@article{5389aec1c6f041dcbc399656626003b3,
title = "Common Trends of Chiral Induced Spin Selectivity and Optical Dichroism with Varying Helix Pitch: A First-Principles Study",
abstract = "Electrons ransported through a chiral molecule become spin−polarized; this phenomenon is known as chiral induced spin selectivity (CISS). It has implications for spintronics, for electrochemical and enantioselective reactions, and for electron transfer in biological systems. The CISS-induced spin polarization in simulations and in experiment differs by orders of magnitude, and the detailed underlying mechanism is still an open question. Structure−property relationships can help elucidate this question. For this purpose, the effect of helix pitch is studied for a model helix of 20 carbon atoms for two quantities which have been found to correlate in some experiments: spin-polarization in transmitted electrons and electronic circular dichroism (ECD). We find that even though the chirality of these model helices goes down with increased pitch, ECD and CISS go up, along with ultraviolet−visible (UV/Vis) spectra and magnetic and electric transition dipole moments. Orbital contributions to the most intense UV/Vis transition do not show a consistent qualitative picture. Tentatively, we can assign the increase in these properties to an increase of the electric polarizability with spatial extension of these helices by changing pitch.",
keywords = "chiral induced spin selectivity, chirality, circular dichroism, density functional theory, polarizability, response properties, spin−orbit coupling",
author = "Sumit Naskar and Aida Saghatchi and Vladimiro Mujica and Carmen Herrmann",
note = "Funding Information: We thank Michael Deffner (University of Hamburg), Arka Bandopadhyay (IISC Bangalore), Narcis Avarvari (CNRS – University of Angers), David Waldeck (University of Pittsburgh), and Ron Naaman (Weizmann Institute of Science) for helpful discussions, and the high-performance computing centre at the University of Hamburg for computational resources. This work is supported by the Cluster of Excellence “Advanced Imaging of Matter” of the Deutsche Forschungsgemeinschaft (DFG) – EXC 2056 – project ID 390715994. V.M. acknowledges a Fellowship from Ikerbasque, the Basque Foundation for Science. Open Access funding enabled and organized by Projekt DEAL. Funding Information: We thank Michael Deffner (University of Hamburg), Arka Bandopadhyay (IISC Bangalore), Narcis Avarvari (CNRS – University of Angers), David Waldeck (University of Pittsburgh), and Ron Naaman (Weizmann Institute of Science) for helpful discussions, and the high‐performance computing centre at the University of Hamburg for computational resources. This work is supported by the Cluster of Excellence “Advanced Imaging of Matter” of the Deutsche Forschungsgemeinschaft (DFG) – EXC 2056 – project ID 390715994. V.M. acknowledges a Fellowship from Ikerbasque, the Basque Foundation for Science. Open Access funding enabled and organized by Projekt DEAL. Publisher Copyright: {\textcopyright} 2022 The Authors. Israel Journal of Chemistry published by Wiley-VCH GmbH.",
year = "2022",
month = dec,
doi = "10.1002/ijch.202200053",
language = "English (US)",
volume = "62",
journal = "Israel Journal of Chemistry",
issn = "0021-2148",
publisher = "Wiley-VCH Verlag",
number = "11-12",
}