{"title":"揭示卤代二聚体中非共价相互作用的能量复杂性","authors":"Fang Liu, Likai Du","doi":"10.1002/qua.27445","DOIUrl":null,"url":null,"abstract":"<p>The understanding of noncovalent interactions is crucial in explaining critical phenomena such as self-assembly, chemical reactivity, and crystallization. This work examines the energetic diversity of conformations and local minima for several halogenated dimers, represented as R-X (R = H, F, CH<sub>3</sub>, CF<sub>3</sub>; X = Cl, Br, I). Thousands of configurations are randomly generated and refined through geometric optimizations to yield a diverse set of molecular conformers. Frequency calculations were performed for all optimized conformers to confirm that they are local minima. The noncovalent interactions in optimized dimers of halogen-containing molecules were analyzed with atom in molecules (AIM) method and symmetry-adapted perturbation theory (SAPT). Additionally, a protocol for generating machine learning models to recover accurate predictions of the physically meaningful SAPT energy components with minor computational cost is presented. These results deepen our understanding of the intricate energy balance and dedicated equilibrium of different noncovalent interactions in halogenated dimers.</p>","PeriodicalId":182,"journal":{"name":"International Journal of Quantum Chemistry","volume":"124 14","pages":""},"PeriodicalIF":2.3000,"publicationDate":"2024-07-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Unveiling the energetic complexity of noncovalent interactions in halogenated dimers\",\"authors\":\"Fang Liu, Likai Du\",\"doi\":\"10.1002/qua.27445\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p>The understanding of noncovalent interactions is crucial in explaining critical phenomena such as self-assembly, chemical reactivity, and crystallization. This work examines the energetic diversity of conformations and local minima for several halogenated dimers, represented as R-X (R = H, F, CH<sub>3</sub>, CF<sub>3</sub>; X = Cl, Br, I). Thousands of configurations are randomly generated and refined through geometric optimizations to yield a diverse set of molecular conformers. Frequency calculations were performed for all optimized conformers to confirm that they are local minima. The noncovalent interactions in optimized dimers of halogen-containing molecules were analyzed with atom in molecules (AIM) method and symmetry-adapted perturbation theory (SAPT). Additionally, a protocol for generating machine learning models to recover accurate predictions of the physically meaningful SAPT energy components with minor computational cost is presented. These results deepen our understanding of the intricate energy balance and dedicated equilibrium of different noncovalent interactions in halogenated dimers.</p>\",\"PeriodicalId\":182,\"journal\":{\"name\":\"International Journal of Quantum Chemistry\",\"volume\":\"124 14\",\"pages\":\"\"},\"PeriodicalIF\":2.3000,\"publicationDate\":\"2024-07-11\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"International Journal of Quantum Chemistry\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://onlinelibrary.wiley.com/doi/10.1002/qua.27445\",\"RegionNum\":3,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q3\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"International Journal of Quantum Chemistry","FirstCategoryId":"92","ListUrlMain":"https://onlinelibrary.wiley.com/doi/10.1002/qua.27445","RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q3","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Unveiling the energetic complexity of noncovalent interactions in halogenated dimers
The understanding of noncovalent interactions is crucial in explaining critical phenomena such as self-assembly, chemical reactivity, and crystallization. This work examines the energetic diversity of conformations and local minima for several halogenated dimers, represented as R-X (R = H, F, CH3, CF3; X = Cl, Br, I). Thousands of configurations are randomly generated and refined through geometric optimizations to yield a diverse set of molecular conformers. Frequency calculations were performed for all optimized conformers to confirm that they are local minima. The noncovalent interactions in optimized dimers of halogen-containing molecules were analyzed with atom in molecules (AIM) method and symmetry-adapted perturbation theory (SAPT). Additionally, a protocol for generating machine learning models to recover accurate predictions of the physically meaningful SAPT energy components with minor computational cost is presented. These results deepen our understanding of the intricate energy balance and dedicated equilibrium of different noncovalent interactions in halogenated dimers.
期刊介绍:
Since its first formulation quantum chemistry has provided the conceptual and terminological framework necessary to understand atoms, molecules and the condensed matter. Over the past decades synergistic advances in the methodological developments, software and hardware have transformed quantum chemistry in a truly interdisciplinary science that has expanded beyond its traditional core of molecular sciences to fields as diverse as chemistry and catalysis, biophysics, nanotechnology and material science.