Mid-infrared molecular spectroscopy in the quantum noise limit

Masaya Arahata, Yu Mukai, Toshiyuki Tashima +2 more

Xiaoqing Zheng, Hui Zhou, Ying Chen +5 more

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.

Morgan W. Mitchell, Vito Giovanni Lucivero, Aleksandra Dimić +2 more

Z. Ficek, R. Tanaś

Yujie Cai, Yu Chen, Xiaoning Xin +2 more

Promoting the sensitivity of mid-infrared (MIR) spectroscopy to the single-photon level is a critical need for investigating photosensitive biological samples and chemical reactions. MIR spectroscopy based on frequency upconversion is a compelling pioneer allowing high-efficiency MIR spectral measurement with well-developed single-photon detectors, which overcomes the main limitations of high thermal noise of current MIR detectors. However, noise from other nonlinear processes caused by strong pump fields hinders the development of the upconversion-based MIR spectroscopy to reach the single-photon level. Here, a broadband MIR single-photon frequency upconversion spectroscopy is demonstrated based on the temporal-spectral quantum correlation of non-degenerate photon pairs, which is well preserved in the frequency upconversion process and is fully used in extracting the signals from tremendous noise caused by the strong pump. A correlation spectrum broader than 660 nm is achieved and applied for the demonstration of sample identification under a low incident photon flux of 0.09 average photons per pulse. The system is featured with non-destructive and robust operation, which makes single-photon-level MIR spectroscopy an appealing option in biochemical applications.

Kōichi Shimoda, Tadao Shimizu