Valentin Zimmermann | Search arXiv

arXiv2023

Spin-orbit excitons in a correlated metal: Raman scattering study of Sr2RhO4

Using Raman spectroscopy to study the correlated 4$d$-electron metal Sr$_2$RhO$_4$, we observe pronounced excitations at 220 meV and 240 meV with $A_\mathrm{1g}$ and $B_\mathrm{1g}$ symmetries, respectively. We identify them as transitions between the spin-orbit multiplets of the Rh ions, in close analogy to the spin-orbit excitons in the Mott insulators Sr$_2$IrO$_4$ and $\alpha$-RuCl$_3$. This observation provides direct evidence for the unquenched spin-orbit coupling in Sr$_2$RhO$_4$. A quantitative analysis of the data reveals that the tetragonal crystal field $\Delta$ in Sr$_2$RhO$_4$ has a sign opposite to that in insulating Sr$_2$IrO$_4$, which enhances the planar $xy$ orbital character of the effective $J=1/2$ wave function. This supports a metallic ground state, and suggests that $c$-axis compression of Sr$_2$RhO$_4$ may transform it into a quasi-two-dimensional antiferromagnetic insulator.

cond-mat.str-el↗

arXiv2019

Near-unity light absorption in a monolayer WS2 van der Waals heterostructure cavity

Excitons in monolayer transition-metal-dichalcogenides (TMDs) dominate their optical response and exhibit strong light-matter interactions with lifetime-limited emission. While various approaches have been applied to enhance light-exciton interactions in TMDs, the achieved strength have been far below unity, and a complete picture of its underlying physical mechanisms and fundamental limits has not been provided. Here, we introduce a TMD-based van der Waals heterostructure cavity that provides near-unity excitonic absorption, and emission of excitonic complexes that are observed at ultra-low excitation powers. Our results are in full agreement with a quantum theoretical framework introduced to describe the light-exciton-cavity interaction. We find that the subtle interplay between the radiative, non-radiative and dephasing decay rates plays a crucial role, and unveil a universal absorption law for excitons in 2D systems. This enhanced light-exciton interaction provides a platform for studying excitonic phase-transitions and quantum nonlinearities and enables new possibilities for 2D semiconductor-based optoelectronic devices.

physics.optics↗