A General Route to Include Pauli Repulsion and Quantum Dispersion Effects in QM/MM Approaches
A methodology to account for nonelectrostatic interactions in Quantum Mechanical (QM)/Molecular Mechanics (MM) approaches is developed. Formulations for Pauli repulsion and dispersion energy, explicitly depending on the QM density, are derived. Such expressions are based on the definition of an auxi...
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| Veröffentlicht in: | Journal of chemical theory and computation 2017-10, Vol.13 (10), p.4854-4870 |
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| container_end_page | 4870 |
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| container_issue | 10 |
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| container_title | Journal of chemical theory and computation |
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| creator | Giovannini, Tommaso Lafiosca, Piero Cappelli, Chiara |
| description | A methodology to account for nonelectrostatic interactions in Quantum Mechanical (QM)/Molecular Mechanics (MM) approaches is developed. Formulations for Pauli repulsion and dispersion energy, explicitly depending on the QM density, are derived. Such expressions are based on the definition of an auxiliary density on the MM portion and the Tkatchenko–Scheffler (TS) approach, respectively. The developed method is general enough to be applied to any QM/MM method and partition, provided an accurate tuning of a small number of parameters is obtained. The coupling of the method with both nonpolarizable and fully polarizable QM/fluctuating charge (FQ) approaches is reported and applied. A suitable parametrization for the aqueous solution, so that its most representative features are well reproduced, is outlined. Then, the obtained parametrization and method are applied to calculate the nonelectrostatic (repulsion and dispersion) interaction energy of nicotine in aqueous solution. |
| doi_str_mv | 10.1021/acs.jctc.7b00776 |
| format | Article |
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Formulations for Pauli repulsion and dispersion energy, explicitly depending on the QM density, are derived. Such expressions are based on the definition of an auxiliary density on the MM portion and the Tkatchenko–Scheffler (TS) approach, respectively. The developed method is general enough to be applied to any QM/MM method and partition, provided an accurate tuning of a small number of parameters is obtained. The coupling of the method with both nonpolarizable and fully polarizable QM/fluctuating charge (FQ) approaches is reported and applied. A suitable parametrization for the aqueous solution, so that its most representative features are well reproduced, is outlined. Then, the obtained parametrization and method are applied to calculate the nonelectrostatic (repulsion and dispersion) interaction energy of nicotine in aqueous solution.</description><identifier>ISSN: 1549-9618</identifier><identifier>EISSN: 1549-9626</identifier><identifier>DOI: 10.1021/acs.jctc.7b00776</identifier><identifier>PMID: 28898079</identifier><language>eng</language><publisher>United States: American Chemical Society</publisher><subject>Aqueous solutions ; Coupling (molecular) ; Dispersion ; Formulations ; Mathematical analysis ; Molecular chains ; Nicotine ; Parameterization ; Quantum mechanics ; Variations</subject><ispartof>Journal of chemical theory and computation, 2017-10, Vol.13 (10), p.4854-4870</ispartof><rights>Copyright © 2017 American Chemical Society</rights><rights>Copyright American Chemical Society Oct 10, 2017</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-a364t-af77ff1b17b68dbd352aad7adc83a682df95be26c7baac43095c1590f9a994053</citedby><cites>FETCH-LOGICAL-a364t-af77ff1b17b68dbd352aad7adc83a682df95be26c7baac43095c1590f9a994053</cites><orcidid>0000-0002-5637-2853 ; 0000-0002-4872-4505</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktopdf>$$Uhttps://pubs.acs.org/doi/pdf/10.1021/acs.jctc.7b00776$$EPDF$$P50$$Gacs$$H</linktopdf><linktohtml>$$Uhttps://pubs.acs.org/doi/10.1021/acs.jctc.7b00776$$EHTML$$P50$$Gacs$$H</linktohtml><link.rule.ids>315,781,785,2766,27080,27928,27929,56742,56792</link.rule.ids><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/28898079$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink></links><search><creatorcontrib>Giovannini, Tommaso</creatorcontrib><creatorcontrib>Lafiosca, Piero</creatorcontrib><creatorcontrib>Cappelli, Chiara</creatorcontrib><title>A General Route to Include Pauli Repulsion and Quantum Dispersion Effects in QM/MM Approaches</title><title>Journal of chemical theory and computation</title><addtitle>J. Chem. Theory Comput</addtitle><description>A methodology to account for nonelectrostatic interactions in Quantum Mechanical (QM)/Molecular Mechanics (MM) approaches is developed. Formulations for Pauli repulsion and dispersion energy, explicitly depending on the QM density, are derived. Such expressions are based on the definition of an auxiliary density on the MM portion and the Tkatchenko–Scheffler (TS) approach, respectively. The developed method is general enough to be applied to any QM/MM method and partition, provided an accurate tuning of a small number of parameters is obtained. The coupling of the method with both nonpolarizable and fully polarizable QM/fluctuating charge (FQ) approaches is reported and applied. A suitable parametrization for the aqueous solution, so that its most representative features are well reproduced, is outlined. Then, the obtained parametrization and method are applied to calculate the nonelectrostatic (repulsion and dispersion) interaction energy of nicotine in aqueous solution.</description><subject>Aqueous solutions</subject><subject>Coupling (molecular)</subject><subject>Dispersion</subject><subject>Formulations</subject><subject>Mathematical analysis</subject><subject>Molecular chains</subject><subject>Nicotine</subject><subject>Parameterization</subject><subject>Quantum mechanics</subject><subject>Variations</subject><issn>1549-9618</issn><issn>1549-9626</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2017</creationdate><recordtype>article</recordtype><recordid>eNp1kDtPwzAURi0EoqWwMyFLLAy09SOJ47EqpVRqBa1gRNaNY4tUaRLieODfkz4HJCZb1vm-e30QuqVkQAmjQ9BusNaNHoiEECGiM9SlYSD7MmLR-elO4w66cm5NCOcB45eow-JYxkTILvoc4akpTA05XpW-Mbgp8azQuU8NfgOfZ3hlKp-7rCwwFCleeigav8FPmatMvXueWGt043BW4OViuFjgUVXVJegv467RhYXcmZvD2UMfz5P38Ut__jqdjUfzPvAoaPpghbCWJlQkUZwmKQ8ZQCog1TGHKGaplWFiWKRFAqADTmSoaSiJlSBlQELeQw_73nbwtzeuUZvMaZPnUJjSO0Ulj6P2-zRo0fs_6Lr0ddFupxgJGOM0ZLylyJ7Sdelcbayq6mwD9Y-iRG3Vq1a92qpXB_Vt5O5Q7JONSU-Bo-sWeNwDu-hx6L99v88ljuQ</recordid><startdate>20171010</startdate><enddate>20171010</enddate><creator>Giovannini, Tommaso</creator><creator>Lafiosca, Piero</creator><creator>Cappelli, Chiara</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/0000-0002-5637-2853</orcidid><orcidid>https://orcid.org/0000-0002-4872-4505</orcidid></search><sort><creationdate>20171010</creationdate><title>A General Route to Include Pauli Repulsion and Quantum Dispersion Effects in QM/MM Approaches</title><author>Giovannini, Tommaso ; Lafiosca, Piero ; Cappelli, Chiara</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-a364t-af77ff1b17b68dbd352aad7adc83a682df95be26c7baac43095c1590f9a994053</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2017</creationdate><topic>Aqueous solutions</topic><topic>Coupling (molecular)</topic><topic>Dispersion</topic><topic>Formulations</topic><topic>Mathematical analysis</topic><topic>Molecular chains</topic><topic>Nicotine</topic><topic>Parameterization</topic><topic>Quantum mechanics</topic><topic>Variations</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Giovannini, Tommaso</creatorcontrib><creatorcontrib>Lafiosca, Piero</creatorcontrib><creatorcontrib>Cappelli, Chiara</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>Giovannini, Tommaso</au><au>Lafiosca, Piero</au><au>Cappelli, Chiara</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>A General Route to Include Pauli Repulsion and Quantum Dispersion Effects in QM/MM Approaches</atitle><jtitle>Journal of chemical theory and computation</jtitle><addtitle>J. Chem. Theory Comput</addtitle><date>2017-10-10</date><risdate>2017</risdate><volume>13</volume><issue>10</issue><spage>4854</spage><epage>4870</epage><pages>4854-4870</pages><issn>1549-9618</issn><eissn>1549-9626</eissn><abstract>A methodology to account for nonelectrostatic interactions in Quantum Mechanical (QM)/Molecular Mechanics (MM) approaches is developed. Formulations for Pauli repulsion and dispersion energy, explicitly depending on the QM density, are derived. Such expressions are based on the definition of an auxiliary density on the MM portion and the Tkatchenko–Scheffler (TS) approach, respectively. The developed method is general enough to be applied to any QM/MM method and partition, provided an accurate tuning of a small number of parameters is obtained. The coupling of the method with both nonpolarizable and fully polarizable QM/fluctuating charge (FQ) approaches is reported and applied. A suitable parametrization for the aqueous solution, so that its most representative features are well reproduced, is outlined. Then, the obtained parametrization and method are applied to calculate the nonelectrostatic (repulsion and dispersion) interaction energy of nicotine in aqueous solution.</abstract><cop>United States</cop><pub>American Chemical Society</pub><pmid>28898079</pmid><doi>10.1021/acs.jctc.7b00776</doi><tpages>17</tpages><orcidid>https://orcid.org/0000-0002-5637-2853</orcidid><orcidid>https://orcid.org/0000-0002-4872-4505</orcidid></addata></record> |
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| source | American Chemical Society Journals |
| subjects | Aqueous solutions Coupling (molecular) Dispersion Formulations Mathematical analysis Molecular chains Nicotine Parameterization Quantum mechanics Variations |
| title | A General Route to Include Pauli Repulsion and Quantum Dispersion Effects in QM/MM Approaches |
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