Mixed-quantum-classical or fully-quantized dynamics? A unified code to compare methods

Coonjobeeharry, J.; Spinlove, K. E.; Sanz Sanz, Cristina; Sapunar, Marin; Došlić, Nađa; Worth, Graham A. (2022) Mixed-quantum-classical or fully-quantized dynamics? A unified code to compare methods. Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences, 380 (2223). ISSN 1364-503X

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Abstract

Three methods for non-adiabatic dynamics are compared to highlight their capabilities. Multiconfigurational time-dependent Hartree is a full gridbased solution to the time-dependent Schrödinger equation, variational multi-configurational Gaussian (vMCG) uses a less flexible but unrestricted Gaussian wavepacket basis, and trajectory surface hopping (TSH) replaces the nuclear wavepacket with a swarm of classical trajectories. Calculations with all methods using a model Hamiltonian were performed. The vMCG and TSH were also then run in a direct dynamics mode, with the potential energy surfaces calculated on-the-fly using quantum chemistry calculations. All dynamics calculations used the QUANTICS package, with the TSH calculations using a new interface to a surface hopping code. A novel approach to calculate adiabatic populations from grid-based quantum dynamics using a time-dependent discrete variable representation is presented, allowing a proper comparison of methods. This article is part of the theme issue ‘Chemistry without the Born–Oppenheimer approximation’.

Item Type:	Article
Uncontrolled Keywords:	trajectory surface hopping ; nonadiabatic dynamics
Subjects:	NATURAL SCIENCES > Chemistry > Theoretical Chemistry
Divisions:	Division of Physical Chemistry
Projects:	Project title Project leader Project code Project type Svjetlo na molekulama: istraživanje spregnute elektronske i nuklearne dinamike-LightMol Nađa Došlić IP-2016-06-1142 HRZZ Efekt kvantnog tuneliranja: dinamika molekula s kvantnim jezgrama-QuanTunMol Marko Tomislav Cvitaš IP-2020-02-9932 HRZZ
Depositing User:	Marin Sapunar
Date Deposited:	30 Apr 2026 09:30
URI:	https://fulir.irb.hr:/id/eprint/11833
DOI:	10.1098/rsta.2020.0386

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