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Strong nonlinear optical effects in micro-confined atmospheric air

Historically, nonlinear optical phenomena such as spectral broadening by harmonic generation have been associated with crystals owing to their strong nonlinear refractive indices, which are in the range of ∼10−14  cm2/W. This association was also the result of the limited optical power available from early lasers and the limited interaction length that the laser–crystal interaction architecture could offer. Consequently, these limitations disqualified a large number of materials whose nonlinear coefficient is lower than n2∼10−16  cm2/W as suitable materials for nonlinear optics applications. For example, it is a common practice in most of optical laboratories to consider ambient or atmospheric air as a “nonlinear optically” inert medium due to its very low nonlinear coefficient (∼10.10−19  cm2/W) and low density. Today, the wide spread of high-power ultra-short pulse lasers on one hand, and low transmission loss and high-power handling of Kagome hollow-core photonic crystal fiber on the other hand, provide the necessary ingredients to excite strong nonlinear optical effects in practically any gas media, regardless of how low its optical nonlinear response is. By using a single table-top 1 mJ ultra-short pulse laser and an air exposed inhibited-coupling guiding hollow-core photonic crystal fiber, we observed generation of supercontinuum and third harmonic generation when the laser pulse duration was set at 600 fs and Raman comb generation when the duration was 300 ps. The supercontinuum spectrum spans over ∼1000  THz and exhibits a typical spectral-density energy of 150 nJ/nm. The dispersion profile of inhibited-coupling hollow-core fiber imprints a distinctive sequence in the supercontinuum generation, which is triggered by the generation of a cascade of four-wave mixing lines and concluded by solitonic dynamics. The Raman comb spans over 300 THz and exhibits multiple sidebands originating from N2 vibrational and ro-vibrational Raman transitions. With the growing use of hollow-core photonic crystal fiber in different fields, the results can be applied to mitigate air nonlinear response when it is not desired or to use ambient air as a convenient nonlinear medium.