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arXiv:2403.05423 · Communications Physics

Fourier-transform infrared spectroscopy with undetected photons from high-gain spontaneous parametric down-conversion

Kazuki Hashimoto, D. B. Horoshko, Mikhail I. Kolobov, Yoad Michael, Ziv Gefen, Maria V. Chekhova

Published Jul 4, 2024• 21 citations
arXivHTMLPDF

Abstract

Abstract Fourier-transform infrared spectroscopy (FTIR) is an indispensable analytical method that allows label-free identification of substances via fundamental molecular vibrations. However, traditional FTIR spectrometers require mid-infrared (MIR) elements, including low-efficiency MIR photodetectors. SU(1,1) interferometry has previously enabled FTIR with undetected MIR photons via spontaneous parametric down-conversion in the low-parametric-gain regime, where the number of photons per mode is much less than one and sensitive photodetectors are needed. In this work, we develop a high-parametric-gain SU(1,1) interferometer for MIR-range FTIR with undetected photons. Using our method, we demonstrate three major advantages: a high photon number at the interferometer output, a considerably lower photon number at the sample, and improved interference contrast. In addition, we broaden the spectral range of the interferometer by aperiodic poling in the gain medium. Exploiting the broadband SU(1,1) interferometer, we measure and evaluate the MIR absorption spectra of polymers in the 3-μm region.

DOI
10.1038/s42005-024-01717-3

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Abstract Nonlinear interferometry with entangled photons allows for characterizing a sample without detecting the photons interacting with it. This method enables highly sensitive optical sensing in the wavelength regions where efficient detectors are still under development. Recently, nonlinear interferometry has been applied to interferometric measurement techniques with broadband light sources, such as Fourier‐transform infrared spectroscopy and infrared optical coherence tomography. However, they have been demonstrated with photon pairs produced through spontaneous parametric down‐conversion (SPDC) at a low parametric gain, where the average number of photons per mode is much smaller than one. The regime of high‐gain SPDC offers several important advantages, such as the amplification of light after its interaction with the sample and a large number of photons per mode at the interferometer output. This work presents broadband spectroscopy and high‐resolution optical coherence tomography with undetected photons generated via high‐gain SPDC in an aperiodically poled lithium niobate crystal. To prove the principle, reflective Fourier‐transform near‐infrared spectroscopy with a spectral bandwidth of 17 THz and optical coherence tomography with an axial resolution of 11 µm are demonstrated.
We develop a high-parametric-gain SU(1,1) interferometer based on an aperiodically poled potassium titanyl phosphate (apKTP) crystal, enabling frequency-domain low-coherence interferometry with undetected mid-infrared photons. The system achieves a signal-to-noise ratio as high as 40 dB and axial resolution of 30 μm, with a 3 μm-centered idler beam. By increasing the poling-period range, we also improve the axial resolution to 17 μm, demonstrating a straightforward route to enhance the performance by working on the crystal design.
Mid-infrared (MIR) spectroscopy serves as a powerful tool for molecular structure identification and chemical composition analysis. However, conventional Fourier-transform infrared spectrometers (FTIR) demonstrate compromised signal-to-noise ratios (SNR) under low-light conditions, which severely limit their performance in high-sensitivity applications. Although MIR superconducting nanowire single-photon detectors (SNSPDs) offer high detection efficiency and low timing jitter, their performance is hindered by background dark counts caused by room-temperature blackbody radiation. In this work, we present a quantum-correlated absorption spectroscopy platform that combines MIR-SNSPDs with entangled photon pairs to overcome these limitations. Leveraging the intrinsic temporal and spectral correlations of the photon pairs, coincidence detection effectively distinguishes signal photons from dominant thermal noise, achieving a remarkable improvement of two orders of magnitude in SNR under ultralow pump power conditions. The system achieves a spectral coverage of 3350-3540 nm with a resolution of 3.7 cm -1 at 3.4 µm, operating at an ultralow illumination photon flux of 4.4 × 10 6 photons/s. Validation experiments using polystyrene and polyethylene samples successfully detected CH 2 vibrational modes, demonstrating the platform’s capability for ultrasensitive biochemical analysis and material characterization. By integrating quantum correlation with MIR-SNSPDs, this work establishes a new paradigm for high-performance MIR spectroscopy in low-light scenarios.