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We use a 3.3 µm high-power continuous wave pump and a 1.67 µm comb probe to detect transitions in the 3ν3 ← ν3 range of methane with sub-Doppler resolution over 6 THz of bandwidth. We achieve high absorption sensitivity for the comb probe using an enhancement cavity and a Fourier transform spectrometer with auto-balanced detection.

Accurate parameters of molecular transitions are needed for data analysis in many applications, ranging from atmospheric research to astrophysics and determination of fundamental constants. Optical frequency comb Fourier transform spectroscopy (OFC-FTS) is particularly well-suited for high-precision measurements of broadband molecular spectra. From these spectra, the parameters of individual transitions - all measured simultaneously under the same experimental conditions - can be determined. We use a mechanical OFC-FTS spectrometer with sub-nominal resolution [1, 2] to perform precise broadband measurements of entire molecular bands of CO2 using either direct absorption spectroscopy or cavity-enhanced complex refractive index spectroscopy (CE-CRIS) [3] and we extract line parameters for line shapes beyond the Voigt profile.

An absorption spectrum of (H2O)-O-16 at 1950 K is recorded in a premixed methane/air flat flame using a cavity-enhanced optical frequency comb-based Fourier transform spectrometer. 2417 absorption lines are identified in the 6250-6670 cm(-1) region with an accuracy of about 0.01 cm(-1). Absolute line intensities are retrieved using temperature and concentration values obtained by tunable diode laser absorption spectroscopy. Line assignments are made using a combination of empirically known energy levels and predictions from the new POKAZATEL variational line list. 2030 of the observed lines are assigned to 2937 transitions, once blends are taken into account. 126 new energy levels of (H2O)-O-16 are identified. The assigned transitions belong to 136 bands and span rotational states up to J = 27.

We present broadband cavity-enhanced complex refractive index spectroscopy (CE-CRIS), a technique for calibration-free determination of the complex refractive index of entire molecular bands via direct measurement of transmission modes of a Fabry-Perot cavity filled with the sample. The measurement of the cavity transmission spectrum is done using an optical frequency comb and a mechanical Fourier transform spectrometer with sub-nominal resolution. Molecular absorption and dispersion spectra (corresponding to the imaginary and real parts of the refractive index) are obtained from the cavity mode broadening and shift retrieved from fits of Lorentzian profiles to the individual cavity modes. This method is calibration-free because the mode broadening and shift are independent of the cavity parameters such as the length and mirror reflectivity. In this first demonstration of broadband CE-CRIS we measure simultaneously the absorption and dispersion spectra of three combination bands of CO2 in the range between 1525 nm and 1620 nm and achieve good agreement with theoretical models. This opens up for precision spectroscopy of the complex refractive index of several molecular bands simultaneously. 

We retrieve high precision absorption and dispersion spectra of the 3v(1)+v(3) band of CO2 from direct measurement of cavity transmission modes using an optical frequency comb and a mechanical Fourier transfolin spectrometer with sub-nominal resolution.

We demonstrate broadband calibration-free complex refractive index spectroscopy of entire molecular bands by direct measurement of transmission modes of a Fabry-Perot cavity using frequency comb-based Fourier transform spectrometer with sub-nominal resolution.

We measure absorption spectra of the CO₂ 3ν₁+ν₃ band at 1.57 μm using optical frequency comb Fourier transform spectroscopy with sub-nominal resolution and retrieve line shape parameters using multiline fitting with the speed-dependent Voigt profile.

We demonstrate a high-temperature water absorption spectrum measured in a flame using cavity-enhanced frequency comb-based Fourier transform spectroscopy. The retrieved transition intensities and frequencies are assigned using the POKAZATEL line list.

Broadband precision spectroscopy is indispensable for providing high fidelity molecular parameters for spectroscopic databases. We have recently shown that mechanical Fourier transform spectrometers based on optical frequency combs can measure broadband high-resolution molecular spectra undistorted by the instrumental line shape (ILS) and with a highly precise frequency scale provided by the comb. The accurate measurement of the power of the comb modes interacting with the molecular sample was achieved by acquiring single-burst interferograms with nominal resolution matched to the comb mode spacing. Here we describe in detail the experimental and numerical steps needed to achieve sub-nominal resolution and retrieve ILS-free molecular spectra, i.e. with ILS-induced distortion below the noise level. We investigate the accuracy of the transition line centers retrieved by fitting to the absorption lines measured using this method. We verify the performance by measuring an ILS-free cavity-enhanced low-pressure spectrum of the 3ν1 + ν3 band of CO2 around 1575 nm with line widths narrower than the nominal resolution. We observe and quantify collisional narrowing of absorption line shape, for the first time with a comb-based spectroscopic technique. Thus retrieval of line shape parameters with accuracy not limited by the Voigt profile is now possible for entire absorption bands acquired simultaneously.

We present optical frequency comb Fourier transform spectroscopy of the entire CO 2 band at 1.57 μm with high enough signal-to-noise ratio to outreach the limit of validity of the Voigt profile.