Nonadiabatic molecular dynamics with solvent effects: A LR-TDDFT QM/MM study of ruthenium (II) tris (bipyridine) in water

Ivano Tavernelli; Basile F E Curchod; Ursula Rothlisberger

doi:10.1016/j.chemphys.2011.03.021

Nonadiabatic molecular dynamics with solvent effects: A LR-TDDFT QM/MM study of ruthenium (II) tris (bipyridine) in water

Ivano Tavernelli^*, Basile F E Curchod, Ursula Rothlisberger

^*Corresponding author for this work

School of Chemistry

Research output: Contribution to journal › Article (Academic Journal)

74 Citations (Scopus)

Abstract

The previously derived trajectory-based nonadiabatic molecular dynamics scheme [E. Tapavicza, I. Tavernelli, U. Rothlisberger, Phys. Rev. Lett. 98 (2007) 023001] is extended to include the coupling of the quantum system with a classically described environment. The dynamics is performed using LR-TDDFT energies and forces computed on-the-fly together with the nonadiabatic coupling vectors needed for the propagation of the nuclear coefficients according to Tully's fewest-switches surface hopping algorithm. The resulting LR-TDDFT-QM/MM approach is applied to the study of the ultrafast relaxation of the photoexcited singlet metal-to-ligand-charge-transfer state (¹MLCT) of [Ru(bpy)₃]²⁺ (bpy = 2,2′-bipyridine) in water. The observed intersystem crossing dynamics with the triplet MLCT is in good agreement with available experimental results.

Original language	English
Pages (from-to)	101-109
Number of pages	9
Journal	Chemical Physics
Volume	391
Issue number	1
DOIs	https://doi.org/10.1016/j.chemphys.2011.03.021
Publication status	Published - 24 Nov 2011

Keywords

Inorganic dyes
LR-TDDFT
Nonadiabatic dynamics
QM/MM
Ruthenium (II) tris (bipyridine)
Surface hopping

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10.1016/j.chemphys.2011.03.021

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Tavernelli, I., Curchod, B. F. E., & Rothlisberger, U. (2011). Nonadiabatic molecular dynamics with solvent effects: A LR-TDDFT QM/MM study of ruthenium (II) tris (bipyridine) in water. Chemical Physics, 391(1), 101-109. https://doi.org/10.1016/j.chemphys.2011.03.021

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abstract = "The previously derived trajectory-based nonadiabatic molecular dynamics scheme [E. Tapavicza, I. Tavernelli, U. Rothlisberger, Phys. Rev. Lett. 98 (2007) 023001] is extended to include the coupling of the quantum system with a classically described environment. The dynamics is performed using LR-TDDFT energies and forces computed on-the-fly together with the nonadiabatic coupling vectors needed for the propagation of the nuclear coefficients according to Tully's fewest-switches surface hopping algorithm. The resulting LR-TDDFT-QM/MM approach is applied to the study of the ultrafast relaxation of the photoexcited singlet metal-to-ligand-charge-transfer state (1MLCT) of [Ru(bpy)3]2+ (bpy = 2,2′-bipyridine) in water. The observed intersystem crossing dynamics with the triplet MLCT is in good agreement with available experimental results.",

keywords = "Inorganic dyes, LR-TDDFT, Nonadiabatic dynamics, QM/MM, Ruthenium (II) tris (bipyridine), Surface hopping",

author = "Ivano Tavernelli and Curchod, {Basile F E} and Ursula Rothlisberger",

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AU - Rothlisberger, Ursula

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