期刊
JOURNAL OF COMPUTATIONAL CHEMISTRY
卷 37, 期 1, 页码 83-92出版社
WILEY
DOI: 10.1002/jcc.24025
关键词
computational organic chemistry; replica exchange molecular dynamics; ab initio molecular dynamics; density functional tight binding
资金
- European Research Council [306528]
- EPFL
- Competence Centre for Materials Science and Technology (CCMX)
- European Research Council (ERC) [306528] Funding Source: European Research Council (ERC)
Computational studies of organic systems are frequently limited to static pictures that closely align with textbook style presentations of reaction mechanisms and isomerization processes. Of course, in reality chemical systems are dynamic entities where a multitude of molecular conformations exists on incredibly complex potential energy surfaces (PES). Here, we borrow a computational technique originally conceived to be used in the context of biological simulations, together with empirical force fields, and apply it to organic chemical problems. Replica-exchange molecular dynamics (REMD) permits thorough exploration of the PES. We combined REMD with density functional tight binding (DFTB), thereby establishing the level of accuracy necessary to analyze small molecular systems. Through the study of four prototypical problems: isomer identification, reaction mechanisms, temperature-dependent rotational processes, and catalysis, we reveal new insights and chemistry that likely would be missed using static electronic structure computations. The REMD-DFTB methodology at the heart of this study is powered by i-PI, which efficiently handles the interface between the DFTB and REMD codes. (C) 2015 Wiley Periodicals, Inc.
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