Nanoscale Femtosecond Dynamics of Mott Insulator (Ca0.99Sr0.01)2RuO4

R. A. Vitalone, A. J. Sternbach, B. A. Foutty, A. S. McLeod, C. Sow, D. Golez, F. Nakamura, Y. Maeno, A. N. Pasupathy, A. Georges, A. J. Millis and D. N. Basov

Nano Letters 22, 5689 (2022)
Ca2RuO4 is a transition-metal oxide that exhibits a Mott insulator–metal transition (IMT) concurrent with a symmetry-preserving Jahn–Teller distortion (JT) at 350 K. The coincidence of these two transitions demonstrates a high level of coupling between the electronic and structural degrees of freedom in Ca2RuO4. Using spectroscopic measurements with nanoscale spatial resolution, we interrogate the interplay of the JT and IMT through the temperature-driven transition. Then, we introduce photoexcitation with subpicosecond temporal resolution to explore the coupling of the JT and IMT via electron–hole injection under ambient conditions. Through the temperature-driven IMT, we observe phase coexistence in the form of a stripe phase existing at the domain wall between macroscopic insulating and metallic domains. Through ultrafast carrier injection, we observe the formation of midgap states via enhanced optical absorption. We propose that these midgap states become trapped by lattice polarons originating from the local perturbation of the JT.