Tracing the dynamics of superconducting order via transient terahertz third-harmonic generation.

Ultrafast optical control of quantum systems is an emerging field of physics. In particular, the possibility of light-driven superconductivity has attracted much of attention. To identify nonequilibrium superconductivity, it is necessary to measure fingerprints of superconductivity on ultrafast timescales. Recently, nonlinear THz third-harmonic generation (THG) was shown to directly probe the collective degrees of freedoms of the superconducting condensate, including the Higgs mode. Here, we extend this idea to light-driven nonequilibrium states in superconducting La2-xSrxCuO4, establishing an optical pump-THz-THG drive protocol to access the transient superconducting order-parameter quench and recovering on few-picosecond timescales. We show in particular the ability of two-dimensional TH spectroscopy to disentangle the effects of optically excited quasiparticles from the pure order-parameter dynamics, which are unavoidably mixed in the pump-driven linear THz response. Benchmarking the gap dynamics to existing experiments shows the ability of driven THG spectroscopy to overcome these limitations in ordinary pump-probe protocols.

THz non-linear optical response in cuprates: predominance of the BCS response over the Higgs mode.

Recent experiments with strong THz fields in unconventional cuprate superconductors have clearly evidenced an increase of the non-linear optical response below the superconducting critical temperature Tc. As in the case of conventional superconductors, a theoretical estimate of the various effects contributing to the non-linear response is needed in order to interpret the experimental findings. Here, we report a detailed quantitative analysis of the non-linear THz optical kernel in cuprates within a realistic model, accounting for the band structure and disorder level appropriate for these systems. We show that the BCS quasiparticle response is the dominant contribution for cuprates, and its polarization dependence accounts very well for the third-harmonic generation measurements. On the other hand, the polarization dependence of the THz Kerr effect is only partly captured by our calculations, suggesting the presence of additional effects when the system is probed using light pulses with different central frequencies.

Non-linear Terahertz driving of plasma waves in layered cuprates.

The hallmark of superconductivity is the rigidity of the quantum-mechanical phase of electrons, responsible for superfluid behavior and Meissner effect. The strength of the phase stiffness is set by the Josephson coupling, which is strongly anisotropic in layered cuprates. So far, THz light pulses have been used to achieve non-linear control of the out-of-plane Josephson plasma mode, whose frequency lies in the THz range. However, the high-energy in-plane plasma mode has been considered insensitive to THz pumping. Here, we show that THz driving of both low-frequency and high-frequency plasma waves is possible via a general two-plasmon excitation mechanism. The anisotropy of the Josephson couplings leads to markedly different thermal effects for the out-of-plane and in-plane response, linking in both cases the emergence of non-linear photonics across Tc to the superfluid stiffness. Our results show that THz light pulses represent a preferential knob to selectively drive phase excitations in unconventional superconductors.

Raman Response in the Nematic Phase of FeSe.

Raman experiments on bulk FeSe revealed that the low-frequency part of the B_{1g} Raman response R_{B1g}(Ω), which probes nematic fluctuations, rapidly decreases below the nematic transition at T_{n}∼85 K. Such behavior is expected when a gap opens up and at a first glance is inconsistent with the fact that FeSe remains a metal below T_{n}. We argue that the drop of R_{B1g}(Ω) can be ascribed to the fact that the nematic order drastically changes the orbital content of low-energy excitations near hole and electron pockets, making them nearly mono-orbital. In this situation, the B_{1g} Raman response gets reduced by the same vertex corrections that enforce charge conservation in the symmetric Raman channel. The reduction holds at low frequencies and gives rise to gaplike behavior of R_{B1g}(Ω). We also show that the enhancement of the B_{1g} Raman response near T_{n} is consistent with the sign change of the nematic order parameter between hole and electron pockets.