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-lineresolving spectroscopy of gaseous samples in a spectral bandwidth of over 700 cm −1 . We use methane transmission spectra around 3.3 µm 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.

We present dispersive Fourier-transform spectroscopy with undetected photons using a nonlinear interferometer based on spontaneous parametric down-conversion. The interferometer transfers mid-infrared information of sample interaction to the near-infrared, which allows using low-noise silicon-based detectors, enabling accurate measurements with extremely low light exposure. We demonstrate a dispersion measurement of gaseous methane with an accuracy greater than 1 part in 106, which is limited by random phase noise. The Fourier-transform approach allows high resolution, rotational-line resolving spectroscopy of both, the absorptive and dispersive properties of a sample in a simple and robust measurement concept.

Nonlinear interferometers based on non-degenerate spontaneous parametric down-conversion (SPDC) create a link between separate spectral ranges. This allows for measurements in remote spectral regions while detecting light in easily accessible wavelengths. In our work, we use periodically poled lithium niobate to create correlated signal (visible or near-infrared) and idler (mid-infrared) photon pairs. Using a nonlinear interferometer in Michelson geometry, we obtain broadband mid-infrared spectra from light detected with a silicon avalanche photodiode. Combining the nonlinear interferometer with a measurement scheme in close analogy to classical Fourier-transform infrared spectroscopy allows for sub-wavenumber spectral resolution, which opens up possibilities for applications such as precise spectroscopic gas analysis.

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 the 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 the wide applicability of the novel sensing concept. Here, we demonstrate a nonlinear interferometer based on pump-enhanced SPDC with strongly improved emission rates while maintaining broadband spontaneous emission. For validation of the concept, we demonstrate high-resolution mid-infrared spectroscopy with near-infrared detection, showcasing 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 using correlated photon pairs allow mid-infrared spectroscopy with near-infrared detection. In our work, we combine nonlinear interferom- etry with a measurement scheme and analysis in analogy to classical Fourier-transform spectroscopy, which enhances the spectroscopic performance.