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Title: Framework for scalable adsorbate–adsorbate interaction models

Abstract

Here, we present a framework for physically motivated models of adsorbate–adsorbate interaction between small molecules on transition and coinage metals based on modifications to the substrate electronic structure due to adsorption. We use this framework to develop one model for transition and one for coinage metal surfaces. The models for transition metals are based on the d-band center position, and the models for coinage metals are based on partial charges. The models require no empirical parameters, only two first-principles calculations per adsorbate as input, and therefore scale linearly with the number of reaction intermediates. By theory to theory comparison with explicit density functional theory calculations over a wide range of adsorbates and surfaces, we show that the root-mean-squared error for differential adsorption energies is less than 0.2 eV for up to 1 ML coverage.

Authors:
 [1];  [1];  [1]
  1. Stanford Univ., Stanford, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1349405
Grant/Contract Number:  
AC02-76SF00515
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. C
Additional Journal Information:
Journal Volume: 120; Journal Issue: 24; Journal ID: ISSN 1932-7447
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE

Citation Formats

Hoffmann, Max J., Medford, Andrew J., and Bligaard, Thomas. Framework for scalable adsorbate–adsorbate interaction models. United States: N. p., 2016. Web. https://doi.org/10.1021/acs.jpcc.6b03375.
Hoffmann, Max J., Medford, Andrew J., & Bligaard, Thomas. Framework for scalable adsorbate–adsorbate interaction models. United States. https://doi.org/10.1021/acs.jpcc.6b03375
Hoffmann, Max J., Medford, Andrew J., and Bligaard, Thomas. Thu . "Framework for scalable adsorbate–adsorbate interaction models". United States. https://doi.org/10.1021/acs.jpcc.6b03375. https://www.osti.gov/servlets/purl/1349405.
@article{osti_1349405,
title = {Framework for scalable adsorbate–adsorbate interaction models},
author = {Hoffmann, Max J. and Medford, Andrew J. and Bligaard, Thomas},
abstractNote = {Here, we present a framework for physically motivated models of adsorbate–adsorbate interaction between small molecules on transition and coinage metals based on modifications to the substrate electronic structure due to adsorption. We use this framework to develop one model for transition and one for coinage metal surfaces. The models for transition metals are based on the d-band center position, and the models for coinage metals are based on partial charges. The models require no empirical parameters, only two first-principles calculations per adsorbate as input, and therefore scale linearly with the number of reaction intermediates. By theory to theory comparison with explicit density functional theory calculations over a wide range of adsorbates and surfaces, we show that the root-mean-squared error for differential adsorption energies is less than 0.2 eV for up to 1 ML coverage.},
doi = {10.1021/acs.jpcc.6b03375},
journal = {Journal of Physical Chemistry. C},
number = 24,
volume = 120,
place = {United States},
year = {2016},
month = {6}
}

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