Revealing umbrella bending as a reporter mode in the D+CH4 reaction

Abstract How the non-reacting moiety of a molecule influences a polyatomic reaction has been a topic of much research interest. Here we present a comprehensive investigation of the D + CH4 → HD + CH3 reaction, a benchmark polyatomic elementary reaction with CH3 as the non-reacting moiety, employing...

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Main Authors: Yuxin Tan, Bin Zhao, Daofu Yuan, Fan Li, Shanshan Yu, Mengda Jin, Yu Zhang, Chang Luo, Wentao Chen, Tao Wang, Jikai Zhu, Ziwei Wang, Tiangang Yang, Shu Liu, Uwe Manthe, Xingan Wang, Dong H. Zhang, Xueming Yang
Format: Article
Language:English
Published: Nature Portfolio 2025-07-01
Series:Nature Communications
Online Access:https://doi.org/10.1038/s41467-025-61117-1
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author Yuxin Tan
Bin Zhao
Daofu Yuan
Fan Li
Shanshan Yu
Mengda Jin
Yu Zhang
Chang Luo
Wentao Chen
Tao Wang
Jikai Zhu
Ziwei Wang
Tiangang Yang
Shu Liu
Uwe Manthe
Xingan Wang
Dong H. Zhang
Xueming Yang
author_facet Yuxin Tan
Bin Zhao
Daofu Yuan
Fan Li
Shanshan Yu
Mengda Jin
Yu Zhang
Chang Luo
Wentao Chen
Tao Wang
Jikai Zhu
Ziwei Wang
Tiangang Yang
Shu Liu
Uwe Manthe
Xingan Wang
Dong H. Zhang
Xueming Yang
author_sort Yuxin Tan
collection DOAJ
description Abstract How the non-reacting moiety of a molecule influences a polyatomic reaction has been a topic of much research interest. Here we present a comprehensive investigation of the D + CH4 → HD + CH3 reaction, a benchmark polyatomic elementary reaction with CH3 as the non-reacting moiety, employing a high-resolution crossed molecular beams apparatus and an accurate seven-dimensional wave packet method. An interesting angular distribution of the CH3(v’ = 1) product umbrella bending vibrational state is observed to scatter more in the sideways direction than the CH3(v’ = 0) one. By monitoring the wave functions on a dividing surface in the transition state region, the CH3 umbrella bending mode is established as a reporter mode that faithfully reveals how the D atom dynamically approaches CH4 at different total angular momenta or impact parameters. This discovery of the reporter mode provides an opportunity for the detailed study of polyatomic reaction dynamics.
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institution Kabale University
issn 2041-1723
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publishDate 2025-07-01
publisher Nature Portfolio
record_format Article
series Nature Communications
spelling doaj-art-fb8ed5fc248e44328523647deec95c2d2025-08-20T04:01:35ZengNature PortfolioNature Communications2041-17232025-07-011611910.1038/s41467-025-61117-1Revealing umbrella bending as a reporter mode in the D+CH4 reactionYuxin Tan0Bin Zhao1Daofu Yuan2Fan Li3Shanshan Yu4Mengda Jin5Yu Zhang6Chang Luo7Wentao Chen8Tao Wang9Jikai Zhu10Ziwei Wang11Tiangang Yang12Shu Liu13Uwe Manthe14Xingan Wang15Dong H. Zhang16Xueming Yang17State Key Laboratory of Chemical Reaction Dynamics and Department of Chemical Physics, University of Science and Technology of ChinaDepartment of Chemistry, College of Science, Southern University of Science and TechnologyHefei National Research Center for Physical Science at Microscale, University of Science and Technology of ChinaState Key Laboratory of Chemical Reaction Dynamics and Department of Chemical Physics, University of Science and Technology of ChinaState Key Laboratory of Chemical Reaction Dynamics and Department of Chemical Physics, University of Science and Technology of ChinaState Key Laboratory of Chemical Reaction Dynamics and Department of Chemical Physics, University of Science and Technology of ChinaState Key Laboratory of Chemical Reaction Dynamics and Department of Chemical Physics, University of Science and Technology of ChinaState Key Laboratory of Chemical Reaction Dynamics and Department of Chemical Physics, University of Science and Technology of ChinaState Key Laboratory of Chemical Reaction Dynamics and Department of Chemical Physics, University of Science and Technology of ChinaDepartment of Chemistry, College of Science, Southern University of Science and TechnologyDepartment of Chemistry, College of Science, Southern University of Science and TechnologyDepartment of Chemistry, College of Science, Southern University of Science and TechnologyDepartment of Chemistry, College of Science, Southern University of Science and TechnologyState Key Laboratory of Chemical Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of SciencesTheoretische Chemie, Fakultät für Chemie, Universität BielefeldState Key Laboratory of Chemical Reaction Dynamics and Department of Chemical Physics, University of Science and Technology of ChinaState Key Laboratory of Chemical Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of SciencesDepartment of Chemistry, College of Science, Southern University of Science and TechnologyAbstract How the non-reacting moiety of a molecule influences a polyatomic reaction has been a topic of much research interest. Here we present a comprehensive investigation of the D + CH4 → HD + CH3 reaction, a benchmark polyatomic elementary reaction with CH3 as the non-reacting moiety, employing a high-resolution crossed molecular beams apparatus and an accurate seven-dimensional wave packet method. An interesting angular distribution of the CH3(v’ = 1) product umbrella bending vibrational state is observed to scatter more in the sideways direction than the CH3(v’ = 0) one. By monitoring the wave functions on a dividing surface in the transition state region, the CH3 umbrella bending mode is established as a reporter mode that faithfully reveals how the D atom dynamically approaches CH4 at different total angular momenta or impact parameters. This discovery of the reporter mode provides an opportunity for the detailed study of polyatomic reaction dynamics.https://doi.org/10.1038/s41467-025-61117-1
spellingShingle Yuxin Tan
Bin Zhao
Daofu Yuan
Fan Li
Shanshan Yu
Mengda Jin
Yu Zhang
Chang Luo
Wentao Chen
Tao Wang
Jikai Zhu
Ziwei Wang
Tiangang Yang
Shu Liu
Uwe Manthe
Xingan Wang
Dong H. Zhang
Xueming Yang
Revealing umbrella bending as a reporter mode in the D+CH4 reaction
Nature Communications
title Revealing umbrella bending as a reporter mode in the D+CH4 reaction
title_full Revealing umbrella bending as a reporter mode in the D+CH4 reaction
title_fullStr Revealing umbrella bending as a reporter mode in the D+CH4 reaction
title_full_unstemmed Revealing umbrella bending as a reporter mode in the D+CH4 reaction
title_short Revealing umbrella bending as a reporter mode in the D+CH4 reaction
title_sort revealing umbrella bending as a reporter mode in the d ch4 reaction
url https://doi.org/10.1038/s41467-025-61117-1
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