Nonempirical Meta-Generalized Gradient Approximations for Modeling Chemisorption at Metal Surfaces

Garza, Alejandro J.; Bell, Alexis T.; Head-Gordon, Martin

doi:10.1021/acs.jctc.8b00288

Nonempirical Meta-Generalized Gradient Approximations for Modeling Chemisorption at Metal Surfaces

Journal Article · Thu May 10 00:00:00 EDT 2018 · Journal of Chemical Theory and Computation

DOI:https://doi.org/10.1021/acs.jctc.8b00288· OSTI ID:1477305

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Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Univ. of California, Berkeley, CA (United States)

We assess the accuracy of popular nonempirical GGAs (PBE, PBEsol, RPBE) and meta-GGAs (TPSS, revTPSS, and SCAN) for describing chemisorption reactions at metal surfaces. Except for RPBE, all the functionals tend to overbind the adsorbate significantly. We then propose a nonempirical meta-GGA, denoted as RTPSS, that is based on RPBE in the same way that TPSS is based on PBE. The RTPSS functional remedies the overbinding problem and improves the description of chemisorption energies. As an example of an application of RTPSS, we study the adsorption of CO on Cu surfaces (a notably difficult problem for semilocal functionals) and find that RTPSS is the only tested functional that predicts accurate chemisorption energies and the preferred adsorption site of CO. Although RTPSS gives an accurate description of chemisorption, nonlocal correlation may be necessary to describe physisorption if long-range van der Waals interactions are involved (however, this is true for semilocal functionals in general). We suggest that RTPSS can be a useful meta-GGA for studying chemisorption processes and mechanisms of heterogeneous catalysis.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22), Chemical Sciences, Geosciences & Biosciences Division (SC-22.1)

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1477305

Journal Information:: Journal of Chemical Theory and Computation, Journal Name: Journal of Chemical Theory and Computation Journal Issue: 6 Vol. 14; ISSN 1549-9618

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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