water liquid and vapor at room temperature was determined by isothermal calorimetry. Compared with water liquid, the heat of wetting by sorption of water vapor at 80% relative humidity and 25 °C was larger, which can raise the temperature of RDF and MBM more than 30 and 56 °C, respectively. Heat generation due to fermentation occurred and the temperature of RDF and MBM reached or exceeded 80 °C after 5 days for RDF and 4 days for MBM at 100% RH. The spontaneous ignition for RDF and MBM results from heat of wetting and fermentation at room temperature and a further exothermic reaction at higher temperature.     

Molecular dynamics simulation of self-diffusion coefficients for several alkanols

The transfer properties and microscopic structures of methanol, ethanol, 1-propanol, 2-propanol, and 1-pentanol in the temperature range from 290 to 450 K and pressure range from 0.1 to 200 MPa were studied by molecular dynamics (MD) simulation through the calculation of the self-diffusion coefficients, velocity autocorrelation functions (VACF), and radial distribution function (RDF). The calculated self-diffusion coefficients conform to the experimental values on the whole, and the temperature has greater influence, which weaken with the increase of the carbon chain, on self-diffusion coefficient than pressure. The factors affecting self-diffusion coefficients were also analyzed from micro perspective by calculation of VACF and RDF, which is helpful to understand the relationship between microscopic structures of fluid and its transfer properties. This work not only provides a reliable simulation method for transfer properties of alkanols, but also provides the prediction data for design and development of chemical processes.