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.

Coherent Laser Ranging of Deforming Objects in Fires at Sub-Millimeter Precision.

Light Detection and Ranging (LiDAR) is a powerful tool to characterize and track the surface geometry of solid objects. In a fire, however, no method has excelled at measuring three-dimensional shapes at millimeter precision while offering some immunity to the effects of flames. This paper applies coherent Frequency Modulated Continuous Wave Light Detection and Ranging to capture three-dimensional measurements of objects in fire at meters of stand-off distance. We demonstrate that despite the presence of natural gas flame depths up to 1.5 m obscuring the target, measurements with millimeter precision can be obtained. This is a significant improvement over previous work making the technique useful for many fire research applications. An approach to achieve sub-millimeter precision using spatial and temporal averaging during post-processing is presented. The technology is demonstrated in case studies of structural connection and vegetation response in fires.

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.

Initial validation of the German version of the Attentional Function Index in a sample of haematological cancer survivors.

OBJECTIVE: To date, no German instrument exists to assess subjective levels of cancer-related cognitive impairments (CRCI) in cancer survivors. We translated the validated Attentional Function Index (AFI) into German and explored its psychometric properties. METHODS: The validation sample consisted of 1,111 haematological cancer survivors mainly recruited from two cancer registries. Factorial structure was explored using principal component analysis, internal consistency via Cronbach's α, construct validity through correlational analyses (Pearson's r) and associations of patient characteristics with the AFI score via regression analyses. RESULTS: In line with the original version, we revealed three factors, that is "effective action" (seven items), "attentional lapses" (three items) and "interpersonal effectiveness" (three items). The overall reliability α was .91. Verifying construct validity, the AFI score correlated positively with cognitive functioning (r = .64, p ≤ .01) and global QoL (r = .44, p ≤ .01), but negatively with fatigue (r = -.60, p ≤ .01) and depressive symptomatology (r = -.6, p ≤ .01). Older age (ß = .12, p < .001), higher comorbidity (ß = -.07, p = .02) and being male patient (ß = .07, p = .01) were significantly associated with the AFI scores, but effect sizes were small. CONCLUSION: The German translation of the AFI shows good psychometric properties and thus may be reasonably applied to measure the subjective level of CRCI in German-speaking oncological populations.

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.

Comparing Optical Oscillators across the Air to Milliradians in Phase and 10

We demonstrate carrier-phase optical two-way time-frequency transfer (carrier-phase OTWTFT) through the two-way exchange of frequency comb pulses. Carrier-phase OTWTFT achieves frequency comparisons with a residual instability of 1.2×10^{-17} at 1 s across a turbulent 4-km free space link, surpassing previous OTWTFT by 10-20 times and enabling future high-precision optical clock networks. Furthermore, by exploiting the carrier phase, this approach is able to continuously track changes in the relative optical phase of distant optical oscillators to 9 mrad (7 as) at 1 s averaging, effectively extending optical phase coherence over a broad spatial network for applications such as correlated spectroscopy between distant atomic clocks.

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.

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.

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.

Open-path measurement of stable water isotopologues using mid-infrared dual-comb spectroscopy.

We present an open-path mid-infrared dual-comb spectroscopy (DCS) system capable of precise measurement of the stable water isotopologues H216O and HD16O. This system ran in a remote configuration at a rural test site for 3.75 months with 60% uptime and achieved a precision of < 2‰ on the normalized ratio of H216O and HD16O (δD) in 1000s. Here, we compare the δD values from the DCS system to those from the National Ecological Observatory Network (NEON) isotopologue point sensor network. Over the multi-month campaign, the mean difference between the DCS δD values and the NEON δD values from a similar ecosystem is < 2‰ with a standard deviation of 18‰, which demonstrates the inherent accuracy of DCS measurements over a variety of atmospheric conditions. We observe time-varying diurnal profiles and seasonal trends that are mostly correlated between the sites on daily timescales. This observation motivates the development of denser ecological monitoring networks aimed at understanding regional- and synoptic-scale water transport. Precise and accurate open-path measurements using DCS provide new capabilities for such networks.

Open-path dual-comb spectroscopy of methane and VOC emissions from an unconventional oil well development in Northern Colorado.

We present results from a field study monitoring methane and volatile organic compound emissions near an unconventional oil well development in Northern Colorado from September 2019 to May 2020 using a mid-infrared dual-comb spectrometer. This instrument allowed quantification of methane, ethane, and propane in a single measurement with high time resolution and integrated path sampling. Using ethane and propane as tracer gases for methane from oil and gas activity, we observed emissions during the drilling, hydraulic fracturing, millout, and flowback phases of well development. Large emissions were seen in drilling and millout phases and emissions decreased to background levels during the flowback phase. Ethane/methane and propane/methane ratios varied widely throughout the observations.

Microwave generation with low residual phase noise from a femtosecond fiber laser with an intracavity electro-optic modulator.

Low phase-noise microwave generation has previously been demonstrated using self-referenced frequency combs to divide down a low noise optical reference. We demonstrate an approach based on a fs Er-fiber laser that avoids the complexity of self-referenced stabilization of the offset frequency. Instead, the repetition rate of the femtosecond Er-fiber laser is phase locked to two cavity-stabilized cw fiber lasers that span 3.74 THz by use of an intracavity electro-optic modulator with over 2 MHz feedback bandwidth. The fs fiber laser effectively divides the 3.74 THz difference signal to produce microwave signals at harmonics of the repetition rate. Through comparison of two identical dividers, we measure a residual phase noise on a 1.5 GHz carrier of -120 dBc/Hz at 1 Hz offset.

Dual-comb photoacoustic spectroscopy.

Spectrally resolved photoacoustic imaging is promising for label-free imaging in optically scattering materials. However, this technique often requires acquisition of a separate image at each wavelength of interest. This reduces imaging speeds and causes errors if the sample changes in time between images acquired at different wavelengths. We demonstrate a solution to this problem by using dual-comb spectroscopy for photoacoustic measurements. This approach enables a photoacoustic measurement at thousands of wavelengths simultaneously. In this technique, two optical-frequency combs are interfered on a sample and the resulting pressure wave is measured with an ultrasound transducer. This acoustic signal is processed in the frequency-domain to obtain an optical absorption spectrum. For a proof-of-concept demonstration, we measure photoacoustic signals from polymer films. The absorption spectra obtained from these measurements agree with those measured using a spectrophotometer. Improving the signal-to-noise ratio of the dual-comb photoacoustic spectrometer could enable high-speed spectrally resolved photoacoustic imaging.

Photodetectors based on intersubband transitions using III-nitride superlattice structures.

We review our recent progress on the fabrication of near-infrared photodetectors based on intersubband transitions in AlN/GaN superlattice structures. Such devices were first demonstrated in 2003, and have since then seen a quite substantial development both in terms of detector responsivity and high speed operation. Nowadays, the most impressive results include characterization up to 3 GHz using a directly modulated semiconductor laser and up to 13.3 GHz using an ultra-short pulse solid state laser.

Tight real-time synchronization of a microwave clock to an optical clock across a turbulent air path.

The ability to distribute the precise time and frequency from an optical clock to remote platforms could enable future precise navigation and sensing systems. Here we demonstrate tight, real-time synchronization of a remote microwave clock to a master optical clock over a turbulent 4-km open air path via optical two-way time-frequency transfer. Once synchronized, the 10-GHz frequency signals generated at each site agree to 10-14 at one second and below 10-17 at 1000 seconds. In addition, the two clock times are synchronized to ±13 fs over an 8-hour period. The ability to phase-synchronize 10-GHz signals across platforms supports future distributed coherent sensing, while the ability to time-synchronize multiple microwave-based clocks to a high-performance master optical clock supports future precision navigation/timing systems.

Synchronization of Clocks Through 12 km of Strongly Turbulent Air Over a City.

We demonstrate real-time, femtosecond-level clock synchronization across a low-lying, strongly turbulent, 12-km horizontal air path by optical two-way time transfer. For this long horizontal free-space path, the integrated turbulence extends well into the strong turbulence regime corresponding to multiple scattering with a Rytov variance up to 7 and with the number of signal interruptions exceeding 100 per second. Nevertheless, optical two-way time transfer is used to synchronize a remote clock to a master clock with femtosecond-level agreement and with a relative time deviation dropping as low as a few hundred attoseconds. Synchronization is shown for a remote clock based on either an optical or microwave oscillator and using either tip-tilt or adaptive-optics free-space optical terminals. The performance is unaltered from optical two-way time transfer in weak turbulence across short links. These results confirm that the two-way reciprocity of the free-space time-of-flight is maintained both under strong turbulence and with the use of adaptive optics. The demonstrated robustness of optical two-way time transfer against strong turbulence and its compatibility with adaptive optics is encouraging for future femtosecond clock synchronization over very long distance ground-to-air free-space paths.

High-performance, vibration-immune, fiber-laser frequency comb.

We demonstrate an environmentally robust optical frequency comb based on a polarization-maintaining, all-fiber, figure-eight laser. The comb is phase locked to a cavity-stabilized cw laser by use of an intracavity electro-optic phase modulator yielding 1.6 MHz feedback bandwidth. This high bandwidth provides close to shot-noise-limited residual phase noise between the comb and cw reference laser of -94 dBc/Hz from 20 Hz to 200 kHz and an integrated in-loop phase noise of 32 mrad from 1 Hz to 1 MHz. Moreover, the comb remains phase locked under significant mechanical vibrations of over 1 g. This level of environmental robustness is an important step toward a fieldable fiber frequency comb.