We demonstrate an optical parametric oscillator (OPO) based on random phase matching in a polycrystalline χ(2) material, ZnSe. The subharmonic OPO utilized a 1.5-mm-long polished ZnSe ceramic sample placed at the Brewster's angle and was synchronously pumped by a Kerr-lens mode-locked Cr:ZnS laser with a central wavelength of 2.35 μm, a pulse duration of 62 fs, and a repetition frequency of 79 MHz. The OPO had a 90-mW pump threshold, and produced an ultrabroadband spectrum spanning 3-7.5 μm. The observed pump depletion was as high as 79%. The key to success in achieving the OPO action was choosing the average grain size of the ZnSe ceramic to be close to the coherence length (~ 100 μm) for our 3-wave interaction. This is the first OPO that uses random polycrystalline material with quadratic nonlinearity and the first OPO based on ZnSe. Very likely, random phase matching in ZnSe and similar random polycrystalline materials (ZnS, CdS, CdSe, GaP) represents a viable route for generating few-cycle pulses and multi-octave frequency combs, thanks to a very broadband nonlinear response.
Degenerate (subharmonic) optical parametric oscillators (OPO) show great promise for the generation of broadband mid-infrared (MIR) frequency combs. Their main features are low pump threshold, dramatic extension of the spectrum of the pump laser, and phase locking to the pump frequency comb. Here we report on obtaining instantaneous spectrum ranging from 2.85 to 8.40 μm at -40 dB level from a subharmonic OPO pumped by an ultrafast Cr2+:ZnS laser. Our experimental setup includes a free running Kerr lens mode locked 2.35 μm Cr2+:ZnS laser, with 62-fs time-bandwidth limited pulse duration, 630-mW average power, and 79 MHz repetition rate that synchronously pumps a ring-cavity orientation-patterned (OP-GaAs) based OPO. A 0.5-mm-long OP-GaAs crystal has a quasi-phase-matching (QPM) period of 88 μm and is designed to provide a broadband parametric gain at OPO degeneracy. A 0.3-mm-thick ZnSe wedge inside the cavity was used to minimize group velocity dispersion. Spectral span of 1.56 octaves in the MIR that we achieved can be further improved by fabricating an in-coupling dielectric mirror with (i) broader reflectivity range and (ii) with compensation of the residual group velocity dispersion. The broad spectrum achieved, 2.85 - 8.40 μm (2320 cm-1 wide instantaneous span), overlaps with a plethora of fundamental molecular IR resonances and can be used for frequency comb spectroscopic detection applied to such fields as remote sensing, study of fast combustion dynamics and medical diagnostics, to name a few.
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