Recent experiments with strong THz fields in both conventional and unconventional superconductors have clearly evidenced a marked third-harmonic generation below the superconducting temperature $T_c$. Its interpretation challenged substantial theoretical work aimed at establishing the relative efficiency of quasiparticle excitations and collective modes in triggering such a resonant response. Here we compute the nonlinear current by implementing a time-dependent Bogoljubov–de Gennes approach, with the twofold aim to account nonperturbatively for the effect of local disorder, and to include the contribution of all collective modes, i.e., superconducting amplitude (Higgs) and phase fluctuations, and charge fluctuations. We show that, in agreement with previous work, already at small disorder the quasiparticle response is dominated by paramagnetic effects. We further demonstrate that paramagnetic processes mediate also the response of all collective modes, with a substantial contribution of charge/phase fluctuations. These processes, which have been overlooked so far, turn out to dominate the third-order current at strong disorder. In addition, we show that disorder strongly influences the polarization dependence of the nonlinear response, with a marked difference between the clean and the disordered case. Our results are particularly relevant for recent experiments in cuprates, whose band structure is in a first approximation reproduced by our lattice model.

• Received 6 November 2020
• Revised 4 January 2021
• Accepted 6 January 2021

DOI:https://doi.org/10.1103/PhysRevB.103.014512