Journal
CHEMICAL PHYSICS
Volume 391, Issue 1, Pages 50-61Publisher
ELSEVIER
DOI: 10.1016/j.chemphys.2011.04.014
Keywords
Quantum optimal control theory; Time-dependent density-functional theory
Funding
- Deutsche Forschungsgemeinschaft [SFB 658]
- MICINN, Spain [FIS2009-13364-C02-01]
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We present some approaches to the computation of ultra-fast laser pulses capable of selectively breaking molecular bonds. The calculations are based on a mixed quantum-classical description: The electrons are treated quantum mechanically (making use of time-dependent density-functional theory), whereas the nuclei are treated classically. The temporal shape of the pulses is tailored to maximize a control target functional which is designed to produce the desired molecular cleavage. The precise definition of this functional is a crucial ingredient: we explore expressions based on the forces, on the momenta and on the velocities of the nuclei. The algorithm used to find the optimum pulse is also relevant; we test both direct gradient-free algorithms, as well as schemes based on formal optimal control theory. The tests are performed both on one dimensional models of atomic chains, and on first-principles descriptions of molecules. (C) 2011 Elsevier B. V. All rights reserved.
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