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We present a microscopic model of the spin-gap quantum magnet (CuCl)LaNb2O7that was previously suggested as a realization of the spin-1/2 frustratedsquare lattice. Taking advantage of the precise atomic positions from recentcrystal structure refinement, we evaluate individual exchange integrals andconstruct a minimum model that naturally explains all the availableexperimental data. Surprisingly, the deviation from tetragonal symmetry leadsto the formation of spin dimers between fourth neighbors due to a Cu-Cl-Cl-Cupathway with a leading antiferromagnetic exchange J4 ~ 25 K. The totalinterdimer exchange amounts to 12 - 15 K. Our model is in agreement withinelastic neutron scattering results and is further confirmed by quantumMonte-Carlo simulations of the magnetic susceptibility and the high-fieldmagnetization. Our results establish (CuCl)LaNb2O7 as a non-frustrated systemof coupled spin dimers with predominant antiferromagnetic interactions andprovide a general perspective for related materials with unusuallow-temperature magnetic properties.

Microscopic model of (CuCl)LaNb2O7: coupled spin dimers replace a frustrated square lattice