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Abstract:

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(ClxBr1-x)4·2H2O (QuinH = Quinolinium, C9H8N+), with 0≤x≤1. Pulsed-field magnetization measurements allow us to estimate an effective in-plane exchange strength J in a regime where exchange fosters short-range order, while the temperature TN at which long-range order (LRO) occurs is found using muon-spin relaxation, allowing us to construct a phase diagram for the series. We evaluate the effectiveness of disorder in suppressing TN and the ordered moment size, and we 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. Furthermore, we demonstrate experimentally that the ground-state disorder is driven by quantum effects of the exchange randomness, which is a feature that has been predicted theoretically and has implications for other disordered quasi-two-dimensional QHAFs.

Abstract:

© 2020 authors. We report on a comprehensive characterization of the newly synthesized Cu2+-based molecular magnet [Cu(pz)2(2-HOpy)2](PF6)2 (CuPOF), where pz=C4H4N2 and 2-HOpy=C5H4NHO. From a comparison of theoretical modeling to results of bulk magnetometry, specific heat, μ+SR, ESR, and NMR spectroscopy, this material is determined as an excellent realization of the two dimensional square-lattice S=12 antiferromagnetic Heisenberg model with a moderate intraplane nearest-neighbor exchange coupling of J/kB=6.80(5) K, and an extremely small interlayer interaction of about 1 mK. At zero field, the bulk magnetometry reveals a temperature-driven crossover of spin correlations from isotropic to XY type, caused by the presence of a weak intrinsic easy-plane anisotropy. A transition to long-range order, driven by the low-temperature XY anisotropy under the influence of the interlayer coupling, occurs at TN=1.38(2) K, as revealed by μ+SR. In applied magnetic fields, our H1-NMR data reveal a strong increase of the magnetic anisotropy, manifested by a pronounced enhancement of the transition temperature to commensurate long-range order at TN=2.8 K and 7 T.