Broadband UV-Vis vibrational coherence spectrometer based on a hollow fiber compressor.

We describe a broadband transient absorption (TA) spectrometer devised to excite and probe, in the blue to UV range, vibrational coherence dynamics in organic molecules in condensed phase. A 800-nm Ti:Sa amplifier and a hollow fiber compressor are used to generate a 6-fs short pulse at 1 kHz. Broadband sum frequency generation with the fundamental pulse is implemented to produce a 400-nm, 8-fs Fourier limited short pulse. A UV-Vis white-light supercontinuum is implemented as a probe with intensity self-referencing to achieve a shot-noise-limited sensitivity. Rapid scanning of the pump-probe delay is shown very efficient in suppressing the noise resulting from low-frequency pump intensity fluctuations. Using either of the 800-nm or 400-nm broadband pulses as the pump for TA spectroscopy of organic molecules in solution, we resolve oscillatory signals down to the 320 nm probing wavelength with a 3200 cm-1 FWHM bandwidth. Their Fourier transformation reveals the corresponding molecular vibrational spectra. Finally, we demonstrate the use of this setup as a vibrational coherence spectrometer for the investigation of the vibrational dynamics accompanying the sub-ps C=C photoisomerization of a retinal-like molecular switch through a conical intersection.

Two MHz tunable non collinear optical parametric amplifiers with pulse durations down to 6 fs.

We report on the development of a 2 MHz non collinear optical parametric amplifier (NOPA) for high repetition rate time resolved X-ray or optical spectroscopy. Our modular and very flexible device is pumped by the second and third harmonics of a commercial femtosecond Ytterbium-doped fiber laser. The amplified pulses are tunable from 520 nm to 1000 nm with pulse durations between 15 and 30 fs over the full tuning range. The same setup is also suitable for broadband amplification and we demonstrate the generation of 6 fs pulses at a central wavelength of 850 nm as well as the generation of a broadband spectrum supporting 4.2 fs transform limited pulse duration at a central wavelength of 570 nm. Very high stability and compactness is achieved thanks to an optimized mechanical design.