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arXiv:2509.03936 · Physical review. B./Physical review. B

Two-dimensional coherent spectroscopy of disordered superconductors in the narrow-band and broad-band limits

Naoto Tsuji

Published May 11, 2026• 1 citation
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Abstract

We theoretically analyze two-dimensional coherent spectroscopy (2DCS) signals for disordered superconductors in two limits: One is the narrow-band limit with sinusoidal pulse waves, and the other is the broad-band limit with delta-function pulses. While the 2DCS signal in the narrow-band limit is related to the third-order nonlinear susceptibilities $χ^{(3)}(3Ω; Ω, Ω, Ω)$ (third harmonic generation) and $χ^{(3)}(Ω; Ω, Ω, -Ω)$ (ac Kerr effect), we find that in the broad-band limit the signal along the diagonal and horizontal lines in the two-dimensional frequency space is related to another nonlinear susceptibility $χ^{(3)}(Ω; Ω, 0, 0)$ (dc Kerr effect). We numerically evaluate those susceptibilities for a lattice model of superconductors based on the BCS mean-field theory and self-consistent Born approximation for impurities. The 2DCS signals in the narrow-band and broad-band limits show threshold and resonance behaviors at the superconducting-gap frequency, respectively, whose physical origin is discussed in light of quasiparticle and Higgs-mode excitations.

DOI
10.1103/68kq-n6g8

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We theoretically analyze two-dimensional coherent spectroscopy (2DCS) signals for disordered superconductors in two limits: One is the narrow-band limit with sinusoidal pulse waves, and the other is the broad-band limit with delta-function pulses. While the 2DCS signal in the narrow-band limit is related to the third-order nonlinear susceptibilities χ(3)(3Ω;Ω,Ω,Ω)χ^{(3)}(3Ω; Ω, Ω, Ω)χ(3)(3Ω;Ω,Ω,Ω) (third harmonic generation) and χ(3)(Ω;Ω,Ω,−Ω)χ^{(3)}(Ω; Ω, Ω, -Ω)χ(3)(Ω;Ω,Ω,−Ω) (ac Kerr effect), we find that in the broad-band limit the signal along the diagonal and horizontal lines in the two-dimensional frequency space is related to another nonlinear susceptibility χ(3)(Ω;Ω,0,0)χ^{(3)}(Ω; Ω, 0, 0)χ(3)(Ω;Ω,0,0) (dc Kerr effect). We numerically evaluate those susceptibilities for a lattice model of superconductors based on the BCS mean-field theory and self-consistent Born approximation for impurities. The 2DCS signals in the narrow-band and broad-band limits show threshold and resonance behaviors at the superconducting-gap frequency, respectively, whose physical origin is discussed in light of quasiparticle and Higgs-mode excitations.
Two-dimensional coherent spectroscopy (2DCS) provides insights into the nonlinear response of correlated lattice systems. We simulate multipulse excitations in the Hubbard model using nonequilibrium dynamical mean-field theory to extract the 2DCS signal of weak-coupling antiferromagnets with and without local potential disorder. By comparing calculations with static and dynamic Hartree terms, and analyzing the waiting-time dependence of the signal, we identify the contribution of the collective amplitude mode to the spectroscopic features and the relevant underlying processes. With broadband pulses, the rephasing and nonrephasing peaks at the gap energy are found to be of predominant amplitude mode character. Using narrow-band pulses, we also demonstrate a strong enhancement of these amplitude mode-related signals at a pulse frequency of half the gap size.
Two-dimensional coherent spectroscopy (2DCS) is a nonlinear spectroscopy technique capable of identifying whether apparent continua in linear response are made out of multiplets of sharp deconfined quasiparticles. This makes it a potent tool for experimental identification of fractionalized phases. Previous discussions have focused on limits where the quasiparticles in question are infinitely long lived. In this paper we discuss 2DCS in the regime where the fractionalized quasiparticles can themselves decay. We introduce a powerful path-integral-based approach, whereby the computation of nonlinear susceptibilities reduces to an efficient exercise in diagrammatic perturbation theory. We apply this method to compute the 2DCS response of the one-dimensional transverse field Ising model, in the presence of integrability-breaking perturbations. We discuss aspects of the self-energy of the fractionalized quasiparticles that may be extracted via 2DCS, such as the momentum-dependent decay rate.
We study electric field induced two-dimensional coherent nonlinear optical spectroscopy (2DCS) in a Kitaev magnet at finite temperature. We show that 2DCS is susceptible to both types of fractional quasiparticles of this quantum spin-liquid, i.e., fermions and flux visons. Focusing on the second order response, we find a strong antidiagonal feature in the two-dimensional frequency plane, related to the galvanoelectric effect of the fractional fermions. Perpendicular to the antidiagonal, the width of this feature is set by quasiparticle relaxation rates beyond the bare Kitaev magnet, thereby providing access to single-particle characteristics within the multi-particle 2DCS continuum. While the structure of the 2DCS susceptibility stems from the fermionic quasiparticles and displays Fermi blocking versus temperature, the emergent bond randomness which arises due to thermally populated visons strongly modifies the fermionic spectrum. Therefore also the presence of gauge excitations is manifest in the 2DCS susceptibility as the temperature is increased beyond the flux proliferation crossover. Our results are consistent with and extend previous findings on second harmonic generation in Kitaev magnets.
We investigate the spatially resolved dynamics of the collective amplitude Schmid-Higgs (SH) mode in disordered s-wave superconductors and fermionic superfluids. By analyzing the analytic structure of the zero-temperature SH susceptibility in the complex frequency plane, we find that, when the coherence length greatly exceeds the mean free path, (i) the SH response at fixed wave vectors exhibits late-time oscillations decaying as 1/t^{2} with frequency 2Δ, where Δ is the superconducting gap; (ii) subdiffusive oscillations with a dynamical exponent z=4 emerge at late times and large distances; and (iii) spatial oscillations at a fixed frequency decay exponentially, with a period that diverges as the frequency approaches 2Δ from above. When the coherence length is comparable to the mean free path, additional exponentially decaying oscillations at fixed wave vectors appear with a frequency above 2Δ. Furthermore, we show that the SH mode induces an extra peak in the third-harmonic generation current at finite wave vectors. The frequency of this peak is shifted from the conventional resonance at Δ, thereby providing an unambiguous signature of order parameter amplitude dynamics.
Multidimensional spectroscopy has become an established tool for disentangling microscopic processes that remain unresolved in conventional linear spectroscopy. Its extension to the terahertz regime now enables analogous questions to be addressed for low-energy collective excitations in quantum materials and synthetic many-body systems. Unlike isolated few-level systems, however, these collective modes generally cannot be described within the standard framework of nonlinear spectroscopy based on a few-level description. Their response is instead governed by their extended nature, interplay of interactions, fluctuations, disorder, dissipation, and coupling to additional degrees of freedom. This thesis develops a theoretical framework for computing and interpreting multidimensional nonlinear spectroscopy in quantum many-body systems. Using real-time nonequilibrium field theory, we formulate nonlinear susceptibilities diagrammatically in terms of propagators, interaction vertices, and self-energies, with particular emphasis on the third-order susceptibility relevant to infrared-active collective excitations. This approach places the established concepts and capabilities of multidimensional spectroscopy within a systematic many-body field-theoretical framework. Furthermore, this formulation makes it possible to move beyond the established probing capabilities, extending multidimensional spectroscopy beyond few-level descriptions and revealing new signatures and functionalities specific to interacting many-body systems. At the same time, it provides a controlled framework for constructing approximations that preserve the underlying symmetries and conservation laws of the system while remaining amenable to both analytical and numerical calculations. By incorporating quantum and thermal fluctuations within the random-phase approximation, we demonstrate that two-dimensional spectra can reveal the growth of fluctuations, identify field-theoretical bound states, and characterize their coupling to many-body continua. We further develop a diagrammatic description of rephasing in extended bosonic systems in the presence of static disorder. We identify the disorder vertex corrections responsible for echo formation and show how echo spectroscopy separates disorder-induced broadening from intrinsic relaxation. This framework is extended to coupled modes and strongly interacting regimes, where interactions can either enhance or suppress rephasing. A further result is the identification of a nonrephasing four-wave-mixing signal that is critically enhanced near a phase transition, in contrast to simpler nonlinear protocols like third-harmonic generation. We apply this framework to electromagnons in NiI2_22​, Josephson plasmons in La2−x_{2-x}2−x​Srx_xx​CuO4_44​, and the low-energy collective excitations in coupled one-dimensional Bose-Einstein condensates. Across these systems, we show how multidimensional spectroscopy can disentangle disorder from intrinsic relaxation, reveal the effects of interactions and fluctuations, identify coupling between collective modes and continua, and extract microscopic information that remains obscured in conventional spectroscopy. Taken together, the results of this thesis provide a diagrammatic framework for calculating and interpreting multidimensional nonlinear spectroscopic signals in many-body systems, while establishing this technique as a selective probe of collective dynamics across a broad range of quantum materials and synthetic platforms.
Two-dimensional coherent spectroscopy (2DCS) with terahertz radiation offers a promising new avenue for the exploration of many-body phenomena in quantum magnets. This includes the potential diagnosis of fractionalized excitations, for which linear response often struggles due to the indistinguishability of a continuum of fractional excitations from that caused by disorders or impurities. However, the interpretation of the complex results produced by 2DCS remains a challenge. Here, we explore a numerical approach based on exact diagonalization (ED) to help push forward our understanding of 2DCS and, as an example, use it to study the impact of confinement in the one-dimensional transverse field Ising (TFIM) model. We first validate our approach by comparing numerical ED and exact analytical results for the spectroscopic signatures of fractionalized spinons in the model, which exhibits a sharp spinon-echo signal in 2DCS, and show how to understand the finite-size effects inevitable with the inherently small system sizes in ED calculations. By augmenting the model with a longitudinal field, which breaks integrability and introduces confinement of spinon pairs, we observe significant changes to the 2DCS spectrum, such as nonsymmetric broadening of the spinon-echo signal. To further elucidate these changes, we introduce a ``four-kink'' approximation, an effective model that captures the interactions between multiple (confined) spinon pairs. Comparing ED data to these four-kink results provides understanding of the multiple features of the 2DCS spectra, allowing us to interpolate between finite-system size data and the thermodynamic limit. One advantage of our ED approach is its possible extension to finite temperatures, which we explore using thermally pure quantum states and demonstrate how the intensity and spectroscopic patterns of 2DCS change when going beyond the integrable model. Our numerically exact results provide a benchmark for future experiments and theoretical studies relying on approximation methods and pave the way for the exploration of fractionalized excitations in quantum magnets.