Mid-infrared Comb Research Articles

Mid-infrared dual frequency comb spectroscopy for combustion analysis from 2.8 to 5 µm

We demonstrate the application of mode-locked mid-infrared dual frequency comb spectroscopy for combustion analysis. With two settings of the same dual-comb system, the measurement spans 1500 cm−1 from 2.8 to 5 µm with 0.0067 cm−1 (200 MHz) point spacing, or almost a quarter-million discrete comb modes. Using this broadband spectrometer, we quantify the pyrolysis and smoldering combustion of wood samples. Specifically, we measure 20-second time-resolved mole fractions of CH4, H2O, two isotopologues of CO2 (12C16O2, 13C16O2), two isotopologues of CO (12C16O, 13C16O), ethane, formaldehyde, methanol, formic acid, as well as gas temperature directly above radiatively heated wood samples. The combination of the fine spectral resolution and the broad bandwidth of the dual-comb spectrometer allows for precise separation of absorption signatures of individual molecules from the congested spectra.

Precision Spectroscopy of Nitrous Oxide Isotopocules with a Cross-Dispersed Spectrometer and a Mid-Infrared Frequency Comb.

As a potent greenhouse gas and an ozone-depleting agent, nitrous oxide (N2O) plays a critical role in the global climate. Effective mitigation relies on understanding global sources and sinks, which can be supported through isotopic analysis. We present a cross-dispersed spectrometer, coupled with a mid-infrared frequency comb, capable of simultaneously monitoring all singly substituted, stable isotopic variants of N2O. Rigorous evaluation of the instrument lineshape function and data treatment using a Doppler-broadened, low-pressure gas sample are discussed. Laboratory characterization of the spectrometer demonstrates sub-GHz spectral resolution and an average precision of 6.7 × 10-6 for fractional isotopic abundance retrievals in 1 s.

Nanophotonic supercontinuum-based mid-infrared dual-comb spectroscopy

High resolution and fast detection of molecular vibrational absorption is important for organic synthesis, pharmaceutical processes, and environmental monitoring, and is enabled by mid-infrared (mid-IR) laser frequency combs via dual-comb spectroscopy. Here, we demonstrate a novel and highly simplified approach to broadband mid-IR dual-comb spectroscopy via supercontinuum generation, achieved using unprecedented nanophotonic dispersion engineering that allows for ultra-broadband and flat-envelope mid-IR frequency combs. Our mid-IR dual-comb spectrometer has an instantaneous bandwidth covering the functional group region from 2800 – 3600 c m − 1 , comprising more than 100,000 comb lines, enabling parallel gas-phase detection with a high sensitivity, sub-Doppler spectral resolution, and a high speed. In addition to the traditional functional groups, their isotopologues are also resolved in this supercontinuum-based dual-comb spectroscopy. Our approach combines well established fiber laser combs, digital coherent data averaging, and integrated nonlinear photonics, each in itself a state-of-the-art technology, signaling the emergence of mid-IR dual-comb spectroscopy for use outside of the protected laboratory environment.

Line positions and intensities of the ν4 band of methyl iodide using mid-infrared optical frequency comb Fourier transform spectroscopy

We use optical frequency comb Fourier transform spectroscopy to measure high-resolution spectra of iodomethane, CH3I, in the CH stretch region from 2800 to 3160 cm-1. The fast-scanning Fourier transform spectrometer with auto-balanced detection is based on a difference frequency generation comb with repetition rate, frep, of 125 MHz. A series of spectra with sample point spacing equal to frep are measured at different frep settings and interleaved to yield sampling point spacing of 11 MHz. Iodomethane is introduced into a 76 m long multipass absorption cell by its vapor pressure at room temperature. The measured spectrum contains three main ro-vibrational features: the parallel vibrational overtone and combination bands centered around 2850 cm-1, the symmetric stretch ν1 band centered at 2971 cm-1, and the asymmetric stretch ν4 band centered at 3060 cm-1. The spectra of the ν4 band and the nearby ν3+ν4-ν3 hot band are simulated using PGOPHER and a new assignment of these bands is presented. The resolved ro-vibrational structures are used in a least square fit together with the microwave data to provide the upper state parameters. We assign 2603 transitions to the ν4 band with a standard deviation (observed – calculated) of 0.00034 cm-1, and 831 transitions to the ν3+ν4-ν3 hot band with a standard deviation of 0.00084 cm-1. For comparison, in the earlier work using standard FT-IR with 162 MHz resolution [Anttila, et al., J. Mol. Spectrosc. 1986; 119:190–200] 1830 transition were assigned to the ν4 band, and 380 transitions to the ν3+ν4-ν3 hot band, with standard deviations of 0.00083 cm-1 and 0.0013 cm-1, respectively. The hyperfine splittings due to the 127I nuclear quadrupole moment are observed for transitions with J ≤ 2 × K. Finally, intensities of 157 isolated transitions in the ν4 band are reported for the first time using the Voigt line shape as a model in multispectral fitting.

Dispersion-engineered T-type germanium waveguide for mid-infrared supercontinuum and frequency comb generations in all-normal dispersion region

In this paper, a T-type germanium (Ge) waveguide with an all-normal dispersion profile is designed for mid-infrared (MIR) supercontinuum (SC) and frequency comb generations. The nonlinearity coefficient of the designed waveguide is calculated as 30.48 W-1·m-1 at the initial pump wavelength of 3.0 µm. Moreover, the group-velocity dispersion is kept low and flat in the considered wavelength range. Simulation results show that with the designed waveguide, the highly coherent and octave-spanning MIR SC can be generated in the wavelength range from 1.85 to 9.98 µm (more than 2.4 octaves) when the pump pulse with wavelength of 3.0 µm, peak power of 900 W, and duration of 120 fs is launched into the 5 mm long waveguide. When the pulse train including 50 pulses at a repetition rate of 100 MHz is used as the pump source, the SC-based frequency comb is obtained.

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.

All-fiber frequency comb at 2 µm providing 1.4-cycle pulses.

We report an all-fiber approach to generating sub-2-cycle pulses at 2 µm and a corresponding octave-spanning optical frequency comb. Our configuration leverages mature erbium:fiber laser technology at 1.5 µm to provide a seed pulse for a thulium-doped fiber amplifier that outputs 330 mW average power at a 100 MHz repetition rate. Following amplification, nonlinear self-compression in fiber decreases the pulse duration to 9.5 fs, or 1.4 optical cycles. The spectrum of the ultrashort pulse spans from 1 to beyond 2.4 µm and enables direct measurement of the carrier-envelope offset frequency. Our approach employs only commercially available fiber components, resulting in a design that is easy to reproduce in the larger community. As such, this system should be useful as a robust frequency comb source in the near-infrared or as a pump source to generate mid-infrared frequency combs.

Interleaved difference-frequency generation for microcomb spectral densification in the mid-infrared

With their compact size and semiconductor-chip-based operation, frequency microcombs can be an invaluable light source for gas spectrcoscopy. However, the generation of mid-infrared (mid-IR) frequency combs with gigahertz line spacing as required to resolve many gas spectra represents a significant challenge for these devices. Here, a technique referred to as interleaved difference-frequency generation (iDFG) is introduced that densifies the spectral line spacing upon conversion of near-IR comb light into the mid-IR light. A soliton microcomb is used as both a comb light source and microwave oscillator in a demonstration, and the spectrum of methane is measured to illustrate how the resulting mid-IR comb avoids spectral undersampling. Beyond demonstration of the iDFG technique, this work represents an important feasibility step towards more compact and potentially chip-based mid-IR gas spectroscopy modules.

Mid-Infrared Frequency Comb Generation and Spectroscopy with Few-Cycle Pulses and χ^{(2)} Nonlinear Optics.

The mid-infrared atmospheric window of 3-5.5 μm holds valuable information regarding molecular composition and function for fundamental and applied spectroscopy. Using a robust, mode-locked fiber-laser source of <11 fs pulses in the near infrared, we explore quadratic (χ^{(2)}) nonlinear optical processes leading to frequency comb generation across this entire mid-infrared atmospheric window. With experiments and modeling, we demonstrate intrapulse difference frequency generation that yields few-cycle mid-infrared pulses in a single pass through periodically poled lithium niobate. Harmonic and cascaded χ^{(2)} nonlinearities further provide direct access to the carrier-envelope offset frequency of the near infrared driving pulse train. The high frequency stability of the mid-infrared frequency comb is exploited for spectroscopy of acetone and carbonyl sulfide with simultaneous bandwidths exceeding 11THz and with spectral resolution as high as 0.003 cm^{-1}. The combination of low noise and broad spectral coverage enables detection of trace gases with concentrations in the part-per-billion range.

Intensity noise optimization of a mid-infrared frequency comb difference-frequency generation source

We experimentally demonstrate in a difference-frequency generation mid-infrared frequency comb source the effect of temporal overlap between pump and signal pulses on the relative intensity noise (RIN) of the idler pulse. When scanning the temporal delay between our 130 fs long signal and pump pulses, we observe a RIN minimum with a 3 dB width of 20 fs delay and a RIN increase of 20 dB in 40 fs delay at the edges of this minimum. We also demonstrate active long-term stabilization of the mid-infrared frequency comb source to the temporal overlap setting corresponding to the lowest RIN operation point by an online RIN detector and active feedback control of the pump-signal pulse delay. This active stabilization setup allows us to dramatically increase the signal-to-noise ratio of mid-infrared absorption spectra.

Frequency noise correlation between the offset frequency and the mode spacing in a mid-infrared quantum cascade laser frequency comb.

The generation of frequency combs in the mid-infrared (MIR) spectral range by quantum cascade lasers (QCLs) has the potential for revolutionizing dual-comb multi-heterodyne spectroscopy in the molecular fingerprint region. However, in contrast to frequency combs based on passively mode-locked ultrafast lasers, their operation relies on a completely different mechanism resulting from a four-wave mixing process occurring in the semiconductor gain medium that locks the modes together. As a result, these lasers do not emit pulses and no direct self-referencing of a QCL comb spectrum has been achieved so far. Here, we present a detailed frequency noise characterization of a MIR QCL frequency comb operating at a wavelength of 8 µm with a mode spacing of ∼7.4 GHz. Using a beat measurement with a narrow-linewidth single-mode QCL in combination with a dedicated electrical scheme, we measured the frequency noise properties of an optical mode of the QCL comb, and indirectly of its offset frequency for the first time, without detecting it by the standard approach of nonlinear interferometry applied to ultrafast mode-locked lasers. In addition, we also separately measured the noise of the comb mode spacing extracted electrically from the QCL. We observed a strong anti-correlation between the frequency fluctuations of the offset frequency and mode spacing, leading to optical modes with a linewidth slightly below 1 MHz in the free-running QCL comb (at 1-s integration time), which is narrower than the individual contributions of the offset frequency and mode spacing that are at least 2 MHz each.

Mid-infrared frequency comb with 6.7 W average power based on difference frequency generation.

We report on the development of a high-power mid-infrared frequency comb with 100 MHz repetition rate and 100 fs pulse duration. Difference frequency generation is realized between two branches derived from an Er:fiber comb, amplified separately in Yb:fiber and Er:fiber amplifiers. Average powers of 6.7 W and 14.9 W are generated in the 2.9 µm idler and 1.6 µm signal, respectively. With high average power, excellent beam quality, and passive carrier-envelope phase stabilization, this light source is a promising platform for generating broadband frequency combs in the far infrared, visible, and deep ultraviolet.

A rapid, spatially dispersive frequency comb spectrograph aimed at gas phase chemical reaction kinetics

This New Views article will highlight some recent advances in high sensitivity gas detection using direct infrared absorption frequency comb laser spectroscopy, with a focus on frequency comb use in chemical reaction kinetics and our own contribution to this field. Our recently implemented detection technique uses a combination of a 12.9 GHz free spectral range virtually imaged phased array and diffraction grating to spatially disperse the mid-infrared frequency comb onto a camera. Individual frequencies or ‘comb teeth’ of a 250 MHz repetition-rate frequency comb are able to be resolved. High molecular sensitivity is achieved by increasing the interaction path length using a Herriott multipass cell. High spectral resolution, broadband spectral coverage, and high molecular sensitivity are all achieved on an adjustable 1–50 µs timescale, making this frequency comb apparatus ideal for measuring chemical reaction kinetics where multiple absorbing species can be monitored simultaneously. This New Views article will also discuss some of the challenges and decisions that chemists might face in implementing this advanced physics technology in their own laboratory. Spatially dispersed 250 MHz mid-infrared frequency comb laser, with absorption of some frequencies by a dilute sample of methane.

Sensitivity of SWIFT spectroscopy.

SWIFT spectroscopy (Shifted Wave Interference Fourier Transform Spectroscopy) is a coherent beatnote technique that can be used to measure the temporal profiles of periodic optical signals. While it has been essential in understanding the physics of various mid-infrared and terahertz frequency combs, its ultimate limits have not been discussed. We show that the envelope of a SWIFTS interferogram is physically meaningful and is directly related to autocorrelation. We derive analytical expressions for the SWIFTS signals of two prototypical cases-chirped pulses from a mode-locked laser and a frequency-modulated comb-and derive scaling laws for the noise of these measurements, showing how it can be mitigated. Finally, we confirm this analysis by performing the first SWIFTS measurements of near-infrared pulses from femtosecond lasers, establishing the validity of the technique for highly-dispersed sub-picojoule pulses.

Mid-infrared frequency comb from a ring quantum cascade laser

The effect of spatial hole burning on mode proliferation has been shown both theoretically and experimentally to be important for frequency comb operation in quantum cascade lasers (QCLs). It is therefore of great interest to investigate the frequency comb operation from integrated ring cavities where this effect is absent. Here we report a mid-infrared quantum cascade laser based on a buried heterostructure ring cavity that exhibits unidirectional lasing with a frequency comb spectrum displaying a predominantly s e c h 2 profile over a bandwidth of ∼ 10 − 1 . A single beat note with 3 dB linewidth of &lt; 900 H z was observed over the last 85% of the whole current dynamic range. To further verify the frequency comb operation, a multiheterodyne experiment was carried out using a standard Fabry–Pérot QCL comb as a reference laser. This measurement allowed the retrieval of the spectral phases, indicating an operation with strong amplitude modulation.

Mid-infrared optical frequency comb in the 2.7–4.0 μm range via difference frequency generation from a compact laser system

Abstract We report on the generation of a mid-infrared (mid-IR) frequency comb with a maximum average output power of 250 mW and tunability in the 2.7–4.0 μm region. The approach is based on a single-stage difference frequency generation (DFG) starting from a compact Yb-doped fiber laser system. The repetition rate of the near-infrared (NIR) comb is locked at 75 MHz. The phase noise of the repetition rate in the offset-free mid-IR comb system is measured and analyzed. Except for the intrinsic of NIR comb, environmental noise at low frequency and quantum noise at high frequency from the amplifier chain and nonlinear spectral broadening are the main noise sources of broadening the linewidth of comb teeth, which limits the precision of mid-IR dual-comb spectroscopy.

Mid-Infrared Supercontinuum and Frequency Comb Generations by Different Optical Modes in a Multimode Chalcogenide Strip Waveguide

Supercontinuum (SC) with broad bandwidth and high coherence is crucial in the SC-based frequency comb source generation. In this paper, we numerically investigate the mid-infrared (MIR) SC generations with the three optical modes (TE <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">00</sub> , TE <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">10</sub> , and TE <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">20</sub> ) in a multimode chalcogenide (As <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">2</sub> Se <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">3</sub> ) strip waveguide. The waveguide structure is carefully engineered to ensure that the pump pulses are propagated in the normal dispersion regions of the considered three optical modes. Highly coherent and octave-spanning MIR SCs are generated when the optimized pump pulse with 80-fs pulse duration, 3-kW peak power, and 3-μm center wavelength is used. Moreover, the nonlinear dynamics of the SC generation are numerically analyzed. Finally, the SC-based frequency combs are numerically demonstrated when a pulse train with a repetition rate of 50 MHz is used as the pump source and launched into the multimode As <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">2</sub> Se <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">3</sub> -based strip waveguide. It is believed that the generated MIR SC and SC-based frequency comb sources have important applications in biophotonics, metrology, and sensing.

Wideband Mid-Infrared Comb for Biomedical Applications

Wideband Mid-Infrared Comb for Biomedical Applications

Low-Threshold 4/5 Octave-Spanning Mid-Infrared Frequency Comb in a LiNbO$_3$ Microresonator

Mid-infrared (MIR) optical frequency combs (OFCs) are ideal light sources for precision metrology and can find extensive applications, especially in molecular spectroscopy and gas detection. Here the generation of mode-locked MIR frequency comb in a LiNbO 3 microring through optimized slot-waveguide design is proposed. Such microcomb can span over four-fifths of an octave (ranging from ~2810 nm to ~4630 nm) with pump power as low as 50 mW, which can be applied to the 2f-3f self-referencing for fully stabilization and helpful to monolithic integration of the whole system. Further investigations on complex dynamical processes for the microcomb generation suggest that the intracavity soliton drifting caused by the third-order dispersion could be compensated by the self-steepening effect as introducing an additional drift through proper dispersion tailoring. This work could facilitate the low-threshold broadband MIR frequency comb generation technique, as well as provide a way to realize more delicate control of soliton microcombs in both temporal and spectral domain.

Near-infrared frequency comb generation in mid-infrared interband cascade lasers.

The interband cascade laser (ICL) is an ideal candidate for low-power mid-infrared frequency comb spectroscopy. In this work, we demonstrate that its intracavity second-order optical nonlinearity induces a coherent up-conversion of the generated mid-infrared light to the near-infrared through second-harmonic and sum-frequency generation. At 1.8 µm, 10 mW of light at 3.6 µm convert into sub-nanowatt levels of optical power, spread across 30 nm of spectral coverage. The observed linear-to-nonlinear conversion efficiency exceeds ${3\;{\unicode{x00B5} {\rm W/W}}^2}$3µW/W2 in continuous wave operation. We use a dual-band ICL frequency comb source to characterize water vapor absorption in both spectral bands.