There is, I think, something ethereal about i —the square root of minus one. I remember first hearing about it at school. It seemed an odd beast at that time—an intruder hovering on the edge of reality.

Usually familiarity dulls this sense of the bizarre, but in the case of i it was the reverse: over the years the sense of its surreal nature intensified. It seemed that it was impossible to write mathematics that described the real world in …

I and i

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

Dual-comb spectroscopy is an emerging new spectroscopic tool that exploits the frequency resolution, frequency accuracy, broad bandwidth, and brightness of frequency combs for ultrahigh-resolution, high-sensitivity broadband spectroscopy. By using two coherent frequency combs, dual-comb spectroscopy allows a sample’s spectral response to be measured on a comb tooth-by-tooth basis rapidly and without the size constraints or instrument response limitations of conventional spectrometers. This review describes dual-comb spectroscopy and summarizes the current state of the art. As frequency comb technology progresses, dual-comb spectroscopy will continue to mature and could surpass conventional broadband spectroscopy for a wide range of laboratory and field applications.

Dual-comb spectroscopy

Ultrafast fibre lasers are an important optical system with industrial, medical and purely scientific applications. Essential components and the operation regimes of ultrafast fibre laser systems are reviewed, as are their use in various applications.

Ultrafast fibre lasers

A laser frequency comb is a broad spectrum composed of equidistant narrow lines. Initially invented for frequency metrology, such combs enable new approaches to spectroscopy over broad spectral bandwidths, of particular relevance to molecules. The performance of existing spectrometers — such as crossed dispersers employing, for example, virtual imaging phase array etalons, or Michelson-based Fourier transform interferometers — can be dramatically enhanced with optical frequency combs. A new class of instruments, such as dual-comb spectrometers without moving parts, enables fast and accurate measurements over broad spectral ranges. The direct self-calibration of the frequency scale of the spectra within the accuracy of an atomic clock and the negligible contribution of the instrumental line-shape will enable determinations of all spectral parameters with high accuracy for stringent comparisons with theories in atomic and molecular physics. Chip-scale frequency comb spectrometers promise integrated devices for real-time sensing in analytical chemistry and biomedicine. This Review gives a summary of the developments in the emerging and rapidly advancing field of atomic and molecular broadband spectroscopy with frequency combs. Frequency comb spectroscopy is a recent field of research that has blossomed in the past five years. This Review discusses developments in the emerging and rapidly advancing field of atomic and molecular broadband spectroscopy with frequency combs.

Frequency comb spectroscopy

We report on the generation of mid-infrared (mid-IR) pulses with a maximum average optical power of 4 mW and wide tunability in the 8–14 μm range via difference frequency generation (DFG) in GaSe from an Er:fiber laser oscillator. The DFG process is seeded with self-frequency shifted Raman solitons that are shown to be phase coherent within the whole tuning range, from 1.76 to 1.93 μm. Interference measurements between adjacent pulses at the idler wavelengths attest coherence transfer to the mid-IR.

Milliwatt-level frequency combs in the 8–14 μm range via difference frequency generation from an Er:fiber oscillator

We demonstrate passive mode-locking by means of a semiconductor saturable-absorber mirror in a diode-pumped Yb:YLF laser. We present crystal growth process, spectroscopic measurements, and investigation of mode-locking performance. Pulse trains with minimum duration of 196 fs, average power of 54 mW and a repetition rate of 55 MHz were obtained. The optical spectrum, centered at 1028 nm, has a 7.1-nm bandwidth leading to nearly transform-limited pulses.

Diode-pumped passively mode-locked Yb:YLF laser.

Room-temperature continuous-wave laser action in a novel Tm-doped LiLuF(4) crystal emitting at around 1.9 microm is demonstrated. The crystal growth process, spectroscopic measurements, and laser performance are presented for different Tm concentrations. An overall tunability extending from 1817 to 2056 nm, a slope efficiency of 46%, and a maximum output power in excess of 1.1 W are reported.

Tm-doped LiLuF 4 crystal for efficient laser action in the wavelength range from 1.82 to 2.06 μm

Modeling a real laser diode stack based on Zemax ray tracing software that operates in a nonsequential mode is reported. The implementation of the model is presented together with the geometric and optical parameters to be adjusted to calibrate the model and to match the simulated intensity irradiance profiles with the experimental profiles. The calibration of the model is based on a near-field and a far-field measurement. The validation of the model has been accomplished by comparing the simulated and experimental transverse irradiance profiles at different positions along the caustic formed by a lens. Spot sizes and waist location are predicted with a maximum error below 6%.

Nonsequential modeling of laser diode stacks using Zemax: simulation, optimization, and experimental validation.

An ideal optical frequency-comb system should combine both single-line spectral resolution and a bandwidth broad enough to cover as many lines as possible. Here, the authors incorporate a fibre spectrometer to detect approximately 500 comb-lines with an instrument resolution of 120 megahertz.

Nicola Coluccelli

Papers

Milliwatt-level frequency combs in the 8–14 μm range via difference frequency generation from an Er:fiber oscillator

Diode-pumped passively mode-locked Yb:YLF laser.

Tm-doped LiLuF 4 crystal for efficient laser action in the wavelength range from 1.82 to 2.06 μm

Nonsequential modeling of laser diode stacks using Zemax: simulation, optimization, and experimental validation.

The optical frequency comb fibre spectrometer.