The entire magnetization process of ${\mathrm{TlCuCl}}_3$ has been experimentally investigated up to 100 T employing the single-turn technique. The upper critical field $H_{c2}$ is observed to be 86.1 T at 2 K. A convex slope of the $M\text{−}H$ curve between the lower and upper critical fields ($H_{c1}$ and $H_{c2}$) is clearly observed, which indicates that a particle-hole symmetry is broken in ${\mathrm{TlCuCl}}_3$. By quantum Monte Carlo simulation and the bond-operator theory method, we find that the particle-hole symmetry breaking results from strong interdimer interactions.

• Received 26 August 2020
• Accepted 30 November 2020

DOI:https://doi.org/10.1103/PhysRevLett.125.267207