TY - JOUR
T1 - Chiral-Induced Spin Selectivity and Non-equilibrium Spin Accumulation in Molecules and Interfaces
T2 - A First-Principles Study
AU - Naskar, Sumit
AU - Mujica, Vladimiro
AU - Herrmann, Carmen
N1 - Funding Information:
The authors thank the high-performance computing center at the University of Hamburg for computational resources. This work is supported by the Cluster of Excellence “CUI: Advanced Imaging of Matter” of the Deutsche Forschungsgemeinschaft (DFG) (EXC 2056, Project ID 390715994). V.M. acknowledges the support of Ikerbasque, the Basque Foundation for Science, and the W. M. Keck Foundation through the grant “Chirality, spin coherence and entanglement in quantum biology”. a
Publisher Copyright:
© 2023 American Chemical Society. All rights reserved.
PY - 2023/1/26
Y1 - 2023/1/26
N2 - Electrons moving through chiral molecules are selected according to their spin orientation and the helicity of the molecule, an effect known as chiral-induced spin selectivity (CISS). The underlying physical mechanism is not yet completely understood. To help elucidate this mechanism, a non-equilibrium Green's function method, combined with a Landauer approach and density functional theory, is applied to carbon helices contacted by gold electrodes, resulting in spin polarization of transmitted electrons. Spin polarization is also observed in the non-equilibrium electronic structure of the junctions. While this spin polarization is small, its sign changes with the direction of the current and with the handedness of the molecule. While these calculations were performed with a pure exchange-correlation functional, previous studies suggest that computationally more expensive hybrid functionals may lead to considerably larger spin polarization in the electronic structure. Thus, non-equilibrium spin polarization could be a key component in understanding the CISS mechanism.
AB - Electrons moving through chiral molecules are selected according to their spin orientation and the helicity of the molecule, an effect known as chiral-induced spin selectivity (CISS). The underlying physical mechanism is not yet completely understood. To help elucidate this mechanism, a non-equilibrium Green's function method, combined with a Landauer approach and density functional theory, is applied to carbon helices contacted by gold electrodes, resulting in spin polarization of transmitted electrons. Spin polarization is also observed in the non-equilibrium electronic structure of the junctions. While this spin polarization is small, its sign changes with the direction of the current and with the handedness of the molecule. While these calculations were performed with a pure exchange-correlation functional, previous studies suggest that computationally more expensive hybrid functionals may lead to considerably larger spin polarization in the electronic structure. Thus, non-equilibrium spin polarization could be a key component in understanding the CISS mechanism.
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U2 - 10.1021/acs.jpclett.2c03747
DO - 10.1021/acs.jpclett.2c03747
M3 - Article
C2 - 36638217
AN - SCOPUS:85146386078
SN - 1948-7185
VL - 14
SP - 694
EP - 701
JO - Journal of Physical Chemistry Letters
JF - Journal of Physical Chemistry Letters
IS - 3
ER -