An algorithm for very high pressure molecular dynamics simulations.

Autor: Tesi M; Dipartimento di Chimica e Chimica Industriale, Università di Pisa, Pisa, Italy., Cammi R; Dipartimento di Scienze Chimiche, della Vita e della Sostenibilità Ambientale, Università di Parma, Parma, Italy., Granucci G; Dipartimento di Chimica e Chimica Industriale, Università di Pisa, Pisa, Italy., Persico M; Dipartimento di Chimica e Chimica Industriale, Università di Pisa, Pisa, Italy.
Jazyk: angličtina
Zdroj: Journal of computational chemistry [J Comput Chem] 2024 Dec 15; Vol. 45 (32), pp. 2848-2861. Date of Electronic Publication: 2024 Aug 29.
DOI: 10.1002/jcc.27461
Abstrakt: We describe a method to run simulations of ground or excited state dynamics under extremely high pressures. The method is based on the introduction of a fictitious ideal gas that exerts the required pressure on a molecular sample and is therefore called XP-GAS (eXtreme Pressure by Gas Atoms in a Sphere). The algorithm is most suitable for approximately spherical clusters of molecules described by quantum chemistry methods, Molecular Mechanics or mixed QM/MM approaches. We compare the results obtained by the algorithm here presented and by the XP-PCM approach, based on a continuum description of the environment. As a test case, we study the conformational dynamics of 1,3-butadiene either as an isolated molecule ("naked" butadiene) or embedded in a cluster of argon atoms, under pressures up to 15 GPa. Overall, our results show that the XP-GAS QM/MM simulation method is in good agreement with the XP-PCM QM/Continuum model (Cammi model) in describing the effect of the pressure on static properties as the equilibrium geometry of butadiene in the ground state. Furthermore, the comparison of XP-GAS simulations with naked butadiene and butadiene in argon shows the importance, for XP-GAS and related methods, of a realistic representation of the medium in modelling pressure effects.
(© 2024 The Author(s). Journal of Computational Chemistry published by Wiley Periodicals LLC.)
Databáze: MEDLINE
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