Direct temporal characterization of sub-3-fs deep UV pulses generated by resonant dispersive wave emission.

We report on the complete temporal characterization of ultrashort pulses, generated by resonant dispersive wave emission in gas-filled hollow-capillary fibers, with energy in the microjoule range and continuously tunable from the deep-ultraviolet to the ultraviolet. Temporal characterization of such ultrabroad pulses, particularly challenging in this spectral region, was performed using an all-in-vacuum setup for self-diffraction frequency resolved optical gating (SD-FROG). Sub-3-fs pulses were measured, tunable from 250 nm to 350 nm, with a minimum pulse duration of 2.4 ± 0.1 fs.

Electron and ion spectroscopy of azobenzene in the valence and core shells.

Azobenzene is a prototype and a building block of a class of molecules of extreme technological interest as molecular photo-switches. We present a joint experimental and theoretical study of its response to irradiation with light across the UV to x-ray spectrum. The study of valence and inner shell photo-ionization and excitation processes combined with measurement of valence photoelectron-photoion coincidence and mass spectra across the core thresholds provides a detailed insight into the site- and state-selected photo-induced processes. Photo-ionization and excitation measurements are interpreted via the multi-configurational restricted active space self-consistent field method corrected by second order perturbation theory. Using static modeling, we demonstrate that the carbon and nitrogen K edges of azobenzene are suitable candidates for exploring its photoinduced dynamics thanks to the transient signals appearing in background-free regions of the NEXAFS and XPS.

Fourier transform spectroscopy in the vibrational fingerprint region with a birefringent interferometer.

We introduce a birefringent interferometer for Fourier transform (FT) spectroscopy in the mid-infrared, covering the vibrational fingerprint region (5-10 µm, 1000-2000 cm-1), which is crucial for molecular identification. Our interferometer employs the crystal calomel (Hg2Cl2), which combines high birefringence (ne-no≈0.55) with a broad transparency range (0.38-20 µm). We adopt a design based on birefringent wedges, which is simple and compact and guarantees excellent delay accuracy and long-term stability. We demonstrate FTIR spectroscopy, with a frequency resolution of 3 cm-1, as well as two-dimensional IR (2DIR) spectroscopy. Our setup can be extended to other spectroscopic modalities such as vibrational circular dichroism and step-scan FT spectroscopy.

Wavelength tuning of femtosecond pulses generated in nonlinear crystals by using diffractive lenses.

We demonstrate that diffractive lenses (DLs) can be used as a simple method to tune the central wavelength of femtosecond pulses generated from second-order nonlinear optical processes in birefringent crystals. The wavelength tunability is achieved by changing the relative distance between the nonlinear crystal and the DL, which acts in a focusing configuration. Besides the many practical applications of the so-generated pulses, the proposed method might be extended to other wavelength ranges by demonstrated similar effects on other nonlinear processes, such as high-order harmonic generation.