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 4 He/graphene by determining the energies of the low-lying selective adsorption states, finding an excellent agreement with the best available the- oretical 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 4 He droplets with a single graphene sheet. It is found that dispersion effects play a key role in the fast spreading of the 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.

Communication: A combined periodic density functional and incremental wave-function-based approach for the dispersion-accounting time-resolved dynamics of 4He nanodroplets on surfaces: 4He/graphene

CIVALLERI, Bartolomeo;
2014-01-01

Abstract

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 4 He/graphene by determining the energies of the low-lying selective adsorption states, finding an excellent agreement with the best available the- oretical 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 4 He droplets with a single graphene sheet. It is found that dispersion effects play a key role in the fast spreading of the 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.
2014
141
151102-1
151102-5
María Pilar de Lara-Castells;Hermann Stoll;Bartolomeo Civalleri;Mauro Causà;Elena Voloshina;Alexander O. Mitrushchenkov;Martí Pi...espandi
File in questo prodotto:
File Dimensione Formato  
he-graphene_delara-castells_jcp2014.pdf

Accesso aperto

Tipo di file: POSTPRINT (VERSIONE FINALE DELL’AUTORE)
Dimensione 930.08 kB
Formato Adobe PDF
930.08 kB Adobe PDF Visualizza/Apri
he-graphene_delara-castells_jcp2014_supp.pdf

Accesso aperto

Tipo di file: POSTPRINT (VERSIONE FINALE DELL’AUTORE)
Dimensione 39.63 kB
Formato Adobe PDF
39.63 kB Adobe PDF Visualizza/Apri

I documenti in IRIS sono protetti da copyright e tutti i diritti sono riservati, salvo diversa indicazione.

Utilizza questo identificativo per citare o creare un link a questo documento: https://hdl.handle.net/2318/157862
Citazioni
  • ???jsp.display-item.citation.pmc??? ND
  • Scopus 35
  • ???jsp.display-item.citation.isi??? 36
social impact