Theory of the Spinon-Mediated Witness Spin Glass in Herbertsmithite

Abstract

Herbertsmithite is a prototypical candidate quantum spin liquid (QSL), believed to feature a long-range entangled ground state and deconfined fractionalised spinon excitations. Confirmation of these properties has been hindered by the presence of magnetic impurities (spin-1/2 Cu2+ spins substituted onto non-magnetic Zn2+ sites). Recently these impurities were reconceptualised as 'witnesses' of the QSL, inheriting long-range interactions and entanglement mediated by the QSL spinons, leading to spin glass formation amongst witnesses below 260 mK. Here we present a full theoretical account of this idea. Despite having only one free parameter (the witness-kagome spin coupling), our model captures the full range of experimental data, including: the formation of a spin glass amongst witnesses; the frequency and temperature dependence of the magnetic noise; a sharp peak in the DC magnetic susceptibility as a function of temperature; and the static neutron scattering structure factor at 2 K. Both candidate QSLs (Z2 and U(1)) give similar agreement with all data; however, our model predicts a qualitative difference between the Z2 and U(1) neutron scattering intensities below 260 mK, providing a long-sought definitive test to distinguish the two cases. We also predict phase diagrams as a function of temperature and witness concentration, finding a phase transition to different long-range ordered witness states for Z2 and U(1) at high concentration.