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Journal Article

Influence of spin and orbital fluctuations on Mott-Hubbard exciton dynamics in LaVO3 thin films


Kennes,  D. M.
Institut für Theorie der Statistischen Physik, RWTH Aachen University and JARA-Fundamentals of Future Information Technology;
Theory Group, Theory Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society;
Center for Free Electron Laser Science;

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Lovinger, D. J., Brahlek, M., Kissin, P., Kennes, D. M., Millis, A. J., Engel-Herbert, R., et al. (2020). Influence of spin and orbital fluctuations on Mott-Hubbard exciton dynamics in LaVO3 thin films. Physical Review B, 102(11): 115143. doi:10.1103/PhysRevB.102.115143.

Cite as: http://hdl.handle.net/21.11116/0000-0007-1F57-6
Recent optical conductivity measurements reveal the presence of Hubbard excitons in certain Mott insulators. In light of these results, it is important to revisit the dynamics of these materials to account for excitonic correlations. We investigate time-resolved excitation and relaxation dynamics as a function of temperature in perovskite-type LaVO3 thin films using ultrafast optical pump-probe spectroscopy. LaVO3 undergoes a series of phase transitions at roughly the same critical temperature TC≅140 K, including a second-order magnetic phase transition (PM→AFM) and a first-order structural phase transition, accompanied by C-type spin order and G-type orbital order. Ultrafast optical pump-probe spectroscopy at 1.6 eV monitors changes in the spectral weight of the Hubbard exciton resonance which serves as a sensitive reporter of spin and orbital fluctuation dynamics. We observe dramatic slowing down of the spin, and orbital dynamics in the vicinity of TC≅140 K, reminiscent of a second-order phase transition, despite the (weakly) first-order nature of the transition. We emphasize that since it is spectral weight changes that are probed, the measured dynamics are not reflective of conventional exciton generation and recombination, but are related to the dynamics of Hubbard exciton formation in the presence of a fluctuating many-body environment.