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电子转移中手性诱导自旋选择性的多体模型

Many-Body Models for Chirality-Induced Spin Selectivity in Electron Transfer.

作者信息

Chiesa Alessandro, Garlatti Elena, Mezzadri Matteo, Celada Leonardo, Sessoli Roberta, Wasielewski Michael R, Bittl Robert, Santini Paolo, Carretta Stefano

机构信息

Dipartimento di Scienze Matematiche, Fisiche e Informatiche, Università di Parma, I-43124 Parma, Italy.

INFN-Sezione di Milano-Bicocca, gruppo collegato di Parma, 43124 Parma, Italy.

出版信息

Nano Lett. 2024 Oct 2;24(39):12133-12139. doi: 10.1021/acs.nanolett.4c02912. Epub 2024 Sep 22.

DOI:10.1021/acs.nanolett.4c02912
PMID:39306768
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC11450995/
Abstract

We present the first microscopic model for the chirality-induced spin selectivity effect in electron-transfer, in which the internal degrees of freedom of the chiral bridge are explicitly included. By exactly solving this model on short chiral chains we demonstrate that a sizable spin polarization on the acceptor arises from the interplay of coherent and incoherent dynamics, with strong electron-electron correlations yielding many-body states on the bridge as crucial ingredients. Moreover, we include the coherent and incoherent dynamics induced by interactions with vibrational modes and show that they can play an important role in determining the long-time polarized state probed in experiments.

摘要

我们提出了第一个用于电子转移中手性诱导自旋选择性效应的微观模型,其中明确包含了手性桥的内部自由度。通过在短手性链上精确求解该模型,我们证明了受体上可观的自旋极化源于相干和非相干动力学的相互作用,强电子-电子关联在桥上产生多体状态是关键因素。此外,我们考虑了与振动模式相互作用引起的相干和非相干动力学,并表明它们在确定实验中探测的长时间极化状态方面可以发挥重要作用。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2044/11450995/754caa72fe2d/nl4c02912_0004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2044/11450995/2e724ca319d8/nl4c02912_0001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2044/11450995/7fe657fd120d/nl4c02912_0002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2044/11450995/f7697654ded5/nl4c02912_0003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2044/11450995/754caa72fe2d/nl4c02912_0004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2044/11450995/2e724ca319d8/nl4c02912_0001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2044/11450995/7fe657fd120d/nl4c02912_0002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2044/11450995/f7697654ded5/nl4c02912_0003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2044/11450995/754caa72fe2d/nl4c02912_0004.jpg

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本文引用的文献

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Chiral Induced Spin Selectivity.手性诱导自旋选择性
Chem Rev. 2024 Feb 28;124(4):1950-1991. doi: 10.1021/acs.chemrev.3c00661. Epub 2024 Feb 16.
2
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Science. 2023 Oct 13;382(6667):197-201. doi: 10.1126/science.adj5328. Epub 2023 Oct 12.
3
Efficient Spin-Selective Electron Transport at Low Voltages of Thia-Bridged Triarylamine Hetero[4]helicenes Chemisorbed Monolayer.硫桥连三芳基胺杂[4]螺旋烯化学吸附单层在低电压下的高效自旋选择性电子传输
分子水平上的手性诱导自旋选择性:理解和利用该现象的不同视角
J Phys Chem Lett. 2025 May 29;16(21):5358-5372. doi: 10.1021/acs.jpclett.5c00755. Epub 2025 May 21.
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Chiral Induced Spin Polarized Electron Current: Origin of the Chiral Induced Spin Selectivity Effect.手性诱导自旋极化电子电流:手性诱导自旋选择性效应的起源
J Phys Chem Lett. 2025 May 1;16(17):4346-4353. doi: 10.1021/acs.jpclett.5c00104. Epub 2025 Apr 24.
ACS Nano. 2023 Aug 8;17(15):15189-15198. doi: 10.1021/acsnano.3c04878. Epub 2023 Jul 26.
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Spin selective charge recombination in chiral donor-bridge-acceptor triads.手性给体-桥-受体三联体中的自旋选择性电荷复合。
J Chem Phys. 2023 May 21;158(19). doi: 10.1063/5.0150269.
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Chirality-Induced Spin Selectivity: An Enabling Technology for Quantum Applications.手性诱导自旋选择性:量子应用的一项使能技术。
Adv Mater. 2023 Jul;35(28):e2300472. doi: 10.1002/adma.202300472. Epub 2023 May 12.
6
Chiral-Induced Spin Selectivity and Non-equilibrium Spin Accumulation in Molecules and Interfaces: A First-Principles Study.手性诱导的自旋选择性和分子与界面中非平衡自旋积累:第一性原理研究。
J Phys Chem Lett. 2023 Jan 26;14(3):694-701. doi: 10.1021/acs.jpclett.2c03747. Epub 2023 Jan 13.
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J Phys Chem Lett. 2022 Jan 27;13(3):808-814. doi: 10.1021/acs.jpclett.1c03925. Epub 2022 Jan 24.
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Theory of Chirality Induced Spin Selectivity: Progress and Challenges.手性诱导自旋选择性理论:进展与挑战
Adv Mater. 2022 Apr;34(13):e2106629. doi: 10.1002/adma.202106629. Epub 2022 Feb 10.
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