Eur. Phys. J. D 28, 211-218 (2004)
https://doi.org/10.1140/epjd/e2003-00306-3

Excited states dynamics in time-dependent density functional theory

High-field molecular dissociation and harmonic generation

¹ Departamento de Física Teórica, Universidad de Valladolid, 47011 Valladolid, Spain
² Donostia International Physics Centre (DIPC), 20018 San Sebastián, Spain
³ Physics Department and Institute for Nuclear Theory, University of Washington, Seattle WA 98195, USA
⁴ Institut für Theoretische Physik, Freie Universität Berlin, 14175 Berlin, Germany
⁵ Departamento de Física de Materiales and Centro Mixto CSIC-UPV/EHU, Facultad de Químicas, Universidad del País Vasco, 20018 San Sebastián, Spain

Corresponding author: ^a alberto.castro@tddft.org

Received: 22 January 2003
Revised: 15 October 2003
Published online: 2 December 2003

Abstract

We present numerical simulations of femtosecond laser induced dynamics of some selected simple molecules — hydrogen, singly ionized sodium dimer, singly ionized helium trimer and lithium cyanide. The simulations were performed within a real-space, real-time, implementation of time-dependent density functional theory (TDDFT). High harmonic generation, Coulomb explosion and laser induced photo-dissociation are observed. The scheme also describes non-adiabatic effects, such as the appearance of even harmonics for homopolar but isotopically asymmetric dimers, even if the ions are treated classically. This TDDFT-based method is reliable, scalable, and extensible to other phenomena such as photoisomerization, molecular transport and chemical reactivity.