Strong Dimerization and Field-Induced Reconstruction of the Low-Energy Spectrum in $\mathrm{Cu}_3(\mathrm{OH})_4(\mathrm{HCO}_2)_2$

Abstract

We investigate the field-dependent low-energy thermodynamics of the distorted triangular quantum antiferromagnet $\mathrm{Cu}_3(\mathrm{OH})_4(\mathrm{HCO}_2)_2$ using a sector-resolved Superblock Diagonalization Method (SBDM) supplemented by a transfer-matrix treatment of weakly coupled layers. The strong exchange hierarchy, dominated by the Cu1--Cu1 intradimer coupling $J_2=150\,\mathrm{K}$, separates a high-energy dimer sector from a much softer magnetic manifold formed predominantly by the Cu2 moments. In the 24-site cluster, sixteen Cu1 spins form the strongly bound sector while eight Cu2 spins remain magnetically active; polarization of these eight spins gives $S^z=4$ compared with $S^z_{\rm sat}=12$, providing a direct microscopic origin for the one-third magnetization scale. The finite-temperature thermodynamics reveals a non-monotonic field evolution of the low-energy scale: the dominant $C/T$ feature softens with increasing field, reaches a minimum near the field region around $2\,\mathrm{T}$, and subsequently hardens as the low-temperature magnetization approaches $M_{\rm sat}/3$. Temperature and field sweeps thus expose a common field-induced spectral reconstruction, while the strongly reduced entropy reflects the restricted number of thermally active degrees of freedom below the dimer excitation scale. Our results identify strong-dimer-induced reduction of the active magnetic Hilbert space, followed by field-driven reorganization of the residual spin sector, as the common microscopic origin of the one-third magnetic response and the non-monotonic low-temperature thermodynamics.