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Physical Review Applied

Quantum Fourier-Transform Infrared Spectroscopy for Complex Transmittance Measurements

Yu Mukai, Masaya Arahata, Toshiyuki Tashima, Ryo Okamoto, Shigeki Takeuchi

Published Mar 8, 2021• 48 citations
Publisher

Abstract

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.

DOI
10.1103/physrevapplied.15.034019

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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.
Infrared quantum absorption spectroscopy is one of the quantum sensing techniques, by which the infrared optical properties of a sample can be estimated through visible or near infrared photon detection without need for infrared optical source or detector, which has been an obstacle for higher sensitivity and spectrometer miniaturization. However, experimental demonstrations have been limited to wavelengths shorter than 5 µm or in the terahertz region, and have not been realized in the so-called fingerprint region of 1500–500 cm−1 (6.6 to 20 µm), which is commonly used to identify chemical compounds or molecules. Here we report the experimental demonstration of quantum Fourier-transform infrared (QFTIR) spectroscopy in the fingerprint region, by which both absorption and phase spectra (complex spectra) can be obtained from Fourier transformed quantum interferograms obtained with a single pixel visible-light detector. As demonstrations, we obtained the transmittance spectrum of a silicon wafer at around 10 µm (1000 cm−1) and complex transmittance spectrum of a synthetic fluoropolymer sheet, polytetrafluoroethylene, in the wavelength range of 8 to 10.5 µm (1250 to 950 cm−1), where absorption due to stretching modes of C-F bonds is clearly observed. These results open the way for new forms of spectroscopic devices based on quantum technologies.
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.
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.
We demonstrate a new scheme for infrared spectroscopy with visible light sources and detectors. The technique relies on the nonlinear interference of correlated photons, produced via spontaneous parametric down conversion in a nonlinear crystal. Visible and infrared photons are split into two paths and the infrared photons interact with the sample under study. The photons are reflected back to the crystal, resembling a conventional Michelson interferometer. Interference of the visible photons is observed and it is dependent on the phases of all three interacting photons: pump, visible and infrared. The transmission coefficient and the refractive index of the sample in the infrared range can be inferred from the interference pattern of visible photons. The method does not require the use of potentially expensive and inefficient infrared detectors and sources, it can be applied to a broad variety of samples, and it does not require a priori knowledge of sample properties in the visible range.