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Femtosecond Studies of the Influence of Solvent on Chemical Reaction Dynamics

溶剂对化学反应动力学影响的飞秒研究

基本信息

批准号：
1665532
负责人：
Stephen Bradforth
金额：
$ 46.4万
依托单位：
University of Southern California
依托单位国家：
美国
项目类别：
Standard Grant
财政年份：
2017
资助国家：
美国
起止时间：
2017-08-01 至 2023-07-31
项目状态：
已结题

来源：
https://www.nsf.gov/awardsearch/showAward?AWD_ID=1665532&HistoricalAwards=false
关键词：
Femtosecond Studies Influence Solvent Chemical

项目摘要

In this project funded by the Chemical Structure Dynamics and Mechanism (CDSM-A) program of the Chemistry Division, Professor Stephen Bradforth of the University of Southern California is using photo-electron spectroscopy (PES) and other laser-based techniques to study the structure of liquid ammonia. PES is a technique that uses light to remove electrons from an atom or molecule. By measuring the energy of these electrons, information can be obtained about the structure of the molecule as well as its interactions with other nearby molecules. The Bradforth group is also studying what happens to the interactions between ammonia molecules when extra electrons are dissolved in the liquid. Liquid ammonia was chosen because it can dissolve higher concentrations of electrons, is similar to water in its structure, and because ammonia is relevant to a number of important industrial processes. Since the PES technique involves removal of electrons from molecules caused by light, the research may also provide insights into similar processes such as the damage to living cells caused by light (for example, during cancer radiation therapy). Students and postdocs involved in the project receive training in building instrumentation for new instruments and benefit from training in international labs. As part of the broader impact of this project, Professor Bradforth is continuing an outreach project that provides hands-on summer internships for students from Cerritos College, a minority-serving community college.This research project explores the electronic structure of the hydrogen-bonding liquid ammonia, and the relationship of this structure to that of water. A central focus of the project is to establish how the electronic density of states can be manipulated by solute dopants. The specific objectives of the project are: (i) to determine the liquid valence band orbital delocalization from experimental photoelectron spectroscopy (PES) and photoelectron angular distribution (PAD) measurements; (ii) to identify isolated solvated electrons, spin-paired dielectrons, and the metal-insulator transition at high excess electron concentration using pump-probe PES measurements of liquid ammonia containing solvated electrons (supplied by alkali metals), and (iii) to characterize low-lying conduction band states and their coupling to localized molecular doorway states using continuous two-photon absorption spectroscopy. The transient absorption and photoelectron spectroscopy work is being done in Professor Bradforth's laboratory at USC. The angle-resolved tunable X-ray photoelectron spectroscopy (PAD) studies are being conducted at the Hamburg and Berlin synchrotron light sources.

在这个由化学系化学结构动力学和机制（CDSM-A）项目资助的项目中，南加州大学的Stephen Bradforth教授正在使用光电子能谱（PES）和其他基于激光的技术来研究液氨的结构。 PES是一种利用光从原子或分子中去除电子的技术。通过测量这些电子的能量，可以获得有关分子结构及其与附近其他分子相互作用的信息。布拉德福斯小组还在研究当额外的电子溶解在液体中时，氨分子之间的相互作用会发生什么。选择液氨是因为它可以溶解更高浓度的电子，在结构上与水相似，并且因为氨与许多重要的工业过程有关。由于PES技术涉及从光引起的分子中去除电子，因此该研究还可以提供对类似过程的见解，例如光引起的活细胞损伤（例如，在癌症放射治疗期间）。参与该项目的学生和博士后接受为新仪器建造仪器的培训，并从国际实验室的培训中受益。作为该项目更广泛影响的一部分，Bradforth教授正在继续一个外展项目，为Cerritos学院（一所为少数民族服务的社区学院）的学生提供暑期实习机会，该研究项目探讨了氢键液态氨的电子结构，以及这种结构与水的结构之间的关系。该项目的一个中心焦点是建立如何通过溶质掺杂剂来操纵电子态密度。该项目的具体目标是：（一）通过实验光电子能谱和光电子角分布测量确定液体价带轨道离域;（ii）识别孤立的溶剂化电子，自旋配对双电子，以及利用泵浦-探测PES测量含有溶剂化电子的液氨在高过量电子浓度下的金属-绝缘体转变（由碱金属提供），和（iii）使用连续双光子吸收光谱来表征低位导带态及其与局部分子门口态的耦合。瞬态吸收和光电子能谱的工作正在南加州大学的布拉德福德教授的实验室进行。角分辨可调谐X射线光电子能谱（PAD）的研究正在汉堡和柏林同步加速器光源进行。

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）

New Insights into the Charge-Transfer-to-Solvent Spectrum of Aqueous Iodide: Surface versus Bulk

DOI：
10.1021/acs.jpclett.9b03857
发表时间：
2020-03-05
期刊：
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
影响因子：
5.7
作者：
Bhattacharyya, Dhritiman;Mizuno, Hikaru;Bradforth, Stephen E.
通讯作者：
Bradforth, Stephen E.

Spectroscopic evidence for a gold-coloured metallic water solution

DOI：
10.1038/s41586-021-03646-5
发表时间：
2021-07-29
期刊：
NATURE
影响因子：
64.8
作者：
Mason, Philip E.;Schewe, H. Christian;Jungwirth, Pavel
通讯作者：
Jungwirth, Pavel

Electronic Structure of Liquid Methanol and Ethanol from Polarization-Dependent Two-Photon Absorption Spectroscopy

通过偏振相关双光子吸收光谱研究液体甲醇和乙醇的电子结构

DOI：
10.1021/acs.jpca.9b04040
发表时间：
2019
期刊：
The Journal of Physical Chemistry A
影响因子：
0
作者：
Bhattacharyya, Dhritiman;Zhang, Yuyuan;Elles, Christopher G.;Bradforth, Stephen E.
通讯作者：
Bradforth, Stephen E.

Electronic Structure of Liquid Alkanes: A Representative Case of Liquid Hexanes and Cyclohexane Studied Using Polarization-Dependent Two-Photon Absorption Spectroscopy

液体烷烃的电子结构：使用偏振相关双光子吸收光谱研究液体己烷和环己烷的代表案例

DOI：
10.1021/acs.jpca.1c06230
发表时间：
2021
期刊：
The Journal of Physical Chemistry A
影响因子：
0
作者：
Bhattacharyya, Dhritiman;Zhang, Yuyuan;Elles, Christopher G.;Bradforth, Stephen E.
通讯作者：
Bradforth, Stephen E.

Valence and Core-Level X-ray Photoelectron Spectroscopy of a Liquid Ammonia Microjet