Dynamic fingerprint of fractionalized excitations in single-crystalline Cu${}_3$Zn(OH)${}_6$FBr

Abstract

Quantum spin liquid (QSL) represents a new class of condensed matter states characterized by the long-range many-body entanglement of topological orders. The most prominent feature of the elusive QSL state is the existence of fractionalized spin excitations. Subject to the strong quantum fluctuations, the spin-1/2 antiferromagnetic system on a kagome lattice is the promising candidate for hosting a QSL ground state, but the structurally ideal realization is rare. Here, we report Raman scattering on the single crystalline Cu${}_3$Zn(OH)${}_6$FBr, and confirm that the ideal kagome structure remains down to low temperatures without any lattice distortion by the angle-resolved polarized Raman responses and second-harmonic-generation measurements. Furthermore, at low temperatures the Raman scattering reveals a continuum of the spin excitations in Cu${}_3$Zn(OH)${}_6$FBr, in contrast to the sharp magnon peak in the ordered kagome antiferromagnet EuCu${}_3$(OH)${}_6$Cl${}_3$. Such magnetic Raman continuum, in particular, the substantial low-energy one-pair spinon excitation serves as strong evidence for fractionalized spin excitations in Cu${}_3$Zn(OH)${}_6$FBr.

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