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

Research Project

Project/Area Number 06453017
Research Category

Grant-in-Aid for General Scientific Research (B)

Allocation TypeSingle-year Grants
Research Field Physical chemistry
Research InstitutionTokyo Institute of Technology

Principal Investigator

OGUNI Masaharu  Tokyo Institute of Technology, Faculty of Science Professor, 理学部, 教授 (50144423)

Project Period (FY) 1994 – 1995
Project Status Completed (Fiscal Year 1995)
Budget Amount *help
¥7,400,000 (Direct Cost: ¥7,400,000)
Fiscal Year 1995: ¥1,100,000 (Direct Cost: ¥1,100,000)
Fiscal Year 1994: ¥6,300,000 (Direct Cost: ¥6,300,000)
KeywordsSupercooled Liquid / Glass Transition / Enthalpy Relaxation / Nonlinearity / Irreversible Process / beta-relaxation / Homogeneous Crystal Nucleation / 結晶核生成 / 液体 / 不可逆性
Research Abstract

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.

Report

(3 results)
  • 1995 Annual Research Report   Final Research Report Summary
  • 1994 Annual Research Report
  • Research Products

    (32 results)

All Other

All Publications (32 results)

  • [Publications] Hiroki Fujimori: "Calorimetric Study of D,L-propene Carbonate : Observation of the β-as α-glass Transition in the Supercooled Liquids and Glasses" J.Chem.Thermodyn.26. 367-378 (1994)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1995 Final Research Report Summary
  • [Publications] Hiroki Fujimori: "Non-exponentiality of the Enthalpy Relaxation under Constant Temperature Conditions in the Time Domain in Supercooled liquids and Glasses" J.Non-Cryst.Solids. 172-174. 601-607 (1994)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1995 Final Research Report Summary
  • [Publications] Minoru Hanaya: "Remarkable Non-exponentiality of the Enthalpy Relaxation in Fast Ion Conducting Glass (AgI) _<0.5> (AgPO_3) _<0.5> Far from Equilibrium" J.Non-Cryst.Solids. 172-174. 608-614 (1994)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1995 Final Research Report Summary
  • [Publications] Hiroki Fujimori: "Nonlinearity of the Enthalpic Response Function to a Temperature Jump and Its Interpretation Based on Fragilty in Liquid Glasses" Bull.Chem.Soc.Japan. 68. 447-455 (1995)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1995 Final Research Report Summary
  • [Publications] Takaaki Hikima: "Determination of Potentially Homogeneous-Nucleation-Based Crystallization in o-Terphenyl and Interpretation of the Nucleation Enhancement Mechanism" Phys.Rev.B52. 3900-3908 (1995)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1995 Final Research Report Summary
  • [Publications] Hiroki Fujimori: "Correlation Index [Tg_α-Tg_β] /Tg_α and Activation Energy Ratio Δ_<εaα>/Δ_<εaβ> as Parameters Characterizing the Structure of Liquid and Glass" Solid State Commun.94. 157-162 (1995)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1995 Final Research Report Summary
  • [Publications] Takaaki Hikima: "Discovery of a Potentially Homogeneous-Nucleation-Based Crystallization around the Glass Transition Temperature in Salol" Solid State Commun.93. 713-717 (1995)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1995 Final Research Report Summary
  • [Publications] 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)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1995 Final Research Report Summary
  • [Publications] Takaaki Hikima: "‘β-Molecular Rearrangement Process,but not α -process,as goverming a Homogeneous Crystal-Nucleation Rate in Supercooled Liquid" Submitted to Bull.Chem.Soc.Japan.

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1995 Final Research Report Summary
  • [Publications] 藤森裕基: "ガラス性液体における構造揺らぎと不可逆的非線形緩和過程の温度ジャンプ法による特性化" 物性研究. 62. 321-323 (1994)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1995 Final Research Report Summary
  • [Publications] 藤森裕基: "過冷却液体におけるスローダイナミクスの熱的特性化" 熱測定. (印刷中). (1996)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1995 Final Research Report Summary
  • [Publications] 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)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1995 Final Research Report Summary
  • [Publications] Hiroki Fujimori: "Non-exponentiality of the Enthalpy Relaxation under Constant Temperature Conditions in the Time Domain in Supercooled liquids and Glasses" J.Non-Cryst.Solids. 172-174. 601-607 (1994)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1995 Final Research Report Summary
  • [Publications] Minoru Hanaya: "Remarkable Non-exponentiality of the Enthalpy Relaxation in Fast Ion Conducting Glass (AgI)_<0.5>(AgPO_3)_<0.5> Far from Equilibrium" J.Non-Cryst.Solids. 172-174. 608-614 (1994)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1995 Final Research Report Summary
  • [Publications] 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 [2]. 447-455 (1995)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1995 Final Research Report Summary
  • [Publications] Takaaki Hikima: "Determination of Potentially Homogeneous-Nucleation-Based Crystallization in o-Terphenyl and Interpretation of the Nucleation Enhancement Mechanism" Phys.Rev.B52 [6]. 3900-3908 (1995)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1995 Final Research Report Summary
  • [Publications] Hiroki Fujimori: "Correlation Index [Tg_<alpha>^-Tg_<beta>]/Tg_<alpha> and Activation Energy Ratio DELTA_<epsilonaalpha>/DELTA_<epsilonabeta> as Parameters Characterizing the Structure of Liquid and Glass" Solid State Commun.94 [2]. 157-162 (1995)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1995 Final Research Report Summary
  • [Publications] Takaaki Hikima: "Discovery of a Potentially Homogeneous-Nucleation-Based Crystallization around the Glass Transition Temperature in Salol" Solid State Commun. 93 [8]. 713-717 (1995)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1995 Final Research Report Summary
  • [Publications] Hiroki Fujimori: "Calorimetric Study of 1,3-diphenyl-1,1,3,3-tetramethyldisiloxane : Emergence of alpha-, beta-, and Crystalline-glass Transitions" J.Non-Cryst.Solids. (in press). (1996)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1995 Final Research Report Summary
  • [Publications] 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).

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1995 Final Research Report Summary
  • [Publications] 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)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1995 Final Research Report Summary
  • [Publications] Hiroki Fujimori: "Thermal Characterization of Slow Dynamics in Supercooled Liquids" Netsusokutei. (in press). (1996)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1995 Final Research Report Summary
  • [Publications] Takaaki Hikima: "Determination of Potentially Homogeneous-Nucleation-Based Crystallization in o-Terphenyl and an Interpretation of the Nucleation Enhancement Mechanism" Phys. Rev.B52. 3900-3908 (1995)

    • Related Report
      1995 Annual Research Report
  • [Publications] Takaaki Hikima: "Discovery of a Potentially Homogeneous-Nucleation-Based Crystallization around the Glass Transition Temperature in Salol" Solid State Commun.93. 713-717 (1995)

    • Related Report
      1995 Annual Research Report
  • [Publications] Hiroki Fujimori: "Correlation Index [T_<gα>-T_<gβ>]/T_<gα> and Activation Energy Ratio Δ ε_<aα> Δ ε_<αβ> as Parameters Characterizing the Structure of Liquid and Glass" Solid State Commun.68. 447-455 (1995)

    • Related Report
      1995 Annual Research Report
  • [Publications] 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)

    • Related Report
      1995 Annual Research Report
  • [Publications] 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)

    • Related Report
      1994 Annual Research Report
  • [Publications] Hiroki FUJIMORI: "Calorimetric Study of D,L-propene Carbonate: Observation of the β-as well as α-glass Transition in the Supercooled Liquid" J. Chem. Thermodyn.26. 367-378 (1994)

    • Related Report
      1994 Annual Research Report
  • [Publications] Hiroki FUJIMORI: "Non-exponentiality of the Enthalpy Relaxation under Constant-Temperature Conditions in the Time Domain in Supercooled Liquids and Glasses" J. Non-Cryst. Solids. 172-174. 601-607 (1994)

    • Related Report
      1994 Annual Research Report
  • [Publications] Minoru HANAYA: "Remarkable Non-exponentiality of the Enthalpy Relaxation in Fast Ion Conducting Glass (AgI)_<0.5>(AgPO_3)_<0.5> Far from Equilibrium" J. Non-Cryst. Solids. 172-174. 608-614 (1994)

    • Related Report
      1994 Annual Research Report
  • [Publications] C. A. ANGELL: "Liquid Fragility and the Glass Transition in Water and Aqueous Solutions" J. Food Engineering. 22. 115-142 (1994)

    • Related Report
      1994 Annual Research Report
  • [Publications] 藤森 裕基: "ガラス性液体における構造揺らぎと不可逆的非線形緩和過程の温度ジャンプ法による特性化" 物性研究. 62. 321-323 (1994)

    • Related Report
      1994 Annual Research Report

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Published: 1994-04-01   Modified: 2016-04-21  

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