New Potential Energy Surface for the H + Cl 2 Reaction and Quantum Dynamics Studies
The reaction of H + Cl → HCl + Cl plays a crucial role in various fields. However, no previous study has investigated this reaction using accurate quantum mechanical methods. In this paper, we construct a global potential energy surface (PES) using the neural network method with more than 20,000 ene...
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| Veröffentlicht in: | The journal of physical chemistry. A, Molecules, spectroscopy, kinetics, environment, & general theory Molecules, spectroscopy, kinetics, environment, & general theory, 2024-06, Vol.128 (22), p.4425-4438 |
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| container_title | The journal of physical chemistry. A, Molecules, spectroscopy, kinetics, environment, & general theory |
| container_volume | 128 |
| creator | Chang, Hanwen Li, Wentao Sun, Zhigang |
| description | The reaction of H + Cl
→ HCl + Cl plays a crucial role in various fields. However, no previous study has investigated this reaction using accurate quantum mechanical methods. In this paper, we construct a global potential energy surface (PES) using the neural network method with more than 20,000
energies obtained by the MRCI-F12+Q method with the aug-cc-pV5Z basis and extrapolated to the complete basis set limit. The spin-orbit coupling of the Cl atom has been considered in the PES. With this new PES, product state-resolved quantum dynamics calculations for the H + Cl
(
= 0,
= 0-2) → HCl + Cl reaction was carried out. Numerical results show that the initial rotational excitation of the Cl
has negligible effects on the reactivity. Product state-resolved integral cross sections (ICS) and rate constants reveal that the HCl is most favorably produced in its
' = 2 vibrational state. The calculated product vibrational state-resolved and total reaction rate constants suggest that the new global PES is accurate enough, as compared with the available experimental measurements. |
| doi_str_mv | 10.1021/acs.jpca.4c00542 |
| format | Article |
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→ HCl + Cl plays a crucial role in various fields. However, no previous study has investigated this reaction using accurate quantum mechanical methods. In this paper, we construct a global potential energy surface (PES) using the neural network method with more than 20,000
energies obtained by the MRCI-F12+Q method with the aug-cc-pV5Z basis and extrapolated to the complete basis set limit. The spin-orbit coupling of the Cl atom has been considered in the PES. With this new PES, product state-resolved quantum dynamics calculations for the H + Cl
(
= 0,
= 0-2) → HCl + Cl reaction was carried out. Numerical results show that the initial rotational excitation of the Cl
has negligible effects on the reactivity. Product state-resolved integral cross sections (ICS) and rate constants reveal that the HCl is most favorably produced in its
' = 2 vibrational state. The calculated product vibrational state-resolved and total reaction rate constants suggest that the new global PES is accurate enough, as compared with the available experimental measurements.</description><identifier>ISSN: 1089-5639</identifier><identifier>EISSN: 1520-5215</identifier><identifier>DOI: 10.1021/acs.jpca.4c00542</identifier><identifier>PMID: 38805307</identifier><language>eng</language><publisher>United States</publisher><ispartof>The journal of physical chemistry. A, Molecules, spectroscopy, kinetics, environment, & general theory, 2024-06, Vol.128 (22), p.4425-4438</ispartof><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><cites>FETCH-LOGICAL-c647-f6b8c36e83298ebe26dfc5e12612cc0d742ad22e5bd254a52e2a5c9114da1a003</cites><orcidid>0000-0002-6600-4923</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><link.rule.ids>314,776,780,2752,27901,27902</link.rule.ids><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/38805307$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink></links><search><creatorcontrib>Chang, Hanwen</creatorcontrib><creatorcontrib>Li, Wentao</creatorcontrib><creatorcontrib>Sun, Zhigang</creatorcontrib><title>New Potential Energy Surface for the H + Cl 2 Reaction and Quantum Dynamics Studies</title><title>The journal of physical chemistry. A, Molecules, spectroscopy, kinetics, environment, & general theory</title><addtitle>J Phys Chem A</addtitle><description>The reaction of H + Cl
→ HCl + Cl plays a crucial role in various fields. However, no previous study has investigated this reaction using accurate quantum mechanical methods. In this paper, we construct a global potential energy surface (PES) using the neural network method with more than 20,000
energies obtained by the MRCI-F12+Q method with the aug-cc-pV5Z basis and extrapolated to the complete basis set limit. The spin-orbit coupling of the Cl atom has been considered in the PES. With this new PES, product state-resolved quantum dynamics calculations for the H + Cl
(
= 0,
= 0-2) → HCl + Cl reaction was carried out. Numerical results show that the initial rotational excitation of the Cl
has negligible effects on the reactivity. Product state-resolved integral cross sections (ICS) and rate constants reveal that the HCl is most favorably produced in its
' = 2 vibrational state. The calculated product vibrational state-resolved and total reaction rate constants suggest that the new global PES is accurate enough, as compared with the available experimental measurements.</description><issn>1089-5639</issn><issn>1520-5215</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2024</creationdate><recordtype>article</recordtype><recordid>eNo90E9PwkAQhvGN0Yiid09m76Y4O9st7dEgignxH9yb6e5US2hLdtsYvr0Q0NPM5XkPPyFuFIwUoLonG0arjaVRbAFMjCfiQhmEyKAyp7sf0iwyic4G4jKEFQAojfG5GOg0BaNhfCEWr_wj39uOm66itZw27L-2ctH7kizLsvWy-2Y5k3dyspYoP5lsV7WNpMbJj56arq_l47ahurJBLrreVRyuxFlJ68DXxzsUy6fpcjKL5m_PL5OHeWSTeByVSZFanXCqMUu5YExcaQ0rTBRaC24cIzlENoVDE5NBRjI2Uyp2pAhADwUcZq1vQ_Bc5htf1eS3uYJ8z5PvePI9T37k2SW3h2TTFzW7_-DPQ_8C7cJhdg</recordid><startdate>20240606</startdate><enddate>20240606</enddate><creator>Chang, Hanwen</creator><creator>Li, Wentao</creator><creator>Sun, Zhigang</creator><scope>NPM</scope><scope>AAYXX</scope><scope>CITATION</scope><orcidid>https://orcid.org/0000-0002-6600-4923</orcidid></search><sort><creationdate>20240606</creationdate><title>New Potential Energy Surface for the H + Cl 2 Reaction and Quantum Dynamics Studies</title><author>Chang, Hanwen ; Li, Wentao ; Sun, Zhigang</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c647-f6b8c36e83298ebe26dfc5e12612cc0d742ad22e5bd254a52e2a5c9114da1a003</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2024</creationdate><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Chang, Hanwen</creatorcontrib><creatorcontrib>Li, Wentao</creatorcontrib><creatorcontrib>Sun, Zhigang</creatorcontrib><collection>PubMed</collection><collection>CrossRef</collection><jtitle>The journal of physical chemistry. A, Molecules, spectroscopy, kinetics, environment, & general theory</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Chang, Hanwen</au><au>Li, Wentao</au><au>Sun, Zhigang</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>New Potential Energy Surface for the H + Cl 2 Reaction and Quantum Dynamics Studies</atitle><jtitle>The journal of physical chemistry. A, Molecules, spectroscopy, kinetics, environment, & general theory</jtitle><addtitle>J Phys Chem A</addtitle><date>2024-06-06</date><risdate>2024</risdate><volume>128</volume><issue>22</issue><spage>4425</spage><epage>4438</epage><pages>4425-4438</pages><issn>1089-5639</issn><eissn>1520-5215</eissn><abstract>The reaction of H + Cl
→ HCl + Cl plays a crucial role in various fields. However, no previous study has investigated this reaction using accurate quantum mechanical methods. In this paper, we construct a global potential energy surface (PES) using the neural network method with more than 20,000
energies obtained by the MRCI-F12+Q method with the aug-cc-pV5Z basis and extrapolated to the complete basis set limit. The spin-orbit coupling of the Cl atom has been considered in the PES. With this new PES, product state-resolved quantum dynamics calculations for the H + Cl
(
= 0,
= 0-2) → HCl + Cl reaction was carried out. Numerical results show that the initial rotational excitation of the Cl
has negligible effects on the reactivity. Product state-resolved integral cross sections (ICS) and rate constants reveal that the HCl is most favorably produced in its
' = 2 vibrational state. The calculated product vibrational state-resolved and total reaction rate constants suggest that the new global PES is accurate enough, as compared with the available experimental measurements.</abstract><cop>United States</cop><pmid>38805307</pmid><doi>10.1021/acs.jpca.4c00542</doi><tpages>14</tpages><orcidid>https://orcid.org/0000-0002-6600-4923</orcidid></addata></record> |
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| ispartof | The journal of physical chemistry. A, Molecules, spectroscopy, kinetics, environment, & general theory, 2024-06, Vol.128 (22), p.4425-4438 |
| issn | 1089-5639 1520-5215 |
| language | eng |
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| source | American Chemical Society Publications |
| title | New Potential Energy Surface for the H + Cl 2 Reaction and Quantum Dynamics Studies |
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