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Optical and Quantum Sensing and Precision Metrology II

High resolution Fourier-transform mid-infrared spectroscopy using nonlinear interferometers

Jachin Kunz, Chiara Lindner, Simon J. Herr, Sebastian Wolf, Jens Kießling, Frank Kühnemann

Published Mar 8, 2023• 1 citation
Publisher

Abstract

Nonlinear interferometers based on correlated photon pairs allow mid-infrared spectroscopy by measuring only near-infrared photons with a silicon-based detector, which offers higher detectivities than mid-infrared detectors. Here, we use the nonlinear interferometer not only to determine the transmission of a sample but also for spectral analysis - analogue to classical Fourier transform infrared (FTIR) spectrometers. The Quantum FTIR analyzes the absorption of gas mixtures with high spectral resolution over a broad mid-infrared wavelength range. Improved emission rates of the photon pair source yield sensitivities similar to a classical FTIR despite an extremely low light exposure on the sample.

DOI
10.1117/12.2650157

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Nonlinear interferometers based on correlated photon pairs allow mid-infrared spectroscopy by measuring only near-infrared photons with a silicon-based detector, which offers higher detectivities than mid-infrared detectors. Here, we use the nonlinear interferometer not only to determine the transmission of a sample but also for spectral analysis - analogue to classical Fourier transform infrared (FTIR) spectrometers. The Quantum FTIR analyzes the absorption of gas mixtures with high spectral resolution over a broad mid-infrared wavelength range. Improved emission rates of the photon pair source yield sensitivities similar to a classical FTIR despite an extremely low light exposure on the sample.
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.
Harnessing the quantum interference of the pair generation processes, infrared quantum spectroscopy, based on nonlinear interferometers with visible-infrared photon-pair sources, enables the extraction of the infrared optical properties of a sample through visible photon detection without the need for an infrared optical source or detector. We develop a theoretical framework for quantum Fourier-transform infrared (QFTIR) spectroscopy. The proposed Fourier analysis method, which fully utilizes the phase information in the interferogram, allows us to determine the complex transmittance and optical constants for a sample in a simple setup without the use of any dispersive optics for spectral selection. In the experimental demonstrations, the transmittance spectrum of a bandpass filter and the refractive index of silica glass are measured in the near-infrared region using QFTIR operated in a low gain regime; these results agree well with the independently measured spectrum using a conventional spectrometer and an value estimated from references. These demonstrations prove the validity and great potential of QFTIR spectroscopy.
In recent years, nonlinear quantum interferometry has been widely explored for applications like spectroscopy, optical coherence tomography, and imaging [1]. Quantum infrared spectroscopy (QIRS) uses quantum interference of generation processes of frequency-entangled visible-IR photon pairs to perform infrared spectroscopy using visible light sources and silicon-based detectors [2]. This technique utilizes a nonlinear quantum interferometer configuration where the generated IR photons pass through the sample, and the correlated visible photons are detected. The change in the detected visible photon flux with and without the sample helps extract the complex transmittance of the sample in the IR region.
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In recent years, quantum Fourier transform infrared (QFTIR) spectroscopy has emerged as an alternative to conventional absorption spectroscopy in the mid-infrared region of the spectrum. By harnessing induced coherence and spectral correlations of photon pairs in a nonlinear Michelson interferometer, this technique offers promising potential for the practical detection of organic gases. However, little research was conducted to bring QFTIR spectrometers closer to domestic or in-field usage. In this work, we present the first use of a QFTIR spectrometer for open-path detection of multiple interfering organic gases in ambient air. We built a nonlinear Michelson interferometer with 1.7 m-long arms to increase the absorption length, coupled with analysis techniques from classical differential absorption spectroscopy used for gas-traces detection. We thus characterize our spectrometer’s sensitivity to acetone, methanol, and ethanol vapors and demonstrate the accurate identification of mixtures of these gases released in ambient air. We show this characteristic is preserved over time by performing a measurement overnight and tracking the evolution of different gases’ average concentrations. These results constitute the first use-case of a QFTIR spectrometer as a detector of organic gases and, thus, represent an important milestone toward the development of such detectors in practical situations.