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Bibliographic Details
Main Authors: Katsumi, Kota, Fiore, Jacopo, Udina, Mattia, Romero III, Ralph, Barbalas, David, Jesudasan, John, Raychaudhuri, Pratap, Seibold, Goetz, Benfatto, Lara, Armitage, N. P.
Format: Preprint
Published: 2023
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Online Access:https://arxiv.org/abs/2311.16449
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Table of Contents:
  • Recently developed terahertz (THz) two-dimensional coherent spectroscopy (2DCS) is a powerful technique to obtain materials information in a fashion qualitatively different from other spectroscopies. Here, we utilized THz 2DCS to investigate the THz nonlinear response of conventional superconductor NbN. Using broad-band THz pulses as light sources, we observed a third-order nonlinear signal whose spectral components are peaked at twice the superconducting gap energy $2Δ$. With narrow-band THz pulses, a THz nonlinear signal was identified at the driving frequency $Ω$ and exhibited a resonant enhancement at temperature when $Ω= 2Δ$. General theoretical considerations show that such a resonance can only arise from a disorder-activated paramagnetic coupling between the light and the electronic current. This proves that the nonlinear THz response can access processes distinct from the diamagnetic Raman-like density fluctuations, which are believed to dominate the nonlinear response at optical frequencies in metals. Our numerical simulations reveal that even for a small amount of disorder, the $Ω=2Δ$ resonance is dominated by the superconducting amplitude mode over the entire investigated disorder range. This is in contrast to other resonances, whose amplitude-mode contribution depends on disorder. Our findings demonstrate the unique ability of THz 2DCS to explore collective excitations inaccessible in other spectroscopies.