Giant Pressure Dependence and Dimensionality Switching in a Metal-Organic Quantum Antiferromagnet

Wehinger, B.; Fiolka, Christoph; Lanza, Arianna; Scatena, Rebecca; Kubus, Mariusz; Grockowiak, A.; Coniglio, W. A.; Graf, D.; Skoulatos, M.; Chen, J.-H.; Gukelberger, J.; Casati, N.; Zaharko, O.; Macchi, Piero; Krämer, Karl; Tozer, S.; Mudry, C.; Normand, B.; Rüegg, Ch. (2018). Giant Pressure Dependence and Dimensionality Switching in a Metal-Organic Quantum Antiferromagnet. Physical review letters, 121(11), p. 117201. American Physical Society 10.1103/PhysRevLett.121.117201

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We report an extraordinary pressure dependence of the magnetic interactions in the metal-organic system [(CuF2(H2O)2)2pyrazine]. At zero pressure, this material realizes a quasi-two-dimensional (Q2D) spin-1/2 square-lattice Heisenberg antiferromagnet. By high-pressure, high-field susceptibility measurements we show that the dominant exchange parameter is reduced continuously by a factor of 2 upon compression. Above 18 kbar, a phase transition occurs, inducing an orbital re-ordering that switches the dimensionality, transforming the Q2D lattice into weakly coupled chains (Q1D). We explain the microscopic mechanisms for both phenomena by combining detailed x-ray and neutron diffraction results with quantitative modeling using spin-polarized density functional theory.

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