Chiesa Alessandro, Garlatti Elena, Mezzadri Matteo, Celada Leonardo, Sessoli Roberta, Wasielewski Michael R, Bittl Robert, Santini Paolo, Carretta Stefano
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.
Nano Lett. 2024 Oct 2;24(39):12133-12139. doi: 10.1021/acs.nanolett.4c02912. Epub 2024 Sep 22.
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.
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。