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Ca2RuO4 undergoes a metal-insulator transition at TMI = 357 K, followed by awell-separated transition to antiferromagnetic order at TN = 110 K. Dilute Crdoping for Ru reduces the temperature of the orthorhombic distortion at TMI andinduces ferromagnetic behavior at TC. The lattice volume V of Ca2Ru1-xCrxO4 (0< x < 0.13) abruptly expands with cooling at both TMI and TC, giving rise to atotal volume expansion {\Delta}V/V {\simeq} 1 %, which sharply contrasts thesmooth temperature dependence of the few known examples of negative volumethermal expansion driven by anharmonic phonon modes. In addition, the nearabsence of volume thermal expansion between TC and TMI represents an Invareffect. The two phase transitions suggest an exotic ground state driven by anextraordinary coupling between spin, orbit and lattice degrees of freedom.

Ca2Ru1-xCrxO4 (0 < x < 0.13): Negative volume thermal expansion via orbital and magnetic orders