Kareem Hegazy, Phil Bucksbaum, Martin Centurion, James Cryan, Renkai Li, Ming-Fu Lin, Bryan Moore, Pedro Nunes, Xiaozhe Shen, Stephen Weathersby, Jie Yang, Xijie Wang, Thomas Wolf
{"title":"通过兆电子伏特超快电子衍射跟踪硝基苯的解离路径","authors":"Kareem Hegazy, Phil Bucksbaum, Martin Centurion, James Cryan, Renkai Li, Ming-Fu Lin, Bryan Moore, Pedro Nunes, Xiaozhe Shen, Stephen Weathersby, Jie Yang, Xijie Wang, Thomas Wolf","doi":"10.1088/1361-6455/ad7431","DOIUrl":null,"url":null,"abstract":"As the simplest nitroaromatic compound, nitrobenzene is an interesting model system to explore the rich photochemistry of nitroaromatic compounds. Previous investigations of nitrobenzene’s photochemical dynamics have probed structural and electronic properties. These investigations paint, at times, a convoluted and sometimes contradictory description of the photochemical landscape. We investigate the ultrafast dynamics of nitrobenzene triggered by photoexcitation at 267 nm for the first time using a structural probe with femtosecond time resolution. Our probe complements previous measurements of nitrobenzene’s electronic structure evolution and aids in determining the photochemical dynamics with less ambiguity. We employ megaelectronvolt ultrafast electron diffraction to follow nitrobenzene’s structural evolution within the first 5 ps after photoexcitation. We observe ground state recovery within <inline-formula>\n<tex-math><?CDATA $160 \\pm 60$?></tex-math><mml:math overflow=\"scroll\"><mml:mrow><mml:mn>160</mml:mn><mml:mo>±</mml:mo><mml:mn>60</mml:mn></mml:mrow></mml:math><inline-graphic xlink:href=\"bad7431ieqn1.gif\"></inline-graphic></inline-formula> fs through nonadiabatic dynamics. Based on comparisons of the experimental signal with molecular dynamics simulations, we exclude a significant population of the triplet manifold. Furthermore, we do not observe fragmentation of nitrobenzene within the investigated time window, which indicates that previously observed photofragmentation reactions take place in the vibrationally ‘hot’ ground state on timescales considerably beyond 5 ps.","PeriodicalId":16826,"journal":{"name":"Journal of Physics B: Atomic, Molecular and Optical Physics","volume":null,"pages":null},"PeriodicalIF":1.5000,"publicationDate":"2024-09-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Tracking dissociation pathways of nitrobenzene via mega-electron-volt ultrafast electron diffraction\",\"authors\":\"Kareem Hegazy, Phil Bucksbaum, Martin Centurion, James Cryan, Renkai Li, Ming-Fu Lin, Bryan Moore, Pedro Nunes, Xiaozhe Shen, Stephen Weathersby, Jie Yang, Xijie Wang, Thomas Wolf\",\"doi\":\"10.1088/1361-6455/ad7431\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"As the simplest nitroaromatic compound, nitrobenzene is an interesting model system to explore the rich photochemistry of nitroaromatic compounds. Previous investigations of nitrobenzene’s photochemical dynamics have probed structural and electronic properties. These investigations paint, at times, a convoluted and sometimes contradictory description of the photochemical landscape. We investigate the ultrafast dynamics of nitrobenzene triggered by photoexcitation at 267 nm for the first time using a structural probe with femtosecond time resolution. Our probe complements previous measurements of nitrobenzene’s electronic structure evolution and aids in determining the photochemical dynamics with less ambiguity. We employ megaelectronvolt ultrafast electron diffraction to follow nitrobenzene’s structural evolution within the first 5 ps after photoexcitation. We observe ground state recovery within <inline-formula>\\n<tex-math><?CDATA $160 \\\\pm 60$?></tex-math><mml:math overflow=\\\"scroll\\\"><mml:mrow><mml:mn>160</mml:mn><mml:mo>±</mml:mo><mml:mn>60</mml:mn></mml:mrow></mml:math><inline-graphic xlink:href=\\\"bad7431ieqn1.gif\\\"></inline-graphic></inline-formula> fs through nonadiabatic dynamics. Based on comparisons of the experimental signal with molecular dynamics simulations, we exclude a significant population of the triplet manifold. Furthermore, we do not observe fragmentation of nitrobenzene within the investigated time window, which indicates that previously observed photofragmentation reactions take place in the vibrationally ‘hot’ ground state on timescales considerably beyond 5 ps.\",\"PeriodicalId\":16826,\"journal\":{\"name\":\"Journal of Physics B: Atomic, Molecular and Optical Physics\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":1.5000,\"publicationDate\":\"2024-09-06\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of Physics B: Atomic, Molecular and Optical Physics\",\"FirstCategoryId\":\"101\",\"ListUrlMain\":\"https://doi.org/10.1088/1361-6455/ad7431\",\"RegionNum\":4,\"RegionCategory\":\"物理与天体物理\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q3\",\"JCRName\":\"OPTICS\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Physics B: Atomic, Molecular and Optical Physics","FirstCategoryId":"101","ListUrlMain":"https://doi.org/10.1088/1361-6455/ad7431","RegionNum":4,"RegionCategory":"物理与天体物理","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q3","JCRName":"OPTICS","Score":null,"Total":0}
Tracking dissociation pathways of nitrobenzene via mega-electron-volt ultrafast electron diffraction
As the simplest nitroaromatic compound, nitrobenzene is an interesting model system to explore the rich photochemistry of nitroaromatic compounds. Previous investigations of nitrobenzene’s photochemical dynamics have probed structural and electronic properties. These investigations paint, at times, a convoluted and sometimes contradictory description of the photochemical landscape. We investigate the ultrafast dynamics of nitrobenzene triggered by photoexcitation at 267 nm for the first time using a structural probe with femtosecond time resolution. Our probe complements previous measurements of nitrobenzene’s electronic structure evolution and aids in determining the photochemical dynamics with less ambiguity. We employ megaelectronvolt ultrafast electron diffraction to follow nitrobenzene’s structural evolution within the first 5 ps after photoexcitation. We observe ground state recovery within 160±60 fs through nonadiabatic dynamics. Based on comparisons of the experimental signal with molecular dynamics simulations, we exclude a significant population of the triplet manifold. Furthermore, we do not observe fragmentation of nitrobenzene within the investigated time window, which indicates that previously observed photofragmentation reactions take place in the vibrationally ‘hot’ ground state on timescales considerably beyond 5 ps.
期刊介绍:
Published twice-monthly (24 issues per year), Journal of Physics B: Atomic, Molecular and Optical Physics covers the study of atoms, ions, molecules and clusters, and their structure and interactions with particles, photons or fields. The journal also publishes articles dealing with those aspects of spectroscopy, quantum optics and non-linear optics, laser physics, astrophysics, plasma physics, chemical physics, optical cooling and trapping and other investigations where the objects of study are the elementary atomic, ionic or molecular properties of processes.