6533b828fe1ef96bd1288626

RESEARCH PRODUCT

Surface Hopping Dynamics Including Intersystem Crossing using the Algebraic Diagrammatic Construction Method

Felix PlasserMathias PabstSebastian MaiAndreas KöhnAndreas KöhnFrank NeeseLeticia González

subject

PhysicsCouplingChemical Physics (physics.chem-ph)010304 chemical physicsAb initioGeneral Physics and AstronomyFOS: Physical sciencesSurface hoppingElectronic structure010402 general chemistry01 natural sciences0104 chemical sciencesIntersystem crossingPhysics - Chemical Physics0103 physical sciencesComplete active spaceStatistical physicsPhysical and Theoretical ChemistryPerturbation theoryWave function

description

We report an implementation for employing the algebraic diagrammatic construction to second order [ADC(2)] ab initio electronic structure level of theory in nonadiabatic dynamics simulations in the framework of the SHARC (surface hopping including arbitrary couplings) dynamics method. The implementation is intended to enable computationally efficient, reliable, and easy-to-use nonadiabatic dynamics simulations of intersystem crossing in organic molecules. The methodology is evaluated for the 2-thiouracil molecule. It is shown that ADC(2) yields reliable excited-state energies, wave functions, and spin-orbit coupling terms for this molecule. Dynamics simulations are compared to previously reported results using high-level multi-state complete active space perturbation theory, showing favorable agreement.

yearjournalcountryeditionlanguage
2017-11-14
10.1063/1.4999687http://arxiv.org/abs/1901.03241