Principles of 2D terahertz spectroscopy of collective excitations: the case of Josephson plasmons in layered superconductors

Two-dimensional terahertz spectroscopy (2DTS), a terahertz analogue of nuclear magnetic resonance, is a new technique poised to address many open questions in complex condensed matter systems. The conventional theoretical framework used ubiquitously for interpreting multidimensional spectra of discrete quantum level systems is, however, insufficient for the continua of collective excitations in strongly correlated materials. Here, we develop a theory for 2DTS of a model collective excitation, the Josephson plasma resonance in layered superconductors. Starting from a mean-field approach at temperatures well below the superconducting phase transition, we obtain expressions for the multidimensional nonlinear responses that are amenable to intuition derived from the conventional single-mode scenario. We then consider temperatures near the superconducting critical temperature $T_c$, where dynamics beyond mean-field become important and conventional intuition fails. As fluctuations proliferate near $T_c$, the dominant contribution to nonlinear response comes from an optical parametric drive of counter-propagating Josephson plasmons, which gives rise to 2D spectra that are qualitatively different from the mean-field predictions. As such, and in contrast to one-dimensional spectroscopy techniques, such as third harmonic generation, 2DTS can be used to directly probe thermally excited finite-momentum plasmons and their interactions. Our theory provides a clear interpretation of recent 2DTS measurements on cuprates, and we discuss implications beyond the present context of Josephson plasmons.