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Collaborative Research: Electronic Coherence Effects in Multichromophore Systems Probed by Two-Dimensional Electronic Spectroscopy

合作研究：二维电子光谱探测多发色团系统中的电子相干效应

基本信息

批准号：
1955795
负责人：
Felix Castellano
金额：
$ 22.5万
依托单位：
North Carolina State University
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：
2020-08-15 至 2023-07-31
项目状态：
已结题

来源：
https://www.nsf.gov/awardsearch/showAward?AWD_ID=1955795&HistoricalAwards=false
关键词：
Collaborative Research Electronic Coherence Effects

项目摘要

In this collaborative project, co-funded by the Chemical Structure, Dynamics & Mechanisms B and the Chemical Structure, Dynamics & Mechanisms A programs of the Chemistry Division, Professor Lin X. Chen of the Department of Chemistry at Northwestern University and Professor Felix N. Castellano from the Department of Chemistry at North Carolina State University lead a project to understand the effects of coherent electronic motions in energy and electron transfer in distinct classes of multi-chromophoric synthetic platforms. The knowledge obtained through the proposed studies will greatly enhance the ability to rationally design chemical materials/devices for catalysis, optoelectronics, and energy sustainability. The proposed research engages University graduate students to use advanced laser spectroscopy for characterization, incorporates state-of-the-art computational chemistry for quantum mechanical and molecular dynamics modeling, and utilizes advanced chemistry laboratory facilities for molecular syntheses and structural characterization, engendering them with expansive training necessary for the development of multidisciplinary scientific expertise. The proposed research/education activities are integrated with numerous K-12 public outreach activities at both universities, including Photonics Day at North Carolina State University and NU Bond at Northwestern University. Specifically, they will employ newly developed two-dimensional electronic spectroscopy in their studies with very high time resolution of approximately 6 femtoseconds. The rationally designed molecules are engineered to tune electronic coupling in their excited states, which are either responsible for or can be correlated to electronic coherence originating from in-phase motions of electrons induced by photoexcitation. The measured coherences will be correlated with the observation of photoinduced intramolecular energy and/or electron transfer chemistry and rationalized using continuously developing theory to assess the role of electronic and/or vibronic coherence in these fundamental primary processes related to light activation. Two types of molecular designs are targeted for these investigations: (1) Pt(II) dimers bridged by hydroxypyridines featuring metal-metal-to-ligand charge transfer excited states where a metal-metal bond is transiently formed following light excitation; and (2) Pt(II) dimers whose terminal cyclometalating ligands are decorated with bay-substituted naphthalenediimide based energy and/or electron acceptors. The proposed project seeks to glean new insight into excited state chemistry and how this knowledge can be leveraged to control reactivity in condensed phases, molecular photonics, and photocatalysis.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B和化学结构、动力学和机理A项目共同资助的合作项目中，西北大学化学系的陈林教授和北卡罗来纳州立大学化学系的Felix N.Castellano教授领导了一个项目，以了解相干电子运动在不同类别的多发色合成平台中的能量和电子转移的影响。通过拟议的研究获得的知识将极大地提高合理设计用于催化、光电子学和能源可持续性的化学材料/器件的能力。这项拟议的研究邀请大学研究生使用先进的激光光谱学进行表征，结合最先进的计算化学进行量子力学和分子动力学建模，并利用先进的化学实验室设施进行分子合成和结构表征，为他们提供发展多学科科学专业知识所需的广泛培训。拟议的研究/教育活动与两所大学的许多K-12公共推广活动相结合，包括北卡罗来纳州立大学的光子学日和西北大学的Nu Bond。具体地说，他们将在研究中使用新开发的二维电子光谱学，时间分辨率非常高，约为6飞秒。经过合理设计的分子被设计成在其激发态中调节电子耦合，这些激发态要么与由光激发诱导的电子的同相运动产生的电子相干有关，要么与之相关。测量的相干性将与光诱导分子内能量和/或电子转移化学的观测相关联，并使用不断发展的理论来合理地评估电子和/或振动相干性在这些与光激活相关的基本初级过程中的作用。这些研究针对两种类型的分子设计：(1)以羟基吡啶为桥联的二聚体，其特征是金属-金属-配体电荷转移激发态，其中金属-金属键在光激发后瞬间形成；以及(2)铂(II)二聚体，其末端的环化配体用海湾取代的萘亚胺基能量和/或电子受体修饰。拟议的项目旨在收集关于激发态化学以及如何利用这些知识来控制凝聚相、分子光子学和光催化中的反应性的新见解。这一奖项反映了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（11）

专著数量（0）

科研奖励数量（0）

会议论文数量（0）

专利数量（0）

Photochemical H 2 Evolution from Bis(diphosphine)nickel Hydrides Enables Low-Overpotential Electrocatalysis

双(二膦)镍氢化物光化学演化H 2 可实现低过电势电催化

DOI：
10.1021/jacs.1c10628
发表时间：
2021
期刊：
Journal of the American Chemical Society
影响因子：
15
作者：
Stratakes, Bethany M.;Wells, Kaylee A.;Kurtz, Daniel A.;Castellano, Felix N.;Miller, Alexander J.
通讯作者：
Miller, Alexander J.

General Design Rules for Bimetallic Platinum(II) Complexes

DOI：
10.1021/acs.jpca.1c05044
发表时间：
2021-10-26
期刊：
JOURNAL OF PHYSICAL CHEMISTRY A
影响因子：
2.9
作者：
Mills, Alexis W.;Valentine, Andrew J. S.;Li, Xiaosong
通讯作者：
Li, Xiaosong

Metal–Metal-to-Ligand Charge Transfer in Pt(II) Dimers Bridged by Pyridyl and Quinoline Thiols

由吡啶基和喹啉硫醇桥接的 Pt(II) 二聚体中的金属 - 金属到配体的电荷转移

DOI：
10.1021/acs.inorgchem.1c02469
发表时间：
2022
期刊：
Inorganic Chemistry
影响因子：
4.6
作者：
Roy, Subhangi;Lopez, Antonio A.;Yarnell, James E.;Castellano, Felix N.
通讯作者：
Castellano, Felix N.

Ligand-Structure-Dependent Coherent Vibrational Wavepacket Dynamics in Pyrazolate-Bridged Pt(II) Dimers

吡唑酯桥 Pt(II) 二聚体中配体结构依赖性相干振动波包动力学

DOI：
10.1021/acs.jpcc.2c02256
发表时间：
2022
期刊：
The Journal of Physical Chemistry C
影响因子：
0
作者：
Kim, Tae Wu;Kim, Pyosang;Mills, Alexis W.;Chakraborty, Arnab;Kromer, Sarah;Valentine, Andrew J.;Castellano, Felix N.;Li, Xiaosong;Chen, Lin X.
通讯作者：
Chen, Lin X.

Ultrafast Excited-State Dynamics of Photoluminescent Pt(II) Dimers Probed by a Coherent Vibrational Wavepacket