Theoretical Shaping of Femtosecond Laser Pulses for Molecular Photodissociation with Control Techniques Based on Ehrenfest's Dynamics and Time-Dependent Density Functional Theory
Resumen: The combination of nonadiabatic Ehrenfest-path molecular dynamics (EMD) based on time-dependent density functional theory (TDDFT) and quantum optimal control formalism (QOCT) was used to optimize the shape of ultra-short laser pulses to achieve photodissociation of a hydrogen molecule and the trihydrogen cation H3 +. This work completes a previous one A. Castro, ChemPhysChem, 2013, 14, 1488-1495], in which the same objective was achieved by demonstrating the combination of QOCT and TDDFT for many-electron systems on static nuclear potentials. The optimization model, therefore, did not include the nuclear movement and the obtained dissociation mechanism could only be sequential: fast laser-assisted electronic excitation to nonbonding states (during which the nuclei are considered to be static), followed by field-free dissociation. Here, in contrast, the optimization was performed with the QOCT constructed on top of the full dynamic model comprised of both electrons and nuclei, as described within EMD based on TDDFT. This is the first numerical demonstration of an optimal control formalism for a hybrid quantum-classical model, that is, a molecular dynamics method.
Idioma: Inglés
DOI: 10.1002/cphc.201600077
Año: 2016
Publicado en: CHEMPHYSCHEM 17, 11 (2016), 1601-1607
ISSN: 1439-4235

Factor impacto JCR: 3.075 (2016)
Categ. JCR: PHYSICS, ATOMIC, MOLECULAR & CHEMICAL rank: 8 / 35 = 0.229 (2016) - Q1 - T1
Categ. JCR: CHEMISTRY, PHYSICAL rank: 54 / 145 = 0.372 (2016) - Q2 - T2

Factor impacto SCIMAGO: 1.284 - Physical and Theoretical Chemistry (Q1) - Atomic and Molecular Physics, and Optics (Q1)

Financiación: info:eu-repo/grantAgreement/ES/MINECO/FIS2013-46159-C2-2-P
Tipo y forma: Article (PostPrint)
Área (Departamento): Área Física Teórica (Dpto. Física Teórica)

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