Traditionally, infrared molecular spectroscopy has been performed with frequency-domain measurement techniques. Recent experiments have exploited the outstanding temporal coherence of state-of-the-art femtosecond lasers to overcome long-standing sensitivity and dynamic range limitations of these traditional techniques, with time-domain measurements. Here, we show how state-of-the-art 2-µm femtosecond technology provides (i) Watt-level infrared sources covering the entire molecular fingerprint region, with a spectral brightness exceeding even that of synchrotrons, (ii) background-free, high-sensitivity and high-dynamic range time-domain detection of molecular vibrations via electro-optical sampling with (iii) attosecond temporal accuracy. These advances herald a new regime for time-, frequency- and space-resolved molecular vibrational metrology.
We study coherence properties of a more-than-octave-wide (2.6-7.5 μm) mid-IR frequency comb based on a 2-μm Tmfiber- laser-pumped degenerate (subharmonic) optical parametric oscillator (OPO) that uses orientation-patterned gallium arsenide (OP-GaAs) as gain element. By varying intracavity dispersion, we observed a 'phase' transition from a singlecomb state (at exactly OPO degeneracy) to a two-comb state (near-degenerate operation), characterized by two spectrally overlapping combs (signal and idler) with distinct carrier-envelope offset frequencies. We achieve this by generating a supercontinuum (SC) from the mode-locked Tm laser that spans most of the near-IR range, and observing RF beats between the SC and parasitic sum-frequency light (pump + OPO) that also falls into the near-IR. We found RF linewidth to be <15 Hz (a resolution of our spectrum analyzer), which proves that coherence of the pump laser comb is preserved to a high degree in a subharmonic OPO. Transition to a two-comb state was characterized by a symmetric splitting of the RF peak. Low pump threshold (down to 7 mW), high (73 mW) average power and high (up to 90%) pump depletion make this comb source very attractive for numerous applications including trace molecular detection and chemical sensing with massively parallel spectral data acquisition.
We review our work on a femtosecond erbium-doped all-fiber laser mode-locked with graphene oxide saturable absorber, which can be conveniently obtained from natural graphite by simple oxidation and ultra-sonication process. The laser directly generated 200 fs pulses at a repetition rate of 22.9 MHz. The stable passively Q-switched operation by graphene oxide saturable absorber in the 1 μm ytterbium-, 1.5 μm erbium-, and 2 μm thulium-doped fiber lasers will be demonstrated as well. These results are comparable with those of graphene saturable absorbers and the superiority of easy fabrication and hydrophilic property of graphene oxide will facilitate its potential applications for ultrafast photonics.