Multi-Dimensional Coherent Spectroscopy of Light-Driven States and their Collective Modes in Multi-Band Superconductors

Abstract

We present a comprehensive theory of light-controlled multi-band superconductivity and apply it to predict distinctive signatures of light-driven superconducting (SC) states in terahertz multi-dimensional coherent spectroscopy (THz-MDCS) experiments. We first derive gauge-invariant Maxwell-Bloch equations for multi-band BCS superconductors. For this, we go beyond previously considered Anderson pseudo-spin precession models to include quantum transport effects. By calculating the THz-MDCS spectra measured experimentally, we then identify unique signatures of finite-momentum Cooper-pairing states that live longer than the laser pulse. These non-equilibrium SC states are characterized by long-lived canting of Anderson pseudo-spins. The pseudo-spin oscillators that describe the properties of these SC states are parametrically driven by both finite-momentum Cooper pairing and by time oscillations of the order parameter relative phase. We show that such strong parametric driving leads to drastic changes in the THz-MDCS spectral shape from the predictions of third-order nonlinear susceptibility calculations. These spectral changes strongly depend on the interband-to-intraband interaction ratio and on the collective modes of the light-driven state.

arXiv comment27 pages, 10 figures

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• Advanced Data Processing of THz-Time Domain Spectroscopy Data with Sinusoidally Moving Delay Lines
• Discovery of an Unconventional Quantum Echo by Interference of Higgs Coherence
• Unlocking Quantum Control and Multi-Order Correlations via Terahertz Two-Dimensional Coherent Spectroscopy
• Theory of symmetry-resolved quench-drive spectroscopy: Nonlinear response of phase-fluctuating superconductors
• Two-dimensional coherent spectroscopy of disordered superconductors in the narrow-band and broad-band limits
• Two-dimensional THz spectroscopy in electronic systems: a many-body diagrammatic approach