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The telecommunications industry's deployment of billions of kilometers of optical fiber has created a vast global network that can be exploited for additional applications such as environmental sensing, quantum networking and international clock comparisons. However, for reasons such as the unidirectionality of long-haul fiber links, telecom fiber networks cannot always be adapted for important applications beyond data transmission. Fortunately, new multicore optical fibers create the opportunity for application coexistence with data traffic, creating expansive multifunctional networks. Towards that end, we propose and demonstrate the faithful transfer of ultrastable optical signals through multicore fiber in a way that is compatible with the unidirectionality of long-haul fiber optic systems, demonstrating a fractional frequency instability of 3x10-19 at 10,000 seconds. This opens the door towards intercontinental optical clock comparisons, with applications in fundamental physics and the redefinition of the second.

We introduce a new parallelized approach to photothermal microscopy that utilizes mid-infrared dual-comb lasers, enabling simultaneous measurements at hundreds of wavelengths. This technology allows for high-speed, label-free chemical identification with super-resolution infrared imaging, overcoming the limitations of slow, single-wavelength-laser methods.

Mid-infrared microscopy is an important tool for biological analyses, allowing a direct probe of molecular bonds in their low energy landscape. In addition to the label-free extraction of spectroscopic information, the application of broadband sources can provide a third dimension of chemical specificity. However, to enable widespread deployment, mid-infrared microscopy platforms need to be compact and robust while offering high speed, broad bandwidth and high signal-to-noise ratio (SNR). In this study, we experimentally showcase the integration of a broadband, high-repetition-rate dual-comb spectrometer (DCS) in the mid-infrared range with a scanning microscope. We employ a set of 1-GHz mid-infrared frequency combs, demonstrating their capability for high-speed and broadband hyperspectral imaging of polymers and ovarian tissue. The system covers 1000 $\mathrm{cm^{-1}}$ at $\mathrm{\nu_c=2941 \; cm^{-1}}$ with 12.86 kHz spectra acquisition rate and 5 $\mathrm{\mu m}$ spatial resolution. Taken together, our experiments and analysis elucidate the trade-off between bandwidth and speed in DCS as it relates to microscopy. This provides a roadmap for the future advancement and application of high-repetition-rate DCS hyperspectral imaging.

We demonstrate a vacuum-gap ultrastable optical reference cavity that does not require a vacuum enclosure. Our simple method of optical contact bonding in a vacuum environment allows for cavity operation in air while maintaining vacuum between the cavity mirrors. Vacuum is maintained long term, with no observed degradation in cavity stability for over 1 year after bonding. For a 1550 nm laser stabilized to a 9.7 mL in-vacuum bonded cavity, the measured Allan deviation is $2.4\times 10^{-14}$ at 1 s and its phase noise is thermal-noise-limited from 0.1 Hz to 10 kHz, reaching about -105 dBc/Hz at 10 kHz offset frequency. This represents the highest stability of any oscillator operated without a vacuum enclosure. Furthermore, we demonstrate a 0.5 mL in-vacuum bonded cavity created using microfabricated mirrors and cavity dicing, with phase noise reaching -95 dBc/Hz at 10 kHz offset frequency. By relieving the need for high-vacuum enclosures, we greatly enhance the portability and utility of low noise, compact cavity-stabilized lasers, with applications ranging from environmental sensing to mobile optical clocks to ultralow noise microwave generation., Comment: 10 pages, 6 figures

The detection of light of thermal origin is the principal means by which humanity has learned about our world and the cosmos. In optical astronomy, in particular, direct detection of thermal photons and the resolution of their spectra have enabled discoveries of the broadest scope and impact. Such measurements, however, do not capture the phase of the thermal fields--a parameter that has proven crucial to transformative techniques in radio astronomy such as synthetic aperture imaging. Over the last 25 years, tremendous progress has occurred in laser science, notably in the phase-sensitive, broad bandwidth, high resolution, and traceable spectroscopy enabled by the optical frequency comb. In this work, we directly connect the fields of frequency comb laser spectroscopy and passive optical sensing as applied to astronomy, remote sensing, and atmospheric science. We provide fundamental sensitivity analysis of dual-comb correlation spectroscopy (DCCS), whereby broadband thermal light is measured via interferometry with two optical frequency combs. We define and experimentally verify the sensitivity scaling of DCCS at black body temperatures relevant for astrophysical observations. Moreover, we provide comparison with direct detection techniques and more conventional laser heterodyne radiometry. Our work provides the foundation for future exploration of comb-based broadband synthetic aperture hyperspectral imaging across the infrared and optical spectrum., Comment: 54 pages, 7 figures

Accurate diagnostics of the combustor region of ramjet engines can improve engine design and create benchmarks for computational fluid dynamics models. Previous works demonstrate that dual frequency comb spectroscopy can provide low uncertainty diagnostics of multiple flow parameters in the non-combusting regions of ramjets. However, the high temperatures present in the combustor present a challenge for broadband spectroscopic absorption models that are used to interpret measurements in these regions. Here, we utilize a new water vapor absorption database created for high temperature water-air mixtures to fit spectra measured in a ground-test ramjet engine with a broadband near-infrared dual comb absorption spectrometer. We extract 2D profiles of pressure, temperature, water mole fraction, and velocity using this new database. We demonstrate that the new database provides the lowest fit residuals compared to other water vapor absorption databases. We compare computational fluid dynamics simulations of the combustor with the measured data to demonstrate that the simulations overpredict heat release and water vapor production., Comment: This work has been cleared by the Air Force under case number AFRL-2023-4205

Molecular diagnostics are a primary tool of modern chemistry, enabling researchers to map chemical reaction pathways and rates to better design and control chemical systems. Many chemical reactions are complex and fast, and existing diagnostic approaches provide incomplete information. For example, mass spectrometry is optimized to gather snapshots of the presence of many chemical species, while conventional laser spectroscopy can quantify a single chemical species through time. Here we optimize for multiple objectives by introducing a high-speed and broadband, mid-infrared dual frequency comb absorption spectrometer. The optical bandwidth of >1000 cm-1 covers absorption fingerprints of many species with spectral resolution <0.03 cm-1 to accurately discern their absolute quantities. Key to this advance are 1 GHz pulse repetition rate frequency combs covering the 3-5 um region that enable microsecond tracking of fast chemical process dynamics. We demonstrate this system to quantify the abundances and temperatures of each species in the complete reactants-to-products breakdown of 1,3,5-trioxane, which exhibits a formaldehyde decomposition pathway that is critical to modern low temperature combustion systems. By maximizing the number of observed species and improving the accuracy of temperature and concentration measurements, this spectrometer advances understanding of chemical reaction pathways and rates and opens the door for novel developments such as combining high-speed chemistry with machine learning.

Supersonic engine development requires accurate and detailed measurements of fluidic and thermodynamic parameters to optimize engine designs and benchmark computational fluid dynamic (CFD) simulations. Here, we demonstrate that dual frequency comb spectroscopy (DCS) with mode-locked frequency combs can provide simultaneous absolute measurements of several flow parameters with low uncertainty across a range of conditions owing to the broadband and ultrastable optical frequency output of the lasers. We perform DCS measurements across a 6800-7200 cm-1 bandwidth covering hundreds of H2O absorption features resolved with a spectral point spacing of 0.0067 cm-1 and point spacing precision of 1.68 x 10-10 cm-1. We demonstrate 2D profiles of velocity, temperature, pressure, water mole fraction, and air mass flux in a ground-test dual-mode ramjet at Wright-Patterson Air Force Base. The narrow angles of the measurement beams offer sufficient spatial resolution to resolve properties across an oblique shock train in the isolator and the thermal throat of the combustor. We determine that the total measurement uncertainties for the various parameters range from 1% for temperature to 9% for water vapor mole fraction, with the absorption database/model that is used to interpret the data typically contributing the most uncertainty (leaving the door open for even lower uncertainty in the future). CFD at the various measurement locations show good agreement, largely falling within the DCS measurement uncertainty for most profiles and parameters.

Providing an accurate, representative sample of mass flux across large open areas for atmospheric studies or the extreme conditions of a hypersonic engine is challenging for traditional intrusive or point-based sensors. Here, we demonstrate that laser absorption spectroscopy with mode-locked frequency combs can simultaneously measure all of the components of mass flux (velocity, temperature, pressure, and species mole fraction) with low uncertainty, spatial resolution corresponding to the laser line of sight, and no supplemental sensor readings. The low uncertainty is provided by the broad spectral bandwidth, high resolution, and extremely well-known and controlled frequency axis of stabilized, mode-locked frequency combs. We demonstrate these capabilities using dual frequency comb spectroscopy (DCS) in the isolator of a ground-test supersonic propulsion engine at Wright-Patterson Air Force Base. The mass flux measurements are consistent within 3.6% of the facility-level engine air supply values. A vertical scan of the laser beams in the isolator measures the spatially resolved mass flux, which is compared with computational fluid dynamics simulations. A rigorous uncertainty analysis demonstrates a instrument uncertainty of ~0.4%, and total uncertainty (including non-instrument sources) of ~7% for mass flux measurements. These measurements demonstrate DCS with mode-locked frequency combs as a low-uncertainty mass flux sensor for a variety of applications.

Mid-infrared (MIR) spectrometers are invaluable tools for molecular fingerprinting and hyper-spectral imaging. Among the available spectroscopic approaches, GHz MIR dual-comb absorption spectrometers have the potential to simultaneously combine the high-speed, high spectral resolution, and broad optical bandwidth needed to accurately study complex, transient events in chemistry, combustion, and microscopy. However, such a spectrometer has not yet been demonstrated due to the lack of GHz MIR frequency combs with broad and full spectral coverage. Here, we introduce the first broadband MIR frequency comb laser platform at 1 GHz repetition rate that achieves spectral coverage from 3 to 13 {\mu}m. This frequency comb is based on a commercially available 1.56 {\mu}m mode-locked laser, robust all-fiber Er amplifiers and intra-pulse difference frequency generation (IP-DFG) of few-cycle pulses in \c{hi}(2) nonlinear crystals. When used in a dual comb spectroscopy (DCS) configuration, this source will simultaneously enable measurements with {\mu}s time resolution, 1 GHz (0.03 cm-1) spectral point spacing and a full bandwidth of >5 THz (>166 cm-1) anywhere within the MIR atmospheric windows. This represents a unique spectroscopic resource for characterizing fast and non-repetitive events that are currently inaccessible with other sources.

Single-cycle pulses with deterministic carrier-envelope phase enable the study and control of light-matter interactions at the sub-cycle timescale, as well as the efficient generation of low-noise multi-octave frequency combs. However, current single-cycle light sources are difficult to implement and operate, hindering their application and accessibility in a wider range of research. In this paper, we present a single-cycle 100 MHz frequency comb in a compact, turn-key, and reliable all-silica-fiber format. This is achieved by amplifying 2 $\mu$m seed pulses in heavily-doped Tm:fiber, followed by cascaded self-compression to yield 6.8 fs pulses with 215 kW peak power and 374 mW average power. The corresponding spectrum covers more than two octaves, from below 700 nm up to 3500 nm. Driven by this single-cycle pump, supercontinuum with 180 mW of integrated power and a smooth spectral amplitude between 2100 and 2700 nm is generated directly in silica fibers. To broaden applications,few-cycle pulses extending from 6 $\mu$m to beyond 22 $\mu$m with long-term stable carrier-envelope phase are created using intra-pulse difference frequency, and electro-optic sampling yields comb-tooth-resolved spectra. Our work demonstrates the first all-fiber configuration that generates single-cycle pulses, and provides a practical source to study nonlinear optics on the same timescale., Comment: Revised version

Accurate absorption models for gases at high pressure and temperature support advanced optical combustion diagnostics and aid in the study of harsh planetary atmospheres. Developing and validating absorption models for these applications requires recreating the extreme temperature and pressure conditions of these environments in static, uniform, well-known conditions in the laboratory. Here, we present the design of a new gas cell to enable reference-quality absorption spectroscopy at high pressure and temperature. The design centers on a carefully controlled quartz sample cell housed at the core of a pressurized ceramic furnace. The half-meter sample cell is relatively long compared to past high- pressure and temperature absorption cells, and is surrounded by a molybdenum heat spreader that enables high temperature uniformity over the full length of the absorbing gas. We measure the temperature distribution of the sample gas using in situ thermocouples, and fully characterize the temperature uniformity across a full matrix of conditions up to 1000 K and 50 bar. The results demonstrate that the new design enables highly uniform and precisely known conditions across the full absorbing path length. Uniquely, we test the new gas cell with a broadband, high-resolution dual frequency comb spectrometer that enables highly resolved absorption spectroscopy across a wide range of temperature and pressure conditions. With this system, we measure the spectrum of CO$_2$ between 6800 and 7000 cm$^{-1}$ at pressures between 0.2 and 20 bar, and temperatures up to 1000 K. The measurements reveal discrepancies from spectra predicted by the HITRAN2016 database with a Voigt line shape at both low- and high-pressure conditions. These results motivate future work to expand absorption models and databases to accurately model high-pressure and -temperature spectra in combustion and planetary science research.

Broadband dual-comb spectroscopy (DCS) based on portable mode-locked fiber frequency combs is a powerful tool for in situ, calibration free, multi-species spectroscopy. While the acquisition of a single spectrum with mode-locked DCS typically takes microseconds to milliseconds, the applications of these spectrometers have generally been limited to systems and processes with time changes on the order of seconds or minutes due to the need to average many spectra to reach a high signal-to-noise ratio (SNR). Here, we demonstrate high-speed, continuous, fiber mode-locked laser DCS with down to 11 $\mu$s time resolution. We achieve this by filtering the comb spectra using portable Fabry-Perot cavities to generate filtered combs with 1 GHz tooth spacing. The 1 GHz spacing increases the DCS acquisition speed and SNR for a given optical bandwidth while retaining a sufficient spacing to resolve absorption features over a wide range of conditions. We measure spectra of methane inside a rapid compression machine throughout the 16 ms compression cycle with 133 cm$^{-1}$ bandwidth (4000 comb teeth) and 1.4 ms time resolution by spectrally filtering one of the combs. By filtering both combs, we measured a single-shot, 25 cm$^{-1}$ (750 comb teeth) spectrum of CO around 6330 cm$^{-1}$ in 11 $\mu$s. The technique enables simultaneously high-speed and high-resolution DCS measurements, and can be applied anywhere within the octave-spanning spectrum of robust and portable fiber mode-locked frequency combs.

Low noise and high repetition rate optical frequency combs are desirable for many applications from timekeeping to precision spectroscopy. For example, gigahertz repetition rate sources greatly increase the acquisition speed of spectra in a dual-comb modality when compared to lower repetition rate sources, while still maintaining sufficient instantaneous resolution to resolve ro-vibrational signatures from molecules in a variety of conditions. In this paper, we present the stabilization and characterization of a turnkey commercial 1~GHz mode-locked laser that operates at telecom wavelengths (1.56 $\mu$m). Fiber amplification and spectral broadening result in the high signal-to-noise ratio detection and stabilization of $\textit{f}_{\textit{ceo}}$ with 438 mrad of residual phase noise (integrated from 10$^2$ to 10$^7$ Hz). Simultaneously, we stabilize the beatnote between the nearest comb mode and a cavity stabilized continuous-wave laser at 1.55 $\mu$m with 41 mrad of residual phase noise (integrated from 10$^2$ to 10$^7$ Hz). This robust, self-referenced comb system is built with off-the-shelf polarization-maintaining fiber components and will be useful for a wide range of low noise frequency comb applications that benefit from the increased repetition rate., Comment: 8 pages, 5 figures

The accuracy of quantitative absorption spectroscopy depends on correctly distinguishing molecular absorption signatures in a measured transmission spectrum from the varying intensity or "baseline" of the light source. Baseline correction becomes particularly difficult when the measurement involves complex, broadly absorbing molecules or non-ideal transmission effects such as etalons. We demonstrate a technique that eliminates the need to account for the laser intensity in absorption spectroscopy by converting the measured transmission spectrum of a gas sample to a modified form of the time-domain molecular free induction decay (m-FID) using a cepstral analysis technique developed for audio signal processing. Much of the m-FID signal is temporally separated from and independent of the source intensity, and this portion can be fit directly with a model to determine sample gas properties without correcting for the light source intensity. We validate the new approach in several complex absorption spectroscopy scenarios and discuss its limitations. The technique is applicable to spectra obtained with any absorption spectrometer and provides a fast and accurate approach for analyzing complex spectra.

We demonstrate fiber mode-locked dual frequency comb spectroscopy for broadband, high resolution measurements in a rapid compression machine (RCM). We apply an apodization technique to improve the short-term signal-to-noise-ratio (SNR), which enables broadband spectroscopy at combustion-relevant timescales. We measure the absorption on 24345 individual wavelength elements (comb teeth) between 5967 and 6133 cm-1 at 704 microsecond time resolution during a 12-ms compression of a CH4-N2 mixture. We discuss the effect of the apodization technique on the absorption spectra, and apply an identical effect to the spectral model during fitting to recover the mixture temperature. The fitted temperature is compared against an adiabatic model, and found to be in good agreement with expected trends. This work demonstrates the potential of DCS to be used as an in situ diagnostic tool for broadband, high resolution, measurements in engine-like environments.

Optical frequency combs provide the clockwork to relate optical frequencies to radio frequencies. Hence, combs allow to measure optical frequencies with respect to a radio frequency where the accuracy is limited only by the reference signal. In order to provide a stable link between the radio and optical frequencies, the two parameters of the frequency comb must be fixed: the carrier envelope offset frequency $f_{\rm ceo}$ and the pulse repetition-rate $f_{\rm rep}$. We have developed the first optical frequency comb based on difference frequency generation (DFG) that eliminates $f_{\rm ceo}$ by design - specifically tailored for applications in cold atom physics. An $f_{\rm ceo}$-free spectrum at 1550 nm is generated from a super continuum spanning more than an optical octave. Established amplification and frequency conversion techniques based on reliable telecom fiber technology allow generation of multiple wavelength outputs. In this paper we discuss the frequency comb design, characterization, and optical frequency measurement of Sr Rydberg states. The DFG technique allows for a compact and robust, passively $f_{\rm ceo}$ stable frequency comb significantly improving reliability in practical applications.