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Realizing square and diamond lattice <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"><mml:mrow><mml:mi>S</mml:mi><mml:mo>=</mml:mo><mml:mn>1</mml:mn><mml:mo>/</mml:mo><mml:mn>2</mml:mn></mml:mrow></mml:math> Heisenberg antiferromagnet models in the <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"><mml:mi>α</mml:mi></mml:math> and <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"><mml:mi>β</mml:mi></mml:math> phases of the coordination framework, <mml:math xmlns:mml="http…
We report the crystal structures and magnetic properties of two pseudopolymorphs of the $S=1/2 {\mathrm{Ti}}^{3+}$ coordination framework, $\mathrm{K}\mathrm{Ti}{({\mathrm{C}}_{2}{\mathrm{O}}_{4})}_{2}\ifmmode\cdot\else\textperiodcentered\fi{}x{\mathrm{H}}_{2}\mathrm{O}$. Single-crystal x-ray and powder neutron diffraction measurements on $\ensuremath{\alpha}\ensuremath{-}\mathrm{K}\mathrm{Ti}{({\mathrm{C}}_{2}{\mathrm{O}}_{4})}_{2}\ifmmode\cdot\else\textperiodcentered\fi{}x{\mathrm{H}}_{2}\mathrm{O}$ confirm its structure in the tetragonal $I4/mcm$ space group with a square planar arrangement of ${\mathrm{Ti}}^{3+}$ ions. Magnetometry and specific heat measurements reveal …