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

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

Optical frequency combs consist of equally spaced discrete optical frequency components and are essential tools for optical communications and for precision metrology, timing and spectroscopy. To date, wide-spanning combs are most often generated by mode-locked lasers or dispersion-engineered resonators with third-order Kerr nonlinearity. An alternative comb generation method uses electro-optic (EO) phase modulation in a resonator with strong second-order nonlinearity, resulting in combs with excellent stability and controllability. Previous EO combs, however, have been limited to narrow widths by a weak EO interaction strength and a lack of dispersion engineering in free-space systems. In this work, we overcome these limitations by realizing an integrated EO comb generator in a thin-film lithium niobate photonic platform that features a large electro-optic response, ultra-low optical loss and highly co-localized microwave and optical felds, while enabling dispersion engineering. Our measured EO frequency comb spans more than the entire telecommunications L-band (over 900 comb lines spaced at ~ 10 GHz), and we show that future dispersion engineering can enable octave-spanning combs. Furthermore, we demonstrate the high tolerance of our comb generator to modulation frequency detuning, with frequency spacing finely controllable over seven orders of magnitude (10 Hz to 100 MHz), and utilize this feature to generate dual frequency combs in a single resonator. Our results show that integrated EO comb generators, capable of generating wide and stable comb spectra, are a powerful complement to integrated Kerr combs, enabling applications ranging from spectroscopy to optical communications.

Broadband electro-optic frequency comb generation in an integrated microring resonator

Optical frequency combs consist of equally spaced discrete optical frequency components and are essential tools for optical communication, precision metrology, timing and spectroscopy1-9. At present, combs with wide spectra are usually generated by mode-locked lasers10 or dispersion-engineered resonators with third-order Kerr nonlinearity11. An alternative method of comb production uses electro-optic (EO) phase modulation in a resonator with strong second-order nonlinearity, resulting in combs with excellent stability and controllability12-14. Previous EO combs, however, have been limited to narrow widths by a weak EO interaction strength and a lack of dispersion engineering in free-space systems. Here we overcome these limitations by realizing an integrated EO comb generator in a thin-film lithium niobate photonic platform that features a large EO response, ultralow optical loss and highly co-localized microwave and optical fields15, while enabling dispersion engineering. Our measured EO comb spans more frequencies than the entire telecommunications L-band (over 900 comb lines spaced about 10 gigahertz apart), and we show that future dispersion engineering can enable octave-spanning combs. Furthermore, we demonstrate the high tolerance of our comb generator to modulation frequency detuning, with frequency spacing finely controllable over seven orders of magnitude (10 hertz to 100 megahertz), and we use this feature to generate dual-frequency combs in a single resonator. Our results show that integrated EO comb generators are capable of generating wide and stable comb spectra. Their excellent reconfigurability is a powerful complement to integrated Kerr combs, enabling applications ranging from spectroscopy16 to optical communications8.

Broadband electro-optic frequency comb generation in a lithium niobate microring resonator

A topical review of numerical and experimental studies of supercontinuum generation in photonic crystal fiber is presented over the full range of experimentally reported parameters, from the femtosecond to the continuous-wave regime. Results from numerical simulations are used to discuss the temporal and spectral characteristics of the supercontinuum, and to interpret the physics of the underlying spectral broadening processes. Particular attention is given to the case of supercontinuum generation seeded by femtosecond pulses in the anomalous group velocity dispersion regime of photonic crystal fiber, where the processes of soliton fission, stimulated Raman scattering, and dispersive wave generation are reviewed in detail. The corresponding intensity and phase stability properties of the supercontinuum spectra generated under different conditions are also discussed.

Supercontinuum generation, photonic crystal fiber

Scientists propose and experimentally demonstrate a new architecture for dual-comb spectroscopy based on all-fibre tunable frequency comb sources using standard telecommunication fibre optics components, opening the way for practical dual-comb spectroscopy.

Frequency-agile dual-comb spectroscopy

We investigate spectral peculiarities of multilayer system, consisting of two identical CLC layers and
a Rhodamine 6G doped polymethyl metacrylate thin film sandwiched between them. We measure
transmission and reflection spectra of the system. A small mismatch between Selective reflection band and
corresponding dip in transmission spectrum is observed. Also we investigate luminescence spectrum of this
system at pulsed and CW mode pumping at various temperatures. The results show that maximal intensity of
luminescence spectrum at constant pumping power is observed at 18°C and the weakest luminescence is
observed at 20°C, the luminescence spectra at higher and lower temperatures are “confined” between these
two spectral curves.

Tatevik Hovhannisyan

Papers

Frequency-agile dual-comb spectroscopy

Spectral investigation of chiral photonic structure with laser dye-doped isotropic polymer film