Adsorption of a single Pt atom on graphene: spin crossing between physisorbed triplet and chemisorbed singlet states

Ahn, Jeonghwan; Hong, Iuegyun; Lee, Gwangyoung; Shin, Hyeondeok; Benali, Anouar; Kwon, Yongkyung

doi:10.1039/d1cp02473f

Adsorption of a single Pt atom on graphene: spin crossing between physisorbed triplet and chemisorbed singlet states

Journal Article · Tue Sep 21 00:00:00 EDT 2021 · Physical Chemistry Chemical Physics. PCCP

DOI:https://doi.org/10.1039/d1cp02473f· OSTI ID:1844193

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Konkuk University, Seoul (Korea)
Argonne National Lab. (ANL), Argonne, IL (United States)

Diffusion Monte Carlo (DMC) calculations have been performed to study the adsorption of a single Pt atom on pristine graphene. In this work, we obtain the adsorption energy curves of a single Pt atom adsorbed at three different adsorption sites (bridge, on-top, hollow) as functions of the vertical distance from a graphene surface for both spin singlet and triplet states. The bridge-site adsorption in a singlet spin state is found to be energetically most stable, which is consistent with previous theoretical predictions. As the Pt atom moves away from a graphene surface, spin triplet states are favored over spin singlet states for all three adsorption sites, reflecting that the ground state of an isolated Pt atom is in a spin triplet state. Furthermore, our DMC calculations reveal local-minimum features in the triplet region which is understood to be due to van der Waals interaction between the Pt atom and graphene. This provides a comprehensive understanding for a spin crossing from a physisorbed triplet state to a chemisorbed singlet state in the adsorption process of a single Pt atom on graphene.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States). Argonne Leadership Computing Facility (ALCF)

Sponsoring Organization:: Korea Institute of Science and Technology (KIST); USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1844193

Alternate ID(s):: OSTI ID: 1822534

Journal Information:: Physical Chemistry Chemical Physics. PCCP, Journal Name: Physical Chemistry Chemical Physics. PCCP Journal Issue: 38 Vol. 23; ISSN 1463-9076

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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