Probing amplified Josephson plasmons in YBa2Cu3O6+x by multidimensional spectroscopy

Abstract The nonlinear driving of collective modes in quantum materials can lead to a number of striking non-equilibrium functional responses, which merit a comprehensive exploration of underlying dynamics. However, the coherent coupling between nonlinearly-driven modes frequently involves multiple...

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Main Authors: N. Taherian, M. Först, A. Liu, M. Fechner, D. Pavicevic, A. von Hoegen, E. Rowe, Y. Liu, S. Nakata, B. Keimer, E. Demler, M. H. Michael, A. Cavalleri
Format: Article
Language:English
Published: Nature Portfolio 2025-06-01
Series:npj Quantum Materials
Online Access:https://doi.org/10.1038/s41535-025-00776-1
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Summary:Abstract The nonlinear driving of collective modes in quantum materials can lead to a number of striking non-equilibrium functional responses, which merit a comprehensive exploration of underlying dynamics. However, the coherent coupling between nonlinearly-driven modes frequently involves multiple mode coordinates at once, and is often difficult to capture by one-dimensional pump probe spectroscopy. One example is phonon-mediated amplification of Josephson plasmons in YBa2Cu3O6+x, a phenomenon likely associated with the mysterious superconducting-like optical response observed in this material. Here, we report two-dimensional nonlinear spectroscopy measurements in driven YBa2Cu3O6+x. We excite apical oxygen phonons with pairs of mutually-delayed carrier envelope phase stable mid-infrared pump pulses, and detect time-modulated second-order nonlinear optical susceptibility. We find that the driven phonons parametrically amplify coherent pairs of fluctuating opposite-momentum Josephson plasma polaritons, corresponding to a squeezed state of the Josephson plasma.
ISSN:2397-4648