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Theory of Chirality Induced Spin Selectivity: Progress and Challenges (2108.09998v1)

Published 23 Aug 2021 in cond-mat.mtrl-sci

Abstract: We provide a critical overview of the theory of the chirality-induced spin selectivity (CISS) effect, i.e., phenomena in which the chirality of molecular species imparts significant spin selectivity to various electron processes. Based on discussions in a recently held workshop, and further work published since, we review the status of CISS effects - in electron transmission, electron transport, and chemical reactions. For each, we provide a detailed discussion of the state-of-the-art in theoretical understanding and identify remaining challenges and research opportunities.

Citations (168)

Summary

Overview of "Theory of Chirality Induced Spin Selectivity: Progress and Challenges"

The paper "Theory of Chirality Induced Spin Selectivity: Progress and Challenges" presents a comprehensive review of the current theoretical understanding and challenges associated with the chirality-induced spin selectivity (CISS) effect. Authored by Ferdinand Evers and a diverse group of researchers, this work synthesizes findings discussed during a workshop along with recent developments published in the field.

Introduction to CISS

CISS describes the phenomenon where the chirality of molecular configurations imparts selective control over the electron spin states in various processes, such as electron transmission, transport, and chemical reactions. Despite its growing experimental validation and potential applications in spintronics and chemistry, the theoretical foundation lagged due to complexities involving spin-orbit coupling (SOC) and quantum mechanics.

Experimental Context

The paper delineates the experimental observations of CISS, primarily in three areas:

  1. Electron Transmission: Characterized by a notable spin polarization of electrons transmitted through chiral molecules, initially detected by photoemission experiments with chiral monolayers.
  2. Electron Transport: Spin-selective electron transport through chiral media has been achieved experimentally in setups using various chiral compounds, showcasing high levels of spin polarization in electron currents.
  3. Chemical Reactions: The ability to drive enantioselective chemical reactions via spin-polarized electrons introduced a new dimension to CISS applications.

Theoretical Developments

The authors review a series of theoretical models addressing CISS across these domains:

  • Scattering Theory: Early efforts focused on SOC-mediated spin scattering in chiral potentials, indicating qualitative agreement but failing quantitatively in reproducing experimental magnitudes without enhancement from substrates with strong SOC.
  • Transport Mechanisms: The spin transport through helical structures under non-equilibrium conditions has been explored through tight-binding and first-principles calculations. The models encountered limitations regarding SOC strength and symmetry-induced constraints.
  • Beyond SOC: Leveraging additional mechanisms like orbital polarization from electrodes or involvement of decoherence baths introduced concepts that circumvent some no-go theorems related to two-terminal devices.

Challenges and Future Directions

Despite advancements, a unified quantitative theory of CISS remains elusive. Major challenges include:

  • SOC Magnitude: Current theoretical models underestimate the effect's magnitude observed in realistic molecular systems, suggesting additional factors might contribute to the pronounced experimental spin polarization.
  • Symmetry Considerations: The integration of mechanisms that break traditional symmetry constraints remains pivotal for accurately modeling CISS.
  • Multi-Disciplinary Approaches: The possible involvement of nuclear dynamics or vibrational effects necessitates cross-disciplinary efforts to accurately depict the phenomenon.

Implications and Speculation

Understanding CISS could significantly impact spintronic applications, offering pathways to develop magnetless spin-based devices. Additionally, enantioselective chemical processes supervised by spin polarization broaden potential chemistry and biochemistry applications. Future advances are likely to depend on resolving SOC prediction disparities and exploring non-electronic contributions to spin transport.

In summary, "Theory of Chirality Induced Spin Selectivity: Progress and Challenges" contributes an in-depth synthesis of CISS, identifying key challenges and recommending directions for future studies to refine our understanding of this complex quantum effect.