{"title":"通过分子动力学模拟和微观理论预测过冷小分子的结构弛豫","authors":"Anh D. Phan , Ngo T. Que , Nguyen T.T. Duyen","doi":"10.1016/j.chemphys.2025.112947","DOIUrl":null,"url":null,"abstract":"<div><div>Understanding and predicting the glassy dynamics of small organic molecules is critical for applications ranging from pharmaceuticals to energy and food preservation. In this work, we present a theoretical framework that combines molecular dynamics simulations and Elastically Collective Nonlinear Langevin Equation (ECNLE) theory to predict the structural relaxation behavior of small organic glass-formers. By using propanol, glucose, fructose, and trehalose as model systems, we estimate the glass transition temperature (<span><math><msub><mrow><mi>T</mi></mrow><mrow><mi>g</mi></mrow></msub></math></span>) from stepwise cooling simulations and volume–temperature analysis. These computed <span><math><msub><mrow><mi>T</mi></mrow><mrow><mi>g</mi></mrow></msub></math></span> values are then inserted into the ECNLE theory to calculate temperature-dependent relaxation times and diffusion coefficients. Numerical results agree well with experimental data in prior works. This approach provides a predictive and experimentally-independent route for characterizing glassy dynamics in molecular materials.</div></div>","PeriodicalId":272,"journal":{"name":"Chemical Physics","volume":"601 ","pages":"Article 112947"},"PeriodicalIF":2.4000,"publicationDate":"2025-09-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Predicting structural relaxation in supercooled small molecules via molecular dynamics simulations and microscopic theory\",\"authors\":\"Anh D. Phan , Ngo T. Que , Nguyen T.T. Duyen\",\"doi\":\"10.1016/j.chemphys.2025.112947\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>Understanding and predicting the glassy dynamics of small organic molecules is critical for applications ranging from pharmaceuticals to energy and food preservation. In this work, we present a theoretical framework that combines molecular dynamics simulations and Elastically Collective Nonlinear Langevin Equation (ECNLE) theory to predict the structural relaxation behavior of small organic glass-formers. By using propanol, glucose, fructose, and trehalose as model systems, we estimate the glass transition temperature (<span><math><msub><mrow><mi>T</mi></mrow><mrow><mi>g</mi></mrow></msub></math></span>) from stepwise cooling simulations and volume–temperature analysis. These computed <span><math><msub><mrow><mi>T</mi></mrow><mrow><mi>g</mi></mrow></msub></math></span> values are then inserted into the ECNLE theory to calculate temperature-dependent relaxation times and diffusion coefficients. Numerical results agree well with experimental data in prior works. This approach provides a predictive and experimentally-independent route for characterizing glassy dynamics in molecular materials.</div></div>\",\"PeriodicalId\":272,\"journal\":{\"name\":\"Chemical Physics\",\"volume\":\"601 \",\"pages\":\"Article 112947\"},\"PeriodicalIF\":2.4000,\"publicationDate\":\"2025-09-19\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Chemical Physics\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0301010425003489\",\"RegionNum\":3,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q4\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Chemical Physics","FirstCategoryId":"92","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0301010425003489","RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q4","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Predicting structural relaxation in supercooled small molecules via molecular dynamics simulations and microscopic theory
Understanding and predicting the glassy dynamics of small organic molecules is critical for applications ranging from pharmaceuticals to energy and food preservation. In this work, we present a theoretical framework that combines molecular dynamics simulations and Elastically Collective Nonlinear Langevin Equation (ECNLE) theory to predict the structural relaxation behavior of small organic glass-formers. By using propanol, glucose, fructose, and trehalose as model systems, we estimate the glass transition temperature () from stepwise cooling simulations and volume–temperature analysis. These computed values are then inserted into the ECNLE theory to calculate temperature-dependent relaxation times and diffusion coefficients. Numerical results agree well with experimental data in prior works. This approach provides a predictive and experimentally-independent route for characterizing glassy dynamics in molecular materials.
期刊介绍:
Chemical Physics publishes experimental and theoretical papers on all aspects of chemical physics. In this journal, experiments are related to theory, and in turn theoretical papers are related to present or future experiments. Subjects covered include: spectroscopy and molecular structure, interacting systems, relaxation phenomena, biological systems, materials, fundamental problems in molecular reactivity, molecular quantum theory and statistical mechanics. Computational chemistry studies of routine character are not appropriate for this journal.