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

TL;DR

This study uses Raman scattering to provide evidence of fractionalized spin excitations in a structurally ideal kagome lattice compound, supporting its candidacy as a quantum spin liquid with topological order.

Contribution

It demonstrates the presence of a magnetic Raman continuum and fractionalized excitations in Cu$_3$Zn(OH)$_6$FBr, confirming its status as an ideal quantum spin liquid candidate.

Findings

Raman scattering reveals a continuum of spin excitations.

The kagome structure remains undistorted at low temperatures.

Evidence of fractionalized spin excitations in the material.

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.