Efficient hierarchical models for reactivity of organic layers on semiconductor surfaces.

density functional theory hybrid organic-inorganic materials interfaces model hierarchy semiconductor functionalization

Journal

Journal of computational chemistry
ISSN: 1096-987X
Titre abrégé: J Comput Chem
Pays: United States
ID NLM: 9878362

Informations de publication

Date de publication:
05 May 2021
Historique:
revised: 20 01 2021
received: 14 12 2020
accepted: 03 02 2021
pubmed: 23 2 2021
medline: 23 2 2021
entrez: 22 2 2021
Statut: ppublish

Résumé

Computational modeling of organic interface formation on semiconductors poses a challenge to a density functional theory-based description due to structural and chemical complexity. A hierarchical approach is presented, where parts of the interface are successively removed in order to increase computational efficiency while maintaining the necessary accuracy. First, a benchmark is performed to probe the validity of this approach for three model reactions and five dispersion corrected density functionals. Reaction energies are generally well reproduced by generalized gradient approximation-type functionals but accurate reaction barriers require the use of hybrid functionals. Best performance is found for the model system that does not explicitly consider the substrate but includes its templating effects. Finally, this efficient model is used to provide coverage dependent reaction energies and suggest synthetic principles for the prevention of unwanted growth termination reactions for organic layers on semiconductor surfaces.

Identifiants

pubmed: 33617671
doi: 10.1002/jcc.26503
doi:

Types de publication

Journal Article

Langues

eng

Sous-ensembles de citation

IM

Pagination

827-839

Subventions

Organisme : German Research Foundation (DFG)
ID : SFB 1083

Informations de copyright

© 2021 The Authors. Journal of Computational Chemistry published by Wiley Periodicals LLC.

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Auteurs

Jan-Niclas Luy (JN)

Fachbereich Chemie, Philipps-Universität Marburg, Marburg, Germany.
Wilhelm-Ostwald-Institut für Physikalische und Theoretische Chemie, Universität Leipzig, Linnéstraße 2, Leipzig, Germany.

Mahlet Molla (M)

Fachbereich Chemie, Philipps-Universität Marburg, Marburg, Germany.

Lisa Pecher (L)

Fachbereich Chemie, Philipps-Universität Marburg, Marburg, Germany.

Ralf Tonner (R)

Fachbereich Chemie, Philipps-Universität Marburg, Marburg, Germany.
Wilhelm-Ostwald-Institut für Physikalische und Theoretische Chemie, Universität Leipzig, Linnéstraße 2, Leipzig, Germany.

Classifications MeSH