Reaction Dynamics of Polyatomic Molecules: Low Temperature Reactions and Coherent Photodissociation

多原子分子的反应动力学:低温反应和相干光解离

基本信息

  • 批准号:
    1955239
  • 负责人:
  • 金额:
    $ 51.7万
  • 依托单位:
  • 依托单位国家:
    美国
  • 项目类别:
    Standard Grant
  • 财政年份:
    2020
  • 资助国家:
    美国
  • 起止时间:
    2020-07-01 至 2023-06-30
  • 项目状态:
    已结题

项目摘要

In this project funded by the Chemical Structure, Dynamics, and Mechanism-A (CSDM-A) program of the Chemistry Division, Professor Arthur Suits and his research team at the University of Missouri, Columbia are developing new tools for studying how chemical reactions occur, in other words, how the atoms within the molecules move, how bonds are broken and new ones formed. The Suits laboratory is developing reaction chambers where the starting materials are injected as uniform supersonic flows of gas. After a pulse of laser light is applied, the changes in molecular structure caused by the laser are observed at different downstream distances. Since the flow rate is known precisely, the downstream distances correspond to time since the laser pulse, and the rates at which the molecules change structure can be calculated. The use of supersonic flows allows very fast chemical reactions to be studied. The downstream events are captured using other laser or microwave spectroscopy techniques. Microwave light causes some molecules to rotate in very specific ways, which in turn reveals information about their structure. The reactions being studied include oxygen atoms reacting with hydrocarbons with double carbon-carbon bonds (C=C) and triple bonds (C≡C), and the light-induced dissociation of ethylene sulfide (C2H4S) and nitrogen dioxide (NO2). These studies are providing new insights into how chemical reactions occur in general. The specific reactions being studied are also important for more accurate modeling of chemical reactions in the atmosphere and in astronomical environments. This project is providing training for a graduate student and a post-doctoral fellow. Data analysis software developed during the research is made available to other research groups worldwide.The research takes advantage of two unique new instruments to probe the reaction dynamics, spectroscopy, and low temperature kinetics of polyatomic molecules. The first of these instruments combines the revolutionary Chirped-pulse Fourier-transform microwave (CPTMW) technique with intense low-temperature pulsed uniform supersonic flows for kinetics and dynamics studies. The research also involves an instrument that combines the same uniform supersonic flows with high-resolution ultra-sensitive continuous-wave cavity ring-down spectroscopy (CRDS), providing capabilities complementary to those of the microwave-based system. The latter instrument has recently demonstrated Simultaneous Kinetics and Ringdown (SKaR) in a supersonic expansion for the first time. In addition to the studies in low temperature flows, the Suits team is also investigating how coherent orbital polarization reveals effects of the so-called geometric phae, wherein the system wavefunction must undergo a sign change following a transit around a conical intersection (CI). The current studies extend investigations of the geometric phase to NO2 and ethylene sulfide, promising novel probes and insights into nonadiabatic dynamics. In terms of scientific Broader Impacts, this project extends capabilities into the mid-IR spectrum, which in turn permits the application of the SKaR kinetics method to many systems of astrochemical and astronomical interest.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.
在这个由化学部化学结构、动力学和机理a (CSDM-A)项目资助的项目中,密苏里大学哥伦比亚分校的Arthur Suits教授和他的研究小组正在开发新的工具来研究化学反应是如何发生的,换句话说,分子内的原子是如何移动的,键是如何断裂的,新的键是如何形成的。Suits实验室正在开发反应室,在那里初始材料以均匀的超音速气流注入。在施加激光脉冲后,在不同的下游距离上观察到激光引起的分子结构变化。由于流速是精确已知的,下游距离对应于自激光脉冲以来的时间,分子改变结构的速率可以计算出来。超声速流动的使用可以研究非常快的化学反应。下游事件使用其他激光或微波光谱技术捕获。微波光使一些分子以非常特殊的方式旋转,这反过来揭示了它们的结构信息。正在研究的反应包括氧原子与具有双键(C=C)和三键(C≡C)的碳氢化合物的反应,以及光诱导的硫化乙烯(C2H4S)和二氧化氮(NO2)的解离。这些研究为化学反应如何发生提供了新的见解。正在研究的特定反应对于更准确地模拟大气和天文环境中的化学反应也很重要。该项目为一名研究生和一名博士后提供培训。在研究期间开发的数据分析软件可供世界各地的其他研究小组使用。本研究利用两种独特的新仪器来探测多原子分子的反应动力学、光谱学和低温动力学。这些仪器中的第一个将革命性的啁啾脉冲傅立叶变换微波(CPTMW)技术与强低温脉冲均匀超音速流相结合,用于动力学和动力学研究。该研究还涉及一种仪器,该仪器将相同的均匀超音速流与高分辨率超灵敏连续波腔衰荡光谱(CRDS)相结合,为基于微波的系统提供补充功能。后一种仪器最近首次在超音速膨胀中展示了同步动力学和Ringdown (SKaR)。除了低温流的研究之外,Suits团队还在研究相干轨道偏振如何揭示所谓的几何相位的影响,其中系统波函数必须经历一个符号变化,之后围绕圆锥形相交(CI)的过境。目前的研究将几何相的研究扩展到NO2和硫化乙烯,为非绝热动力学提供了新的探测和见解。就更广泛的科学影响而言,该项目将能力扩展到中红外光谱,这反过来又允许将SKaR动力学方法应用于许多天体化学和天文学兴趣系统。该奖项反映了美国国家科学基金会的法定使命,并通过使用基金会的知识价值和更广泛的影响审查标准进行评估,被认为值得支持。

项目成果

期刊论文数量(8)
专著数量(0)
科研奖励数量(0)
会议论文数量(0)
专利数量(0)
Uniform supersonic flow sampling for detection by chirped-pulse rotational spectroscopy
用于通过啁啾脉冲旋转光谱检测的均匀超音速流采样
  • DOI:
    10.1063/5.0073527
  • 发表时间:
    2022
  • 期刊:
  • 影响因子:
    0
  • 作者:
    Gurusinghe, Ranil M.;Dias, Nureshan;Krueger, Ritter;Suits, Arthur G.
  • 通讯作者:
    Suits, Arthur G.
Radical–Radical Reaction Dynamics Probed Using Millimeterwave Spectroscopy: Propargyl + NH 2 /ND 2
使用毫米波光谱探测自由基 - 自由基反应动力学:丙炔 NH 2 /ND 2
  • DOI:
    10.1021/acs.jpclett.1c03813
  • 发表时间:
    2022
  • 期刊:
  • 影响因子:
    0
  • 作者:
    Gurusinghe, Ranil M.;Dias, Nureshan;Mebel, Alexander M.;Suits, Arthur G.
  • 通讯作者:
    Suits, Arthur G.
Coherent atomic orbital polarization probes the geometric phase in photodissociation of polyatomic molecules
相干原子轨道偏振探测多原子分子光解离的几何相位
  • DOI:
    10.1002/ntls.20220013
  • 发表时间:
    2022
  • 期刊:
  • 影响因子:
    0
  • 作者:
    Weeraratna, Chaya;Suits, Arthur G.;Vasyutinskii, Oleg S.
  • 通讯作者:
    Vasyutinskii, Oleg S.
Imaging rotational energy transfer: comparative stereodynamics in CO + N 2 and CO + CO inelastic scattering
旋转能量转移成像:CO N 2 和 CO CO 非弹性散射的立体动力学比较
  • DOI:
    10.1039/d3cp02229c
  • 发表时间:
    2023
  • 期刊:
  • 影响因子:
    3.3
  • 作者:
    Sun, Zhong-Fa;Scheidsbach, Roy J.;van Hemert, Marc C.;van der Avoird, Ad;Suits, Arthur G.;Parker, David H.
  • 通讯作者:
    Parker, David H.
Direct D-atom Incorporation in Radicals: An Overlooked Pathway for Deuterium Fractionation
自由基中直接掺入 D 原子:一种被忽视的氘分馏途径
  • DOI:
    10.3847/1538-4357/acac1d
  • 发表时间:
    2023
  • 期刊:
  • 影响因子:
    0
  • 作者:
    Dias, Nureshan;Gurusinghe, Ranil M.;Broderick, Bernadette M.;Millar, Tom J.;Suits, Arthur G.
  • 通讯作者:
    Suits, Arthur G.
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Arthur Suits其他文献

Arthur Suits的其他文献

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{{ truncateString('Arthur Suits', 18)}}的其他基金

New Tools and Applications for Kinetics and Dynamics with Broadband Rotational Spectroscopy
宽带旋转光谱动力学和动力学的新工具和应用
  • 批准号:
    2247776
  • 财政年份:
    2023
  • 资助金额:
    $ 51.7万
  • 项目类别:
    Standard Grant
New Tools and New Approaches for Spectroscopy, Kinetics and Dynamics in Uniform Supersonic Flows
均匀超音速流中光谱学、动力学和动力学的新工具和新方法
  • 批准号:
    1665207
  • 财政年份:
    2017
  • 资助金额:
    $ 51.7万
  • 项目类别:
    Standard Grant
Chemical Dynamics of Polyatomic Molecules: New Probes for New Insights
多原子分子的化学动力学:新探针带来新见解
  • 批准号:
    1634760
  • 财政年份:
    2016
  • 资助金额:
    $ 51.7万
  • 项目类别:
    Standard Grant
Chemical Dynamics of Polyatomic Molecules: New Probes for New Insights
多原子分子的化学动力学:新探针带来新见解
  • 批准号:
    1361906
  • 财政年份:
    2014
  • 资助金额:
    $ 51.7万
  • 项目类别:
    Standard Grant
MRI: Development of a Chirped-Pulse, Fourier-Transform mm-Wave Pulsed Uniform Supersonic Flow Spectrometer
MRI:啁啾脉冲、傅立叶变换毫米波脉冲均匀超声速流谱仪的开发
  • 批准号:
    1126380
  • 财政年份:
    2011
  • 资助金额:
    $ 51.7万
  • 项目类别:
    Standard Grant
Experimental Probes of Nonadiabatic Dynamics and Novel Reaction Pathways in Polyatomic Molecules
多原子分子非绝热动力学和新反应途径的实验探索
  • 批准号:
    1111348
  • 财政年份:
    2011
  • 资助金额:
    $ 51.7万
  • 项目类别:
    Standard Grant
High-Resolution Imaging of Photodissociation Dynamics in Ions and Neutral Molecules
离子和中性分子光解离动力学的高分辨率成像
  • 批准号:
    0715300
  • 财政年份:
    2007
  • 资助金额:
    $ 51.7万
  • 项目类别:
    Continuing Grant
IDBR: Development of an Electrostatic Ion Trap Tandem Mass Spectrometer
IDBR:静电离子阱串联质谱仪的开发
  • 批准号:
    0551958
  • 财政年份:
    2006
  • 资助金额:
    $ 51.7万
  • 项目类别:
    Continuing Grant
Imaging Probes of Collisional Ionization, Ion Pair Dissociation and Superexcited State Dynamics
碰撞电离、离子对解离和超激发态动力学的成像探针
  • 批准号:
    0415393
  • 财政年份:
    2004
  • 资助金额:
    $ 51.7万
  • 项目类别:
    Continuing Grant
Ion Pair Imaging Spectroscopy
离子对成像光谱
  • 批准号:
    0102174
  • 财政年份:
    2001
  • 资助金额:
    $ 51.7万
  • 项目类别:
    Continuing Grant

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Visualizing Photon Induced Dynamics in Polyatomic Molecules using Femtosecond Pump-Probe Laser Pulses
使用飞秒泵浦探测激光脉冲可视化多原子分子中的光子诱发动力学
  • 批准号:
    2306982
  • 财政年份:
    2023
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RUI: Strong-Field Control of Intramolecular Dynamics in Polyatomic Molecules
RUI:多原子分子内分子动力学的强场控制
  • 批准号:
    2309192
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    2023
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    $ 51.7万
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    Continuing Grant
Collaborative Research: Attosecond Electron Dynamics in Polyatomic Molecules Probed by Water Window X-Rays
合作研究:水窗 X 射线探测多原子分子中的阿秒电子动力学
  • 批准号:
    2207674
  • 财政年份:
    2022
  • 资助金额:
    $ 51.7万
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    Continuing Grant
Collaborative Research: Attosecond Electron Dynamics in Polyatomic Molecules Probed by Water Window X-Rays
合作研究:水窗 X 射线探测多原子分子中的阿秒电子动力学
  • 批准号:
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Quantum Mechanics and Dynamics of Open Polyatomic Systems
开放多原子系统的量子力学和动力学
  • 批准号:
    RGPIN-2020-04017
  • 财政年份:
    2022
  • 资助金额:
    $ 51.7万
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    Discovery Grants Program - Individual
State-to-State Photodissociation of Polyatomic Free Radicals: Nonadiabatic Dynamics and Quantum Coherence
多原子自由基的状态到状态光解离:非绝热动力学和量子相干性
  • 批准号:
    2155232
  • 财政年份:
    2022
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Quantum Mechanics and Dynamics of Open Polyatomic Systems
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使用飞秒泵浦探测激光脉冲可视化多原子分子中的光子诱发动力学
  • 批准号:
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  • 财政年份:
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