Communication: A combined periodic density functional and incremental wave-function-based approach for the dispersion-accounting time-resolved dynamics of {sup 4}He nanodroplets on surfaces: {sup 4}He/graphene
- Institut für Theoretische Chemie, Universität Stuttgart, D-70550 Stuttgart (Germany)
- Dipartimento di Chimica e Centro Interdipartimentale NIS, Universitá di Torino, Via P. Giuria 7, 10125 Torino (Italy)
- Dipartimento di Ingegneria Chimica, dei Materiali e delle Produzioni Industriali, Universiá di Napoli Federico II, Piazzale Tecchio, 80126 Napoli (Italy)
- Humboldt-Universität zu Berlin, Institut für Chemie, Brook-Taylor-Str. 2, 12489 Berlin (Germany)
- Université Paris-Est, Laboratoire Modélisation et Simulation Multi Echelle, MSME UMR 8208 CNRS, 5 bd Descartes, 77454 Marne-la-Vallée (France)
- Department ECM, Facultat de Física, and IN"2UB, Universitat de Barcelona, Diagonal 645, E-08028 Barcelona (Spain)
In this work we propose a general strategy to calculate accurate He–surface interaction potentials. It extends the dispersionless density functional approach recently developed by Pernal et al. [Phys. Rev. Lett. 103, 263201 (2009)] to adsorbate-surface interactions by including periodic boundary conditions. We also introduce a scheme to parametrize the dispersion interaction by calculating two- and three-body dispersion terms at coupled cluster singles and doubles and perturbative triples (CCSD(T)) level via the method of increments [H. Stoll, J. Chem. Phys. 97, 8449 (1992)]. The performance of the composite approach is tested on {sup 4}He/graphene by determining the energies of the low-lying selective adsorption states, finding an excellent agreement with the best available theoretical data. Second, the capability of the approach to describe dispersionless correlation effects realistically is used to extract dispersion effects in time-dependent density functional simulations on the collision of {sup 4}He droplets with a single graphene sheet. It is found that dispersion effects play a key role in the fast spreading of the {sup 4}He nanodroplet, the evaporation-like process of helium atoms, and the formation of solid-like helium structures. These characteristics are expected to be quite general and highly relevant to explain experimental measurements with the newly developed helium droplet mediated deposition technique.
- OSTI ID:
- 22436593
- Journal Information:
- Journal of Chemical Physics, Vol. 141, Issue 15; Other Information: (c) 2014 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA); ISSN 0021-9606
- Country of Publication:
- United States
- Language:
- English
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