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Register a new userPolarization-resolved terahertz third-harmonic generation in a superconductor NbN: dominance of Higgs mode beyond the BCS approximation
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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.
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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 by supercurrent injection. We demonstrate that the phase of the second-harmonic (SH) signal flips when the direction of supercurrent is inverted, i.e., the signal is ascribed to the nonreciprocal response that occurs under broken $mathcal{P}$- and $mathcal{T}$-symmetries. The temperature dependence of the SH signal exhibits a sharp resonance, which is accounted for by the vortex motion driven by the THz electric field in an anharmonic pinning potential. The maximum conversion ratio $eta_{mathrm{SHG}}$ reaches $approx10^{-2}$ in a thin film NbN with the thickness of 25 nm after the field cooling with a very small magnetic field of $approx1$ Oe, for a relatively weak incident THz electric field of 2.8 kV/cm at 0.48 THz.
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 system with intense narrowband THz pulses. For the pump-pulse frequencies $f=$ 0.3, 0.4, and 0.5 THz, temperature-dependent evolution of the THG signals exhibits a resonance maximum at the temperature where $2f=2Delta_pi(T)$, for the dirty-limit superconducting gap $2Delta_pi=$ 1.03 THz at 4 K. In contrast, for $f=$ 0.6 and 0.7 THz with $2f>2Delta_pi$, the THG intensity increases monotonically with decreasing temperature. Moreover, for $2f<2Delta_pi$ the THG is found nearly isotropic with respect to the pump-pulse polarization. These results suggest the predominant contribution of the driven Higgs amplitude mode of the dirty-limit gap, pointing to the importance of scattering for observation of the Higgs mode in superconductors.
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 driving with THz light, which shows resonances in the third-harmonic generation (THG) signal if twice the driving frequency matches the energy of the Higgs mode. We derive expressions of the driven gap oscillations for arbitrary gap symmetry and calculate the THG response. We demonstrate that the possible Higgs modes for superconductors with non-trivial gap symmetry can lead to additional resonances if twice the driving frequency matches the energy of these Higgs modes and we disentangle the influence of charge density fluctuations (CDF) to the THG signal within our clean-limit analysis. With this we show that THG experiments on unconventional superconductors allow for a detection of their Higgs modes. This paves the way for future studies on realistic systems including additional features to understand the collective excitation spectra of unconventional superconductors.
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 this common understanding, here, we demonstrate that, if the dc supercurrent is introduced into the superconductor, the Higgs mode becomes infrared active and is directly observed in the linear optical conductivity measurement. We observed a sharp resonant peak at $omega=2Delta$ in the optical conductivity spectrum of a thin-film NbN in the presence of dc supercurrent, showing a reasonable agreement with the recent theoretical prediction. The method as proven by this work opens a new pathway to study the Higgs mode in a wide variety of superconductors.
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 oscillation emerges in the electromagnetic response in the BCS gap energy region. The oscillation frequency coincides with the asymptotic value of the BCS gap energy, indicating the appearance of the theoretically-anticipated collective amplitude mode of the order parameter, namely the Higgs amplitude mode. Our result opens a new pathway to the ultrafast manipulation of the superconducting order parameter by optical means.
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