Abstract

Using inelastic neutron scattering, x-ray, neutron diffraction, and the first-principle calculation techniques, we show that the crystal structure of the two-dimensional quantum spin system (CuCl)LaNb2_2O7_7 is orthorhombic with PbamPbam symmetry in which CuCl4_4O2_2 octahedra are tilted from their high symmetry positions and the Cu2+(s=1/2)^{2+} (s = 1/2) ions form a distorted square lattice. The dominant magnetic interactions are the fourth nearest neighbor antiferromagnetic interactions with a Cu-Cl--Cl-Cu exchange path, which lead to the formation of spin singlets. The two strongest interactions between the singlets are ferromagnetic, which makes (CuCl)LaNb2_2O7_7 the first system of ferromagnetically coupled Shastry-Sutherland quantum spin singlets.

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