Femtosecond lasers, white light absorption

For 2PA or ESA spectral measurements, it is necessary to use tunable laser sources where optical parametric oscillators/amplifiers (OPOs/OPAs) are extensively used for nonlinear optical measurements. An alternative approach, which overcomes the need of expensive and misalignment prone OPO/OPA sources, is the use of an intense femtosecond white-light continuum (WLC) for Z-scan measurements [71,72]. Balu et al. have developed the WLC Z-scan technique by generating a strong WLC in krypton gas, allowing for a rapid characterization of the nonlinear absorption and refraction spectra in the range of 400-800 nm [72]. 

The femtosecond transient absorption studies were performed with 387 nm laser pulses (1 khz, 150 fs pulse width) from an amplified Ti Sapphire laser system (Model CPA 2101, Clark-MXR Inc). A NOPA optical parametric converter was used to generate ultrashort tunable visible pulses from the pump pulses. The apparatus is referred to as a two-beam setup, where the pump pulse is used as excitation source for transient species and the delay of the probe pulse is exactly controlled by an optical delay rail. As probe (white light continuum), a small fraction of pulses stemming from the CPA laser system was focused by a 50 mm lens into a 2-mm thick sapphire disc. A schematic representation of the setup is given below in Fig. 7.2. 2.0 mm quartz cuvettes were used for all measurements. 

Fig. 7.2 Two-beam experimental setup for femtosecond transient absorption studies using a white light continuum. A commercially available CPA 2101 laser system delivers the pulses. Ultrashort tunable visible pulses are obtained by the NOPA optical parametric converter. A chopper wheel is used to cut every second pump pulse in order to compare the signal with and without the pump. The white light continuum is generated by a sapphire disc. The time delay between the pump and probe pulses is adjusted by the optical delay rail...

Nanosecond laser Flash Photolysis experiments were performed with 355 and 532 nm laser pulses from a Brilland-Quantel Nd YAG system (5 ns pulse width) in a front face (VIS) and side face (NIR) geometry using a pulsed 450 W XBO lamp as white light source. Similarly to the femtosecond transient absorption setup, a two beam arrangement was used. However, the pump and probe pulses were generated separately, namely the pump pulse stemming from the Nd YAG laser and the probe from the XBO lamp. A schematic representation of the setup is given below in Fig. 7.3. 0.5 cm quartz cuvettes were used for all measurements. 

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