Polarization-resolved terahertz third-harmonic generation in a single-crystal superconductor NbN: Dominance of the Higgs mode beyond the BCS approximation

Recent advances in time-domain terahertz (THz) spectroscopy have unveiled that resonantly enhanced strong THz third-harmonic generation (THG) mediated by the collective Higgs amplitude mode occurs in s-wave superconductors, where charge-density fluctuations (CDFs) have been shown to also contribute to the nonlinear third-order susceptibility. It has been theoretically proposed that the nonlinear responses of Higgs and CDF exhibit essentially different polarization dependences. Here we experimentally discriminate the two contributions by polarization-resolved intense THz transmission spectroscopy for a single-crystal NbN film. The result shows that the resonant THG in the transmitted light always appears in the polarization parallel to that of the incident light with no appreciable polarization-angle dependence relative to the crystal axis. When we compare this with the theoretical calculation here with the BCS approximation and the dynamical mean-field theory for a model of NbN constructed from first principles, the experimental result strongly indicates that the Higgs mode rather than the CDF dominates the THG resonance in NbN. A possible mechanism for this is the retardation effect in the phonon-mediated pairing interaction beyond BCS.