Ryusuke Matsunaga, Naoto Tsuji, Kazumasa Makise, Hirotaka Terai, Hideo Aoki, and Ryo Shimano
https://journals.aps.org/prb/accepted/06073Oa1P3bEc21dc38d310718d5f15931783f2ce
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 (CDF) 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.
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