Anharmonic Correction to Adsorption Free Energy from DFT-Based MD Using Thermodynamic Integration
Adsorption processes are often governed by weak interactions for which the estimation of entropy contributions by means of the harmonic approximation is prone to be inaccurate. Thermodynamic integration (TI) from the harmonic to the fully interacting system (λ-path integration) can be used to comput...
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| Veröffentlicht in: | Journal of chemical theory and computation 2021-02, Vol.17 (2), p.1155-1169 |
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| container_title | Journal of chemical theory and computation |
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| creator | Amsler, Jonas Plessow, Philipp N Studt, Felix Bučko, Tomáš |
| description | Adsorption processes are often governed by weak interactions for which the estimation of entropy contributions by means of the harmonic approximation is prone to be inaccurate. Thermodynamic integration (TI) from the harmonic to the fully interacting system (λ-path integration) can be used to compute anharmonic corrections. Here, we combine TI with (curvilinear) internal coordinates in periodic systems to make the formalism available in computational studies. Our implementation of ab initio molecular dynamics in VASP is independent of the reaction path and can be thus applied to study adsorption processes relative to the gas phase and does hence provide a useful tool for computational catalysis. We discuss the application of the approach on three model systems for which exact semianalytical solutions exist and illustrate and quantify the importance of anharmonic vibrations, hindered rotations, and hindered translations (dissociation). Eventually, we apply the method to study the adsorption of small adsorbates in a zeolite (H-SSZ-13). |
| doi_str_mv | 10.1021/acs.jctc.0c01022 |
| format | Article |
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Thermodynamic integration (TI) from the harmonic to the fully interacting system (λ-path integration) can be used to compute anharmonic corrections. Here, we combine TI with (curvilinear) internal coordinates in periodic systems to make the formalism available in computational studies. Our implementation of ab initio molecular dynamics in VASP is independent of the reaction path and can be thus applied to study adsorption processes relative to the gas phase and does hence provide a useful tool for computational catalysis. We discuss the application of the approach on three model systems for which exact semianalytical solutions exist and illustrate and quantify the importance of anharmonic vibrations, hindered rotations, and hindered translations (dissociation). 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Chem. Theory Comput</addtitle><description>Adsorption processes are often governed by weak interactions for which the estimation of entropy contributions by means of the harmonic approximation is prone to be inaccurate. Thermodynamic integration (TI) from the harmonic to the fully interacting system (λ-path integration) can be used to compute anharmonic corrections. Here, we combine TI with (curvilinear) internal coordinates in periodic systems to make the formalism available in computational studies. Our implementation of ab initio molecular dynamics in VASP is independent of the reaction path and can be thus applied to study adsorption processes relative to the gas phase and does hence provide a useful tool for computational catalysis. We discuss the application of the approach on three model systems for which exact semianalytical solutions exist and illustrate and quantify the importance of anharmonic vibrations, hindered rotations, and hindered translations (dissociation). Eventually, we apply the method to study the adsorption of small adsorbates in a zeolite (H-SSZ-13).</description><subject>Adsorbates</subject><subject>Adsorption</subject><subject>Anharmonicity</subject><subject>Condensed Matter, Interfaces, and Materials</subject><subject>Free energy</subject><subject>Molecular dynamics</subject><subject>Software</subject><subject>Translations</subject><subject>Vapor phases</subject><subject>Zeolites</subject><issn>1549-9618</issn><issn>1549-9626</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2021</creationdate><recordtype>article</recordtype><recordid>eNp1kEtPAjEURhujEUT3rkwTNy4cvO08aJfIQ0kwbmA9Ke0FhzAttsOCf28RdGHi6rbN-U7bj5BbBl0GnD0pHbpr3eguaIgH_Iy0WZ7JRBa8OP9dM9EiVyGsAdI04-klacUpOOSyTVTffihfO1tpOnDeo24qZ2njaN8E57ffu7FHpCOLfrWnS-9qOhzPkmcV0NC3IZ2Hyq7o7AOjxuytqqNqYhtceXVIX5OLpdoEvDnNDpmPR7PBazJ9f5kM-tNEpUXWJHkPmQGjMsVN2gNcLmRhtGAaZG5SqVAsdCGQZznTKDVwBDQC2KJXAJPxax3ycPRuvfvcYWjKugoaNxtl0e1CyTMBPM8LISJ6_wddu5238XWRksALyOBAwZHS3oXgcVlufVUrvy8ZlIf6y1h_eai_PNUfI3cn8W5Ro_kN_PQdgccj8B39ufRf3xeD35Ad</recordid><startdate>20210209</startdate><enddate>20210209</enddate><creator>Amsler, Jonas</creator><creator>Plessow, Philipp N</creator><creator>Studt, Felix</creator><creator>Bučko, Tomáš</creator><general>American Chemical Society</general><scope>NPM</scope><scope>AAYXX</scope><scope>CITATION</scope><scope>7SC</scope><scope>7SR</scope><scope>7U5</scope><scope>8BQ</scope><scope>8FD</scope><scope>JG9</scope><scope>JQ2</scope><scope>L7M</scope><scope>L~C</scope><scope>L~D</scope><scope>7X8</scope><orcidid>https://orcid.org/0000-0001-6841-4232</orcidid><orcidid>https://orcid.org/0000-0001-9913-4049</orcidid><orcidid>https://orcid.org/0000-0003-3112-4957</orcidid><orcidid>https://orcid.org/0000-0002-5847-9478</orcidid></search><sort><creationdate>20210209</creationdate><title>Anharmonic Correction to Adsorption Free Energy from DFT-Based MD Using Thermodynamic Integration</title><author>Amsler, Jonas ; Plessow, Philipp N ; Studt, Felix ; Bučko, Tomáš</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-a364t-57e1d0da4a2d370efb96dc81c095d39ae8bc68e2451ce9c02e0ed801b76019003</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2021</creationdate><topic>Adsorbates</topic><topic>Adsorption</topic><topic>Anharmonicity</topic><topic>Condensed Matter, Interfaces, and Materials</topic><topic>Free energy</topic><topic>Molecular dynamics</topic><topic>Software</topic><topic>Translations</topic><topic>Vapor phases</topic><topic>Zeolites</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Amsler, Jonas</creatorcontrib><creatorcontrib>Plessow, Philipp N</creatorcontrib><creatorcontrib>Studt, Felix</creatorcontrib><creatorcontrib>Bučko, Tomáš</creatorcontrib><collection>PubMed</collection><collection>CrossRef</collection><collection>Computer and Information Systems Abstracts</collection><collection>Engineered Materials Abstracts</collection><collection>Solid State and Superconductivity Abstracts</collection><collection>METADEX</collection><collection>Technology Research Database</collection><collection>Materials Research Database</collection><collection>ProQuest Computer Science Collection</collection><collection>Advanced Technologies Database with Aerospace</collection><collection>Computer and Information Systems Abstracts Academic</collection><collection>Computer and Information Systems Abstracts Professional</collection><collection>MEDLINE - Academic</collection><jtitle>Journal of chemical theory and computation</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Amsler, Jonas</au><au>Plessow, Philipp N</au><au>Studt, Felix</au><au>Bučko, Tomáš</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Anharmonic Correction to Adsorption Free Energy from DFT-Based MD Using Thermodynamic Integration</atitle><jtitle>Journal of chemical theory and computation</jtitle><addtitle>J. Chem. Theory Comput</addtitle><date>2021-02-09</date><risdate>2021</risdate><volume>17</volume><issue>2</issue><spage>1155</spage><epage>1169</epage><pages>1155-1169</pages><issn>1549-9618</issn><eissn>1549-9626</eissn><abstract>Adsorption processes are often governed by weak interactions for which the estimation of entropy contributions by means of the harmonic approximation is prone to be inaccurate. Thermodynamic integration (TI) from the harmonic to the fully interacting system (λ-path integration) can be used to compute anharmonic corrections. Here, we combine TI with (curvilinear) internal coordinates in periodic systems to make the formalism available in computational studies. Our implementation of ab initio molecular dynamics in VASP is independent of the reaction path and can be thus applied to study adsorption processes relative to the gas phase and does hence provide a useful tool for computational catalysis. 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| subjects | Adsorbates Adsorption Anharmonicity Condensed Matter, Interfaces, and Materials Free energy Molecular dynamics Software Translations Vapor phases Zeolites |
| title | Anharmonic Correction to Adsorption Free Energy from DFT-Based MD Using Thermodynamic Integration |
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