This paper describes the contents of the 2016 edition of the HITRAN molecular spectroscopic compilation. The new edition replaces the previous HITRAN edition of 2012 and its updates during the intervening years. The HITRAN molecular absorption compilation is composed of five major components: the traditional line-by-line spectroscopic parameters required for high-resolution radiative-transfer codes, infrared absorption cross-sections for molecules not yet amenable to representation in a line-by-line form, collision-induced absorption data, aerosol indices of refraction, and general tables such as partition sums that apply globally to the data. The new HITRAN is greatly extended in terms of accuracy, spectral coverage, additional absorption phenomena, added line-shape formalisms, and validity. Moreover, molecules, isotopologues, and perturbing gases have been added that address the issues of atmospheres beyond the Earth. Of considerable note, experimental IR cross-sections for almost 300 additional molecules important in different areas of atmospheric science have been added to the database. The compilation can be accessed through www.hitran.org. Most of the HITRAN data have now been cast into an underlying relational database structure that offers many advantages over the long-standing sequential text-based structure. The new structure empowers the user in many ways. It enables the incorporation of an extended set of fundamental parameters per transition, sophisticated line-shape formalisms, easy user-defined output formats, and very convenient searching, filtering, and plotting of data. A powerful application programming interface making use of structured query language (SQL) features for higher-level applications of HITRAN is also provided.

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The HITRAN 2008 molecular spectroscopic database

Temporal dissipative solitons are observed in a nonlinear, high-finesse, optical microresonator driven by a continuous-wave laser. This approach enables ultrashort pulses to be generated in spectral regimes lacking broadband laser gain media and saturable absorbers, making it potentially useful for applications in broadband spectroscopy, telecommunications, astronomy and low-phase-noise microwave generation.

Temporal solitons in optical microresonators

The detection and measurement of gas concentrations using the characteristic optical absorption of the gas species is important for both understanding and monitoring a variety of phenomena from industrial processes to environmental change. This study reviews the field, covering several individual gas detection techniques including non-dispersive infrared, spectrophotometry, tunable diode laser spectroscopy and photoacoustic spectroscopy. We present the basis for each technique, recent developments in methods and performance limitations. The technology available to support this field, in terms of key components such as light sources and gas cells, has advanced rapidly in recent years and we discuss these new developments. Finally, we present a performance comparison of different techniques, taking data reported over the preceding decade, and draw conclusions from this benchmarking.

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Optical gas sensing: a review

This paper describes the status circa 2001, of the HITRAN compilation that comprises the public edition available through 2001. The HITRAN compilation consists of several components useful for radiative transfer calculation codes: high-resolution spectroscopic parameters of molecules in the gas phase, absorption cross-sections for molecules with very dense spectral features, aerosol refractive indices, ultraviolet line-by-line parameters and absorption cross-sections, and associated database management software. The line-by-line portion of the database contains spectroscopic parameters for 38 molecules and their isotopologues and isotopomers suitable for calculating atmospheric transmission and radiance properties. Many more molecular species are presented in the infrared cross-section data than in the previous edition, especially the chlorofluorocarbons and their replacement gases. There is now sufficient representation so that quasi-quantitative simulations can be obtained with the standard radiance codes. In addition to the description and justification of new or modified data that have been incorporated since the last edition of HITRAN (1996), future modifications are indicated for cases considered to have a significant impact on remote-sensing experiments. (C) 2003 Elsevier Ltd. All rights reserved.

The HITRAN molecular spectroscopic database: edition of 2000 including updates through 2001

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 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

The sensitivity of molecular fingerprinting is dramatically improved when the absorbing sample is placed in a high-finesse optical cavity, because the effective path length is increased. When the equidistant lines from a laser frequency comb are simultaneously injected into the cavity over a large spectral range, multiple trace gases may be identified1 within a few milliseconds. However, efficient analysis of the light transmitted through the cavity remains challenging. Here, a novel approach—cavity-enhanced, frequency-comb, Fourier-transform spectroscopy—fully overcomes this difficulty and enables measurement of ultrasensitive, broad-bandwidth, high-resolution spectra within a few tens of microseconds without any need for detector arrays, potentially from the terahertz to ultraviolet regions. Within a period of just 18 µs, we recorded the spectra of the ammonia 1.0 µm overtone bands comprising 1,500 spectral elements and spanning 20 nm, with a resolution of 4.5 GHz and a noise equivalent absorption at 1 s averaging of 1 × 10−10 cm−1 Hz−1/2, thus opening a route to time-resolved spectroscopy of rapidly evolving single events. By combining Fourier transform spectroscopy with two frequency-shifted combs and cavity ring-down spectroscopy, scientists demonstrate a powerful new tool for ultrahigh sensitivity spectroscopy. The scheme can measure broadband, high-resolution spectra in tens of microseconds, does not require detector arrays and may allow tuning from terahertz to ultraviolet frequencies.

https://hal.archives-ouvertes.fr/hal-00409826/document

Cavity-enhanced dual-comb spectroscopy

A new multiplex technique of coherent anti-Stokes Raman spectro-imaging with two laser frequency combs is shown to record molecular spectra of broad bandwidth on a microsecond scale.

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Coherent Raman spectro-imaging with laser frequency combs

The spectrum of a laser frequency comb consists of several hundred thousand equally spaced lines over a broad spectral bandwidth. Such frequency combs have revolutionized optical frequency metrology and they now hold much promise for significant advances in a growing number of applications including molecular spectroscopy. Despite an intriguing potential for the measurement of molecular spectra spanning tens of nanometres within tens of microseconds at Doppler-limited resolution, the development of dual-comb spectroscopy is hindered by the demanding stability requirements of the laser combs. Here we overcome this difficulty and experimentally demonstrate a concept of real-time dual-comb spectroscopy, which compensates for laser instabilities by electronic signal processing. It only uses free-running mode-locked lasers without any phase-lock electronics. We record spectra spanning the full bandwidth of near-infrared fibre lasers with Doppler-limited line profiles highly suitable for measurements of concentrations or line intensities. Our new technique of adaptive dual-comb spectroscopy offers a powerful transdisciplinary instrument for analytical sciences.

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Nathalie Picqué

Papers

Mid-infrared frequency combs

Frequency comb spectroscopy

Cavity-enhanced dual-comb spectroscopy

Coherent Raman spectro-imaging with laser frequency combs

Adaptive real-time dual-comb spectroscopy