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Recent years have seen the development of quantum sensing concepts utilizing nonlinear interferometers based on correlated photon pairs generated by spontaneous parametric down-conversion (SPDC). Using SPDC far from frequency degeneracy allows a 'division of labor' between the mid-infrared photon for strongest sample interaction and the correlated near-infrared photon for low-noise detection. The small number of photons provided by SPDC and the resulting inferior signal-to-noise ratio are, however, a limiting factor preventing wide applicability of the novel sensing concept. Here, we demonstrate a nonlinear interferometer based on pump-enhanced SPDC with strongly improved emission rates, but maintaining broadband, spontaneous emission. For validation of the concept, we demonstrate high-resolution mid-infrared spectroscopy with near-infrared detection, showcasing the improved accuracy. Although the number of mid-infrared photons is about five orders of magnitude smaller than in classical spectrometers, the sensitivity of the quantum spectrometer becomes comparable, marking an essential step toward real-world applications.

Nonlinear interferometers allow for mid-infrared spectroscopy with near-infrared detection using correlated photons. Previous implementations have demonstrated a spectral resolution limited by spectrally selective detection. In our work, we demonstrate mid-infrared transmission spectroscopy in a nonlinear interferometer using single-pixel near-infrared detection and Fourier-transform analysis. A sub-wavenumber spectral resolution allows for rotational-line-resolving spectroscopy of gaseous samples in a spectral bandwidth of over 700$\,$cm$^{-1}$. We use methane transmission spectra around 3.3$\,\mu$m wavelength to characterize the spectral resolution, noise limitations and transmission accuracy of our device. The combination of nonlinear interferometry and Fourier-transform analysis paves the way towards performant and efficient mid-infrared spectroscopy with near-infrared detection., Comment: \copyright 2021 Optical Society of America. Users may use, reuse, and build upon the article, or use the article for text or data mining, so long as such uses are for non-commercial purposes and appropriate attribution is maintained. All other rights are reserved

Nonlinear interferometers allow spectroscopy in the mid-infrared range by detecting correlated visible light, for which non-cooled detectors with higher specific detectivity and lower dark count rates are available. We present a new approach for the registration of spectral information, which combines a nonlinear interferometer using non-degenerate spontaneous parametric down-conversion (SPDC) with a Fourier-transform spectroscopy concept. In order to increase the spectral coverage, we use broadband non-collinear SPDC in periodically poled LiNbO$_3$. Without the need for spectrally selective detection, continuous spectra with a spectral bandwidth of more than 100$\,$cm$^{-1}$ are achieved. We demonstrate transmission spectra of a polypropylene sample measured with ~ 6$\,$cm$^{-1}$ resolution in the spectral range between 3.2$\,\mu$m to 3.9$\,\mu$m.