From Classical to Quantum and Back: A Hamiltonian Scheme for Adaptive Multiresolution Classical/Path-Integral Simulations

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• 作者：Karsten Kreis ; Mark E. Tuckerman ; Davide Donadio ; Kurt Kremer ; Raffaello Potestio
• 刊名：Journal of Chemical Theory and Computation
• 出版年：2016
• 出版时间：July 12, 2016
• 年：2016
• 卷：12
• 期：7
• 页码：3030-3039
• 全文大小：548K
• 年卷期：0
• ISSN：1549-9626

文摘

Quantum delocalization of atomic nuclei affects the physical properties of many hydrogen-rich liquids and biological systems even at room temperature. In computer simulations, quantum nuclei can be modeled via the path-integral formulation of quantum statistical mechanics, which implies a substantial increase in computational overhead. By restricting the quantum description to a small spatial region, this cost can be significantly reduced. Herein, we derive a bottom-up, rigorous, Hamiltonian-based scheme that allows molecules to change from quantum to classical and vice versa on the fly as they diffuse through the system, both reducing overhead and making quantum grand-canonical simulations possible. The method is validated via simulations of low-temperature parahydrogen. Our adaptive resolution approach paves the way to efficient quantum simulations of biomolecules, membranes, and interfaces.