Abstract

Recently H3_3LiIr2_2O6_6 has been reported as a spin-orbital entangled quantum spin liquid (QSL) [K. Kitagawa et al., Nature {\bf 554}, 341 (2018)], albeit its connection to Kitaev QSL has not been yet identified. To unveil the related Kitaev physics, we perform the first Raman spectroscopy studies on single crystalline H3_3LiIr2_2O6_6 samples. We implement a soft chemical replacement of Li+^+ with H+^+ from αα-Li2_2IrO3_3 single crystals to synthesize the single crystal samples of the iridate second generation H3_3LiIr2_2O6_6. The Raman spectroscopy can be used to diagnose the QSL state since the magnetic Raman continuum arises from a process involving pairs of fractionalized Majorana fermionic excitation in a pure Kitaev model. We observe a broad dome-shaped magnetic continuum in H3_3LiIr2_2O6_6, in line with theoretical expectations for the two-spin process in the Kitaev QSL. Our results establish the close connection to the Kitaev QSL physics in H3_3LiIr2_2O6_6.

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