Spinon Mediation of Witness-Spin Dynamics and Ground State in Herbertsmithite

The kagome lattice of spin-1/2 Cu atoms in herbertsmithite (ZnCu3(OH)6Cl2) may sustain a quantum spin liquid (QSL) state with spinon quasiparticles. Each kagome plane is separated from its homologues by a layer of spinless Zn atoms. Providentially, however, some spin-1/2 Cu atoms substitute randomly onto these inter-kagome Zn sites. We reconceptualize these 'impurity' atoms as quantum 'witness-spins', an exceptional new interrogative of the conjectured Z2-gauge-symmetric QSL state. Thus we introduce spin-noise spectroscopy to explore herbertsmithite witness-spin dynamics for QSL studies. It reveals the existence, slowing and intensification of spin noise, prefatory to a sharp transition at T* {\approx} 260 mK. Below T* the spin-noise power spectral density S_M(ω,T) {\propto} ω^{-α(T)} stabilizes at α {\approx} 1; the spin noise variance σ_M^2(T) diminishes precipitously; the ultra-low-field magnetic susceptibility χ(T) undergoes a sharp transition into a phase exhibiting an Edwards-Anderson order-parameter and ultra-slow spin-state relaxation. A Z2 QSL theory of spinon-mediated witness-spin interactions corresponds best to all these experimental observations, predicting slowing and intensification of witness-spin fluctuations and noise spectrum S_M(ω,T) with cooling, with a transition into a unique spinon-mediated phase signified by rapidly diminishing spin noise, with S_M(ω,T) {\propto} ω^{-1}, a sharp cusp in the DC magnetic susceptibility χ(T), and the appearance of an Edwards-Anderson order-parameter. We rule out numerous other mechanisms for these effects, so that only spinon-mediation by either a Z2 or U(1) QSL is consistent with all present herbertsmithite empirics, with the former model providing a closer match to data.