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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 also been shown to 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 crystal axis dependence. 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 discussed such as the retardation effect in the phonon-mediated pairing interaction beyond BCS.
Giant second-harmonic generation (SHG) in the terahertz (THz) frequency range is observed in a thin film of an s-wave superconductor NbN, where the time-reversal ($mathcal{T}$-) and space-inversion ($mathcal{P}$-) symmetries are simultaneously broken
We report on time-resolved linear and nonlinear terahertz spectroscopy of the two-band superconductor MgB$_2$ with the superconducting transition temperature $T_c approx$ 36 K. Third-harmonic generation (THG) is observed below $T_c$ by driving the sy
Higgs spectroscopy is a new field in which Higgs modes in nonequilibrium superconductors are analyzed to gain information about the ground state. One experimental setup in which the Higgs mode in s-wave superconductors was observed is periodic drivin
Higgs mode in superconductors, i.e. the collective amplitude mode of the order parameter does not associate with charge nor spin fluctuations, therefore it does not couple to the electromagnetic field in the linear response regime. On the contrary to
Ultrafast responses of BCS superconductor Nb1-xTixN films in a nonadiabatic excitation regime were investigated by using terahertz (THz) pump-THz probe spectroscopy. After an instantaneous excitation with the monocycle THz pump pulse, a transient osc