High-energy electronic excitations in Sr${}_2$IrO${}_4$ observed by Raman scattering

Abstract

Spin-orbit interaction in Sr${}_2$IrO${}_4$ leads to the realization of the $J_{\mathrm{eff}}$ = 1/2 state and also induces an insulating behavior. Using large-shift Raman spectroscopy, we found two high-energy excitations of the d-shell multipletat at 690 meV and 680 meV with $A_{1g}$ and $B_{1g}$ symmetry respectively. As temperature decreases, the $A_{1g}$ and $B_{1g}$ peaks narrow, and the $A_{1g}$ peak shifts to higher energy while the energy of the $B_{1g}$ peak remains the same. When 25$\%$ of Ir is substituted with Rh the $A_{1g}$ peak softens by 10$\%$ but the $B_{1g}$ peak does not. We show that both pseudospin-flip and non-pseudosin-flip dd electronic transitions are Raman active, but only the latter are observed.

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• Square Lattice Iridates
• Two-magnon Raman scattering and pseudospin-lattice interactions in Sr2IrO4 and Sr3Ir2O7
• Covalency-driven collapse of strong spin-orbit coupling in face-sharing iridium octahedra
• Multiple Spin-Orbit Excitons and the Electronic Structure of $\alpha$-RuCl${}_3$
• Compressive-strain induced enhancement of exchange interactions and short-range magnetic order in Sr${}_2$IrO${}_4$ investigated by Raman spectroscopy
• Quest for New Quantum States via Field-Editing Technology
• Spin liquid like Raman signatures in hyperkagome iridate Na${}_4$Ir${}_3$O${}_8$
• Spin-orbit excitons in a correlated metal: Raman scattering study of Sr2RhO4