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Femtosecond laser sources and optical frequency combs in the molecular fingerprint region of the electromagnetic spectrum are crucial for a plethora of applications in natural and life sciences. Here we introduce Cr 2-based lasers as a convenient means for producing super-octave mid-IR electromagnetic transients via optical rectification (or intra-pulse difference frequency generation, IDFG). We demonstrate that a relatively long, 2.5 μm, central wavelength of a few-cycle Cr 2 :ZnS driving source (20 fs pulse duration, 6 W average power, 78 MHz repetition rate) enabled the use of highly nonlinear ZnGeP 2 crystal for IDFG with exceptionally high conversion efficiency (>3%) and output power of 0.15 W, with the spectral span of 5.8-12.5 μm. Even broader spectrum was achieved in GaSe crystal: 4.3-16.6 μm for type I and 5.8-17.6 μm for type II phase matching. The results highlight the potential of this architecture for ultrafast spectroscopy and generation of broadband frequency combs in the longwave infrared.

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Spectroscopic characterization of Fe:ZnSe(Cr:ZnSe) crystals under visible excitation into the charge transfer bands of Transition Metal ions were studied. The excitation efficiencies of mid-IR photoluminescence between (5)T(2)((5)E) and (5)E((5)T(2)) states via direct relaxation to the upper laser levels and via metastable upper (3)T(1) were investigated. It was demonstrated that the latter route is the dominant process for Cr(2+) ions and could provide sufficient pump rate for mid-IR lasing. The pump efficiencies via direct relaxation to the upper laser levels were estimated to be <2% for both ions under 532 nm excitation wavelength.