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Abstract: The nonlinear optical response of a material is conventionally assumed to be very much smaller than its linear response. Here we report that the nonlinear contribution to the refractive index of a sample of indium-tin oxide can be much larger than the linear contribution when the optical wavelength is close to the material’s bulk plasma wavelength, where the material exhibits epsilon-near-zero behavior. In particular, we demonstrate that a change in refractive index as large as 0.7 can be obtained in an ultra-thin indium-tin oxide film using an optical intensity of 140 GW/cm2.
Nonlinear optical phenomena result from the light-induced modification of the optical properties of a material lead to a broad range of applications, including microscopy, all-optical data processing, and quantum information. However, nonlinear (NL) effects are typically extremely weak. The size of nonlinear effects is typically limited by the largest intensity that can be used without permanently damaging of the material. Consequently, the resulting change in refractive index is typically of the order of 0.001 or smaller.
A long-standing goal of nonlinear optics (NLO) has been the development of materials that can display a light-induced change in the refractive index of the order of unity. Such materials would lead to exciting new applications of NLO. Indeed, much effort in the fields of plasmonics and metamaterials is devoted to the development of such materials. Furthermore, it has been suggested that materials with vanishing permittivity, commonly known as epsilon-nearzero (ENZ) materials, can be used to induce highly nonlinear phenomena and unusual phase-matching behavior. In this work, we describe our studies of indium-tin oxide (ITO) at its ENZ wavelength, and we demonstrate a refractive index change of 0.7.
Materials possessing free charges, such as metals and doped semiconductors, exhibit a vanishing permittivity at the bulk plasmon wavelength. The zero-permittivity wavelength in doped semiconductors typically lies at infrared wavelengths and can be fine tuned by controlling the level of doping. Here we study the case of an ultra-thin layer of ITO exhibiting ENZ behavior at wavelengths around 1.24 µm. We show that in this spectral region the nonlinear response (intensity-dependent change in refractive index, Δn) is enhanced approximately 2000-fold with respect to that observed at shorter wavelengths and that a Δn of the order of unity can be observed.
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