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000005524 02470 $$ahttps://doi.org/10.1021/acs.jpclett.2c01915$$2doi
000005524 037__ $$aTEXTUAL$$bArticle
000005524 041__ $$aeng
000005524 245__ $$aPeriodic Density Matrix Embedding for CO Adsorption on the MgO(001) Surface
000005524 269__ $$a2022-08-08
000005524 336__ $$aArticle
000005524 520__ $$aThe adsorption of simple gas molecules to metal oxide surfaces is a primary step in many heterogeneous catalysis applications. Quantum chemical modeling of these reactions is a challenge in terms of both cost and accuracy, and quantum-embedding methods are promising, especially for localized chemical phenomena. In this work, we employ density matrix embedding theory (DMET) for periodic systems to calculate the adsorption energy of CO to the MgO(001) surface. Using coupled-cluster theory with single and double excitations and second-order Møller–Plesset perturbation theory as quantum chemical solvers, we perform calculations with embedding clusters up to 266 electrons in 306 orbitals, with the largest embedding models agreeing to within 1.2 kcal/mol of the non-embedding references. Moreover, we present a memory-efficient procedure of storing and manipulating electron repulsion integrals in the embedding space within the framework of periodic DMET.
000005524 536__ $$oU.S. Department of Energy$$cDE-SC0012702
000005524 536__ $$oUniversity of Minnesota$$aChemical Theory Center summer research fellowship
000005524 540__ $$a<p>Copyright © 2022 The Authors</p> <p>This work is licensed under the <a href="http://creativecommons.org/licenses/by/4.0/" target="_blank">Creative Commons Attribution License</a>.</p>
000005524 542__ $$fCC BY
000005524 690__ $$aPhysical Sciences Division
000005524 690__ $$aPritzker School of Molecular Engineering
000005524 691__ $$aChemistry
000005524 692__ $$aChicago Center for Theoretical Chemistry
000005524 692__ $$aJames Franck Institute
000005524 7001_ $$1https://orcid.org/0000-0002-2974-9600$$2ORCID$$aMitra, Abhishek$$uUniversity of Chicago
000005524 7001_ $$1https://orcid.org/0000-0001-7807-2950$$2ORCID$$aHermes, Matthew R.$$uUniversity of Chicago
000005524 7001_ $$1https://orcid.org/0000-0002-9307-8549$$2ORCID$$aCho, Minsik$$uBrown University
000005524 7001_ $$1https://orcid.org/0000-0003-2989-8013$$2ORCID$$aAgarawal, Valay$$uUniversity of Chicago
000005524 7001_ $$1https://orcid.org/0000-0001-5227-1396$$2ORCID$$aGagliardi, Laura$$uUniversity of Chicago
000005524 773__ $$tThe Journal of Physical Chemistry Letters
000005524 8564_ $$yArticle$$9b863e5e6-c0ee-46e1-9326-cd0b37926d06$$s2625156$$uhttps://knowledge.uchicago.edu/record/5524/files/Periodic-Density-Matrix-Embedding-for-CO-Adsorption-on-the-MgO-001-Surface.pdf$$ePublic
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000005524 908__ $$aI agree
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000005524 983__ $$aArticle