Time-Resolved X-ray Absorption Spectroscopy: An MCTDH Quantum Dynamics Protocol

• DOI: 10.1021/acs.jctc.3c00953
• Publication Date: 2023-12-16T01:18:20Z
• Authors: Francesco Segatta; Daniel Aranda; Flavia Aleotti; Francesco Montorsi; Shaul Mukamel; Marco Garavelli; Fabrizio Santoro; Artur Nenov
• Keywords: Dynamics

Expressions for linear and nonlinear spectroscopy simulation in the X-ray window which time evolution of a photoexcited molecular system is treated via quantum dynamics are derived. By leveraging on peculiar properties core-excited/ionized states, first- third-order response functions recast limit time-scale separation between extremely short core-state lifetime (comparably longer) electronic-state transfer nuclear vibrational motion. This work natural extension Segatta et al. (J. Chem. Theory Comput. 2023, 19, 2075–2091), some present authors coupled MCTDH to at different levels sophistication. Full approximate expressions compared by simulating transient absorption carbon K-edge pyrene molecule.