{"title":"核运动对光诱导双分子相互作用动力学的影响","authors":"Menghang Shi, Hao Huang, Chenxu Lu, Shengzhe Pan, Lianrong Zhou, Zhejun Jiang, Hongcheng Ni, Wenbin Zhang, Jian Wu","doi":"10.1103/physrevx.14.041001","DOIUrl":null,"url":null,"abstract":"In chemical reactions, the nuclear motion of the molecules plays a crucial role in determining the reaction rates and outcomes. Employing the cold target recoil ion momentum spectroscopy and femtosecond pump-probe techniques, we perform a molecular-level study into the influence of nuclear vibrations on light-induced bimolecular reactions within <math display=\"inline\" xmlns=\"http://www.w3.org/1998/Math/MathML\"><mrow><msub><mrow><mi mathvariant=\"normal\">H</mi></mrow><mrow><mn>2</mn></mrow></msub><mtext>−</mtext><msub><mrow><mi mathvariant=\"normal\">D</mi></mrow><mrow><mn>2</mn></mrow></msub></mrow></math> dimers. The study focuses on the formation dynamics of <math display=\"inline\" xmlns=\"http://www.w3.org/1998/Math/MathML\"><mrow><msub><mi mathvariant=\"normal\">D</mi><mn>2</mn></msub><msup><mi mathvariant=\"normal\">H</mi><mo>+</mo></msup></mrow></math> and <math display=\"inline\" xmlns=\"http://www.w3.org/1998/Math/MathML\"><mrow><msub><mi mathvariant=\"normal\">H</mi><mn>2</mn></msub><msup><mi mathvariant=\"normal\">D</mi><mo>+</mo></msup></mrow></math> cations, shedding light on the interplay between translational and vibrational motions of the nuclei steering the bimolecular reactions. Our observations reveal a notable yield ratio of <math display=\"inline\" xmlns=\"http://www.w3.org/1998/Math/MathML\"><mrow><mn>1</mn><mo>:</mo><mn>1.6</mn></mrow></math> between <math display=\"inline\" xmlns=\"http://www.w3.org/1998/Math/MathML\"><mrow><msub><mi mathvariant=\"normal\">H</mi><mn>2</mn></msub><msup><mi mathvariant=\"normal\">D</mi><mo>+</mo></msup></mrow></math> and <math display=\"inline\" xmlns=\"http://www.w3.org/1998/Math/MathML\"><mrow><msub><mi mathvariant=\"normal\">D</mi><mn>2</mn></msub><msup><mi mathvariant=\"normal\">H</mi><mo>+</mo></msup></mrow></math> channels, accompanied with a faster formation of <math display=\"inline\" xmlns=\"http://www.w3.org/1998/Math/MathML\"><mrow><msub><mi mathvariant=\"normal\">D</mi><mn>2</mn></msub><msup><mi mathvariant=\"normal\">H</mi><mo>+</mo></msup></mrow></math> compared to <math display=\"inline\" xmlns=\"http://www.w3.org/1998/Math/MathML\"><mrow><msub><mi mathvariant=\"normal\">H</mi><mn>2</mn></msub><msup><mi mathvariant=\"normal\">D</mi><mo>+</mo></msup></mrow></math>. Molecular dynamics simulations unveil that the faster vibrational motion of <math display=\"inline\" xmlns=\"http://www.w3.org/1998/Math/MathML\"><mrow><msubsup><mrow><mi mathvariant=\"normal\">H</mi></mrow><mrow><mn>2</mn></mrow><mrow><mo>+</mo></mrow></msubsup></mrow></math> than that of <math display=\"inline\" xmlns=\"http://www.w3.org/1998/Math/MathML\"><mrow><msubsup><mrow><mi mathvariant=\"normal\">D</mi></mrow><mrow><mn>2</mn></mrow><mrow><mo>+</mo></mrow></msubsup></mrow></math> upon single ionization within the dimer accounts for these differences. Our findings provide new insight into the time-resolved kinetic isotope effect on the bimolecular reactions, highlighting the critical relationship between nuclear vibrational motions and reaction dynamics.","PeriodicalId":20161,"journal":{"name":"Physical Review X","volume":null,"pages":null},"PeriodicalIF":11.6000,"publicationDate":"2024-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Impact of Nuclear Motion on Light-Induced Bimolecular Interaction Dynamics\",\"authors\":\"Menghang Shi, Hao Huang, Chenxu Lu, Shengzhe Pan, Lianrong Zhou, Zhejun Jiang, Hongcheng Ni, Wenbin Zhang, Jian Wu\",\"doi\":\"10.1103/physrevx.14.041001\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"In chemical reactions, the nuclear motion of the molecules plays a crucial role in determining the reaction rates and outcomes. Employing the cold target recoil ion momentum spectroscopy and femtosecond pump-probe techniques, we perform a molecular-level study into the influence of nuclear vibrations on light-induced bimolecular reactions within <math display=\\\"inline\\\" xmlns=\\\"http://www.w3.org/1998/Math/MathML\\\"><mrow><msub><mrow><mi mathvariant=\\\"normal\\\">H</mi></mrow><mrow><mn>2</mn></mrow></msub><mtext>−</mtext><msub><mrow><mi mathvariant=\\\"normal\\\">D</mi></mrow><mrow><mn>2</mn></mrow></msub></mrow></math> dimers. The study focuses on the formation dynamics of <math display=\\\"inline\\\" xmlns=\\\"http://www.w3.org/1998/Math/MathML\\\"><mrow><msub><mi mathvariant=\\\"normal\\\">D</mi><mn>2</mn></msub><msup><mi mathvariant=\\\"normal\\\">H</mi><mo>+</mo></msup></mrow></math> and <math display=\\\"inline\\\" xmlns=\\\"http://www.w3.org/1998/Math/MathML\\\"><mrow><msub><mi mathvariant=\\\"normal\\\">H</mi><mn>2</mn></msub><msup><mi mathvariant=\\\"normal\\\">D</mi><mo>+</mo></msup></mrow></math> cations, shedding light on the interplay between translational and vibrational motions of the nuclei steering the bimolecular reactions. Our observations reveal a notable yield ratio of <math display=\\\"inline\\\" xmlns=\\\"http://www.w3.org/1998/Math/MathML\\\"><mrow><mn>1</mn><mo>:</mo><mn>1.6</mn></mrow></math> between <math display=\\\"inline\\\" xmlns=\\\"http://www.w3.org/1998/Math/MathML\\\"><mrow><msub><mi mathvariant=\\\"normal\\\">H</mi><mn>2</mn></msub><msup><mi mathvariant=\\\"normal\\\">D</mi><mo>+</mo></msup></mrow></math> and <math display=\\\"inline\\\" xmlns=\\\"http://www.w3.org/1998/Math/MathML\\\"><mrow><msub><mi mathvariant=\\\"normal\\\">D</mi><mn>2</mn></msub><msup><mi mathvariant=\\\"normal\\\">H</mi><mo>+</mo></msup></mrow></math> channels, accompanied with a faster formation of <math display=\\\"inline\\\" xmlns=\\\"http://www.w3.org/1998/Math/MathML\\\"><mrow><msub><mi mathvariant=\\\"normal\\\">D</mi><mn>2</mn></msub><msup><mi mathvariant=\\\"normal\\\">H</mi><mo>+</mo></msup></mrow></math> compared to <math display=\\\"inline\\\" xmlns=\\\"http://www.w3.org/1998/Math/MathML\\\"><mrow><msub><mi mathvariant=\\\"normal\\\">H</mi><mn>2</mn></msub><msup><mi mathvariant=\\\"normal\\\">D</mi><mo>+</mo></msup></mrow></math>. Molecular dynamics simulations unveil that the faster vibrational motion of <math display=\\\"inline\\\" xmlns=\\\"http://www.w3.org/1998/Math/MathML\\\"><mrow><msubsup><mrow><mi mathvariant=\\\"normal\\\">H</mi></mrow><mrow><mn>2</mn></mrow><mrow><mo>+</mo></mrow></msubsup></mrow></math> than that of <math display=\\\"inline\\\" xmlns=\\\"http://www.w3.org/1998/Math/MathML\\\"><mrow><msubsup><mrow><mi mathvariant=\\\"normal\\\">D</mi></mrow><mrow><mn>2</mn></mrow><mrow><mo>+</mo></mrow></msubsup></mrow></math> upon single ionization within the dimer accounts for these differences. Our findings provide new insight into the time-resolved kinetic isotope effect on the bimolecular reactions, highlighting the critical relationship between nuclear vibrational motions and reaction dynamics.\",\"PeriodicalId\":20161,\"journal\":{\"name\":\"Physical Review X\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":11.6000,\"publicationDate\":\"2024-10-02\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Physical Review X\",\"FirstCategoryId\":\"101\",\"ListUrlMain\":\"https://doi.org/10.1103/physrevx.14.041001\",\"RegionNum\":1,\"RegionCategory\":\"物理与天体物理\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"PHYSICS, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Physical Review X","FirstCategoryId":"101","ListUrlMain":"https://doi.org/10.1103/physrevx.14.041001","RegionNum":1,"RegionCategory":"物理与天体物理","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"PHYSICS, MULTIDISCIPLINARY","Score":null,"Total":0}
Impact of Nuclear Motion on Light-Induced Bimolecular Interaction Dynamics
In chemical reactions, the nuclear motion of the molecules plays a crucial role in determining the reaction rates and outcomes. Employing the cold target recoil ion momentum spectroscopy and femtosecond pump-probe techniques, we perform a molecular-level study into the influence of nuclear vibrations on light-induced bimolecular reactions within dimers. The study focuses on the formation dynamics of and cations, shedding light on the interplay between translational and vibrational motions of the nuclei steering the bimolecular reactions. Our observations reveal a notable yield ratio of between and channels, accompanied with a faster formation of compared to . Molecular dynamics simulations unveil that the faster vibrational motion of than that of upon single ionization within the dimer accounts for these differences. Our findings provide new insight into the time-resolved kinetic isotope effect on the bimolecular reactions, highlighting the critical relationship between nuclear vibrational motions and reaction dynamics.
期刊介绍:
Physical Review X (PRX) stands as an exclusively online, fully open-access journal, emphasizing innovation, quality, and enduring impact in the scientific content it disseminates. Devoted to showcasing a curated selection of papers from pure, applied, and interdisciplinary physics, PRX aims to feature work with the potential to shape current and future research while leaving a lasting and profound impact in their respective fields. Encompassing the entire spectrum of physics subject areas, PRX places a special focus on groundbreaking interdisciplinary research with broad-reaching influence.