Simulations of Chemical Reactions and Polarization Effects at Mesoscopic Scale Specific Force Fields

来源 :第十二届全国量子化学会议 | 被引量 : 0次 | 上传用户:herojian
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  Despite the force-field based molecular dynamics(MD)simulation has been widely applied to rationalize the experimental observations and measurements in chemistry,physics,materials,and life science for years,traditional force field suffers from the incapability for describing chemical reactions and electrostatic polarization effects,which are crucial in many important transformation processes.With the rapid development of quantum mechanical(QM)methods for the large-sized systems and with the input of electronic structure information(which was interlinked with the specific force field terms),some specialized force fields,such as the reactive and polarizable models,were introduced to widen applications of force field methods to a broad range of topics in energy storage,biology process,electronics,catalysis,etc.In order to simulate the collective switching process in azobenzene-based self-assemble monolayers on gold surface,reactive MD simulations were implemented.1,2 By using the reactive rotation potential and switching function,the collective effect of numerous reaction centers and the environment influence on the quantum yield in the complex system were explored at mesoscopic scale.The fragment-based polarizable model was developed to simulate the peptide conformations.3,4 To save computational time in comparison with those polarization models using atom-centered dipole moments without much loss of accuracy,the fragment-centered dipole moments,which are obtained from the energy-based fragmentation QM calculations,are introduced to compute dipole-dipole interactions.To further reduce the computational costs,the fragment-based polarization model is extended into a multi-layer coarsed-graining(CG)style.5 Our polarization models were also applied to an electro-switchable oligopeptide surface,in which the polarization of charged oligopeptides under electric field plays an important role in the conformational changes.6 The specific force fields,furnished with QM justified potential functions,will become a practical tool of modeling the chemical reactions in condensed phase.
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