Refine
Has Fulltext
- no (63) (remove)
Year of publication
Document Type
- Article (61)
- Part of a Book (1)
- Doctoral Thesis (1)
Language
- English (63)
Is part of the Bibliography
- yes (63)
Keywords
- surface chemistry (2)
- Basis sets (1)
- Born-Oppenheimer MD (1)
- Chelates (1)
- Chemical calculations (1)
- DFT (1)
- Delta-Kohn-Sham (1)
- Electron dynamics (1)
- Ionization (1)
- Lasers (1)
Institute
We apply the multiconfiguration time-dependent Hartree-Fock method to electronic structure calculations and show that quantum chemical information can be obtained with this explicitly time-dependent approach. Different equations of motion are discussed, as well as the numerical cost. The two-electron integrals are calculated using a natural potential expansion, of which we describe the convergence behavior in detail
In this paper we report dynamical simulations of laser-driven, coupled nuclear-electron dynamics for a molecule- surface system. Specifically, the laser desorption of a small molecule (NO) from a metal slab (Pt) in the so-called DIET limit (Desorption Induced by Electronic Transitions), is studied. The excitation of the metal electrons by a laser pulse followed by the formation of a negative ion resonance, its subsequent decay, and the simultaneous desorption of the molecule are all treated within a single quantum mechanical model. This model is based on an earlier theory of Harris and others [S. M. Harris, S. Holloway, and G. R. Darling, J. Chem. Phys. 102, 8235 (1995)], according to which a nuclear degree of freedom is coupled to an electronic one, both propagated on a single non-Born-Oppenheimer potential energy surface. The goals of the present contribution are (i) to make a conceptual connection of this model to the frequently adopted nonadiabatic "multi-state" models of photodesorption, (ii) to understand details of the desorption mechanism, (iii) to explicitly account for the laser pulse, and (iv) to study the photodesorption as a function of the thickness of the metal film, and the laser parameters. As an important methodological aspect we also present a highly efficient numerical scheme to propagate the wave packet in a problem-adapted diabatic basis
In this paper we report time-dependent configuration interaction singles calculations modeling the laser- induced current through a metal-insulator-metal (MIM) contact. We compare our results to recent experiments [D. Diesing, M. Merschdorf, A. Thon, and W. Pfeiffer, Appl. Phys. B (to be published)]. We use two jellium slabs separated by a vacuum region in a one-dimensional model to describe the MIM contact. The contact is coupled to ultrashort (fs) laser pulses by the semiclassical dipole approximation. We discuss simulated two-pulse correlation spectra in comparison to experimental results