Title:Phonon-Mediated Nonlinear Optical Responses and Quantum Geometry

Abstract:Unraveling the complexities of nonlinear optical (NLO) responses, particularly the intricate many-body interactions among photons, electrons, and phonons, remains a significant challenge in condensed matter physics. Here, we present a diagrammatic approach to explore NLO responses with electron-phonon coupling (EPC), focusing on the phonon-mediated nonlinear optical (Ph-NLO) responses up to the second order in photon perturbation. We systematically analyze the shift and ballistic mechanisms responsible for phonon-mediated electron-photon interactions. By incorporating EPC effects, we elucidate phenomena such as phonon-mediated shift current (Ph-SC) and second-harmonic generation (Ph-SHG) in a comprehensive Ph-NLO framework. This approach enables below-gap resonant responses at terahertz photon frequencies, offering a promising mechanism for terahertz optical applications that surpasses the constraints of conventional pure-electronic NLO theories. Additionally, we explore the geometric and topological consequences of Ph-NLO responses by introducing the EPC Berry curvature, EPC quantum metric, and EPC shift vector. These concepts unveil a unique quantum geometric structure within the Hilbert space, parameterized by both the electronic wavevector and phonon-displacement, thereby extending the established pure-electronic quantum geometry. Using a general Rice-Mele model, we demonstrate the connection between Ph-NLO responses and EPC geometry, discussing the implications and predicting observable effects for future experimental validation. This framework also provides a foundation for advancing first-principles calculations aimed at the discovery and engineering of NLO materials. The insights gained from this study contribute to a more profound understanding of NLO responses and EPC quantum geometry.