{"title":"利用高斯过程回归建立水中多体相互作用模型","authors":"Yulian T Manchev, Paul L A Popelier","doi":"10.1021/acs.jpca.4c05873","DOIUrl":null,"url":null,"abstract":"<p><p>We report a first-principles water dimer potential that captures many-body interactions through Gaussian process regression (GPR). Modeling is upgraded from previous work by using a custom kernel function implemented through the KeOps library, allowing for much larger GPR models to be constructed and interfaced with the next-generation machine learning force field FFLUX. A new synthetic water dimer data set, called WD24, is used for model training. The resulting models can predict 90% of dimer geometries within chemical accuracy for a test set and in a simulation. The curvature of the potential energy surface is captured by the models, and a successful geometry optimization is completed with a total energy error of just 2.6 kJ mol<sup>-1</sup>, from a starting structure where water molecules are separated by nearly 4.3 Å. Dimeric modeling of a flexible, noncrystalline system with FFLUX is shown for the first time.</p>","PeriodicalId":59,"journal":{"name":"The Journal of Physical Chemistry A","volume":null,"pages":null},"PeriodicalIF":2.7000,"publicationDate":"2024-10-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Modeling Many-Body Interactions in Water with Gaussian Process Regression.\",\"authors\":\"Yulian T Manchev, Paul L A Popelier\",\"doi\":\"10.1021/acs.jpca.4c05873\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p><p>We report a first-principles water dimer potential that captures many-body interactions through Gaussian process regression (GPR). Modeling is upgraded from previous work by using a custom kernel function implemented through the KeOps library, allowing for much larger GPR models to be constructed and interfaced with the next-generation machine learning force field FFLUX. A new synthetic water dimer data set, called WD24, is used for model training. The resulting models can predict 90% of dimer geometries within chemical accuracy for a test set and in a simulation. The curvature of the potential energy surface is captured by the models, and a successful geometry optimization is completed with a total energy error of just 2.6 kJ mol<sup>-1</sup>, from a starting structure where water molecules are separated by nearly 4.3 Å. Dimeric modeling of a flexible, noncrystalline system with FFLUX is shown for the first time.</p>\",\"PeriodicalId\":59,\"journal\":{\"name\":\"The Journal of Physical Chemistry A\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":2.7000,\"publicationDate\":\"2024-10-11\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"The Journal of Physical Chemistry A\",\"FirstCategoryId\":\"1\",\"ListUrlMain\":\"https://doi.org/10.1021/acs.jpca.4c05873\",\"RegionNum\":2,\"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":"The Journal of Physical Chemistry A","FirstCategoryId":"1","ListUrlMain":"https://doi.org/10.1021/acs.jpca.4c05873","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q3","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Modeling Many-Body Interactions in Water with Gaussian Process Regression.
We report a first-principles water dimer potential that captures many-body interactions through Gaussian process regression (GPR). Modeling is upgraded from previous work by using a custom kernel function implemented through the KeOps library, allowing for much larger GPR models to be constructed and interfaced with the next-generation machine learning force field FFLUX. A new synthetic water dimer data set, called WD24, is used for model training. The resulting models can predict 90% of dimer geometries within chemical accuracy for a test set and in a simulation. The curvature of the potential energy surface is captured by the models, and a successful geometry optimization is completed with a total energy error of just 2.6 kJ mol-1, from a starting structure where water molecules are separated by nearly 4.3 Å. Dimeric modeling of a flexible, noncrystalline system with FFLUX is shown for the first time.
期刊介绍:
The Journal of Physical Chemistry A is devoted to reporting new and original experimental and theoretical basic research of interest to physical chemists, biophysical chemists, and chemical physicists.