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<p>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 YBa<sub>2</sub>Cu<sub>3</sub>O<sub>6+x</sub>, 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 YBa<sub>2</sub>Cu<sub>3</sub>O<sub>6+x</sub>. We excite apical oxygen phonons with <i>pairs</i> 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.</p>

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Probing amplified Josephson plasmons in YBa2Cu3O6+x by multidimensional spectroscopy

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年6月6日

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  • 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

摘要

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.