Absorptive loss and band non-parabolicity as a physical origin of large nonlinearity in epsilon-near-zero materials

Abstract: For decades, nonlinear optics has been used to control the frequency and propagation of light in unique ways enabling a wide range of applications such as ultrafast lasing, sub-wavelength imaging, and novel sensing methods. Through this, a key thread of research in the field has always been the development of new and improved nonlinear materials to empower these applications. Recently, epsilon-near-zero (ENZ) materials have emerged as a potential platform to enhanced nonlinear interactions, bolstered in large part due to the extreme refractive index tuning ({\Delta}n~ 0.1 - 1) of sub-micron thick films that has been demonstrated in literature. Despite this experimental success, the theory has lagged and is needed to guide future experimental efforts. Here, we construct a theoretical framework for the intensity-dependent refractive index of the most popular ENZ materials, heavily doped semiconductors. We demonstrate that the nonlinearity when excited below bandgap, is due to the modification of the effective mass of the electron sea which produces a shift in the plasma frequency. We discuss trends and trade-offs in the optimization of excitation conditions and material choice (such material loss, band structure, and index dispersion), and provide a figure of merit through which the performance of future materials may be evaluated. By illuminating the framework of the nonlinearity, we hope to propel future applications in this growing field.