Giant pressure dependence and dimensionality switching in a metal-organic quantum antiferromagnet

Abstract

We report an extraordinary pressure dependence of the magnetic interactions in the metal-organic system [(CuF${}_2$(H${}_2$O)${}_2$)${}_2$pyrazine]. 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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• Room-temperature structural phase transition in the quasi-2D spin-1/2 Heisenberg antiferromagnet Cu(pz)${}_2$(ClO${}_4$)${}_2$