Validation of open-path dual-comb spectroscopy against an O2 background: erratum.

This erratum corrects errors that appear in Opt. Express31, 5042 (2023).10.1364/OE.480301.

Pulse interaction induced systematic errors in dual comb spectroscopy.

Systematic errors are observed in dual comb spectroscopy when pulses from the two sources travel in a common fiber before interrogating the sample of interest. When sounding a molecular gas, these errors distort both the line shapes and retrieved concentrations. Simulations of dual comb interferograms based on a generalized nonlinear Schrodinger equation highlight two processes for these systematic errors. Self-phase modulation changes the spectral content of the field interrogating the molecular response but affects the recorded spectral baseline and absorption features differently, leading to line intensity errors. Cross-phase modulation modifies the relative inter-pulse delay, thus introducing interferogram sampling errors and creating a characteristic asymmetric distortion on spectral lines. Simulations capture the shape and amplitude of experimental errors which are around 0.1% on spectral transmittance residuals for 10 mW of total average power in 10 meters of common fiber, scaling up to above 0.6% for 20 mW and 60 m.

Validation of open-path dual-comb spectroscopy against an O2 background.

Dual-comb spectroscopy measures greenhouse gas concentrations over kilometers of open air with high precision. However, the accuracy of these outdoor spectra is challenging to disentangle from the absorption model and the fluctuating, heterogenous concentrations over these paths. Relative to greenhouse gases, O2 concentrations are well-known and evenly mixed throughout the atmosphere. Assuming a constant O2 background, we can use O2 concentration measurements to evaluate the consistency of open-path dual-comb spectroscopy with laboratory-derived absorption models. To this end, we construct a dual-comb spectrometer spanning 1240 nm to 1700nm, which measures O2 absorption features in addition to CO2 and CH4. O2 concentration measurements across a 560 m round-trip outdoor path reach 0.1% precision in 10 minutes. Over seven days of shifting meteorology and spectrometer conditions, the measured O2 has -0.07% mean bias, and 90% of the measurements are within 0.4% of the expected hemisphere-average concentration. The excursions of up to 0.4% seem to track outdoor temperature and humidity, suggesting that accuracy may be limited by the O2 absorption model or by water interference. This simultaneous O2, CO2, and CH4 spectrometer will be useful for measuring accurate CO2 mole fractions over vertical or many-kilometer open-air paths, where the air density varies.

Removing biases in dual frequency comb spectroscopy due to digitizer nonlinearity.

Operation of any dual-comb spectrometer requires digitization of the interference signal before further processing. Nonlinearities in the analog-to-digital conversion can alter the apparent gas concentration by multiple percent, limiting both precision and accuracy of this technique. This work describes both the measurement of digitizer nonlinearity and the development of a model that quantitatively describes observed concentration bias over a range of conditions. We present hardware methods to suppress digitizer-induced bias of concentration retrievals below 0.1%.

Collinear opto-optical loss modulation for carrier-envelope offset stabilization of a fiber frequency comb.

Opto-optical loss modulation (OOM) for stabilization of the carrier-envelope offset (CEO) frequency of a femtosecond all-fiber laser is performed using a collinear geometry. Amplitude-modulated 1064 nm light is fiber coupled into an end-pumped semiconductor saturable absorber mirror (SESAM)-mode-locked all-polarization-maintaining erbium fiber femtosecond laser, where it optically modulates the loss of the SESAM resulting in modulation of the CEO frequency. A noise rejection bandwidth of 150 kHz is achieved when OOM and optical gain modulation are combined in a hybrid analog/digital loop. Collinear OOM provides a simple, all-fiber, high-bandwidth method for improving the CEO frequency stability of SESAM mode-locked fiber lasers.

Monitoring methane emissions from oil and gas operations‡.

The atmospheric concentration of methane has more than doubled since the start of the Industrial Revolution. Methane is the second-most-abundant greenhouse gas created by human activities and a major driver of climate change. This APS-Optica report provides a technical assessment of the current state of monitoring U.S. methane emissions from oil and gas operations, which accounts for roughly 30% of U.S. anthropogenic methane emissions. The report identifies current technological and policy gaps and makes recommendations for the federal government in three key areas: methane emissions detection, reliable and systematized data and models to support mitigation measures, and effective regulation.

Compact mid-infrared dual-comb spectrometer for outdoor spectroscopy.

This manuscript describes the design of a robust, mid-infrared dual-comb spectrometer operating in the 3.1-µm to 4-µm spectral window for future field applications. The design represents an improvement in system size, power consumption, and robustness relative to previous work while also providing a high spectral signal-to-noise ratio. We demonstrate a system quality factor of 2×106 and 30 hours of continuous operation over a 120-meter outdoor air path.

Obtaining more energetic modelocked pulses from a SESAM-based fiber laser.

A major design goal for femtosecond fiber lasers is to increase the output power but not at the cost of increasing the noise level or narrowing the bandwidth. Here, we perform a computational study to optimize the cavity design of a femtosecond fiber laser that is passively modelocked with a semiconductor saturable absorbing mirror (SESAM). We use dynamical methods that are more than a thousand times faster than standard evolutionary methods. We show that we can obtain higher pulse energies and hence higher output powers by simultaneously increasing the output coupling ratio, the gain, and the anomalous group delay dispersion. We can obtain output pulses that are from 5 to 15 times the energy of the pulse in the current experimental design with no penalty in the noise level or bandwidth.

Dual-comb spectroscopy with tailored spectral broadening in Si3N4 nanophotonics.

Si3N4 waveguides, pumped at 1550 nm, can provide spectrally smooth, broadband light for gas spectroscopy in the important 2 µm to 2.5 µm atmospheric water window, which is only partially accessible with silica-fiber based systems. By combining Er+ fiber frequency combs and supercontinuum generation in tailored Si3N4 waveguides, high signal-to-noise dual-comb spectroscopy spanning 2 µm to 2.5 µm is demonstrated. Acquired broadband dual-comb spectra of CO and CO2 agree well with database line shape models and have a spectral-signal-to-noise as high as 48/√s, showing that the high coherence between the two combs is retained in the Si3N4 supercontinuum generation. The dual-comb spectroscopy figure of merit is 6 × 106/√s, equivalent to that of all-fiber dual-comb spectroscopy systems in the 1.6 µm band. based on these results, future dual-comb spectroscopy can combine fiber comb technology with Si3N4 waveguides to access new spectral windows in a robust non-laboratory platform.

Single-Blind Quantification of Natural Gas Leaks from 1 km Distance Using Frequency Combs.

A new method is tested in a single-blind study for detection, attribution, and quantification of methane emissions from the natural gas supply chain, which contribute substantially to annual U.S. emissions. The monitoring approach couples atmospheric methane concentration measurements from an open-path dual frequency comb laser spectrometer with meteorological data in an inversion to characterize emissions. During single-blind testing, the spectrometer is placed >1 km from decommissioned natural gas equipment configured with intentional leaks of controllable rate. Single, steady emissions ranging from 0 to 10.7 g min-1 (0-34.7 scfh) are detected, located, and quantified at three gas pads of varying size and complexity. The system detects 100% of leaks, including leaks as small as 0.96 g min-1 (3.1 scfh). It attributes leaks to the correct pad or equipment group (tank battery, separator battery, wellhead battery) 100% of the time and to the correct equipment (specific separator, tank, or wellhead) 67% of the time. All leaks are quantified to within 3.7 g min-1 (12 scfh); 94% are quantified to within 2.8 g min-1 (9 scfh). These tests are an important initial demonstration of the methodology's viability for continuous monitoring of large regions, with extension to other trace gases and industries.

Speed-dependent Voigt lineshape parameter database from dual frequency comb measurements at temperatures up to 1305 K. Part II: Argon-broadened H2O absorption, 6801-7188 cm-1.

We report argon-broadened water vapor transition parameters and their temperature dependence based on measured spectra spanning 6801-7188 cm-1 from a broad-bandwidth, high-resolution dual frequency comb spectrometer. The 25 collected spectra of 2% water vapor in argon ranged from 296 K to 1305 K with total pressure spanning 100 Torr to 600 Torr. A multispectrum fitting routine was used in conjunction with a quadratic speed-dependent Voigt profile to extract broadening and shift parameters, and a power-law temperature-dependence exponent for both. The measurements represent the first broad bandwidth, argon-broadened water vapor absorption study, and are an important step toward a foreign-gas-perturbed, high-temperature database developed using advanced lineshape profiles.

Speed-dependent Voigt lineshape parameter database from dual frequency comb measurements up to 1305 K. Part I: Pure H2O absorption, 6801-7188 cm-1.

We measure speed-dependent Voigt lineshape parameters with temperature-dependence exponents for several hundred spectroscopic features of pure water spanning 6801-7188 cm-1. The parameters are extracted from broad bandwidth, high-resolution dual frequency comb absorption spectra with multispectrum fitting techniques. The data encompass 25 spectra ranging from 296 K to 1305 K and 1 to 17 Torr of pure water vapor. We present the extracted parameters, compare them to published data, and present speed-dependence, self-shift, and self-broadening temperature-dependent parameters for the first time. Lineshape data is extracted using a quadratic speed-dependent Voigt profile and a single self-broadening power law temperature-dependence exponent over the entire temperature range. The results represent an important step toward a new high-temperature database using advanced lineshape profiles.

Wake mode sidebands and instability in mode-locked lasers with slow saturable absorbers.

Passively mode-locked lasers with semiconductor saturable absorption mirrors are attractive comb sources due to their simplicity, excellent self-starting properties, and their environmental robustness. These lasers, however, can have an increased noise level and wake mode instabilities. Here, we investigate the wake mode dynamics in detail using a combination of evolutionary and dynamical methods. We describe the mode-locked pulse generation from noise when a stable pulse exists and the evolution of the wake mode instability when no stable pulse exists. We then calculate the dynamical spectrum of the mode-locked pulse, and we show that it has six discrete eigenmodes, two of which correspond to wake modes. The wake modes are unstable when the wake mode eigenvalues have a positive real part. We also show that even when the laser is stable, the wake modes lead to experimentally observed sidebands.

Self-referenced frequency combs using high-efficiency silicon-nitride waveguides.

We utilize silicon-nitride waveguides to self-reference a telecom-wavelength fiber frequency comb through supercontinuum generation, using 11.3 mW of optical power incident on the chip. This is approximately 10 times lower than conventional approaches using nonlinear fibers and is enabled by low-loss (<2 dB) input coupling and the high nonlinearity of silicon nitride, which can provide two octaves of spectral broadening with incident energies of only 110 pJ. Following supercontinuum generation, self-referencing is accomplished by mixing 780-nm dispersive-wave light with the frequency-doubled output of the fiber laser. In addition, at higher optical powers, we demonstrate f-to-3f self-referencing directly from the waveguide output by the interference of simultaneous supercontinuum and third harmonic generation, without the use of an external doubling crystal or interferometer. These hybrid comb systems combine the performance of fiber-laser frequency combs with the high nonlinearity and compactness of photonic waveguides, and should lead to low-cost, fully stabilized frequency combs for portable and space-borne applications.

Accurate frequency referencing for fieldable dual-comb spectroscopy.

We describe a dual-comb spectrometer that can operate independently of laboratory-based rf and optical frequency references but is nevertheless capable of ultra-high spectral resolution, high SNR, and frequency-accurate spectral measurements. The instrument is based on a "bootstrapped" frequency referencing scheme in which short-term optical phase coherence between combs is attained by referencing each to a free-running diode laser, whilst high frequency resolution and long-term accuracy is derived from a stable quartz oscillator. The sensitivity, stability and accuracy of this spectrometer were characterized using a multipass cell. We demonstrate comb-resolved spectra spanning from 140 THz (2.14 µm, 4670 cm-1) to 184 THz (1.63 µm, 6140 cm-1) in the near infrared with a frequency sampling of 200 MHz (0.0067 cm-1) and ~1 MHz frequency accuracy. High resolution spectra of water and carbon dioxide transitions at 1.77 µm, 1.96 µm and 2.06 µm show that the molecular transmission acquired with this system operating in the field-mode did not deviate from those measured when it was referenced to a maser and cavity-stabilized laser to within 5.6 × 10-4. When optimized for carbon dioxide quantification at 1.60 µm, a sensitivity of 2.8 ppm-km at 1 s integration time, improving to 0.10 ppm-km at 13 minutes of integration time was achieved.

Mid-infrared optical frequency combs based on difference frequency generation for molecular spectroscopy.

Mid-infrared femtosecond optical frequency combs were produced by difference frequency generation of the spectral components of a near-infrared comb in a 3-mm-long MgO:PPLN crystal. We observe strong pump depletion and 9.3 dB parametric gain in the 1.5 µm signal, which yields powers above 500 mW (3 µW/mode) in the idler with spectra covering 2.8 µm to 3.5 µm. Potential for broadband, high-resolution molecular spectroscopy is demonstrated by absorption spectra and interferograms obtained by heterodyning two combs.

Broadband Phase Spectroscopy over Turbulent Air Paths.

Broadband atmospheric phase spectra are acquired with a phase-sensitive dual-frequency-comb spectrometer by implementing adaptive compensation for the strong decoherence from atmospheric turbulence. The compensation is possible due to the pistonlike behavior of turbulence across a single spatial-mode path combined with the intrinsic frequency stability and high sampling speed associated with dual-comb spectroscopy. The atmospheric phase spectrum is measured across 2 km of air at each of the 70,000 comb teeth spanning 233 cm(-1) across hundreds of near-infrared rovibrational resonances of CO(2), CH(4), and H(2)O with submilliradian uncertainty, corresponding to a 10(-13) refractive index sensitivity. Trace gas concentrations extracted directly from the phase spectrum reach 0.7 ppm uncertainty, demonstrated here for CO(2). While conventional broadband spectroscopy only measures intensity absorption, this approach enables measurement of the full complex susceptibility even in practical open path sensing.

Time-domain stabilization of carrier-envelope phase in femtosecond light pulses.

We report a time-domain method of stabilizing the carrier-envelope phase (CEP) of femtosecond pulses. Temporal variations of the pulse envelope and the carrier electric-field phase were separately detected with the aid of intensity cross-correlation and interferometric cross-correlation. These detected signals were used to stabilize the CEP; the resulting 50-fold improvement in the fractional stability of the carrier-envelop-offset frequency was evaluated as 1.2 × 10(-11) at 0.1 second averaging periods and 1.7 × 10(-9) at 80 seconds, corresponding to a carrier envelope phase noise of 75 microradians and 10 milliradians, respectively. This method can be realized with a low pulse energy of ~10 pJ and does not require subsequent power amplification or spectral broadening. The high efficiency and short-term stability of this method can facilitate the use of femtosecond lasers in the field of industrial surface measurements, telecommunications, and space sciences.

Speckle phase noise in coherent laser ranging: fundamental precision limitations.

Frequency-modulated continuous-wave laser detection and ranging (FMCW LADAR) measures the range to a surface through coherent detection of the backscattered light from a frequency-swept laser source. The ultimate limit to the range precision of FMCW LADAR, or any coherent LADAR, to a diffusely scattering surface will be determined by the unavoidable speckle phase noise. Here, we demonstrate the two main manifestations of this limit. First, frequency-dependent speckle phase noise leads to a non-Gaussian range distribution having outliers that approach the system range resolution, regardless of the signal-to-noise ratio. These outliers are reduced only through improved range resolution (i.e., higher optical bandwidths). Second, if the range is measured during a continuous lateral scan across a surface, the spatial pattern of speckle phase is converted to frequency noise, which leads to additional excess range uncertainty. We explore these two effects and show that laboratory results agree with analytical expressions and numerical simulations. We also show that at 1 THz optical bandwidth, range precisions below 10 µm are achievable regardless of these effects.

Comb-calibrated frequency-modulated continuous-wave ladar for absolute distance measurements.

We demonstrate a comb-calibrated frequency-modulated continuous-wave laser detection and ranging (FMCW ladar) system for absolute distance measurements. The FMCW ladar uses a compact external cavity laser that is swept quasi-sinusoidally over 1 THz at a 1 kHz rate. The system simultaneously records the heterodyne FMCW ladar signal and the instantaneous laser frequency at sweep rates up to 3400 THz/s, as measured against a free-running frequency comb (femtosecond fiber laser). Demodulation of the ladar signal against the instantaneous laser frequency yields the range to the target with 1 ms update rates, bandwidth-limited 130 µm resolution and a ~100 nm accuracy that is directly linked to the counted repetition rate of the comb. The precision is <100 nm at the 1 ms update rate and reaches ~6 nm for a 100 ms average.