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Towards a Merger of Nonadiabatic Molecular Dynamics and Spintronics

非绝热分子动力学与自旋电子学的合并

基本信息

批准号：
2102402
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：
Standard Grant
财政年份：
2021
资助国家：
美国
起止时间：
2021-06-01 至 2024-05-31
项目状态：
已结题

来源：
https://www.nsf.gov/awardsearch/showAward?AWD_ID=2102402&HistoricalAwards=false
关键词：
Towards Merger Nonadiabatic Molecular Dynamics

项目摘要

Joseph Subotnik of The University of Pennsylvania is supported by an award from the Chemical Theory, Models and Computational Methods program in the Division of Chemistry to study how electronic spin affects nuclear relaxation and can shape energy loss via heat production. In particular, Subotnik will develop new and powerful algorithms that quantify exactly how molecules with nuclei and spins relax after they have been excited by light. Subotnik will test both theoretically and computationally which atoms move during relaxation, and will explore the possibility that this atomic motion can lead to a promotion of spin-selectivity for long periods of time. All of the algorithmic developments will be released to the public in an open source fashion. This research program lies at the cutting edge of physical chemistry and spin-chemistry, and in the long term, research here has the potential to help create an entirely new form of device electronics based on electronic spin (so-called spintronics) unlike conventional devices based on electronic charge. The broader impacts include the Subotnik group's support for bringing undergraduate researchers into the lab, with a special emphasis on introducing members of underrepresented groups to hands-on science. The Subotnik research team also invites these students to participate the annual Penn Conference in Theoretical Chemistry (PCTC). Subotnik will develop a semi-classical algorithm for quantifying how coupled nuclear-electronic systems prepared out of equilibrium relax in the presence of spin-orbit coupling. In the presence of spin-orbit coupling, the electronic Hamiltonian becomes complex-valued and the nature of electronic transitions becomes very difficult for modern algorithms because (i) the direction of momentum rescaling becomes unclear and (ii) the presence of Berry magnetic forces can lead to novel reaction pathways. Subotnik is constructing and benchmarking a novel, reliable surface hopping approach to treat such conditions, both for the case of doublets (with two electronic states) as well as for the case of singlet-triplet crossings (with four electronic states). Furthermore, Subotnik will run simulations on reasonably small test cases to investigate whether the presence coupled nuclear-electronic dynamics effects (including Berry forces) may underlie recent experiments displaying a chiral induced spin selectivity (CISS) effect.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）获得了化学系化学理论、模型和计算方法项目的奖励，研究电子自旋如何影响核松弛，以及如何通过产热形成能量损失。特别是，Subotnik将开发新的强大算法，精确量化具有原子核和自旋的分子在被光激发后是如何放松的。Subotnik将从理论上和计算上测试哪些原子在弛豫过程中运动，并探索这种原子运动在很长一段时间内促进自旋选择性的可能性。所有的算法开发都将以开源的方式向公众发布。这个研究项目处于物理化学和自旋化学的前沿，从长远来看，这里的研究有可能帮助创造一种基于电子自旋（所谓的自旋电子学）的全新形式的设备电子学，而不是基于电子电荷的传统设备。更广泛的影响包括Subotnik小组支持将本科生研究人员引入实验室，并特别强调将代表性不足的群体成员引入实践科学。Subotnik研究小组还邀请这些学生参加一年一度的宾夕法尼亚大学理论化学会议（PCTC）。Subotnik将开发一种半经典算法，用于量化在自旋轨道耦合存在下脱离平衡状态的耦合核电子系统是如何松弛的。在存在自旋-轨道耦合的情况下，电子哈密顿量变得复杂，电子跃迁的性质对现代算法来说变得非常困难，因为(i)动量重新缩放的方向变得不清楚，（ii）贝里磁力的存在可能导致新的反应途径。Subotnik正在构建和测试一种新颖可靠的表面跳跃方法来处理这种情况，既适用于双重态（具有两个电子态），也适用于单重态-三重态交叉（具有四个电子态）。此外，Subotnik将在相当小的测试案例上进行模拟，以调查是否存在耦合的核电子动力学效应（包括Berry力）可能是最近显示手性诱导自旋选择性（CISS）效应的实验的基础。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 phase-space semiclassical approach for modeling nonadiabatic nuclear dynamics with electronic spin

用电子自旋模拟非绝热核动力学的相空间半经典方法

DOI：
10.1063/5.0093345
发表时间：
2022
期刊：
The Journal of Chemical Physics
影响因子：
0
作者：
Wu, Yanze;Bian, Xuezhi;Rawlinson, Jonathan I.;Littlejohn, Robert G.;Subotnik, Joseph E.
通讯作者：
Subotnik, Joseph E.

A quantum-classical Liouville formalism in a preconditioned basis and its connection with phase-space surface hopping

预处理基础上的量子经典刘维尔形式及其与相空间表面跳跃的联系