Effect of exchange-bond randomization in a highly two-dimensional quantum Heisenberg antiferromagnet*

We present an investigation of the effect of randomizing exchange coupling strengths in the S = 1/2 square lattice quasi-two-dimensional quantum Heisenberg antiferromagnet (QHAF) (QuinH)₂Cu(Cl_xBr_1−x)₄●2H₂O (QuinH = Quinolinium, C₉H₈N⁺), with 0 ≤ x ≤ 1. Pulsed-field magnetization allows us to estimate an effective in-plane exchange strength in a regime where exchange fosters short-range order, while the temperature at which long-range order occurs (T_N) is found using muon-spin relaxation, allowing us to construct a phase diagram for the series. We evaluate the effectiveness of disorder in suppressing the T_N and the ordered moment size and find an extended disordered phase in the region 0.4 ≤ x ≤ 0.8 where no magnetic order occurs. The observed critical substitution levels are accounted for by an energetics-based competition between different local magnetic orders. We demonstrate experimentally that the ground-state disorder is driven by quantum effects of the exchange randomness, a feature that has been predicted theoretically and has implications for other disordered quasi-two-dimensional QHAFs.