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Henrik R. Larsson

Publications and source records attributed to Henrik R. Larsson.

21 records · Page 2Linked to original sources

Efficient molecular quantum dynamics in coordinate and phase space using pruned bases

We present an efficient implementation of dynamically pruned quantum dynamics, both in coordinate space and in phase space. We combine the ideas behind the biorthogonal von Neumann basis (PvB) with the orthogonalized momentum-symmetrized Gaussians (Weylets) to create a new basis, projected Weylets, that takes the best from both methods. We benchmark pruned dynamics using phase-space-localized PvB, projected Weylets, and coordinate-space-localized DVR bases, with real-world examples in up to six dimensions. We show that coordinate-space localization is most important for efficient pruning and that pruned dynamics is much faster compared to unpruned, exact dynamics. Phase-space localization is useful for more demanding dynamics where many basis functions are required. There, projected Weylets offer a more compact representation than pruned DVR bases.

physics.chem-ph↗

Quantum Dynamics in Phase Space using Projected von Neumann Bases

We describe the mathematical underpinnings of the biorthogonal von Neumann method for quantum mechanical simulations (PvB). In particular, we present a detailed discussion of the important issue of non-orthogonal projection onto subspaces of biorthogonal bases, and how this differs from orthogonal projection. We present various representations of the Schrödinger equation in the reduced basis and discuss their relative merits. We conclude with illustrative examples and a discussion of the outlook and challenges ahead for the PvB representation.

quant-ph↗

Correlation effects in strong-field ionization of heteronuclear diatomic molecules

We develop a time-dependent theory to investigate electron dynamics and photoionization processes of diatomic molecules interacting with strong laser fields including electron-electron correlation effects. We combine the recently formulated time-dependent generalized-active-space configuration interaction theory [D. Hochstuhl and M. Bonitz, Phys. Rev. A 86, 053424 (2012); S. Bauch, et al., Phys. Rev. A 90, 062508 (2014)] with a prolate spheroidal basis set including localized orbitals and continuum states to describe the bound electrons and the outgoing photoelectron. As an example, we study the strong-field ionization of the two-center four-electron lithium hydride molecule in different intensity regimes. By using single-cycle pulses, two orientations of the asymmetric heteronuclear molecule are investigated: Li-H, with the electrical field pointing from H to Li, and the opposite case of H-Li. The preferred orientation for ionization is determined and we find a transition from H-Li, for low intensity, to Li-H, for high intensity. The influence of electron correlations is studied at different levels of approximation, and we find a significant change in the preferred orientation. For certain intensity regimes, even an interchange of the preferred configuration is observed, relative to the uncorrelated simulations. Further insight is provided by detailed comparisons of photoelectron angular distributions with and without correlation effects taken into account.

physics.chem-ph↗