Organic materials are known to feature long spin-diffusion times, originating in a generally small spin-orbit coupling observed in these systems. From that perspective, chiral molecules acting as efficient spin selectors pose a puzzle, that attracted a lot of attention during the recent years. Here we revisit the physical origins of chiral-induced spin selectivity (CISS), and propose a simple analytic minimal model to describe it. The model treats a chiral molecule as an anisotropic wire with molecular dipole moments aligned arbitrarily with respect to the wire's axes, and is therefore quite general. Importantly, it shows that helical structure of the molecule is not necessary to observe CISS and other chiral non-helical molecules can also be considered as a potential candidates for CISS effect. We also show that the suggested simple model captures the main characteristics of CISS observed in experiment, without the need for additional constraints employed in the previous studies. The results pave the way for understanding other related physical phenomena where CISS effect plays an essential role.
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 strength of the spin-orbit interaction relevant to transport in a low dimensional structure depends critically on the relative geometrical arrangement of current carrying orbitals. Recent tight-binding orbital models for spin transport in DNA-like molecules, have surmised that the band spin-orbit coupling arises from the particular angular relations between orbitals of neighboring bases on the helical chain. Such arrangement could be probed by inducing deformations in the molecule in a conductive probe AFM type setup, as it was recently reported by Kiran, Cohen and Naaman\cite{Kiran}. Here…
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…
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.
The chiral induced spin selectivity effect is an excited states phenomenon, which can be probed using photo-spectroscopy as well as transport measurements. On the one hand such measurements represent averaged quantities, on the other hand nearly all theoretical descriptions, with only a few exceptions, have been concerned with energy dependent properties of the pertinent structures. While those properties may or may not be relevant for the chiral induced spin selectivity effect, many of those properties have been attributed as being the, or part of the, origins of the effect. Here, it is demon…
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）
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…
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 …
Chiral-induced spin selectivity (CISS) is a phenomenon in which electron spins are polarized as they are transported through chiral molecules, and the spin polarization depends on the handedness of the chiral molecule. In this study, we show that spin selectivity can be realized in achiral materials by coupling electrons to a single mode of a chiral optical cavity. By investigating spin-dependent electron transport using the nonequilibrium Green's function approach, the spin polarization in a two-terminal setup is demonstrated to approach unity if the rate of dephasing is sufficiently small an…
We study the non-equilibrium dynamics of electron transmission from a straight waveguide to a helix with spin-orbit coupling. Transmission is found to be spin-selective and can lead to large spin polarizations of the itinerant electrons. The degree of spin selectivity depends on the width of the interface region, and no polarization is found for single-point couplings. We show that this is due to momentum conservation conditions arising from extended interfaces. We therefore identify interface structure and conservation of momentum as crucial ingredients for chiral-induced spin selectivity, an…
Understanding chiral induced spin-selectivity (CISS), resulting from charge transport through helical systems, has recently inspired many experimental and theoretical efforts, but is still object of intense debate. In order to assess the nature of CISS, we propose to focus on electron-transfer processes occurring at the single-molecule level. We design simple magnetic resonance experiments, exploiting a qubit as a highly sensitive and coherent magnetic sensor, to provide clear signatures of the acceptor polarization. Moreover, we show that information could even be obtained from time-resolved …
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…
The theoretical explanation for the chiral-induced spin selectivity effect, in which electrons' passage through a chiral system depends on their spin and the handedness of the system, remains vague. Although most experimental work was performed at room temperature, most of the proposed theories did not include vibrations. Here, we present temperature-dependent experiments and a theoretical model that captures all observations and provides spin polarization values that are consistent with the experimental results. The model includes vibrational contribution to the spin orbit coupling. It shows …
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））
The chiral induced spin selectivity (CISS) in layers of helical molecules gained considerable attention in the emerging field of spintronics, because the effect enables spin-filter devices under ambient conditions. Several theoretical studies have been carried out to explain this effect on a microscopic scale, but the origin of the effect is still controversial. In particular the role of spin-flip scattering during electron transport is an open issue. In this study we describe the electron and spin transport by rate equations including spin-dependent losses and spin-flip scattering. We reduce …
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 equati…
The observation of spin-dependent transport through organic chiral structures has sparked numerous fundamental and applicative questions ranging from biology to spintronics. By now, there is a broad consensus that the effect results from the combination of spin-orbit coupling and the systems' unique geometry. However, two key challenges remain. Firstly, accounting for the magnitude of the measured effect in light of the weak spin-orbit coupling in organic systems. Secondly, understanding its observation not only in tunneling-dominated short molecules, but also in longer ones where phonon-assis…
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）
Efficient generation of spin polarization is the central focus of spintronics. In magnetic materials, spin currents can arise from heat currents by the conventional spin Seebeck effect. Recently, chiral phonons with definite handedness and angular momenta have also produced profound impacts on multiple research fields. In this paper, starting with nonequilibrium distribution of chiral phonons under temperature gradient, we find a new spin selectivity effect - chiral phonon activated spin Seebeck (CPASS) effect, in chiral materials without magnetic order nor spin-orbit coupling. With both phono…
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）
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）
Cubic chiral magnets, such as Cu$_{2}$OSeO$_{3}$, exhibit a variety of non-collinear spin textures, including a trigonal lattice of spin whirls, so-called skyrmions. Using magnetic resonant elastic x-ray scattering (REXS) on a crystalline Bragg peak and its magnetic satellites while exciting the sample with magnetic fields at GHz frequencies, we probe the ferromagnetic resonance modes of these spin textures by means of the scattered intensity. Most notably, the three eigenmodes of the skyrmion lattice are detected with large sensitivity. As this novel technique, which we label REXS-FMR, is car…
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-…
We study the binding pattern of the amino acid alanine on the naturally chiral Pt surfaces Pt(531), Pt(321) and Pt(643). These surfaces are all vicinal to the {111} direction but have different local environments of their kink sites and are thus a model for realistic roughened Pt surfaces. Alanine has only a single methyl group attached to its chiral center, which makes the number of possible binding conformations computationally tractable. Additionally, only the amine and carboxyl group are expected to interact strongly with the Pt substrate. On Pt(531) we study the molecule in its pristine a…
