This Review discusses the emerging field of mid-infrared frequency comb generation, including technologies based on novel laser gain media, nonlinear frequency conversion and microresonators, as well as the applications of these combs in precision spectroscopy and direct frequency comb spectroscopy. Laser frequency combs are coherent light sources that emit a broad spectrum of discrete, evenly spaced narrow lines whose absolute frequency can be measured to within the accuracy of an atomic clock. Their development in the near-infrared and visible domains has revolutionized frequency metrology while also providing numerous unexpected opportunities in other fields such as astronomy and attosecond science. Researchers are now exploring how to extend frequency comb techniques to the mid-infrared spectral region. Versatile mid-infrared frequency comb generators based on novel laser gain media, nonlinear frequency conversion or microresonators promise to significantly expand the applications of frequency combs. In particular, novel approaches to molecular spectroscopy in the 'fingerprint region', with dramatically improved precision, sensitivity, recording time and/or spectral bandwidth may lead to new discoveries in the various fields relevant to molecular science.

Mid-infrared frequency combs

A broadband, compact, all-electrically driven mid-infrared frequency comb based on a quantum cascade laser widens the scope of application of combs in this frequency range beyond that of sources which depend on a chain of optical components. Optical frequency combs are light sources that produce a comb-like spectrum, with sharp equidistant frequency modes, and have many uses in metrology and spectroscopy applications. The mid-infrared regime is particularly important for molecular fingerprinting, but so far the comb sources in this wavelength regime are bulky and rely on a chain of optical components. For wide practical applications, an electrically injected, compact scheme is desired. Andreas Hugi et al. now demonstrate a mid-infrared frequency comb generator based on a semiconductor device, a continuous-wave quantum cascade laser. Optical frequency combs1 act as rulers in the frequency domain and have opened new avenues in many fields such as fundamental time metrology, spectroscopy and frequency synthesis. In particular, spectroscopy by means of optical frequency combs has surpassed the precision and speed of Fourier spectrometers. Such a spectroscopy technique is especially relevant for the mid-infrared range, where the fundamental rotational–vibrational bands of most light molecules are found2. Most mid-infrared comb sources are based on down-conversion of near-infrared, mode-locked, ultrafast lasers using nonlinear crystals3. Their use in frequency comb spectroscopy applications has resulted in an unequalled combination of spectral coverage, resolution and sensitivity4,5,6,7. Another means of comb generation is pumping an ultrahigh-quality factor microresonator with a continuous-wave laser8,9,10. However, these combs depend on a chain of optical components, which limits their use. Therefore, to widen the spectroscopic applications of such mid-infrared combs, a more direct and compact generation scheme, using electrical injection, is preferable. Here we present a compact, broadband, semiconductor frequency comb generator that operates in the mid-infrared. We demonstrate that the modes of a continuous-wave, free-running, broadband quantum cascade laser11 are phase-locked. Combining mode proliferation based on four-wave mixing with gain provided by the quantum cascade laser leads to a phase relation similar to that of a frequency-modulated laser. The comb centre carrier wavelength is 7 micrometres. We identify a narrow drive current range with intermode beat linewidths narrower than 10 hertz. We find comb bandwidths of 4.4 per cent with an intermode stability of less than or equal to 200 hertz. The intermode beat can be varied over a frequency range of 65 kilohertz by radio-frequency injection. The large gain bandwidth and independent control over the carrier frequency offset and the mode spacing open the way to broadband, compact, all-solid-state mid-infrared spectrometers.

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Mid-infrared frequency comb based on a quantum cascade laser

Applying metamaterial concepts to dielectric systems offers low losses compared with metallic structures. Here, silicon-based metamaterial and nanophotonic advances are reviewed. The prospect of creating metamaterials with optical properties greatly exceeding the parameter space accessible with natural materials has been inspiring intense research efforts in nanophotonics for more than a decade. Following an era of plasmonic metamaterials, low-loss dielectric nanostructures have recently moved into the focus of metamaterial-related research. This development was mainly triggered by the experimental observation of electric and magnetic multipolar Mie-type resonances in high-refractive-index dielectric nanoparticles. Silicon in particular has emerged as a popular material choice, due to not only its high refractive index and very low absorption losses in the telecom spectral range, but also its paramount technological relevance. This Review overviews recent progress on metamaterial-inspired silicon nanostructures, including Mie-resonant and off-resonant regimes.

Metamaterial-inspired silicon nanophotonics

Dual-comb spectroscopy performed in the mid-infrared-where molecules have their strongest rotovibrational absorption lines-offers the promise of high spectral resolution broadband spectroscopy with very short acquisition times (μs) and no moving parts. Recently, we demonstrated frequency comb operation of a quantum-cascade-laser. We now use that device in a compact, dual-comb spectrometer. The noise properties of the heterodyne beat are close to the shot noise limit. Broadband (15 cm(-1)) high-resolution (80 MHz) absorption spectroscopy of both a GaAs etalon and water vapour is demonstrated, showing the potential of quantum-cascade-laser frequency combs as the basis for a compact, all solid-state, broadband chemical sensor.

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Dual-comb spectroscopy based on quantum-cascade-laser frequency combs

Frequency combs based on terahertz quantum cascade lasers, which combine the high power of lasers with the broadband capabilities of pulsed sources, are demonstrated. The frequency combs generate 5 mW of terahertz power covering a frequency range of almost 500 GHz and produce more than 70 lines at 3.5 THz.

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Terahertz laser frequency combs

In this study, we report the unequivocal demonstration of midinfrared mode-locked pulses from quantum cascade lasers. The train of short pulses was generated by actively modulating the current and hence the gain of an edge-emitting quantum cascade laser (QCL). Pulses with duration of about 3 ps at full-width-at-half-maxima and energy of 0.5 pJ were characterized using a second-order interferometric autocorrelation technique based on a nonlinear quantum well infrared photodetector. The mode-locking dynamics in the QCLs was modeled based on the Maxwell-Bloch equations in an open two-level system. Our model reproduces the overall shape of the measured autocorrelation traces and predicts that the short pulses are accompanied by substantial wings as a result of strong spatial hole burning. The range of parameters where short mode-locked pulses can be formed is found.

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Mode-locked pulses from mid-infrared quantum cascade lasers.

We show that nonlinear phase shifts and third-order dispersion can compensate each other in short-pulse fiber amplifiers. This compen-sation can be exploited in any implementation of chirped-pulse amplification, with stretching and compression accomplished with diffraction gratings, single-mode fiber, microstructure fiber, fiber Bragg gratings, etc. In particular, we consider chirped-pulse fiber amplifiers at wavelengths for which the fiber dispersion is normal. The nonlinear phase shift accumulated in the amplifier can be compensated by the third-order dispersion of the combination of a fiber stretcher and grating compressor. A numerical model is used to predict the compensation, and experimental results that exhibit the main features of the calculations are presented. In the presence of third-order dispersion, an optimal nonlinear phase shift reduces the pulse duration, and enhances the peak power and pulse contrast compared to the pulse produced in linear propagation. Contrary to common belief, fiber stretchers can perform as well or better than grating stretchers in fiber amplifiers, while offering the major practical advantages of a waveguide medium.

Compensation of nonlinear phase shifts with third-order dispersion in short-pulse fiber amplifiers

We report the unequivocal demonstration of mid-infrared mode-locked pulses from a semiconductor laser. The train of short pulses was generated by actively modulating the current and hence the optical gain in a small section of an edge-emitting quantum cascade laser (QCL). Pulses with pulse duration at full-width-at-half-maximum of about 3 ps and energy of 0.5 pJ were characterized using a second-order interferometric autocorrelation technique based on a nonlinear quantum well infrared photodetector. The mode-locking dynamics in the QCLs was modelled and simulated based on Maxwell-Bloch equations in an open two-level system. We anticipate our results to be a significant step toward a compact, electrically-pumped source generating ultrashort light pulses in the mid-infrared and terahertz spectral ranges.

Stable mode-locked pulses from mid-infrared semiconductor lasers

By optimizing the cavity dispersion map, 1.5-nJ, 36-fs pulses are obtained from a Yb-doped fiber laser. Higher-order dispersion currently limits the pulse duration.

Generation of 36-femtosecond pulses from a ytterbium fiber laser

By optimizing the cavity dispersion map, 1.5-nJ pulses as short as 36 fs are obtained from a Yb-doped fiber laser. Residual higher-order dispersion currently limits the pulse duration, and it should be possible to generate pulses as short as 25–30 fs with Yb-doped fiber.

Lyuba Kuznetsova

Papers

Mode-locked pulses from mid-infrared quantum cascade lasers.

Compensation of nonlinear phase shifts with third-order dispersion in short-pulse fiber amplifiers

Stable mode-locked pulses from mid-infrared semiconductor lasers

Generation of 36-femtosecond pulses from a ytterbium fiber laser

Generation of 36-femtosecond pulses from a ytterbium fiber laser