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.

Automated control and stabilization of ultrabroadband laser pulse angular dispersion.

We present an innovative automatic control of angular dispersion for high-power laser systems. A novel, to the best of our knowledge, diagnostic has been developed to visualize angular dispersion in ultrashort near-infrared laser pulses for on-shot analysis. The output of a commercial ultrabroadband oscillator was prepared with an arbitrary chromatic dispersion and sent through a compensation system composed of 4° glass wedges in motorized mounts. These wedges were rotationally controlled in discrete steps about the beam axis in accordance with the diagnostic, via an automated feedback loop, to successfully eliminate angular dispersion to a precision of 5 nrad/nm. The system can be implemented to maintain a zero or nonzero target dispersion for experiments.

Continuous ultraviolet to blue-green astrocomb.

Cosmological and exoplanetary science using transformative telescopes like the ELT will demand precise calibration of astrophysical spectrographs in the blue-green, where stellar absorption lines are most abundant. Astrocombs-lasers providing a broadband sequence of regularly-spaced optical frequencies on a multi-GHz grid-promise an atomically-traceable calibration scale, but their realization in the blue-green is challenging for current infrared-laser-based technology. Here, we introduce a concept achieving a broad, continuous spectrum by combining second-harmonic generation and sum-frequency-mixing in an MgO:PPLN waveguide to generate 390-520 nm light from a 1 GHz Ti:sapphire frequency comb. Using a Fabry-Pérot filter, we extract a 30 GHz sub-comb spanning 392-472 nm, visualizing its thousands of modes on a high-resolution spectrograph. Experimental data and simulations demonstrate how the approach can bridge the spectral gap present in second-harmonic-only conversion. Requiring only [Formula: see text]100 pJ pulses, our concept establishes a new route to broadband UV-visible generation at GHz repetition rates.

GPU-accelerated full-field modelling of highly dispersive ultrafast optical parametric oscillators.

We demonstrate GPU-accelerated modelling of ultrafast optical parametric oscillators (OPOs) via the χ(2) nonlinear envelope equation with 1265× improvement in execution time compared with a CPU-based approach. Incorporating an adaptive step-size algorithm and absorbing boundary conditions, our model is capable of simulating OPOs containing long (>10 mm) nonlinear crystals or significant intracavity dispersion with outputs generated in less than 1 minute, allowing the investigation of systems that were previously computationally prohibitive to explore. We implement real-world parameters such as optical coatings, material absorption, and non-ideal poling domains within quasi-phase matched nonlinear crystals, producing excellent agreement with the spectral tuning behaviour and average power from a previously reported prism-based OPO. Our digital twinning approach provides a low-cost iterative development platform for ultrafast OPOs.

Fiber-delivered heterodyne spectroscopy with a mid-infrared frequency comb.

By exploiting the excellent short-term phase stability between consecutive pulses from a free-running optical parametric oscillator frequency comb, we report the first example of hollow-core fiber-delivered heterodyne spectroscopy in the 3.1-3.8 µm wavelength range. The technique provides a means of spectroscopically interrogating a sample situated at the distal end of a fiber, with all electronics and light sources situated at the proximal end and with an inherent capability to suppress spectroscopically interfering features present in the free-space and in-fiber delivery path. Using a silica anti-resonant, hollow-core delivery fiber, we demonstrate high quality transmission and attenuated total reflectance spectroscopy of a plastic sample for fiber lengths of up to 40 m, significantly exceeding the few-meter lengths typically possible using solid-core fibers. The technique opens a route to implementing multi-species spectroscopic monitoring in remote and / or hostile industrial environments and medical applications.

Multi-target two-photon dual-comb LiDAR.

By substituting two-photon cross-correlation in a wide-bandgap photodiode for the coherent gating conventionally used in dual-comb ranging, two-photon dual-comb LiDAR exchanges data-intensive interferometric acquisition for a single time-stamp from which an absolute distance can be inferred. Here, we report the application of two-photon dual-comb LiDAR to obtain real-time ranging to three independent targets with only a single silicon-photodiode detector. We show precisions of 197-255 nm (2 seconds averaging time) for static targets, and real-time simultaneous ranging to three dynamic targets driven by independent sinusoidal, saw-tooth and square waveforms. Finally, we demonstrate multi-target ranging to three points on a rigid body to provide simultaneous pitch and yaw angular measurements with precisions of 27.1 arcsec (130 µrad) on a 25 mm baseline.

Misalignment-free, Kerr-lens-modelocked Yb:Y2O3 2.2-GHz oscillator, amplified by a semiconductor optical amplifier.

We present a fully bonded, misalignment-free, diode-pumped Yb:ceramic (Yb:Y2O3) oscillator producing 190-fs pulses at a repetition frequency of 2.185 GHz. Self-starting Kerr-lens-modelocked operation was obtained from both outputs of the ring cavity with an average combined output power of 14-30 mW for pump powers from 380-670 mW. The fully bonded design provided self-starting, turnkey operation, with a relative intensity noise of 0.025% from 1 Hz-1 MHz. Tuning of the pulse repetition rate over a 120 kHz range was demonstrated for a 2°C change in temperature. Chirped-pulse amplification in a semiconductor optical amplifier was shown to increase the pulse average power to 69 mW and the pulse energy (peak power) from 2.5 pJ (12 W) to 32 pJ (71 W).

Feed-forward stabilization of a single-frequency, diode-pumped Pr:YLF-Cr:LiCAF laser operating at 813.42†nm.

We introduce a simple and compact diode-pumped Pr:YLF-Cr:LiCAF laser, operating at 813.42 nm and providing a 130-mW, single-frequency output tunable over a 3-GHz range. The laser has a short-term intrinsic linewidth estimated to be 700 Hz (ß-separation method), while exhibiting a free-running wavelength stability of below 1 pm in one hour. Using a feed-forward technique we demonstrate the integration of the laser output into a fully stabilized, 1-GHz Ti:sapphire laser frequency comb, resulting in a heterodyne beat note between the laser and the comb with a bandwidth of 65 kHz. Combining feed-forward control with a low-bandwidth servo feedback loop permits stable long-term locking with an rms beat note variation of 15 kHz over 2 minutes. This performance makes the laser a potential candidate for the lattice laser in a 87Sr optical lattice clock.

Compressive hyperspectral imaging in the molecular fingerprint band.

Spectrally-resolved imaging provides a spectrum for each pixel of an image that, in the mid-infrared, can enable its chemical composition to be mapped by exploiting the correlation between spectroscopic features and specific molecular groups. The compatibility of Fourier-transform interferometry with full-field imaging makes it the spectroscopic method of choice, but Nyquist-limited fringe sampling restricts the increments of the interferometer arm length to no more than a few microns, making the acquisition time-consuming. Here, we demonstrate a compressive hyperspectral imaging strategy that combines non-uniform sampling and a smoothness-promoting prior to acquire data at 15% of the Nyquist rate, providing a significant acquisition-rate improvement over state-of-the-art techniques. By illuminating test objects with a sequence of suitably designed light spectra, we demonstrate compressive hyperspectral imaging across the 700-1400 cm-1 region in transmission mode. A post-processing analysis of the resulting hyperspectral images shows the potential of the method for efficient non-destructive classification of different materials on painted cultural heritage.

Three-element, self-starting Kerr-lens-modelocked 1-GHz Ti:sapphire oscillator pumped by a single laser diode.

We present a Kerr-lens-modelocked, three-element, diode-pumped Ti:sapphire laser producing 111-fs pulses at a repetition frequency of 1.02 GHz. Self-starting soliton-modelocked operation with an output power of 106 mW was obtained when the laser was pumped at 1.0 W with a single 527-nm laser diode. The output exhibits a relative intensity noise of 0.06% (1 Hz - 1 MHz) and locking of the repetition rate to an external reference is demonstrated with a phase error of 1.7 mrad (1 Hz-1 MHz). The simplicity of the laser makes it an attractive candidate as a module for integration into larger systems.

Hollow-core fiber delivery of broadband mid-infrared light for remote spectroscopy.

High-resolution multi-species spectroscopy is achieved by delivering broadband 3-4-µm mid-infrared light through a 4.5-meter-long silica-based hollow-core optical fiber. Absorptions from H37Cl, H35Cl, H2O and CH4 present in the gas within the fiber core are observed, and the corresponding gas concentrations are obtained to 5-ppb precision using a high-resolution Fourier-transform spectrometer and a full-spectrum multi-species fitting algorithm. We show that by fully fitting the narrow absorption features of these light molecules their contributions can be nulled, enabling further spectroscopy of C3H6O and C3H8O contained in a Herriott cell after the fiber. As a demonstration of the potential to extend fiber-delivered broadband mid-infrared spectroscopy to significant distances, we present a high-resolution characterization of the transmission of a 63-meter length of hollow-core fiber, fully fitting the input and output spectra to obtain the intra-fiber gas concentrations. We show that, despite the fiber not having been purged, useful spectroscopic windows are still preserved which have the potential to enable hydrocarbon spectroscopy at the distal end of fibers with lengths of tens or even hundreds of meters.

Towards a space-qualified Kerr-lens mode-locked laser.

We report a 1.5-GHz Kerr-lens mode-locked (KLM) Yb:Y2O3 ring laser constructed by directly bonding the cavity components onto an aluminum baseplate. Stable unidirectional operation with an output power ≥10mW was obtained for pump-diode currents of 300-500 mA, corresponding to a total electrical power consumption of 1.5 W. After repetition rate stabilization, a comparison with a conventionally constructed identical laser showed a 50% reduction in phase noise. In free-running operation the bonded laser showed superior passive repetition rate stability. The bonding process follows an already proven integration approach in space-borne instrumentation, mapping a development pathway for KLM lasers in aerospace applications.

Two-photon dual-comb LiDAR.

The interferometric signals produced in conventional dual-comb laser ranging require femtosecond lasers with long-term carrier-envelope offset frequency stability, and are limited to an upper sampling rate by radio-frequency aliasing considerations. By using cross-polarized dual combs and two-photon detection, we demonstrate carrier-phase-insensitive cross-correlations at sampling rates of up to 12× the conventional dual-comb aliasing limit, recording these in a digitizer-based acquisition system to implement ranging with sub-100 nm precision. We then extend this concept to show how the high data burden of conventional dual-comb acquisition can be eliminated by using a simple microcontroller as a ns-precision stopwatch to record the time intervals separating the two-photon cross-correlation pulses, providing real-time and continuous LiDAR-like distance metrology capable of sub-100 nm precision and dynamic acquisition for unlimited periods.

Development of a deep-ultraviolet pulse laser source operating at 234†nm for direct cooling of Al+ ion clocks.

We report on the development of a 250-MHz 234 nm deep-ultraviolet pulse source based on a flexible wavelength-conversion scheme. The scheme is based on a frequency-doubled optical parametric oscillator (FD-OPO) together with a cascaded frequency conversion process. We use a χ(2) nonlinear envelope equation to guide the design of an intra-cavity OPO crystal, demonstrating a flexible broadband tunable feature and providing as high as watt-level of a frequency-doubled signal output centered at 850 nm, which is served as an input wave for the cascaded frequency conversion process. As much as 3.0 mW of an average power at 234 nm is obtained, with an rms power stability of better than 1% over 20 minutes. This deep-ultraviolet pulse laser source can be used for many applications in quantum optics and for direct laser cooling of Al+ ion clocks.

Dither-free stabilization of a femtosecond doubly resonant OPO using parasitic sum-frequency mixing.

Stable operation of a doubly resonant femtosecond optical parametric oscillator (OPO) requires submicron matching of the OPO and pump laser cavity lengths, which is normally implemented using a dither-locking feedback scheme. Here we show that parasitic sum-frequency mixing between the pump and resonant pulses of a degenerate femtosecond OPO provides an error signal suitable for actuating the cavity length with the precision needed to maintain oscillation on a single fringe and at maximum output power. Unlike commonly used dither-locking approaches, the method introduces no modulation noise and requires no additional optical components, except for one narrowband filter. The scheme is demonstrated on a Ti:sapphire-pumped sub-40-fs PPKTP OPO, from which data are presented showing a tenfold reduction in relative intensity noise compared with dither locking.

Characterization of a carrier-envelope-offset-stabilized blue- and green-diode-pumped Ti:sapphire frequency comb.

Diode-pumping of Ti:sapphire provides a low-cost route to high-quality frequency-comb sources, exploiting the potential of direct diode modulation for wideband control of the carrier-envelope-offset frequency. We present here an fREP- and fCEO-locked, directly diode-pumped Ti:sapphire frequency comb, producing 66-fs pulses at 800 nm and employing f-to-2f interferometry and current modulation of a 462-nm blue laser diode to achieve a stabilization bandwidth extending to ∼70 kHz. Characterizations of the fREP and fCEO phase noise are compared to relative intensity noise spectra of the pump diodes to provide insights into how the diode design and performance transfer into the comb stability, suggesting a lower contribution to fREP and fCEO noise from the blue laser diode than from the green diode.

Open-path multi-species remote sensing with a broadband optical parametric oscillator.

Open-path remote sensing is critical for monitoring fugitive emissions from industrial sites, where a variety of volatile organic compounds may be released. At ranges of only a few tens of metres, spatially coherent broadband mid-infrared sources can access sufficiently large absorption cross-sections to quantify hydrocarbon gas fluctuations above ambient background levels at high signal:noise ratios. Here we report path-integrated simultaneous concentration measurements of water, methane and ethane implemented in the 3.1-3.5-µm range using 0.05-cm-1-resolution Fourier-transform spectroscopy with an ultrafast optical parametric oscillator and a simple, non-compliant target. Real-time concentration changes were observed at a range of 70 m by simulating a fugitive emission with a weak localized release of 2% methane in air. Spectral averaging yielded a methane detection sensitivity of 595 ppb·m, implying a system capability to resolve few-ppb concentrations of many volatile organic compounds at observation ranges of 50-100 m.

Autonomous multi-species environmental gas sensing using drone-based Fourier-transform infrared spectroscopy.

Unmanned aerial vehicles (UAVs)-or drones-present compelling new opportunities for airborne gas sensing in applications such as environmental monitoring, hazardous scene assessment, and facilities' inspection. Instrumenting a UAV for this purpose encounters trade-offs between sensor size, weight, power, and performance, which drives the adoption of lightweight electrochemical and photo-ionisation detectors. However, this occurs at the expense of speed, selectivity, sensitivity, accuracy, resolution, and traceability. Here, we report on the design and integration of a broadband Fourier-transform infrared spectrometer with an autonomous UAV, providing ro-vibrational spectroscopy throughout the molecular fingerprint region from 3 - 11 µm (3333 - 909 cm-1) and enabling rapid, quantitative aerial surveys of multiple species simultaneously with an estimated noise-limited performance of 18 ppm (propane). Bayesian interpolation of the acquired gas concentrations is shown to provide both localization of a point source with approximately one meter accuracy, and distribution mapping of a gas cloud, with accompanying uncertainty quantification.

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.