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Fundamentals of heterodyne wave mixing spectroscopy: a tutorial

This tutorial provides a joint theoretical and experimental overview of heterodyne wave mixing spectroscopy, focusing mainly on four-wave mixing (FWM). This powerful and versatile time-resolved nonlinear optical spectroscopy technique enables the investigation of individual localized single photon emitters, as well as microscopy of extended samples, e.g., two-dimensional transition metal dichalcogenides. Starting with the fundamental theory of optically driven two-level systems, we motivate the utility of wave mixing spectroscopy via a discussion on homogeneous and inhomogeneous linewidths which can be independently measured using FWM. We then provide a detailed overview of the heterodyne wave mixing setup operated by one of the authors (JK) at Institut Néel in Grenoble, supported by theoretical modeling of the signal detection process. Throughout the paper we elaborate on important benefits of heterodyne wave mixing spectroscopy, e.g., background-free detection, measurement of the full signal field including amplitude and phase, and investigation of coupling mechanisms in few-level systems. Within the context of the latter point we discuss the significance of two-dimensional (2D) FWM spectra. This tutorial is dedicated to students, young researchers, as well as experts in the field of nonlinear spectroscopy in general and FWM in particular. It explains the fundamental concepts and building blocks required to operate a heterodyne wave mixing experiment both from the experimental and theoretical side. This joint approach is helpful for theoreticians who want to accurately and quantitatively model wave mixing signals, as well as for experimentalists who aim to interpret their recorded data.