Jahn-Teller states mixed by spin-orbit coupling in an electromagnetic field

24 pages, 8 figuresSpin-orbit coupling plays a pivotal role in condensed matter physics. For instance, spin-orbit interactions affect the magnetization and transport dynamics in solids, while spins and momenta are locked in topological matter. Alternatively, spin-orbit entanglement may play an important role in exotic phenomena, like quantum spin liquids in 4d and 5d systems. An interesting question is how electronic states mixed by spin orbit coupling interact with electromagnetic fields, which may hold potential to tune their properties and reveal interesting physics. Motivated by our recent discovery of large gyrotropic signals in some Jahn-Teller manganites, here we explore the interaction of light with spin-mixed states in a d4 transition metal. We show that spin-orbit mixing enables electronic transitions that are sensitive to circularly polarized light, giving rise to a gyrotropic response that increases with spin-orbit coupling. Interestingly, photoexcited transitions that involve spin reversal are behind such gyrotropic resonances. Additionally, we find that the interaction with the electromagnetic field depends strongly on the relative orientation of the propagation of light with respect to Jahn-Teller distortions and spin quantization. We suggest that such interactions offer the opportunity to use electromagnetic waves at optical wavelengths to entangle orbital and spin degrees of freedom. Our approach, which includes a group-theoretical treatment of spin-orbit coupling, has wide applicability and provides a versatile tool to explore the interaction of electromagnetic fields with electronic states in transition metals with arbitrary spin-orbit coupling strength and pointgroup symmetries.We acknowledge financial support from Projects No. PID2020-118479RBI00 and Severo Ochoa FUNFUTURE (No. CEX2019-000917-S) of the Spanish Ministry of Science and Innovation (Grant No. MCIN/AEI/10.13039/501100011033).With funding from the Spanish government through the ‘Severo Ochoa Centre of Excellence’ accreditation (CEX2019-000917-S).Peer reviewe