Nonadiabatic quantum molecular dynamics with hopping. I. General formalism and case study

• Main Authors: Fischer, Michael, Handt, Jan, Schmidt, Rüdiger
• Other Authors: Technische Universität Dresden, Fakultät Mathematik und Naturwissenschaften
• Format: Article
• Language: English
• Published: Saechsische Landesbibliothek- Staats- und Universitaetsbibliothek Dresden 2014
• Subjects: Moleküldynamik; Quanten- und Molekulardynamik; elektronukleare Korrelation; Fallstudie; quantum molecular dynamics; hopping; case study; electronnuclear correlation; ddc:530; rvk:UA 1000
• Online Access: http://nbn-resolving.de/urn:nbn:de:bsz:14-qucosa-151703; http://nbn-resolving.de/urn:nbn:de:bsz:14-qucosa-151703; http://www.qucosa.de/fileadmin/data/qucosa/documents/15170/PhysRevA.90.012525.pdf

An extension of the nonadiabatic quantum molecular dynamics approach is presented to account for electron-nuclear correlations in the dynamics of atomic many-body systems. The method combines electron dynamics described within time-dependent density-functional or Hartree-Fock theory with trajectory-surface-hopping dynamics for the nuclei, allowing us to take into account explicitly a possible external laser field. As a case study, a model system of H++H collisions is considered where full quantum-mechanical calculations are available for comparison. For this benchmark system the extended surface-hopping scheme exactly reproduces the full quantum results. Future applications are briefly outlined.