Chiral Induced Spin Selectivity (CISS) has attracted significant interest in recent years due to its widespread applications, including spintronic devices, enantiomeric separation, and chemical reaction selectivity. Theoretical models of CISS have consistently underestimated the degree of spin polarization observed in experiment; however, these models do not evaluate the role of the chiral/substrate interface, and recent experiments have indicated that this interface plays a role in some of this as of yet unaccounted for polarization. These experiments, however, have lacked the interfacial specificity to probe the role of the interface directly. We use an interface specific technique, electronic sum frequency generation (eSFG) spectroscopy, to directly probe the interfacial electronic states of DNA covalently attached to MoS<sub>2</sub> – a model system for CISS. We have developed a novel time domain, heterodyne eSFG spectrometer to facilitate this measurement. Our technique employs a piezoelectric driven vibrating mirror, conferring unprecedented phase stability; allowing for longer scans without loss of spectral accuracy. Our eSFG measurements are complemented by transient reflectivity measurements, which probe the dynamics of charge transport to the substrate. Understanding the role of the interface may open up new avenues for CISS engineering, potentially facilitating spin based device design.

Probing the role of the interface in chiral induced spin selectivity

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