Abstract

We present a thorough experimental study of the three-dimensional hyperhoneycomb Kitaev magnet ββ-Li2_2IrO3_3, using a combination of inelastic neutron scattering (INS), time-domain THz spectroscopy, and heat capacity measurements. The main results include a massive low-temperature reorganization of the INS spectral weight that evolves into a broad peak centered around 12 meV, and a distinctive peak in the THz data at 2.8(1) meV. A detailed comparison to powder-averaged spin-wave theory calculations reveals that the positions of these two features are controlled by the anisotropic ΓΓ coupling and the Heisenberg exchange JJ, respectively. The refined microscopic spin model places ββ-Li2_2IrO3_3 in close proximity to the Kitaev spin liquid phase.

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