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arXiv 2503.09286cond-mat.mes-hallphysics.chem-ph
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量子振动效应对分子结中电荷输运自旋极化的作用

The Role of Quantum Vibronic Effects in the Spin Polarization of Charge Transport through Molecular Junctions

Samuel L. Rudge, Christoph Kaspar, Rudolf Smorka, Riley J. Preston, Joseph Subotnik, Michael Thoss

AI总结:

本文利用数值精确的层级运动方程方法研究分子结中量子振动对电荷输运自旋极化的影响,发现低电压非共振区存在显著的振动辅助自旋极化,并将其与振动角动量和激发关联,证明该效应在广泛参数范围内具有鲁棒性。

摘要:

分子振动与通过分子结的电荷输运中的自旋极化之间的联系目前是一个备受关注的话题,对诸如手性诱导自旋选择性(CISS)等多种现象具有重要影响。在本工作中,我们沿此主题探索分子结中振动动力学与非平衡电荷电流相应自旋极化之间的关系。我们采用层级运动方程(HEOM)方法,由于该方法数值精确且对振动自由度进行量子力学处理,它扩展了此前依赖近似输运方法的类似模型分析。我们发现在非共振、低电压区域电荷电流存在显著的自旋极化,在该区域振动必须进行量子力学处理。此外,我们能够将电荷输运中的自旋极化与振动动力学的相应极化联系起来,后者表现为振动角动量和激发。我们的分析涵盖多种分子-电极耦合、温度、轨道能量和自旋轨道耦合,表明振动辅助的自旋极化在广泛的参数范围内具有鲁棒性。

英文摘要:

The connection between molecular vibrations and spin polarization in charge transport through molecular junctions is currently a topic of high interest, with important consequences for a variety of phenomena, such as chirality-induced spin selectivity (CISS). In this work, we follow this theme by exploring the relationship between vibronic dynamics and the corresponding spin polarization of the nonequilibrium charge current in a molecular junction. We employ the hierarchical equations of motion (HEOM) approach, which, since it is numerically exact and treats the vibrational degrees of freedom quantum mechanically, extends previous analyses of similar models that relied on approximate transport methods. We find significant spin polarization of the charge current in the off-resonant, low-voltage regime, where the vibrations must be treated quantum mechanically. Furthermore, we are able to connect the spin polarization in the charge transport to a corresponding polarization of the vibrational dynamics, which manifests itself in the vibrational angular momentum and excitation. Our analysis covers multiple molecule-lead couplings, temperatures, orbital energies, and spin-orbit couplings, demonstrating that the vibrationally assisted spin polarization is robust across a broad range of parameters.

机构、总结、中文摘要均由AI分析而来,可能存在错误,请以论文正文为准。

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