Dynamic fingerprint of fractionalized excitations in single-crystalline Cu3Zn(OH)6FBr

Beyond the absence of long-range magnetic orders, the most prominent feature of the elusive quantum spin liquid (QSL) state is the existence of fractionalized spin excitations, i.e., spinons. When the system orders, the spin-wave excitation appears as the bound state of the spinon-antispinon pair. Although scarcely reported, a direct comparison between similar compounds illustrates the evolution from spinon to magnon. Here, we perform the Raman scattering on single crystals of two quantum kagome antiferromagnets, of which one is the kagome QSL candidate CuZn(OH)FBr, and another is an antiferromagnetically ordered compound EuCu(OH)Cl. In CuZn(OH)FBr, we identify a unique one spinon-antispinon pair component in the E magnetic Raman continuum, providing strong evidence for deconfined spinon excitations. In contrast, a sharp magnon peak emerges from the one-pair spinon continuum in the E magnetic Raman response once EuCu(OH)Cl undergoes the antiferromagnetic order transition. From the comparative Raman studies, we can regard the magnon mode as the spinon-antispinon bound state, and the spinon confinement drives the magnetic ordering.