Photoinduced phase switching at a Mott insulator-to-metal transition

Abstract

Achieving fundamental understanding of insulator-to-metal transitions (IMTs) in strongly correlated systems and their persistent and reversible control via nonequilibrium drive are prime targets of current condensed matter research. Photoinduced switching between competing orders in correlated insulators requires a free-energy landscape with nearly degenerate ground states, which is commonly reached through doping, strain, or static electric field. The associated spatial inhomogeneity leads to a photoinduced phase transition that remains confined near the illuminated region. Here we report optical spectroscopy experiments at the first-order IMT in the 4d-electron compound Ca${}_3$(Ru${}_{0.99}$Ti${}_{0.01}$)${}_2$O${}_7$ and show that specific Ru d-d interband transitions excited by light with a threshold fluence corresponding to the planar density of Ru atoms can trigger reversible, avalanche-like coherent propagation of phase interfaces across the full extent of a macroscopic sample, in the absence of assisting external stimuli. Based on detailed comparison of spectroscopic data to density functional calculations, we attribute the extraordinary photo-sensitivity of the IMT to an exceptionally shallow free-energy landscape generated by the confluence of electron-electron and electron-lattice interactions. Our findings suggest Ca${}_3$(Ru${}_{0.99}$Ti${}_{0.01}$)${}_2$O${}_7$ as an ideal model system for building and testing a theory of Mott transition dynamics in the presence of strong electron-lattice coupling and may pave the way towards nanoscale devices with quantum-level photosensitivity.

24 pages, 8 figures, 3 ancillary video files

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