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A novel Ti3+-based thiospinel ZnTi2S4 is successfully synthesized via alow-temperature ion-exchange reaction. ZnTi2S4 shows a signature of metallicground state evidenced by a contribution of conduction electrons in the heatcapacity and Pauli-like paramagnetic susceptibility. These observationscontrast to the electronic state of similar Ti3+-based spinel MgTi2O4exhibiting the metal-insulator transition associated with a molecular orbitalcrystallization (MOC). Furthermore, the magnetic susceptibility of ZnTi2S4shows a pseudogap-like behavior indicated by a vast peak in the magneticsusceptibility around 110 K, likely originating from the MOC fluctuation. Theorigin of the difference in the electronic states of MgTi2O4 and ZnTi2S4 wouldbe due to the different magnitude of overlap between Ti 3d and p orbitals (O:2p and S: 3p). The presence of a MOC state in the close vicinity ofinsulator-metal transition may suggest the importance of itinerancy in a MOC.

journal of physics. condensed matter

Metallic state in the vicinity of molecular orbital crystallization in  the d$^1$ thiospinel ZnTi$_2$S$_4$ prepared via a reductive ion-exchange  reaction