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

Kim, Min-Jae; Kovalev, Sergey; Udina, Mattia; Haenel, Rafael; Kim, Gideok; Puviani, Matteo; Cristiani, Georg; Ilyakov, Igor et al. · Sci Adv · 2024

basic_science · Level V

Where this comes from

Abstract

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 La<sub>2-<i>x</i></sub>Sr<i><sub>x</sub></i>CuO<sub>4</sub>, 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.