Open AccessLocal Control Theory using Trajectory Surface Hopping and Linear-Response Time-Dependent Density Functional Theory
Author(s) -
Basile F. E. Curchod,
Thomas J. Penfold,
Ursula Röthlisberger,
Ivano Tavernelli
Publication year - 2013
Publication title -
chimia
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 0.387
H-Index - 55
eISSN - 2673-2424
pISSN - 0009-4293
DOI - 10.2533/chimia.2013.218
Subject(s) - surface hopping , trajectory , density functional theory , curvature , photoexcitation , physics , time dependent density functional theory , population , statistical physics , pulse (music) , control theory (sociology) , quantum mechanics , control (management) , computer science , mathematics , excited state , geometry , demography , sociology , voltage , artificial intelligence
The implementation of local control theory using nonadiabatic molecular dynamics within the framework of linear-response time-dependent density functional theory is discussed. The method is applied to study the photoexcitation of lithium fluoride, for which we demonstrate that this approach can efficiently generate a pulse, on-the-fly, able to control the population transfer between two selected electronic states. Analysis of the computed control pulse yields insights into the photophysics of the process identifying the relevant frequencies associated to the curvature of the initial and final state potential energy curves and their energy differences. The limitations inherent to the use of the trajectory surface hopping approach are also discussed.