A Deep Dive into Electron-Neutral Interactions

深入研究电子中性相互作用

基本信息

  • 批准号:
    2053889
  • 负责人:
  • 金额:
    $ 54.23万
  • 依托单位:
  • 依托单位国家:
    美国
  • 项目类别:
    Standard Grant
  • 财政年份:
    2021
  • 资助国家:
    美国
  • 起止时间:
    2021-06-01 至 2025-05-31
  • 项目状态:
    未结题

项目摘要

In this project, funded by the Chemical Structure Dynamics and Mechanism (CSDM-A) program of the Chemistry Division, Professor Caroline Chick Jarrold and her students at Indiana University are studying interactions between electrons and neutral molecules using several sophisticated experimental techniques that are based on the absorption and emission of light by the chemical compounds being studied. Electron-neutral interactions drive many important chemical and physical processes, yet they are difficult to explore experimentally. From a practical standpoint, controlling electrons is challenging because they are thousands of times lighter than atoms, which themselves are tiny particles, while at the same time, the electric charge carried by the electron makes it vulnerable to deflection by the earth’s magnetic field, among other weak influencing forces present in laboratory settings. Professor Jarrold overcomes these hurdles by preparing the free electrons in a controlled way, which is to target negatively charged molecules with a laser pulse that removes an electron with a known amount of energy, and in the desired proximity of a neutral target molecule. The array of molecules selected for study are chosen to sample a broad range of properties that affect their interactions with electrons. The experiments involve the novel use of photoelectrons as a tool for probing valence-bound, non-valence-bound, and temporary anion states of molecules and bimolecular complexes, with an emphasis on preparing and probing systems that do not neatly fall into any of these three categories. This project addresses several hypotheses involving the description of electron-driven chemistry, the increasingly complex landscape for electron-bimolecular interactions, and the rules that govern non-valence-bound anion lifetimes. Probing these systems experimentally with energy-selected electrons is achieved by detachment of anionic precursors, which provides a route to mapping the energy-dependence of electron-neutral interactions, some of which initiate electron-driven chemistry. Additional studies include fluorescence lifetime and dispersed fluorescence measurements on non-valence-bound excited states of anions. Interpretation of data collected on these complex and often transient species is supported by calculations conducted by collaborator Professor Thomas Sommerfeld of Southeastern Louisiana University, who has expertise in the theoretical treatment of non-valence states of anions. The broader impacts include a more complete picture of electron-driven chemical and physical processes, which is a prerequisite for controlling these processes. In addition, participants in this project receive well-rounded graduate or postdoctoral training in a range of techniques in chemical physics, coupled with ample professional development opportunities, in the laboratory of a PI with a deep commitment to diversity and equity.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.
在这个项目中,由化学系的化学结构动力学和机制(CSDM-A)计划资助,印第安纳州大学的Caroline Chick Jarrold教授和她的学生正在使用几种复杂的实验技术研究电子和中性分子之间的相互作用,这些技术是基于被研究的化合物对光的吸收和发射。 电子-中性相互作用驱动许多重要的化学和物理过程,但它们很难通过实验进行探索。 从实际的角度来看,控制电子是一项挑战,因为它们比原子轻数千倍,而原子本身就是微小的粒子,同时,电子携带的电荷使其容易受到地球磁场的偏转,以及实验室环境中存在的其他微弱影响力。 Jarrold教授通过以受控的方式制备自由电子来克服这些障碍,即用激光脉冲靶向带负电荷的分子,该激光脉冲以已知的能量去除电子,并且在中性目标分子的期望附近。选择用于研究的分子阵列是为了对影响其与电子相互作用的广泛性质进行采样。 实验涉及光电子作为探测分子和双分子复合物的价束缚、非价束缚和临时阴离子状态的工具的新用途,重点是准备和探测不完全属于这三类中任何一类的系统。 该项目解决了几个假设,涉及电子驱动化学的描述,电子-双分子相互作用的日益复杂的景观,以及管理非价键结合阴离子寿命的规则。 通过分离阴离子前体来实验性地用能量选择的电子探测这些系统,这提供了一种映射电子-中性相互作用的能量依赖性的途径,其中一些启动了电子驱动的化学。 其他的研究包括荧光寿命和分散荧光测量的非价束缚激发态的阴离子。 对这些复杂且经常是瞬态的物种收集的数据的解释得到了合作者东南路易斯安那大学的托马斯索末菲教授进行的计算的支持,他在阴离子非价态的理论处理方面具有专业知识。更广泛的影响包括更完整地了解电子驱动的化学和物理过程,这是控制这些过程的先决条件。 此外,该项目的参与者在一个致力于多样性和公平的PI实验室接受了一系列化学物理技术的全面研究生或博士后培训,以及充足的专业发展机会。该奖项反映了NSF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(7)
专著数量(0)
科研奖励数量(0)
会议论文数量(0)
专利数量(0)
Trend in the Electron Affinities of Fluorophenyl Radicals ·C 6 H 5-x F x (1 ≤ x ≤ 4)
氟苯基自由基·C 6 H 5-x F x (1 ≤ x ≤ 4) 的电子亲和力变化趋势
  • DOI:
    10.1021/acs.jpca.3c04327
  • 发表时间:
    2023
  • 期刊:
  • 影响因子:
    0
  • 作者:
    McGee, Conor J.;McGinnis, Kristen Rose;Jarrold, Caroline Chick
  • 通讯作者:
    Jarrold, Caroline Chick
Identification of Stable Perfluorocarbons Formed by Hyperthermal Decomposition of Graphite Fluoride Using Anion Photoelectron Spectroscopy
  • DOI:
    10.1021/acs.jpcc.2c02180
  • 发表时间:
    2022-06
  • 期刊:
  • 影响因子:
    0
  • 作者:
    Brett A. Williams;A. Siedle;C. Jarrold
  • 通讯作者:
    Brett A. Williams;A. Siedle;C. Jarrold
Anion Photoelectron Imaging Spectroscopy of C 6 HF 5 – , C 6 F 6 – , and the Absence of C 6 H 2 F 4 –
C 6 HF 5 α、C 6 F 6 α 和不存在的 C 6 H 2 F 4 α 的阴离子光电子成像光谱
  • DOI:
    10.1021/acs.jpca.3c04016
  • 发表时间:
    2023
  • 期刊:
  • 影响因子:
    0
  • 作者:
    McGee, Conor J.;McGinnis, Kristen Rose;Jarrold, Caroline Chick
  • 通讯作者:
    Jarrold, Caroline Chick
Autodetachment over Broad Photon Energy Ranges in the Anion Photoelectron Spectra of [O 2 – M ] − ( M = Glyoxal, Methylglyoxal, or Biacetyl) Complex Anions
[O 2 → M ] →(M = 乙二醛、甲基乙二醛或联乙酰)复合阴离子的阴离子光电子谱中宽光子能量范围内的自分离
  • DOI:
    10.1021/acs.jpca.1c07163
  • 发表时间:
    2021
  • 期刊:
  • 影响因子:
    0
  • 作者:
    Dobulis, Marissa A.;McGee, Conor J.;Sommerfeld, Thomas;Jarrold, Caroline Chick
  • 通讯作者:
    Jarrold, Caroline Chick
Identification of Isoprene Oxidation Reaction Products via Anion Photoelectron Spectroscopy
阴离子光电子能谱鉴定异戊二烯氧化反应产物
  • DOI:
    10.1021/acs.jpca.1c08176
  • 发表时间:
    2021
  • 期刊:
  • 影响因子:
    0
  • 作者:
    Dobulis, Marissa A.;Thompson, Michael C.;Jarrold, Caroline Chick
  • 通讯作者:
    Jarrold, Caroline Chick
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Caroline Jarrold其他文献

Caroline Jarrold的其他文献

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{{ truncateString('Caroline Jarrold', 18)}}的其他基金

A look at atmospheric chemistry through the back door: PEI spectroscopy of anionic precursors to transient species
通过后门观察大气化学:瞬态物质阴离子前体的 PEI 光谱
  • 批准号:
    1664965
  • 财政年份:
    2017
  • 资助金额:
    $ 54.23万
  • 项目类别:
    Continuing Grant
Probing metal catalyst-support interactions using small cluster models: Gas-phase reactivity studies, anion photoelectron spectroscopy, and DFT calculations
使用小簇模型探测金属催化剂-载体相互作用:气相反应性研究、阴离子光电子能谱和 DFT 计算
  • 批准号:
    1265991
  • 财政年份:
    2013
  • 资助金额:
    $ 54.23万
  • 项目类别:
    Continuing Grant
Binary transition metal oxide clusters: Kinetics and mechanisms of catalytically relevant processes probed by gas-phase reactivity studies, spectroscopy, and DFT calculations
二元过渡金属氧化物簇:通过气相反应性研究、光谱学和 DFT 计算探测催化相关过程的动力学和机制
  • 批准号:
    1012641
  • 财政年份:
    2010
  • 资助金额:
    $ 54.23万
  • 项目类别:
    Standard Grant
Studies of the chemical and physical properties of molybdenum-based mixed metal oxide clusters
钼基混合金属氧化物簇化学和物理性质的研究
  • 批准号:
    0718387
  • 财政年份:
    2007
  • 资助金额:
    $ 54.23万
  • 项目类别:
    Continuing Grant
CAREER: Steps Toward Ensuring the Quality of the Next Generation of Chemists, and Probing the Size-Dependent Properties of Catalytically Significant Metal Cluster/Adsorbate Compl
职业生涯:确保下一代化学家的质量,并探索具有催化意义的金属簇/吸附物复合物的尺寸依赖性特性的步骤
  • 批准号:
    0350193
  • 财政年份:
    2003
  • 资助金额:
    $ 54.23万
  • 项目类别:
    Continuing Grant
CAREER: Steps Toward Ensuring the Quality of the Next Generation of Chemists, and Probing the Size-Dependent Properties of Catalytically Significant Metal Cluster/Adsorbate Compl
职业生涯:确保下一代化学家的质量,并探索具有催化意义的金属簇/吸附物复合物的尺寸依赖性特性的步骤
  • 批准号:
    9875046
  • 财政年份:
    1999
  • 资助金额:
    $ 54.23万
  • 项目类别:
    Continuing Grant

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