Third-order optical nonlinearities play a vital role for generation 1,2 and characterization 3-5 of some of the shortest optical pulses to date, for optical switching applications 6,7 , and for spectroscopy 8,9. In many cases, nonlinear optical effects are used far off resonance, and then an instantaneous temporal response is expected. Here, we show for the first time resonant frequency-resolved optical gating measurements 10-12 that indicate substantial nonlinear polarization relaxation times up to 6.5 fs in dielectric media, i.e., significantly beyond the shortest pulses directly available from commercial lasers. These effects are among the fastest effects observed in ultrafast spectroscopy. Numerical solutions of the time-dependent Schrödinger equation 13,14 are in excellent agreement with experimental observations. The simulations indicate that pulse generation and characterization in the ultraviolet may be severely affected by this previously unreported effect. Moreover, our approach opens an avenue for application of frequency-resolved optical gating as a highly selective spectroscopic probe in high-field physics.

A novel algorithm for the ultrashort laser pulse characterization method of interferometric frequency-resolved optical gating (iFROG) is presented. Based on a genetic method, namely, differential evolution, the algorithm can exploit all available information of an iFROG measurement to retrieve the complex electric field of a pulse. The retrieval is subjected to a series of numerical tests to prove the robustness of the algorithm against experimental artifacts and noise. These tests show that the integrated error-correction mechanisms of the iFROG method can be successfully used to remove the effect from timing errors and spectrally varying efficiency in the detection. Moreover, the accuracy and noise resilience of the new algorithm are shown to outperform retrieval based on the generalized projections algorithm, which is widely used as the standard method in FROG retrieval. The differential evolution algorithm is further validated with experimental data, measured with unamplified three-cycle pulses from a mode-locked Ti:sapphire laser. Additionally introducing group delay dispersion in the beam path, the retrieval results show excellent agreement with independent measurements with a commercial pulse measurement device based on spectral phase interferometry for direct electric-field retrieval. Further experimental tests with strongly attenuated pulses indicate resilience of differential-evolution-based retrieval against massive measurement noise.

The near-ultraviolet photoluminescence of ZnO nanorods induced by multiphoton absorption of unamplified Ti:sapphire pulses is investigated. Power dependence measurements have been conducted with an adaptation of the ultrashort pulse characterization method of interferometric frequencyresolved optical gating. These measurements enable the separation of second harmonic and photoluminescence bands due to their distinct coherence properties. A detailed analysis yields fractional power dependence exponents in the range of 3 to 4, indicating the presence of multiple nonlinear processes. The range in measured exponents is attributed to differences in local field enhancement, which is supported by independent photoluminescence and structural measurements. Simulations based on Keldysh theory suggest contributions by three-and four-photon absorption as well as avalanche ionization in agreement with experimental findings.

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Measurement of nonlinear optical reflectivity of saturable absorber devices is discussed. A setup is described that enables absolute accuracy of reflectivity measurements better than 0.3%. A repeatability within 0.02% is shown for saturable absorbers with few-percent modulation depth. The setup incorporates an in situ knife-edge characterization of beam diameters, making absolute reflectivity estimations and determination of saturation fluences significantly more reliable. Additionally, several measures are discussed to substantially improve the reliability of the reflectivity measurements. At its core, the scheme exploits the limits of state-of-the-art digital lock-in technology but also greatly benefits from a fiber-based master-oscillator power-amplifier source, the use of an integrating sphere, and simultaneous comparison with a linear reflectivity standard.