Here we propose a mechanism by which spin polarization can be generated dynamically in chiral molecular systems undergoing photo-induced electron transfer. The proposed mechanism explains how spin polarization emerges in systems where charge transport is dominated by incoherent hopping, mediated by spin orbit and electronic exchange couplings through an intermediate charge transfer state. We derive a simple expression for the spin polarization that predicts a non-monotonic temperature dependence consistent with recent experiments. We validate this theory using approximate quantum master equations and the numerically exact hierarchical equations of motion. The proposed mechanism of chirality induced spin selectivity should apply to many chiral systems, and the ideas presented here have implications for the study of spin transport at temperatures relevant to biology, and provide simple principles for the molecular control of spins in fluctuating environments.
The elucidation of the mechanisms behind chiral-induced spin selectivity remains an outstanding scientific challenge. Here we consider the role of delocalised phonon modes in electron transport in chiral structures and demonstrate that spin selectivity can originate from spin-dependent energy and momentum conservation in electron-phonon scattering events. While this mechanism is robust to the specifical nature of the vibrational modes, the degree of spin polarization depends on environmental factors, such as external driving fields, temperatures and phonon relaxation rates. This dependence is …
Symmetry considerations in chirality-induced spin selectivity
Helmholtz-Institut Mainz（亥姆霍兹美因茨研究所）；GSI Helmholtzzentrum für Schwerionenforschung GmbH（GSI重离子研究中心有限公司）；QUANTUM, Institut für Physik, Johannes Gutenberg-Universität（约翰内斯·古腾堡大学量子物理研究所）；Department of Physics, University of California（加州大学物理系）；Institute of Physics, Johannes Gutenberg-University Mainz（约翰内斯·古腾堡大学美因茨分校物理研究所）
Electron exchange and correlations emerging from the coupling between ionic vibrations and electrons are addressed. Spin-dependent electron-phonon coupling originates from the spin-orbit interaction, and it is shown that such electron-phonon coupling introduces exchange splitting between the spin channels in the structure. By application of these results to a model for a chiral molecular structure mounted between metallic leads, the chirality induced spin selectivity is found to become several tens of percents using experimentally feasible parameters.
We report a new type of spin-orbit coupling (SOC) called geometric SOC. Starting from the relativistic theory in curved space, we derive an effective nonrelativistic Hamiltonian in a generic curve embedded into flat three dimensions. The geometric SOC is $O(m^{-1})$, in which $m$ is the electron mass, and hence much larger than the conventional SOC of $O(m^{-2})$. The energy scale is estimated to be a hundred meV for a nanoscale helix. We calculate the current-induced spin polarization in a coupled-helix model as a representative of the chirality-induced spin selectivity. We find that it depen…
The chirality-induced spin selectivity (CISS) effect gives rise to strongly spin-dependent transport through many organic molecules and structures. Its discovery raises fascinating fundamental questions as well as the prospect of possible applications. The basic phenomenology, a strongly asymmetric magnetoresistance despite the absence of magnetism, is now understood to result from the combination of spin-orbit coupling and chiral geometry. However, experimental signatures of electronic helicity were observed at room temperature, i.e., at an energy scale that exceeds the typical spin-orbit cou…
The chirality-induced spin selectivity (CISS) effect has been confirmed experimentally for a large class of organic molecules. Adequately modeling the effect remains a challenging task, with both phenomenological models and first-principle simulations yielding inconclusive results. Building upon a previously presented model by K. Michaeli and R. Naaman (J. Phys. Chem C 123, 17043 (2019)) we systematically investigate an effective 1-dimensional model derived as the limit of a 3-dimensional quantum system with strong confinement and including spin-orbit coupling. Having a simple analytic structu…
Chirality-induced spin selectivity (CISS) refers to the fact that electrons get spin polarized after passing through organic chiral molecules in a nanoscale device. In CISS, chiral molecules are commonly believed to be a spin filter through which one favored spin transmits and the opposite spin gets reflected, i.e., transmitted and reflected electrons exhibit opposite spin polarization. In this work, we point out that such a spin filter scenario contradicts the principle that equilibrium spin current must vanish. Instead, we find that both transmitted and reflected electrons present the same t…
Chirality induced spin selectivity, discovered about two decades ago in helical molecules, is a non-equilibrium effect that emerges from the interplay between geometrical helicity and spin-orbit interactions. Several model Hamiltonians building on this interplay have been proposed and while these can yield spin-polarized transport properties that agrees with experimental observations, they simultaneously depend on unrealistic values of the spin-orbit interaction parameters. It is likely, however, that a common deficit originates from the fact that all these models are uncorrelated, or, single-…
Real Space Imaging of Spin Scattering in Chirality-Induced Spin Selectivity
Ulsan National Institute of Science and Technology (UNIST)（蔚山科学技术院）；Weizmann Institute of Science（魏茨曼科学研究所）；Pennsylvania State University（宾夕法尼亚州立大学）；Max Planck Institute for the Structure and Dynamics of Matter（物质结构与动力学马普研究所）
Chirality-induced spin selectivity due to an emergent molecular orbital moment
The Institute of Physics of the Czech Academy of Sciences（捷克科学院物理研究所）；Institute of Physics, Johannes Gutenberg-University（约翰内斯·古腾堡大学物理研究所）；Peter Grünberg Institut (PGI-6), Forschungszentrum Jülich GmbH（于利希研究中心彼得·格林伯格研究所（PGI-6））
What Is the Real-Time Atomistic Mechanism Behind Chirality-Induced Spin Selectivity in Donor-Chiral Bridge-Acceptor Molecules?
School of Physics and Wuhan National High Magnetic Field Center, Huazhong University of Science and Technology（华中科技大学物理学院与武汉国家强磁场中心）；Institute for Quantum Science and Engineering, Huazhong University of Science and Technology（华中科技大学量子科学与工程研究院）
Emergent chirality and enantiomeric selectivity in layered NbOX$_2$ crystals
Aalto University（阿尔托大学）；Max Planck Institute for Chemical Physics of Solids（马克斯·普朗克固体化学物理研究所）；Centro de Física de Materiales (CFM-MPC), CSIC-UPV/EHU（材料物理中心，西班牙国家研究委员会-巴斯克国立大学）；University of the Basque Country (UPV/EHU)（巴斯克国立大学）；Donostia International Physics Center (DIPC)（圣塞巴斯蒂安国际物理中心）；Université de Sherbrooke（舍布鲁克大学）；Regroupement Québécois sur les Matériaux de Pointe (RQMP)（魁北克尖端材料联盟）
研究层状NbOX₂晶体的结构和电子性质，揭示其非手性I m m m相与手性C2相之间的联系，通过原理计算发现中间非手性C2/m相，并探讨电场和压力对手性稳定的影响。
A minimal model is exactly solved for electron spin transport on a helix. Electron transport is assumed to be supported by well oriented $p_z$ type orbitals on base molecules forming a staircase of definite chirality. In a tight binding interpretation, the SOC opens up an effective $π_z-π_z$ coupling via interbase $p_{x,y}-p_z$ hopping, introducing spin coupled transport. The resulting continuum model spectrum shows two Kramers doublet transport channels with a gap proportional to the SOC. Each doubly degenerate channel satisfies time reversal symmetry, nevertheless, a bias chooses a transport…
Non-equilibrium angular momentum selectivity and filtering in chiral carbon nanotubes
School of Engineering, Mackenzie Presbyterian University（麦肯锡福音大学工程学院）；MackGraphe Graphene and Nanomaterials Research Institute, Mackenzie Presbyterian University（麦肯锡福音大学MackGraphe石墨烯与纳米材料研究所）；Departamento de Física, Universidade Federal do Ceará（塞阿拉联邦大学物理系）
Central to spintronics is the interconversion between electronic charge and spin currents, and this can arise from the chirality-induced spin selectivity (CISS) effect. CISS is often studied as magnetoresistance (MR) in two-terminal (2T) electronic devices containing a chiral (molecular) component and a ferromagnet. However, fundamental understanding of when and how this MR can occur is lacking. Here, we uncover an elementary mechanism that generates such a MR for nonlinear response. It requires energy-dependent transport and energy relaxation within the device. The sign of the MR depends on c…
Revealing Wavelength- and Size-Dependent CO2 Reduction Selectivity via Operando Scanning Photo-Electrochemical Microscopy
École Polytechnique Fédérale de Lausanne（洛桑联邦理工学院）；Institute of Chemical Research of Catalonia (ICIQ-CERCA), The Barcelona Institute of Science and Technology（加泰罗尼亚化学研究所（ICIQ-CERCA），巴塞罗那科学与技术研究院）；Scuola Superiore Meridionale（南方高等学院）；Rensselaer Polytechnic Institute（伦斯勒理工学院）
Topological aspects of the geometry of DNA and similar chiral molecules have received a lot of attention, while the topology of their electronic structure is less explored. Previous experiments have revealed that DNA can efficiently filter spin-polarized electrons between metal contacts, a process called chiral-induced spin-selectivity (CISS). However, the underlying correlation between chiral structure and electronic spin remains elusive. In this work, we reveal an orbital texture in the band structure, a topological characteristic induced by the chirality. We find that this orbital texture e…
Photon-energy-programmable subnanometric electron birth-site control
Research Institute of Electronics (RIE), Shizuoka University（静冈大学电子研究所）；Department of Energy and Materials Engineering, Faculty of Science and Engineering, Kindai University（近畿大学理工学部能源材料工程系）；RIKEN Center for Quantum Computing (RQC)（理化学研究所量子计算中心）
Max-Born-Institut（马克斯·博恩研究所）；Insitute of Physics, Humboldt University zu Berlin（柏林洪堡大学物理研究所）；Technion - Israel Institute of Technology（以色列理工学院）；School of Molecular Sciences, Arizona State University（亚利桑那州立大学分子科学学院）；Department of Physics, Imperial College London（伦敦帝国理工学院物理系）；Department of Physics, Freie Universität Berlin（柏林自由大学物理系）；Technische Universität Berlin（柏林工业大学）
We report chirality-induced current-in-plane magnetoresistance (CIP-MR) in chiral molecule/ferromagnetic metal bilayer at room temperature. The previously reported chiralityinduced current-perpendicular-to-plane magnetoresistance (CPP-MR) originates from the chiral induced spin-selectivity (CISS) effect that needs charge-current passing through the molecule. In contrast, the observed CIP-MR in the present study requires no bias charge current through the molecule. The temperature dependence of CIP-MR suggests thermally induced spin-polarization in the chiral molecules is the key for the observ…
