Mid-infrared optical coherence tomography with a stabilized OP-GaP optical parametric oscillator.

We demonstrate mid-infrared time-domain optical coherence tomography (OCT) with an orientation-patterned GaP optical parametric oscillator. Instantaneous broadband mid-infrared spectra provide reduced scattering for OCT applications including cultural heritage, quality assurance, and security. B-scan calibrations performed across the wavelength tuning range show depth resolutions of 67 µm at 5.1 µm and 88 µm at 10.5 µm. Volumetric imaging inside a plastic bank card is demonstrated at 5.1 µm, with a 1 Hz A-scan rate that indicates the potential of stable broadband OPO sources to contribute to mid-infrared OCT.

Advanced Solid-State Lasers: feature issue introduction.

This Joint Issue of Optics Express and Optical Materials Express features 40 peer-reviewed articles written by authors who participated in the Advanced Solid State Lasers Conference, part of the Optica Laser Congress and Exhibition held in Barcelona, Spain from December 11-15, 2022. This review provides a brief summary of these articles covering the latest developments in laser host and nonlinear crystals, structured materials, fiber lasers and amplifiers, ultrafast mode-locked lasers and optical parametric amplifiers, frequency-doubled Raman lasers, vortex beams, and novel concepts in laser design.

Sub-Hz relative linewidths from an interferometrically stabilized mid-infrared frequency comb.

Frequency combs present a unique tool for high-precision and rapid molecular spectroscopy. Difference frequency generation (DFG) of near-infrared sources is a common approach to generate passively stabilized mid-infrared combs. However, only little attention has been paid so far to precisely measure the coherence properties of such sources. Here, we investigate these using a Raman-soliton based DFG source driven by an Yb:fiber frequency comb. A heterodyne beat between the second harmonic of the phase-locked DFG comb near 4 µm and a 2 µm Tm:fiber frequency comb locked to the same optical reference is performed. Using this method, we measure the relative phase noise power spectral density of both combs. This results in a sub-Hz relative linewidth between the DFG comb and the Tm:fiber comb. We also introduce a new pump/seed delay locking mechanism based on interferometry for long-term stable intensity noise suppression.

Feature issue introduction: advanced solid-state lasers.

This joint issue of Optics Express and Optical Materials Express features 36 state-of-the art articles written by authors who participated in the international conference advanced solid state lasers held online from October 3-7, 2021. This review provides a summary of these articles covering a wide spectrum of topics around solid-state lasers from materials research to sources and from design innovation to applications.

Simple approach to broadband mid-infrared pulse generation with a mode-locked Yb-doped fiber laser.

Broadband mid-infrared (MIR) molecular spectroscopy demands a bright and broadband light source in the molecular fingerprint region. To this end, intra-pulse difference frequency generation (IDFG) has shown excellent properties among various techniques. Although IDFG systems pumped with 1.5- or 2-µm ultrashort pulsed lasers have been extensively developed, few systems have been demonstrated with 1-µm lasers, which use bulky 100-W-class high-power Yb thin-disk lasers. In this work, we demonstrate a simple and robust approach of 1-µm-pumped broadband IDFG with a conventional mode-locked Yb-doped fiber laser. We first generate 3.3-W, 12.1-fs ultrashort pulses at 50 MHz by a simple combination of spectral broadening with a short single-mode fiber and pulse compression with chirped mirrors. Then, we use them for pumping a thin orientation-patterned gallium phosphide crystal, generating 1.2-mW broadband MIR pulses with the -20-dB bandwidth of 480 cm-1 in the fingerprint region (760-1240 cm-1, 8.1-13.1 µm). The 1-µm-based IDFG system allows for additional generations of ultrashort pulses in the ultraviolet and visible regions, enabling, for example, 50-MHz-level high-repetition-rate vibrational sum-frequency generation spectroscopy or pump-probe spectroscopy.

Efficient second harmonic generation of a high-power picosecond CO2 laser.

A comparative analysis of AgGaSe2, GaSe, CdGeAs2, and Te for second harmonic generation (SHG) of a picosecond CO2 laser at intensities up to 50 GW/cm2 is presented. We demonstrate external energy conversion efficiency of >20% in AgGaSe2. Conversion efficiency >5% is measured in GaSe and CdGeAs2. Self-focusing and multifilamentation are found to severely limit the SHG process in CdGeAs2 and Te at such high fields. Demonstration of ≥150 MW SH pulses for a 10 µm picosecond pump, in combination with femtosecond CO2 laser development, will open new strong-field applications in the 4.5-5.5 µm range.

Mid-infrared frequency combs at 10 GHz.

We demonstrate mid-infrared (MIR) frequency combs at 10 GHz repetition rate via intra-pulse difference-frequency generation (DFG) in quasi-phase-matched nonlinear media. Few-cycle pump pulses (≲15fs, 100 pJ) from a near-infrared electro-optic frequency comb are provided via nonlinear soliton-like compression in photonic-chip silicon-nitride waveguides. Subsequent intra-pulse DFG in periodically poled lithium niobate waveguides yields MIR frequency combs in the 3.1-4.8 µm region, while orientation-patterned gallium phosphide provides coverage across 7-11 µm. Cascaded second-order nonlinearities simultaneously provide access to the carrier-envelope-offset frequency of the pump source via in-line f-2f nonlinear interferometry. The high-repetition rate MIR frequency combs introduced here can be used for condensed phase spectroscopy and applications such as laser heterodyne radiometry.

Infrared electric field sampled frequency comb spectroscopy.

Probing matter with light in the mid-infrared provides unique insight into molecular composition, structure, and function with high sensitivity. However, laser spectroscopy in this spectral region lacks the broadband or tunable light sources and efficient detectors available in the visible or near-infrared. We overcome these challenges with an approach that unites a compact source of phase-stable, single-cycle, mid-infrared pulses with room temperature electric field-resolved detection at video rates. The ultrashort pulses correspond to laser frequency combs that span 3 to 27 µm (370 to 3333 cm-1), and are measured with dynamic range of >106 and spectral resolution as high as 0.003 cm-1. We highlight the brightness and coherence of our apparatus with gas-, liquid-, and solid-phase spectroscopy that extends over spectral bandwidths comparable to thermal or infrared synchrotron sources. This unique combination enables powerful avenues for rapid detection of biological, chemical, and physical properties of matter with molecular specificity.

Terahertz generation by optical rectification in chalcopyrite crystals ZnGeP2, CdGeP2 and CdSiP2.

Optical rectification of near-infrared laser pulses generates broadband terahertz radiation in chalcopyrite crystals CdGeP2, ZnGeP2 and CdSiP2. The emission is characterized using linear-polarized excitation from 0.8 eV to 1.55 eV (1550 nm - 800 nm). All three crystals are (110)-cut and polished to 0.5 mm, thinner than the coherence length across most of the excitation photon energy range, such that they all produce a bandwidth ~2.5 THz when excited with ~100 fs pulses. It is found that CdGeP2 produced the strongest emission at telecoms wavelengths, while CdSiP2 is generally the strongest source. Pump-intensity dependence provides the nonlinear coefficients for each crystal.

White powder identification using broadband coherent light in the molecular fingerprint region.

We show that a variety of white powder samples, including painkillers, amino acids, stimulants and sugars are readily discriminated by diffuse reflectance infrared spectroscopy involving no preparation of the sample and no physical contact with it. Eleven powders were investigated by illuminating each sample with broadband coherent light in the 8-9-µm band from an OPGaP femtosecond optical parametric oscillator. The spectra of the scattered light were obtained using Fourier-transform spectroscopy. Similarities between different spectra were quantified using Pearson's correlation coefficient, confirming that spectral features in the 8-9-µm wavelength region were sufficient to discriminate between all eleven powders evaluated in the study, offering a route to simple and automated non-contact chemical detection.

Systematic spectral shifts in the mid-infrared spectroscopy of aerosols.

Infrared spectroscopy in the spectral fingerprint region from 6.5 to 20 µm has been applied for decades to identify vapor- and condensed-phase chemicals with high confidence. By employing a unique broadband laser operating from 7.2- to 11.5-µm we show that, in this region, wavelength-dependent Mie-scattering effects substantially modulate the underlying chemical absorption signature, undermining the ability of conventional infrared absorption spectroscopy to identify aerosolized liquids and solids. In the aerosol studied, Mie theory predicts that the positions of spectroscopic features will blue-shift by up to 200 nm, and this behavior is confirmed by experiment, illustrating the critical importance of considering Mie contributions to aerosol spectroscopy in the mid infrared. By examining the spectroscopy of light scattered from an aerosol of the chemical diethyl phthalate, we demonstrate excellent agreement with a Mie-scattering model informed by direct measurements of the particle-size-distribution and complex refractive index.

Multi-watt, multi-octave, mid-infrared femtosecond source.

Spectroscopy in the wavelength range from 2 to 11 µm (900 to 5000 cm-1) implies a multitude of applications in fundamental physics, chemistry, as well as environmental and life sciences. The related vibrational transitions, which all infrared-active small molecules, the most common functional groups, as well as biomolecules like proteins, lipids, nucleic acids, and carbohydrates exhibit, reveal information about molecular structure and composition. However, light sources and detectors in the mid-infrared have been inferior to those in the visible or near-infrared, in terms of power, bandwidth, and sensitivity, severely limiting the performance of infrared experimental techniques. This article demonstrates the generation of femtosecond radiation with up to 5 W at 4.1 µm and 1.3 W at 8.5 µm, corresponding to an order-of-magnitude average power increase for ultrafast light sources operating at wavelengths longer than 5 µm. The presented concept is based on power-scalable near-infrared lasers emitting at a wavelength near 1 µm, which pump optical parametric amplifiers. In addition, both wavelength tunability and supercontinuum generation are reported, resulting in spectral coverage from 1.6 to 10.2 µm with power densities exceeding state-of-the-art synchrotron sources over the entire range. The flexible frequency conversion scheme is highly attractive for both up-conversion and frequency comb spectroscopy, as well as for a variety of time-domain applications.

Efficient half-harmonic generation of three-optical-cycle mid-IR frequency comb around 4 µm using OP-GaP.

We report a broadband mid-infrared frequency comb with three-optical-cycle pulse duration centered around 4.2 µm, via half-harmonic generation using orientation-patterned GaP (OP-GaP) with ~43% conversion efficiency. We experimentally compare performance of GaP with GaAs and lithium niobate as the nonlinear element, and show how properties of GaP at this wavelength lead to generation of the shortest pulses and the highest conversion efficiency. These results shed new light on half-harmonic generation of frequency combs, and pave the way for generation of short-pulse intrinsically-locked frequency combs at longer wavelengths in the mid-infrared with high conversion efficiencies.

Continuous-wave whispering-gallery optical parametric oscillator based on CdSiP2.

Continuous-wave (cw) optical parametric oscillators (OPOs) are ideally suited for applications, for example high-resolution spectroscopy, that need coherent sources combining narrow-linewidth emission with good wavelength tunability. Here, we demonstrate for the first time cw OPOs based on a millimeter-sized whispering gallery resonator (WGR) made of cadmium silicon phosphide (CdSiP2). By employing a compact laser diode at 1.57-µm wavelength for pumping, a cw OPO with wavelength tunability from 2.3 µm to 5.1 µm is realized based on such a resonator. The oscillation thresholds are in the milliwatt range. The maximum total power conversion efficiency reaches more than 15%. The intrinsic quality factor at 1.57 µm is determined to be 3.5 × 106. This work suggests that CdSiP2 is a very promising alternative for constructing mid-infrared parametric devices.

All-fiber mid-infrared source tunable from 6 to 9 µm based on difference frequency generation in OP-GaP crystal.

We report the first fully fiberized difference frequency generation (DFG) source, delivering a broadly tunable idler in the 6 to 9 µm spectral range, using an orientation-patterned gallium phosphide (OP-GaP) crystals with different quasi-phase matching periods (QPM). The mid-infrared radiation (MIR) is obtained via mixing of the output of a graphene-based Er-doped fiber laser at 1.55 µm with coherent frequency-shifted solitons at 1.9 µm generated in a highly nonlinear fiber using the same seed. The presented setup is the first truly all-fiber, all-polarization maintaining, alignment-free DFG source reported so far. Its application to laser spectroscopy was demonstrated by the absorption spectrum measurement of ν4 band of methane in 7.5 - 8.3 µm spectral range. The system simplicity and compactness paves the way for applications in field-deployable optical frequency comb spectroscopy systems for gas sensing.

Compact and efficient mid-IR OPO source pumped by a passively Q-switched Tm:YAP laser.

We describe a compact and efficient mid-infrared (mid-IR) source based on zinc germanium phosphide (ZGP) and cadmium silicon phosphide (CSP) optical parametric oscillators (OPOs), operating in near degenerate condition, directly pumped by a 1.94 µm thulium (Tm)-doped yttrium-aluminum-perovskite (YAP) laser. The Tm:YAP laser is passively Q-switched by a chromium-doped zinc sulfide saturable absorber, and is operated to 4 W average power with a peak power of 29 kW. The laser emission was used to pump CSP and ZGP doubly resonant linear OPO cavities, generating a maximum 3.5-4.2 µm mid-IR emission of 2.5 W for CSP and 2.3 W for ZGP, with maximum optical conversion efficiencies of 65% and 58%, respectively, achieved for the two OPO crystals.

Self-referenced octave-wide subharmonic GaP optical parametric oscillator centered at 3 µm and pumped by an Er-fiber laser: erratum.

This erratum reports a correction to the labeling of Figs. 2(b) and 3(b) in the original manuscript, Opt. Lett.42, 4756 (2017)OPLEDP0146-959210.1364/OL.42.004756.

Self-referenced octave-wide subharmonic GaP optical parametric oscillator centered at 3 µm and pumped by an Er-fiber laser.

We report an octave-wide mid-IR spectrum (2.3-4.8 µm) obtained from a subharmonic optical parametric oscillator (OPO) based on a newly developed nonlinear crystal, orientation-patterned gallium phosphide (OP-GaP), which was synchronously pumped by a femtosecond 1560 nm fiber laser. We proved that the octave-wide output is in the form of a single frequency comb. The observed f-to-2f frequency beats, originating directly from the OPO, can be used for self-referencing and phase locking of the pump laser comb with no need for supercontinuum generation. With an average output power of ∼30 mW, this setup might be beneficial for a variety of spectroscopic applications in the mid-IR.

Midinfrared frequency comb by difference frequency of erbium and thulium fiber lasers in orientation-patterned gallium phosphide.

We generate over 60 mW of pulses with wavelengths from 6 to 11 micrometers by difference frequency mixing between erbium and thulium fiber amplifiers in orientation-patterned GaP with a photon conversion efficiency of 0.2. By stabilizing the repetition rate of the shared oscillator and adding a frequency shifter to one arm, the output becomes a frequency comb with tunable carrier envelope offset.

Nanosecond difference-frequency generation in orientation-patterned gallium phosphide.

We report a tunable, single-pass, pulsed nanosecond difference-frequency generation (DFG) source based on the new semiconductor nonlinear material, orientation-patterned gallium phosphide (OP-GaP). The DFG source is realized by mixing the output signal of a nanosecond OPO tunable over 1723-1827 nm with the input pump pulses of the same OPO at 1064 nm in an OP-GaP crystal, resulting in tunable generation over 233 nm in the mid-infrared from 2548 to 2781 nm. Using a 40-mm-long crystal, we have produced ∼14 mW of average DFG output power at 2719 nm for a pump power of 5 W and signal power of 1 W at 80 kHz repetition rate. To the best of our knowledge, this is the first single-pass nanosecond DFG source based on OP-GaP. The DFG output beam has a TEM00 spatial mode profile and exhibits passive power stability better than 1.7% rms over 1.4 h at 2774 nm, compared to 1.6% and 0.1% rms for the signal and pump, respectively. The OP-GaP crystal is recorded to have a temperature acceptance bandwidth of 17.7°C.