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We demonstrate high-sensitivity vibrational absorption spectroscopy in the 2-micron wavelength range by using a mode-locked Cr:ZnS laser. Interferometric subtraction and multichannel detection across the broad laser spectrum realize simultaneous background-free detection of multiple vibrational modes over a spectral span of >380 cm -1 . Importantly, we achieve detection of small absorbance on the order of 10 -4 , which is well below the detection limit of conventional absorption spectroscopy set by the detector dynamic range. The results indicate the promising potential of the background-free method for ultrasensitive and rapid detection of trace gases and chemicals.

We developed a diode-pumped, mode-locked polycrystalline Cr:ZnS oscillator using single-walled carbon nanotubes as a saturable absorber. The oscillator exhibits self-start mode-locking operation, generating sub-100 fs pulses with an average power of 300 mW. We found a unique feature in which the intensity noise originating from relaxation oscillation is suppressed by inherent second harmonic generation in polycrystalline Cr:ZnS. The observed noise suppression is reproduced by a theoretical model that includes an instantaneous nonlinear loss.

We study the saturable absorption properties of single-walled carbon nanotubes (SWCNTs) with a large diameter of 2.2 nm and the corresponding exciton resonance at a wavelength of 2.4 µm. At resonant excitation, a large modulation depth of approximately 30 % and a small saturation fluence of a few tens of µJ/cm 2 are evaluated. The temporal response is characterized by an instantaneous rise and a subpicosecond recovery. We also utilize the SWCNTs to realize sub-50 fs, self-start mode locking in a Cr:ZnS laser, revealing that the film thickness is an important parameter that affects the possible pulse energy and duration. The results prove that semiconductor SWCNTs with tailored diameters exceeding 2 nm are useful for passive mode locking in the mid-infrared range.