TY  - JOUR
AU  - Ruckenbauer, M.
AU  - Barbatti, M.
AU  - Müller, T.
AU  - Lischka, H.
TI  - Nonadiabatic Excited-State Dynamics with Hybrid ab Initio Quantum-Mechanical/Molecular-Mechanical Methods: Solvation of the Pentadieniminium Cation in Apolar Media
JO  - The journal of physical chemistry  / A
VL  - 114
SN  - 1089-5639
CY  - Washington, DC
PB  - Soc.
M1  - PreJuSER-9524
SP  - 6757 - 6765
PY  - 2010
N1  - This work was supported by the Austrian Science Fund within the framework of the Special Research Program F16 (Advanced Light Sources) and Project P18411-N19, by the project FS397001-CPAMMS in the University Priority Research Area Computational Science of the University of Vienna, and by the COST Chemistry Action D37 Gridchem, Working Groups PHOTODYN and ELAMS. Computational resources at the Luna-cluster of the Institute for Computer Science were accessed using the Vienna Grid Environment (VGE. Calculations were partially performed at the Linux PC cluster Schrodinger III of the computer center of the University of Vienna.
AB  - A new implementation of nonadiabatic excited-state dynamics using hybrid methods is presented. The current approach is aimed at the simulation of photoexcited molecules in solution. The chromophore is treated at the ab initio level, and its interaction with the solvent is approximated by point charges within the electrostatic embedding approach and by a Lennard-Jones potential for the nonbonded interactions. Multireference configuration interaction (MRCI) and multiconfiguration self-consistent field (MCSCF) methods can be used. The program implementation has been performed on the basis of the Columbus and Newton-X program systems. For example, the dynamics of penta-2,4-dien-1-iminium (PSB3) and 4-methyl-penta-2,4-dien-1-iminium cations (MePSB3) was investigated in gas phase and in n-hexane solution. The excited-state (S(1)) lifetime and temporal evolution of geometrical parameters were computed. In the case of PSB3 the n-hexane results resemble closely the gas phase data. MePSB3, however, shows a distinct extension of lifetime due to steric hindering of the torsion around the central bond because of solute-solvent interactions.
KW  - Cations: chemistry
KW  - Imines: chemistry
KW  - Models, Molecular
KW  - Molecular Conformation
KW  - Quantum Theory
KW  - Solvents: chemistry
KW  - Time Factors
KW  - Cations (NLM Chemicals)
KW  - Imines (NLM Chemicals)
KW  - Solvents (NLM Chemicals)
KW  - J (WoSType)
LB  - PUB:(DE-HGF)16
C6  - pmid:20518515
UR  - <Go to ISI:>//WOS:000278981900004
DO  - DOI:10.1021/jp103101t
UR  - https://juser.fz-juelich.de/record/9524
ER  -