Photoexcited states of the harmonic honeycomb iridate γ-Li₂IrO₃

We report equilibrium and nonequilibrium optical measurements on the recently synthesized "harmonic" honeycomb iridate \gamma-Li$_2$IrO$_3$ (LIO), as well as the layered honeycomb iridate Na$_2$IrO$_3$ (NIO). Using Fourier transform infrared microscopy we performed reflectance measurements on LIO, from which we obtained the optical conductivity below 2 eV. In addition we measured the photoinduced changed in reflectance, \Delta R, as a function of time, t, temperature, T, and probe field polarization in both LIO and NIO. In LIO, \Delta R(t,T) is anisotropic and comprised of three T dependent components. Two of these components are related to the onset of magnetic order and the third is related to a photoinduced population of metastable electronic excited states. In NIO, \Delta R(t,T) has a single T dependent component that is strikingly similar to the electronic excitation component of \Delta R in LIO. Through analysis and comparison of \Delta R(t,T) for two compounds, we extract information on the onset of magnetic correlations at and above the transition temperature in LIO, the bare spin-flip scattering rate in equilibrium, the lifetime of low-lying quasiparticle excitations, and the polarization dependence of optical transitions that are sensitive to magnetic order.