Chirality-Induced Spin Selectivity in a Coarse-Grained Tight-Binding Model for Helicene

Geyer M, Gutierrez R, Mujica V, Cuniberti G (2019)

Publication Type: Journal article

Publication year: 2019

Journal

Journal of Physical Chemistry C American Chemical Society

Book Volume: 123

Pages Range: 27230-27241

Journal Issue: 44

DOI: 10.1021/acs.jpcc.9b07764

Abstract

Spin-dependent effects in helical molecular systems, leading to the so-called chirality-induced spin selectivity (CISS) effect, have strongly attracted the attention of the chemical and physical community over the past few years. A large amount of experimental material has been collected so far, and different theoretical approaches have been presented to rationalize the CISS effect. The problem is, however, still a subject of debate. We present a semianalytical coarse-grained atomistic description of the electronic structure of a simple helical molecule, including spin-orbit interactions. For reference, we consider helicene, which is a pure carbon-based helical system with no chiral centers, and which has been previously shown experimentally to display a CISS effect. Our model exploits perturbation theory and a Löwdin-like partitioning to obtain an effective Ï-πHamiltonian, where all coupling coefficients depend on the helical geometry and predefined Slater-Koster parameters. As a result, they can be explicitly computed, thus providing physically meaningful orders of magnitude. We further discuss the conditions under which a nonvanishing spin polarization can be obtained in the model. We expect that our approach will serve to bridge the gap between purely phenomenological model Hamiltonians and more advanced first-principles methodologies.

Involved external institutions

Technische Universität Dresden DE Germany (DE) Arizona State University (ASU) US United States (USA) (US)

How to cite

APA:

Geyer, M., Gutierrez, R., Mujica, V., & Cuniberti, G. (2019). Chirality-Induced Spin Selectivity in a Coarse-Grained Tight-Binding Model for Helicene. Journal of Physical Chemistry C, 123(44), 27230-27241. https://doi.org/10.1021/acs.jpcc.9b07764

MLA:

Geyer, Matthias, et al. "Chirality-Induced Spin Selectivity in a Coarse-Grained Tight-Binding Model for Helicene." Journal of Physical Chemistry C 123.44 (2019): 27230-27241.

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