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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：
Caroline Jarrold
金额：
$ 54.23万
依托单位：
Indiana University
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

来源：
https://www.nsf.gov/awardsearch/showAward?AWD_ID=2053889&HistoricalAwards=false
关键词：
Deep Dive into Electron Neutral

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.

在这个由化学系化学结构动力学和机理(CSDM-A)计划资助的项目中，印第安纳大学的Caroline Chick Jarroeld教授和她的学生正在使用几种复杂的实验技术来研究电子和中性分子之间的相互作用，这些技术基于被研究的化合物对光的吸收和发射。电子-中性相互作用推动了许多重要的化学和物理过程，但它们很难在实验上探索。从实用的角度来看，控制电子很有挑战性，因为它们比原子轻几千倍，而原子本身是微小的粒子，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弱影响力量。贾罗尔德教授克服了这些障碍，他以一种受控的方式准备了自由电子，即用激光脉冲瞄准带负电荷的分子，这种脉冲可以移除具有已知能量的电子，并位于中性目标分子所希望的附近。选择用于研究的分子阵列是为了对影响它们与电子相互作用的广泛性质进行采样。这些实验涉及光电子作为探测分子和双分子络合物的价束缚、非价束缚和临时阴离子状态的工具的新用途，重点是制备和探测不整齐地归入这三类中的任何一种的系统。这个项目解决了几个假设，涉及描述电子驱动的化学，电子-双分子相互作用日益复杂的图景，以及支配非价结合阴离子寿命的规则。用能量选择的电子在实验上探测这些体系是通过分离阴离子前体实现的，这为绘制电子-中性相互作用的能量依赖关系提供了一条途径，其中一些相互作用启动了电子驱动的化学。其他研究包括阴离子非价束缚激发态的荧光寿命和色散荧光测量。路易斯安那大学东南分校的合作者Thomas Sommerfeld教授在阴离子非价态的理论处理方面拥有专业知识，他对收集到的关于这些复杂且往往是瞬变的物种的数据的解释得到了合作者托马斯·索默菲尔德教授的计算支持。更广泛的影响包括对电子驱动的化学和物理过程的更完整的了解，这是控制这些过程的先决条件。此外，该项目的参与者在致力于多样性和公平的PI的实验室接受一系列化学物理技术的全面研究生或博士后培训，以及充足的职业发展机会。该奖项反映了NSF的法定使命，并通过使用基金会的智力优势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：
The Journal of Physical Chemistry A
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：
The Journal of Physical Chemistry C
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：
The Journal of Physical Chemistry A
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：
The Journal of Physical Chemistry A
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