弛豫铁电体弥散相变的玻璃化特性研究

根据弛豫铁电材料在相变区域的介电弥散行为和玻璃化 液体材料在过冷状态下黏度与温度的行为所共同满足的Vogel-Fulcher 函数关系, 分析了施主替代钛酸钡系列陶瓷的缺陷补偿原理, 通过引入玻璃化液体的构型熵概念, 研究了弛豫铁电材料中钛阳离子缺陷作用势的温度关系, 得到了如下结论: 施主掺杂含量的增加导致了无序度的增加, 钛离子缺陷浓度的增大和平均极性区域尺寸的减小; 在构型熵满足Vogel-Fulcher 函数关系的条件下, 温度越低, 钛离子缺陷作用的范围越大, 极化区域也越大. 缺陷作用的范围随温度的变化导致了弛豫铁电材料的弥散性. 温度下降到一定程度, 冻结效应发生, 介电弥散现象消失.     

甘氨酸-苯丙氨酸-甘氨酸-甘氨酸四肽气相稳定构型的系统寻找

利用PM3、HF和BHandHLYP方法的结合,系统寻找了甘氨酸-苯丙氨酸-甘氨酸-甘氨酸(GFGG)四肽在气相中的稳定构型．对该构型寻找方法进行了详细的描述,并给出了一些重要构型的基本参数,如电子能、零点振动能、偶极矩、转动常数、垂直电离能和不同温度的构型分布等．通过对重要构型结构特征的分析,发现熵的效应是决定构型稳定性的重要因素,并讨论指出了对构型偶极矩和特征振动模的测量是验证理论预言的有效途径．对GFGG构型与蛋白质二级结构的联系的分析表明,GFGG低能构型出现了类似于α-螺旋的局域结构,以及数量可观的蛋白质β转角和γ转角的局域结构.     

热核物质中单核子势的重排项贡献和三体核力效应

在包含三体核力的有限温度Brueckner-Hartree-Fock理论方法基础上, 利用质量算子的空穴线展开, 研究了热核物质中基态关联所导致的对单核子势的重排修正项的密度和温度依赖性, 并讨论了三体核力对重排项的影响. 结果表明：单核子势的重排项贡献具有较强的密度和温度相关性, 重排项贡献随密度增加而增强并随温度升高而减弱. 在计算中引入三体核力会在一定程度上抑制基态空穴关联 效应, 从而导致单核子势的重排项贡献减小, 而且三体核力对重排项贡献的影响随密度增大而增强.     

Pd基非晶合金动态弛豫机制和应力松弛行为

作为潜在的功能及结构材料,高熵非晶合金在凝聚态物理和力学领域引起广泛的研究兴趣.高熵非晶合金宏观力学性能与微观结构非均匀性之间的关联是当前重要的科学问题之一.本文选取非晶形成能力良好的Pd_42.5Cu₃₀Ni_7.5P₂₀非晶合金和Pd₂₀Pt₂₀Cu₂₀Ni₂₀P₂₀高熵非晶合金作为模型体系,借助于动态弛豫行为及应力松弛实验建立了温度和物理时效对非晶合金高温变形机制与微观结构非均匀性之间的关联.研究结果表明Pd基非晶合金表现出“肩膀峰”β弛豫形式.玻璃转变温度以下物理时效非晶合金体系原子移动性导致β弛豫肩膀峰往更高的温度迁移.在应力松弛过程中,由于高构型熵的引入降低吉布斯自由能,这是高熵非晶合金具有较高激活能的原因.高熵非晶合金更难被激活,需要突破更高的能量势垒.物理时效时间增加,高熵非晶合金流变单元更小,这也得益于多主元高熵非晶合金慢扩散效应.高熵非晶合金激活体积的改变在物理时效下应力松弛...     

熔融Cu57团簇在急冷过程中弛豫和局域结构转变的分子动力学研究

采用基于嵌入原子方法的正则系综分子动力学研究熔融Cu₅₇团簇在急冷过程中的弛豫及其局域结构变化.通过对弛豫过程中均方位移、非相干中间散射函数和非Gauss参数三种函数和原子键对随急冷温度不同所发生变化的分析表明,在经过短时间的原子剧烈运动后,急冷温度极大地影响着团簇内原子结构弛豫过程.急冷温度较高时,原子在经历短时间剧烈运动的β弛豫后,进入α弛豫区后以扩散运动为主,随后原子运动表现为非扩散性的原子局域结构重排,团簇内没有出现明显的成核结构.随着温度的降低,原子局域结构的变化在经过短时间原子剧烈运动的β弛豫后,在α弛豫区原子运动表现为扩散性运动,并出现一定数量的不稳定二十面体结构.当急冷温度很低时,在进入α弛豫区后,团簇结构变化逐渐表现为非扩散性原子局域结构重排,形成相当数量的稳定成核二十面体结构. 关键词： 团簇 分子动力学 计算机模拟 表面     

熔融Cu57团簇在急冷过程中弛豫和局域结构转变的分子动力学研究

采用基于嵌入原子方法的正则系综分子动力学研究熔融Cu₅₇团簇在急冷过程中的弛豫及其局域结构变化.通过对弛豫过程中均方位移、非相干中间散射函数和非Gauss参数三种函数和原子键对随急冷温度不同所发生变化的分析表明,在经过短时间的原子剧烈运动后,急冷温度极大地影响着团簇内原子结构弛豫过程.急冷温度较高时,原子在经历短时间剧烈运动的β弛豫后,进入α弛豫区后以扩散运动为主,随后原子运动表现为非扩散性的原子局域结构重排,团簇内没有出现明显的成核结构.随着温度的降低,原子局域结构的变化在经过短时间原子剧烈运动的β弛豫后,在α弛豫区原子运动表现为扩散性运动,并出现一定数量的不稳定二十面体结构.当急冷温度很低时,在进入α弛豫区后,团簇结构变化逐渐表现为非扩散性原子局域结构重排,形成相当数量的稳定成核二十面体结构.     

正则黑洞熵

应用隧道效应所得到的能量谱计算配分函数,进而计算黑洞熵.当本结论取一级近似时,熵修正的对数项与考虑广义不确定关系对黑洞熵修正的对数项一致,然而在计算中没有不确定因子.虽然对数修正项前的因子与考虑热波动对黑洞熵修正中对数项前的因子相同,但所给结论中当黑洞的热容量为负时也不存在发散项.所以本结论具有普遍性. 关键词： 广义不确定关系 热波动 正则系综 量子修正     

纳柱阵列通道中生物分子等效淌度的宏观输运理论分析

各向异性生物分子或带电布朗粒子在周期性孔隙结构运动的分析在生物医学、水处理、环境工程等无数领域具有非常重要的意义. 本文基于宏观输运理论计算粒子在周期性微纳阵列结构中等效输运 参数, 预测分离结果. 首先通过引入构型熵及有效电荷等参数, 建立各向异性生物分子在纳米级受限环境下的等效布朗粒子模型, 然后应用宏观输运理论和数值方法计算分子的等效淌度. 以小分子DNA 片段在周期性纳柱阵列通道中电泳迁移为例, 证明当通道空隙接近或小于分子尺寸时, 熵受限对分子的等效迁移速度有重要的影响, 是实现生物分子分离的主要机理. 因为熵受限的作用随着外电场的增强而减低,所以在较低电场强度条件下, 分子淌度差别较大, 对应分离效果较佳. 关键词： 生物分子分离 构型熵 微纳阵列 宏观输运理论     

C60分子在有序-无序和玻璃态相变间的取向概率与弛豫行为

用极限动力学模型研究了C60分子在有序-无序相变和玻璃态相变温度区间取向角为98°和38°的取向概率与温度的关系.计算结果在玻璃态相变点附近的85!K,90!K和有序-无序相变点的260!K分别与实验值相吻合,取向概率对实验值更精确的拟合及其对温度的二阶导数预言玻璃态相变点在84!K.导出了弛豫规律,其结果表明:双能级的C60分子从非平衡态到平衡态的弛豫行为与非指数因子β有关,其总的弛豫时间决定于其中一个较短的弛豫时间,展宽指数形式保持不变.讨论了KWW方程的非指数因子β与分子间协同作用的关系,发现与双取向态间的能级差有关,计算值与实验结果相同.     

C60分子在有序-无序和玻璃态相变间的取向概率与弛豫行为

用极限动力学模型研究了Ｃ₆₀分子在有序-无序相变和玻璃态相变温度区间取向 角为98°和38°的取向概率与温度的关系.计算结果在玻璃态相变点附近的85K,90K和有序- 无序相变点的260K分别与实验值相吻合,取向概率对实验值更精确的拟合及其对温度的二阶 导数预言玻璃态相变点在84K.导出了弛豫规律,其结果表明：双能级的Ｃ₆₀分子从非平衡态到平衡态的弛豫行为与非指数因子β有关,其总的弛豫时间决定于其中一个较 短的弛豫时间,展宽指数形式保持不变.讨论了KWW方程的非 关键词： 60')" href="#">Ｃ₆₀ 取向概率 非平衡态弛豫     

Programming configurational changes in systems of functionalised polymers using reversible intramolecular linkages

ABSTRACT

We study polymers functionalised by complexes forming intramolecular linkages. Simulations of chains forming reversible linkages are difficult due to entropic barriers that hamper the sampling of different connectivity states specified by the list of pairs of reacted complexes. We address this problem by devising Monte Carlo (MC) moves that change the connectivity state of the system by regrowing parts of the chain while simultaneously reacting bond-forming complexes. Along with moves that link/unlink pairs of complexes, we develop two types of bond-exchange moves. We use these algorithms to study self-assembly of single chain polymeric nanoparticles. When considering monofunctional precursors, we find branched and linear nanoparticle morphologies dominated by long and short intramolecular loops, respectively, along with hierarchical structures in which complexes belonging to different loops are cross-linked. In the strong association limit, equilibrium structures are only reached when using bond-exchange MC moves. We also consider bifunctional precursors in which two different types of complexes decorate the two halves of the chain. We find different types of morphologies featuring different amounts of linkages between complexes of different types. Such findings corroborate our method as a valuable tool to design and predict self-assembly of functional polymers.     

Inherent Structure Approach to the Study of Glass-Forming Liquids

The inherent structure approach, wherein thermodynamic and structural changes in glass-forming liquids are analyzed in terms of local potential energy minima that the liquid samples, has recently been applied extensively to the study of thermodynamic aspects of glass-forming liquids. The evaluation of the configurational entropy, which arises from the multiplicity of local energy minima, plays a central role in such analyses. Results are presented here concerning the calculation of configurational entropy based on computer simulations of a model liquid; and the application of the inherent structure formalism to the study of the glass transition locus, and the fragility of glass-forming liquids.     

Macrospin limit and configurational anisotropy in nanoscale permalloy triangles

In permalloy submicron triangles, configurational anisotropy—a higher-order form of shape anisotropy—yields three equivalent easy axes, imposed by the structures’ symmetry order. Supported by micromagnetic simulations, an experimental method was devised to evaluate the nanostructure dimensions for which a Stoner-Wohlfarth type of reversal could be used to describe this particular magnetic anisotropy. In this regime, a straightforward procedure using an in-plane rotating field allowed us to quantify experimentally the six-fold anisotropy fields for triangles of different thicknesses and sizes.     

Configurational relaxation of “Van Der Waals complexes” in solution

Novel measurements on the microscopic solvation dynamics of 3-amino-N-methylphthalimide (3ANMP) in nonpolar decalin (decahydronaphthalene) solutions with small concentrations of ethanol and other polar additives have been made, using the time-dependent fluorescence Stokes shift (TDFSS) technique. It is found that the experimentally measured TDFSS slightly differs from that predicted by the theory of the generalized Smoluchowski-Vlasov equation (SVE). The essentially slower character of the TDFSS in binary solutions than given by the SVE approach may be explained by the control of the solvation behavior by the large-wavevector processes involving nearest-neighbor molecules.Abbreviations 3ANMP 3-Amino-N-methylphthalimide - TDFSS time-dependent fluorescence Stokes shift - SVE Smoluchowski-Vlasov equation - VWC van der Waals complexes - DMF dimethylformamide - MSA mean spherical approximation.     

Configurational entropy of systems with non-additive lateral interactions

The configurational entropy per site of a lattice gas model with non-additive interactions between adsorbed particles for square, triangular and honeycomb lattices is discussed in the present study. The model used here assumes that the energy which links a certain atom with any of its nearest-neighbors strongly depends on the state of occupancy in the first coordination sphere of that adatom. By means of Monte Carlo simulations in the canonical ensemble by following the algorithm of parallel tempering and the thermodynamic integration method the configurational entropy per site has been calculated. By analyzing the behavior of the configurational entropy per site, the different low-temperature-ordered phases are described. The dependency of the critical temperature of the system as a function of characteristic parameters of the model is established.     

Nanosized ceria-based ceramics: a comparative study

Ce_(1−x)Gd/Sm _x O_2−δ (x = 0.05–0.2, GDC/SDC) nanometric powder was prepared by glycine-nitrates combustion synthesis, by strictly following uniformity in the preparation route. The thermochemical properties of the obtained precursor were studied by TGA/DTA. Crystallization of the fluorite phase occurred on heating at 800 °C or higher temperature. The grain size of calcined powder was found to be about 15 nm. Densification was studied as a function of dopant content. SDC was found more sinterable than GDC. Crystal structure and microstructure were characterized by means of X-ray diffraction (XRD) and scanning electron microscopy (SEM). Electrical characterization was carried out using the impedance spectroscopy method in the frequency range of 50 Hz–13 MHz. The bulk conductivity of SDC is higher than GDC pellet for all concentration ranges. The results were analyzed by using the concept of change of the chemical bond ionicity due to the replacement of the host by dopant. Guest/host ionic size, valence mismatch ratio and their consequences are counted semiquantitatively into the configurational and thermal entropy.     

Configurational entropy of adsorbed rigid rods: Theory and Monte Carlo simulations

The configurational entropy of straight rigid rods of length k (k-mers) adsorbed on square, honeycomb, and triangular lattices is studied by combining theory and Monte Carlo (MC) simulations in grand canonical and canonical ensembles. Three theoretical models to treat k-mer adsorption on two-dimensional lattices have been discussed: (i) the Flory-Huggins approximation and its modification to address linear adsorbates; (ii) the well-known Guggenheim-DiMarzio approximation; and (iii) a simple semi-empirical model obtained by combining exact one-dimensional calculations, its extension to higher dimensions and Guggenheim-DiMarzio approach. On the other hand, grand canonical and canonical MC calculations of the configurational entropy were obtained by using a thermodynamic integration technique. In the second case, the method relies upon the definition of an artificial Hamiltonian associated with the system of interest for which the entropy of a reference state can be exactly known. Thermodynamic integration is then applied to calculate the entropy in a given state of the system of interest. Comparisons between MC simulations and theoretical results were used to test the accuracy and reliability of the models studied.     

Discretization errors in molecular dynamics simulations with deterministic and stochastic thermostats

We investigate the influence of numerical discretization errors on computed averages in a molecular dynamics simulation of TIP4P liquid water at 300 K coupled to different deterministic (Nosé–Hoover and Nosé–Poincaré) and stochastic (Langevin) thermostats. We propose a couple of simple practical approaches to estimating such errors and taking them into account when computing the averages. We show that it is possible to obtain accurate measurements of various system quantities using step sizes of up to 70% of the stability threshold of the integrator, which for the system of TIP4P liquid water at 300 K corresponds to the step size of about 7 fs.     

Guided-Wave Two-Dimensional Acousto-Optic Scanner Using Proton-Exchanged Lithium Niobate Waveguide

Two-dimensional scanning of a 0.6328 mum guided-light beam has been realized using noncolinear acousto-optic (AO) coplanar Bragg diffraction together with colinear AO guided-mode to substrate radiation-mode conversion in a Z-cut Xpropagation LiNbO3 proton-exchanged (PE) waveguide. The two surface acoustic (SAW) waves utilized are at the center frequencies of 500 and 200 MHz, propagating in the Y and X axes, respectively. Two-dimensional scanning of approximately 720 resolvable light beam spots, namely, 18 40 (horizontal vertical) scanning, has been demonstrated using a light beam of 1.0 mm aperture. The total number of resolvable beam spots can be greatly increased from 720 by simply utilizing SAW transducers of larger bandwidth and a light beam of greater aperture. It should also be possible to significantly increase the diffraction efficiency from 3 % by optimizing the parameters of the PE waveguide and the SAWs.