Spin dynamics and disorder effects in the S=1/2 kagome Heisenberg spin liquid phase of kapellasite

TL;DR

This study investigates the spin dynamics and disorder effects in the gapless spin liquid phase of kapellasite, a frustrated kagome magnet, using multiple experimental techniques to reveal the role of exchange interactions and disorder.

Contribution

It provides detailed experimental validation of the J1-J2-Jd Heisenberg model for kapellasite and uncovers the impact of 27% Cu/Zn site disorder on its magnetic properties.

Findings

Confirmation of ferromagnetic J1 and competing interactions around 10 K

Detection of moderate exchange anisotropy with D/J~3%

Observation of a broad distribution of spin-lattice relaxation times at low temperatures

Abstract

We report $^{35}$Cl NMR, ESR, $\mu$SR and specific heat measurements on the $S=1/2$ frustrated kagom\'e magnet kapellasite, $\alpha-$Cu$_3$Zn(OH)$_6$Cl$_2$, where a gapless spin liquid phase is stabilized by a set of competing exchange interactions. Our measurements confirm the ferromagnetic character of the nearest-neighbour exchange interaction $J_1$ and give an energy scale for the competing interactions $|J| \sim 10$ K. The study of the temperature-dependent ESR lineshift reveals a moderate symmetric exchange anisotropy term $D$, with $|D/J|\sim 3$%. These findings validate a posteriori the use of the $J_1 - J_2 - J_d$ Heisenberg model to describe the magnetic properties of kapellasite [Bernu et al., Phys. Rev. B 87, 155107 (2013)]. We further confirm that the main deviation from this model is the severe random depletion of the magnetic kagom\'e lattice by 27%, due to Cu/Zn site mixing, and specifically address the effect of this disorder by $^{35}$Cl NMR, performed on an oriented polycrystalline sample. Surprisingly, while being very sensitive to local structural deformations, our NMR measurements demonstrate that the system remains homogeneous with a unique spin susceptibility at high temperature, despite a variety of magnetic environments. Unconventional spin dynamics is further revealed by NMR and $\mu$SR in the low-$T$, correlated, spin liquid regime, where a broad distribution of spin-lattice relaxation times is observed. We ascribe this to the presence of local low-energy modes.