{"title":"Studying substituent number effects on vibrational energy transfer by time−resolved CARS spectroscopy","authors":"Xiaosong Liu, Qingxiao Zou, Hui Li, Weilong Liu, Feng Hu, Yanqiang Yang","doi":"10.1140/epjd/s10053-024-00830-w","DOIUrl":null,"url":null,"abstract":"<div><p>Vibrational energy transfer was a key property of chemical reactions that remains deeply understood. In this work, the detail information of vibrational energy transfer in aniline, N,N-dimethylaniline (DMA) and N,N-diethylaniline (DEA) were studied by femtosecond time-resolved coherent anti-Stokes Raman scattering (CARS) spectroscopy, respectively. Low frequency modes of aniline, DMA and DEA were collectively excited, the beats arising from vibrational couplings among these modes were described. With analysis of vibrational coupling, energy transfer flow from one mode to another was visualized. An investigation into the molecular structure and vibrational couplings can be found that vibrational energy transfer is related to vibrational mode symmetry. In addition, substituent groups play an important role in vibrational coupling and energy transfer of aniline, DMA and DEA. A decrease of the number of substituent vibrational modes involved in coupling and energy transfer efficiency with the increase of the amount of relative molecular mass ratio was found out.</p><h3>Graphical abstract</h3><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":789,"journal":{"name":"The European Physical Journal D","volume":"78 4","pages":""},"PeriodicalIF":1.5000,"publicationDate":"2024-04-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"The European Physical Journal D","FirstCategoryId":"4","ListUrlMain":"https://link.springer.com/article/10.1140/epjd/s10053-024-00830-w","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}
引用次数: 0
Abstract
Vibrational energy transfer was a key property of chemical reactions that remains deeply understood. In this work, the detail information of vibrational energy transfer in aniline, N,N-dimethylaniline (DMA) and N,N-diethylaniline (DEA) were studied by femtosecond time-resolved coherent anti-Stokes Raman scattering (CARS) spectroscopy, respectively. Low frequency modes of aniline, DMA and DEA were collectively excited, the beats arising from vibrational couplings among these modes were described. With analysis of vibrational coupling, energy transfer flow from one mode to another was visualized. An investigation into the molecular structure and vibrational couplings can be found that vibrational energy transfer is related to vibrational mode symmetry. In addition, substituent groups play an important role in vibrational coupling and energy transfer of aniline, DMA and DEA. A decrease of the number of substituent vibrational modes involved in coupling and energy transfer efficiency with the increase of the amount of relative molecular mass ratio was found out.
振动能量转移是化学反应的一个关键特性，但人们对这一特性的理解仍然很深。本研究利用飞秒时间分辨相干反斯托克斯拉曼散射（CARS）光谱分别研究了苯胺、N,N-二甲基苯胺（DMA）和N,N-二乙基苯胺（DEA）中振动能量传递的详细信息。对苯胺、DMA 和 DEA 的低频模式进行了集体激发，并描述了这些模式之间振动耦合产生的节拍。通过分析振动耦合，可以直观地看到能量从一个模式传递到另一个模式。通过对分子结构和振动耦合的研究可以发现，振动能量的传递与振动模式的对称性有关。此外，取代基团在苯胺、DMA 和 DEA 的振动耦合和能量传递中起着重要作用。研究发现，随着相对分子质量比的增加，参与耦合和能量传递效率的取代基振动模式数量减少。
期刊介绍：
The European Physical Journal D (EPJ D) presents new and original research results in:
Atomic Physics;
Molecular Physics and Chemical Physics;
Atomic and Molecular Collisions;
Clusters and Nanostructures;
Plasma Physics;
Laser Cooling and Quantum Gas;
Nonlinear Dynamics;
Optical Physics;
Quantum Optics and Quantum Information;
Ultraintense and Ultrashort Laser Fields.
The range of topics covered in these areas is extensive, from Molecular Interaction and Reactivity to Spectroscopy and Thermodynamics of Clusters, from Atomic Optics to Bose-Einstein Condensation to Femtochemistry.
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