Slow dynamics of disordered zigzag chain molecules in layered LiVS2 under electron irradiation

Abstract

Electronic instabilities in transition metal compounds often spontaneously form orbital molecules, which consist of orbital-coupled metal ions at low temperature. Recent local structural studies utilizing the pair distribution function revealed that preformed orbital molecules appear disordered even in the high-temperature paramagnetic phase. However, it is unclear whether preformed orbital molecules are dynamic or static. Here, we provide clear experimental evidence of the slow dynamics of disordered orbital molecules realized in the high-temperature paramagnetic phase of LiVS2, which exhibits vanadium trimerization upon cooling below 314 K. Unexpectedly, the preformed orbital molecules appear as a disordered zigzag chain that fluctuate in both time and space under electron irradiation. Our findings should advance studies on soft matter physics realized in an inorganic material due to disordered orbital molecules.

arXiv comment17 pages, 4 figures and supplemental information

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• Charge-ordered state satisfying the Anderson condition in LiRh2O4 arising from local dimer order
• Zigzag chain order of LiVSe${}_2$ developing away from the vanadium trimer phase transition boundary
• Electronic Self-Organization in the β-Pyrochlore Oxide CsW2O6
• Reexamination of the charge-ordered dimer pattern in the spinel compound CuIr2S4 using single-crystal synchrotron x-ray diffraction
• Structural dimerization and charge-orbital ordering in a ferromagnetic semiconductor LiV2S4 monolayer
• 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