| Title: |
Time-Resolved X-ray Absorption Spectroscopy: An MCTDH Quantum Dynamics Protocol |
| Authors: |
Segatta F.; Aranda D.; Aleotti F.; Montorsi F.; Mukamel S.; Garavelli M.; Santoro F.; Nenov A. |
| Contributors: |
Segatta F.; Aranda D.; Aleotti F.; Montorsi F.; Mukamel S.; Garavelli M.; Santoro F.; Nenov A. |
| Publication Year: |
2023 |
| Collection: |
IRIS Università degli Studi di Bologna (CRIS - Current Research Information System) |
| Subject Terms: |
Time-Resolved; X‐ray Absorption; Spectroscopy; MCTDH; Quantum Dynamics |
| Description: |
Expressions for linear and nonlinear spectroscopy simulation in the X-ray window in which the time evolution of a photoexcited molecular system is treated via quantum dynamics are derived. By leveraging on the peculiar properties of core-excited/ionized states, first- and third-order response functions are recast in the limit of time-scale separation between the extremely short core-state lifetime and the (comparably longer) electronic-state transfer and nuclear vibrational motion. This work is a natural extension of Segatta et al. (J. Chem. Theory Comput. 2023, 19, 2075-2091), in which some of the present authors coupled MCTDH quantum dynamics to spectroscopy simulation at different levels of sophistication. Full quantum dynamics and approximate expressions are compared by simulating X-ray transient absorption spectroscopy at the carbon K-edge in the pyrene molecule. |
| Document Type: |
article in journal/newspaper |
| File Description: |
STAMPA |
| Language: |
English |
| Relation: |
info:eu-repo/semantics/altIdentifier/pmid/38101807; info:eu-repo/semantics/altIdentifier/wos/WOS:001139534200001; volume:20; issue:1; firstpage:307; lastpage:322; numberofpages:16; journal:JOURNAL OF CHEMICAL THEORY AND COMPUTATION; https://hdl.handle.net/11585/953432 |
| DOI: |
10.1021/acs.jctc.3c00953 |
| Availability: |
https://hdl.handle.net/11585/953432; https://doi.org/10.1021/acs.jctc.3c00953; https://pubs.acs.org/doi/10.1021/acs.jctc.3c00953 |
| Rights: |
info:eu-repo/semantics/openAccess |
| Accession Number: |
edsbas.827747C9 |
| Database: |
BASE |