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International audience; The nonlinear refractive indices ( n 2 ) of a selection of bulk (LiB 3 O 5 , KTiOAsO 4 , MgO:LiNbO 3 , LiGaS 2 , ZnSe) and liquid (E7, MLC2132) crystals are measured at 1030 nm in the sub-picosecond regime (200 fs) by nonlinear chirped interferometry. The reported values provide key parameters for the design of near- to mid-infrared parametric sources, as well as all-optical delay lines.

Four-wave mixing processes are ubiquitous in ultrafast optics and the determination of the coefficients of the $\chi^{(3)}$ tensor is thus essential. We introduce a novel time-resolved ultrafast spectroscopic method to characterize the third-order nonlinearity on the femtosecond time-scale. This approach, coined as "nonlinear chirped Doppler interferometry", makes use of the variation of the optical group delay of a transmitted probe under the effect of an intense pump pulse in the nonlinear medium of interest. The observable is the spectral interference between the probe and a reference pulse sampled upstream. We show that the detected signal is enhanced when the pulses are chirped, and that, although interferometric, the method is immune to environmental phase fluctuations and drifts. By chirping adequately the reference pulse, the transient frequency shift of the probe pulses is also detected in the time domain and the detected nonlinear signal is enhanced. Nonlinear phase shifts as low as 10\,mrad, corresponding to a frequency shift of 30\,GHz, i.e. 0.01\% of the carrier frequency, are detected without heterodyne detection or active phase-stabilization. The diagonal and/or non-diagonal terms of reference glasses (SiO$_2$) and crystals (Al$_2$O$_3$, BaF$_2$, CaF$_2$) are characterized. The method is finally applied to measure the soft vibration mode of KTiOAsO$_4$ (KTA).

International audience; We report a novel jitter-free ultrafast spectroscopy method to investigate third-order nonlinearity. The method is applied to assess the nonlinear refractive indices of ori-entated, nematic liquid crystals in the femtosecond regime.

National audience

The stability of the phase difference between two white-light continua, generated from the same 180-fs pulses at ≃ 1035 nm, is assessed by a modified Bellini-Hänsch interferometer. Mutual spectral phase stability is studied and quantified as a function of several parameters: pulse energy, position of the nonlinear crystal with respect to the beam waist and interaction length. Our results show that intrapulse decoherence may significantly contribute to the measured CEP noise floor. In addition, spectrally-resolved intensity-to-phase coupling coefficients are measured and stability regions are identified.

Four-wave mixing processes are ubiquitous in ultrafast optics and the determination of the coefficients of the χ(3) tensor is thus essential. We introduce a novel time-resolved ultrafast spectroscopic method to characterize the third-order nonlinearity on the femtosecond time-scale. This approach, coined as “nonlinear chirped interferometry,” makes use of the variation of the optical group delay of a transmitted probe under the effect of an intense pump pulse in the nonlinear medium of interest. The observable is the spectral interference between the probe and a reference pulse sampled upstream and the metric is the transient swing of the probe group delay. We show that the detected signal is enhanced when the pulses are weakly chirped, and that, although interferometric, the method is intrinsically less sensitive to environmental phase fluctuations and drifts. By chirping adequately the reference pulse, the transient frequency shift of the probe pulses is also detected in the time domain and the detected nonlinear signal is enhanced. Nonlinear phase shifts as low as 10 mrad, corresponding to a frequency shift of 30 GHz, i.e., 0.01% of the carrier frequency, are detected without heterodyne detection or active phase-stabilization. The diagonal and/or non-diagonal terms of reference glasses (SiO2) and crystals (Al2O3, BaF2, CaF2) are characterized. The method is finally applied to measure the soft vibration mode of KTiOAsO4 (KTA).