Spectroscopy from quantum dynamics: a mixed wave function/analytical line shape functions approach

• DOI: 10.1007/s00214-023-03035-3
• Publication Date: 2023-10-03T11:02:16Z
• Authors: Francesco Montorsi; Daniel Aranda; Marco Garavelli; Fabrizio Santoro; Francesco Segatta
• Keywords: MCTDH; Nonlinear spectroscopy simulation; Quantum dynamics; 0103 physical sciences; MCTDH, Nonlinear spectroscopy simulation, Quantum dynamics; 01 natural sciences

Abstract Quantum dynamics is the natural framework in which accurate simulation of spectroscopy nonadiabatically coupled molecular systems can be obtained. Even if efficient quantum approaches have been developed, number degrees freedom that need to considered realistic typically too high explicitly account for all them. Moreover, open-quantum systems, a quasi-continuum low-frequency environment modes included get proper description spectral bands. Here, we describe an approach large modes, based on their partitioning into two sets: set dynamically relevant (so-called active modes) are treated dynamics, and only spectroscopically spectator modes), via analytical line shape functions. Linear nonlinear model system simulated, providing clear domain applicability introduced exact, assessing error when such approximate.