Spectroscopy of fundamental vibrational transitions offers a label-free alternative for
high-chemical contrast measurements. These transitions can be interrogated either
directly by using mid-infrared light or indirectly through Raman scattering. This thesis
aims to advance dual-comb spectroscopy to improve the acquisition speed, resolution
and spectral coverage of vibrational spectroscopy. Dual-comb spectroscopy is a time
domain technique, which combines optical frequency combs -coherent light sources
with a spectrum constituted of discrete evenly spaced lines - and Fourier transform
spectroscopy.
For linear spectroscopy, a mid-infrared optical parametric oscillator was developed and
characterized. Its idler-pulse duration can be as short as a few cycles (~3 to 6 cycles),
with a central wavelength tunable from 2180nm to 3732nm (2679cm-1 - 4587cm-1),
allowing more than 2500nm (2861 cm-1) of total coverage while maintaining an average
power of tens of milliwatts. The high peak power of this system was exploited
for spectral broadening; generation of phase-coherent supercontinua was achieved in
waveguides, made from either silicon or chalcogenide glass, producing octave spanning
spectra ~1500nm to 3300nm (3030cm-1 - 6666cm-1) for silicon and from ~1600nm
beyond 3860nm (2590 cm-1 - 6250 cm-1) for chalcogenide glass). Two optical parametric
oscillator were constructed, advancing toward a dual-comb mid-infrared spectrometer.
Since the optical parametric oscillators are not stabilized, an additional correction scheme
was set up and characterized.
Coherent Raman scattering was also investigated, as a means to access optically active
and inactive fundamental vibrational transitions. Several spectroscopy setups were
developed to measure the Raman blue or red shifted light in forward and backward
scattered direction as well as a differential detection between blue and red shifted light.
There is a dead time between consecutive interferograms existent, up to a factor of 1000
larger than the measurement time. This dead time could be reduced by an order of
magnitude using a laser with ~1GHz and a laser with 100MHz repetition rate instead
of two lasers with ~100MHz repetition rate. All implementations achieved excellent
acquisition times (in the microsecond range), signal-to-noise ratios up to 1000 and
spectral coverage of about ~1200 cm-1). These advantages enabled measuring spectrally
resolved images, in a first rudimentary microscopy-setup.