A time-dependent excited-state molecular dynamics (TDESMD) algorithm addresses photoinduced dynamics in a lanthanide metalorganic complexes driven by a strong laser field. [1] The electronic state experiences hopping between ground state and ligand-to-metal charge-transfer (LMCT) potential energy surfaces. This provides accumulation of nuclear kinetic energy and may lead to different dynamics of interatomic distances, from small oscillations to abrupt elongations, corresponding to fragmentation of the studied compound. The TDESMD algorithm is implementd in basis of Kohn-Sham orbitals as a modification to first-principles molecular dynamics procedure. The TDESMD algorithm was used to explore photodissociation mechanisms for laser-assisted metal-organic chemical vapour deposition (MOCVD) process using lanthanide cyclopentadienyl-type precursors. The computed fragments are compared with the ones elucidated experimentally using photoionisation time-of-flight mass spectrometry.[1] J. Chen, Q. Meng, P. S. May, M. T. Berry, and D. S. Kilin, Molecular Physics (2013) in print, doi:10.1080/00268976.2013.845310The authors acknowledge the NSF/EPSCoR award EPS0903804. The computational resources of DOE, BES � Chemical Sciences, NERSC Contract No. DE-AC02-05CH11231, allocation Award 86185 'Computational Modeling of Photo-catalysis and Photoinduced Charge Transfer Dynamics on Surfaces' are gratefully acknowledged.

Computational analysis of photodissociation of lanthanide complexes for laser-assisted metal-organic chemical vapour deposition by time-dependent excited-state molecular dynamics

247th National Meeting (2014)

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.