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The Dynamics and Spectroscopy of Intersystem-Crossing in Solution and at Metal Surfaces

溶液中和金属表面的系间窜越的动力学和光谱学

基本信息

批准号：
1764365
负责人：
Joseph Subotnik
金额：
$ 45万
依托单位：
University of Pennsylvania
依托单位国家：
美国
项目类别：
Continuing Grant
财政年份：
2018
资助国家：
美国
起止时间：
2018-05-01 至 2022-04-30
项目状态：
已结题

来源：
https://www.nsf.gov/awardsearch/showAward?AWD_ID=1764365&HistoricalAwards=false
关键词：
Dynamics Spectroscopy Intersystem Crossing Solution

项目摘要

Joseph Subotnik of the University of Pennsylvania is supported by an award from the Theory, Models and Computational Methods program in the Chemistry division to develop new computational and theoretical techniques for uncovering when and how molecules change spin state and potentially emit light in the form of phosphorescence (which is commonly observed). Subotnik is also exploring how the presence of a metal surface affects changes in spin state. The software tools developed by this proposal are being released on the PI's github page and in modern electronic structure packages, e.g. Q-Chem. The outreach activities of this proposal include an annual conference in theoretical chemistry (the Penn Conference in Theoretical Chemistry) which is very inexpensive for the public (and often free) and which also offers exceptional graduate students and postdocs the chance to speak. In more detail, Subotnik and his research group are developing computational tools in both electronic structure and dynamics for quantifying spin crossovers, so that one can monitor the flow of energy and population in the condensed phase. On the electronic structure side, they are calculating energies, gradients and derivative couplings that are consistent with most nonadiabatic dynamics algorithms. On the dynamics side, Subotnik and coworkers are formulating a theory of the electronic friction tensor at a metal surface that is consistent with spin-orbit coupling, so that the effects of spin changes near a metal surface can be estimated and the branching of triplet states can be quantified. The Subotnik group is also investigating how spin effects enter into semiclassical electrodynamics, beyond mean-field theory.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.

宾夕法尼亚大学的约瑟夫·苏博特尼克（Joseph Subotnik）获得了化学学部理论、模型和计算方法项目的奖励，他开发了新的计算和理论技术，用于揭示分子何时以及如何改变自旋状态，并可能以磷光的形式发光（这是普遍观察到的）。Subotnik也在探索金属表面的存在如何影响自旋态的变化。由该提案开发的软件工具正在PI的github页面和现代电子结构包（例如Q-Chem）中发布。该提案的推广活动包括一年一度的理论化学会议（宾夕法尼亚大学理论化学会议），该会议对公众来说非常便宜（通常是免费的），并且还为优秀的研究生和博士后提供发言的机会。更详细地说，Subotnik和他的研究小组正在开发用于量化自旋交叉的电子结构和动力学的计算工具，这样人们就可以监控凝聚态中的能量和人口流动。在电子结构方面，他们正在计算与大多数非绝热动力学算法一致的能量、梯度和导数耦合。在动力学方面，Subotnik和同事正在制定一个金属表面的电子摩擦张量理论，该理论与自旋-轨道耦合一致，因此可以估计金属表面附近自旋变化的影响，并且可以量化三重态的分支。Subotnik小组也在研究自旋效应如何超越平均场理论进入半经典电动力学。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）

A “backtracking” correction for the fewest switches surface hopping algorithm

针对最少开关表面跳跃算法的“回溯”修正

DOI：
10.1063/5.0022436
发表时间：
2020
期刊：
The Journal of Chemical Physics
影响因子：
0
作者：
Miao, Gaohan;Bian, Xuezhi;Zhou, Zeyu;Subotnik, Joseph
通讯作者：
Subotnik, Joseph

A Necessary Trade-off for Semiclassical Electrodynamics: Accurate Short-Range Coulomb Interactions versus the Enforcement of Causality?

半经典电动力学的必要权衡：准确的短程库仑相互作用与因果关系的执行？

DOI：
10.1021/acs.jpclett.8b02309
发表时间：
2018
期刊：
The Journal of Physical Chemistry Letters
影响因子：
0
作者：
Li, Tao E.;Chen, Hsing-Ta;Nitzan, Abraham;Sukharev, Maxim;Subotnik, Joseph E.
通讯作者：
Subotnik, Joseph E.

TD-DFT spin-adiabats with analytic nonadiabatic derivative couplings

具有解析非绝热导数耦合的 TD-DFT 自旋绝热

DOI：
10.1063/1.5126440
发表时间：
2020
期刊：
The Journal of Chemical Physics
影响因子：
0
作者：
Bellonzi, Nicole;Alguire, Ethan;Fatehi, Shervin;Shao, Yihan;Subotnik, Joseph E.
通讯作者：
Subotnik, Joseph E.

A demonstration of consistency between the quantum classical Liouville equation and Berry’s phase and curvature for the case of complex Hamiltonians

复数哈密顿量情况下量子经典刘维尔方程与贝里相位和曲率之间的一致性证明