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Ca2RuO4 is a structurally-driven Mott insulator with a metal-insulatortransition at TMI = 357K, followed by a well-separated antiferromagnetic orderat TN = 110 K. Slightly substituting Ru with a 3d transition metal ion Meffectively shifts TMI by weakening the orthorhombic distortion and induceseither metamagnetism or magnetization reversal below TN. Moreover, M doping forRu produces negative thermal expansion in Ca2Ru1-xMxO4 (M = Cr, Mn, Fe or Cu);the lattice volume expands on cooling with a total volume expansion ratio,{\Delta}V/V, reaching as high as 1%. The onset of the negative thermalexpansion closely tracks TMI and TN, sharply contrasting classic negativethermal expansion that shows no relevance to electronic properties. Inaddition, the observed negative thermal expansion occurs near room temperatureand extends over a wide temperature interval up to 300 K. These findingsunderscores new physics driven by a complex interplay between orbital, spin andlattice degrees of freedom.

Magnetic and Orbital Orders Coupled to Negative Thermal Expansion in Mott Insulators, Ca2Ru1-xMxO4 (M = Mn and Fe)