Explaining the magnitude of Chirality-Induced Spin Selectivity via electron-electron exchange

Abstract

Chiral molecular structure can couple to electron spin, leading to unexpected spin polarization effects. This Chirality-Induced Spin Selectivity (CISS) was first reported for DNA molecules adsorbed on gold but its microscopic origin remains unclear. We demonstrated though simulation that the exchange arising from electron-electron Coulomb interactions within the self-consistent mean field (Hartree--Fock) approximation can yield significant ($\sim 2\%$) spin polarisation for $3$-methylcyclohexanone adsorbed on Cu(111) amplifying a much smaller ($\sim 0.0014\%$) initial bias, consistent with experiment. Symmetry considerations ensure the result is physically meaningful, while its ab-initio nature ensures all parameters are physically realistic. This amplification is connected to existing studies on spin-symmetry breaking in Hartree--Fock, providing a new pathway for understanding the magnitude of CISS as an emergent phenomenon of interacting electrons.