Search for Elementary Rearrangement Process and Investigation of Irreversible Structural Relaxation in Simple-Molecular Liquids

简单分子液体中基本重排过程的搜索和不可逆结构弛豫的研究

基本信息

  • 批准号:
    06453017
  • 负责人:
  • 金额:
    $ 4.74万
  • 依托单位:
  • 依托单位国家:
    日本
  • 项目类别:
    Grant-in-Aid for General Scientific Research (B)
  • 财政年份:
    1994
  • 资助国家:
    日本
  • 起止时间:
    1994 至 1995
  • 项目状态:
    已结题

项目摘要

1) beta-glass transition as well as alpha-one were found by an adiabatic calorimetry to occur in the supercooled liquid state of 1,3-diphenyl-1,1,3,3-tetramethyldisiloxane, omicron-terphenyl, propene carbonate and dibutylphthalate. Further, in the plastically crystalline state of cyclohexanol, there were two sets of alpha-and beta-glass transitions and another glass transition found to occur. A possibility was suggested that plural modes of molecular rearrangement motions coupled in liquid were decoupled from each other through the positional ordering of molecules.2) alpha-relaxation processes under constant temperature condition were studied calorimetrically by the temperature jump method for glycerol, propylene glycol, 1,3-diphenyl-1,1,3,3-tetramethyldisiloxane and dibutylphthalate with different fragilities from each other. The relaxation processes were characterized in terms of the nonexponentiality parameter beta of stretched exponential function. A strong correlation was found to exist between the fragility m and the nonlinearity delta=dbeta/dDELTA_jT of relaxation function to the temperature jump. The presence of the correlation was also confirmed by a computer simulation of the ireversible relaxation process based on a thermal activation model.3) The similar enthalpy relaxation processes were tracked by the temperature jump method for fluorene-dibenzofuran solid solutions. The nonexponentiality parameter beta was constant independently of DELTA_jT for each conpound. This result is quite in contrast to that in supercooled liquid, demonstrating that the nonlinearity found in liquid is attributed mainly to a non-Arrhenius property of the average relaxation times.4) A new crystallization process due to the aggregation of homogeneous crystal embryos/nuclei was discovered in omicron-terphenyl and salol in their respective glass transition regions. The growth rate was found to be determined by the beta-relaxation rate but not by the alpha-one commonly recognized.
1)通过绝热量热法发现在1,3-二苯基-1,1,3,3-四甲基二硅氧烷、三联苯、碳酸丙烯酯和邻苯二甲酸二丁酯的过冷液态中发生β-玻璃化转变以及α-酮。此外,在环己醇的塑性结晶状态下,存在两组α-和β-玻璃化转变,并且发现发生另一种玻璃化转变。2)采用温度跃变法对不同脆性的甘油、丙二醇、1,3-二苯基-1,1,3,3-四甲基二硅氧烷和邻苯二甲酸二丁酯在恒温条件下的α弛豫过程进行了量热研究。用拉伸指数函数的非指数性参数β表征弛豫过程。发现脆性m与弛豫函数对温度跃变的非线性度delta=dbeta/dDELTA_jT之间存在很强的相关性。基于热活化模型的不可逆弛豫过程的计算机模拟也证实了相关性的存在。3)采用温度跃变方法跟踪了芴-二苯并呋喃固溶体的类似焓弛豫过程。非指数性参数β是恒定的,独立于每个复合物的DELTA_jT。这一结果与在过冷液体中的结果形成鲜明对比,表明在液体中发现的非线性主要归因于平均弛豫时间的非阿耳忒修斯性质。4)在三联苯和salol的玻璃化转变区发现了一个新的结晶过程,这是由于同质晶胚/晶核的聚集。发现生长速率由β-松弛速率决定,而不是由通常公认的α-松弛速率决定。

项目成果

期刊论文数量(64)
专著数量(0)
科研奖励数量(0)
会议论文数量(0)
专利数量(0)
Hiroki Fujimori: "Calorimetric Study of D,L-propene Carbonate : Observation of the beta-as alpha-glass Transition in the Supercooled Liquids and Glasses" J.Chem.Thermodyn.26. 367-378 (1994)
Hiroki Fujimori:“D,L-丙烯碳酸酯的量热研究:过冷液体和玻璃中 β-as α-玻璃转变的观察”J.Chem.Thermodyn.26。
  • DOI:
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    0
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Hiroki Fujimori: "Calorimetric Study of 1,3-diphenyl-1,1,3,3-tetramethyldisiloxane : Emergence of α-,β-,and Crystalline-glass Transitions" J.Non-Cryst.Solids. (in press). (1996)
Hiroki Fujimori:“1,3-二苯基-1,1,3,3-四甲基二硅氧烷的量热研究:α-、β-和结晶玻璃转变的出现”J.Non-Cryst.Solids(正在出版)。 (1996)
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  • 影响因子:
    0
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Takaaki Hikima: "beta-Molecular Rearrangement Process, but not alpha-process, as goverming a Homogeneous Crystal-Nucleation Rate in Supercooled Liquid" Bull.Chem.Soc.Japan. (Submitted).
Takaaki Hikima:“β 分子重排过程,但不是 α 过程,控制过冷液体中的均质晶体成核速率”Bull.Chem.Soc.Japan。
  • DOI:
  • 发表时间:
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  • 影响因子:
    0
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Hiroki Fujimori: "Characterization of Structural Fluctuation and Irreversible Nonlinear Relaxation Process in Glassy Liquid by a Temperature Jump Method" Bussei Kenkyu. 62 [2]. 321-323 (1994)
Hiroki Fujimori:“通过温度跳跃方法表征玻璃液体中的结构涨落和不可逆非线性弛豫过程”Bussei Kenkyu。
  • DOI:
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  • 期刊:
  • 影响因子:
    0
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Hiroki FUJIMORI: "Nonlinearity of the Enthalpic Response Function to a Temperature Jump and Its Interpretation Based on Fragility in Liquid Glasses" Bull. Chem. Soc. Japan. 68. 447-455 (1995)
Hiroki FUJIMORI:“温度跳跃的焓响应函数的非线性及其基于液体玻璃脆性的解释”公牛。
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OGUNI Masaharu其他文献

OGUNI Masaharu的其他文献

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{{ truncateString('OGUNI Masaharu', 18)}}的其他基金

Ordering and potential appearance of a phase transition in low-tenperature liquid confined within meso-pores
中孔内低温液体中相变的有序性和潜在出现
  • 批准号:
    25610119
  • 财政年份:
    2013
  • 资助金额:
    $ 4.74万
  • 项目类别:
    Grant-in-Aid for Challenging Exploratory Research
Liquid-liquid phase transition and dynamic properties of low-temperature water under pressure, and chemical-pressurization effects on water
低温水在压力下的液-液相变和动态特性以及化学加压对水的影响
  • 批准号:
    21340118
  • 财政年份:
    2009
  • 资助金额:
    $ 4.74万
  • 项目类别:
    Grant-in-Aid for Scientific Research (B)
Low-temperature structure formation and glass transition behaviors oflow-dimensional water
低维水的低温结构形成和玻璃化转变行为
  • 批准号:
    18350003
  • 财政年份:
    2006
  • 资助金额:
    $ 4.74万
  • 项目类别:
    Grant-in-Aid for Scientific Research (B)
Realization of a two-dimensional glass, and the direct observation of its ordered-cluster structure and structural change
二维玻璃的实现及其有序簇结构和结构变化的直接观察
  • 批准号:
    10440169
  • 财政年份:
    1998
  • 资助金额:
    $ 4.74万
  • 项目类别:
    Grant-in-Aid for Scientific Research (B).
Configuration and Rearrangement Rate of Excess Oxygen Atoms in Transition-Metal Oxides Related to Superconductors
超导体相关过渡金属氧化物中过量氧原子的构型和重排率
  • 批准号:
    08454208
  • 财政年份:
    1996
  • 资助金额:
    $ 4.74万
  • 项目类别:
    Grant-in-Aid for Scientific Research (B)
Heat Capacity at Constant Volume and Molecular Motion of Crystal, Orientationally Disordered Crystal and Liquid
晶体、无序晶体和液体的定体积热容和分子运动
  • 批准号:
    02453008
  • 财政年份:
    1990
  • 资助金额:
    $ 4.74万
  • 项目类别:
    Grant-in-Aid for General Scientific Research (B)

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