Ultrasensitive spectroscopy is an essential component in mid-infrared (MIR) technology. However, the drawbacks of MIR detectors pose challenges to robust MIR spectroscopy at the single-photon level. We propose an MIR single-photon frequency upconversion spectroscopy nonlocally mapping the MIR information to the time domain. Broadband MIR photons from spontaneous parametric downconversion are frequency-upconverted to the near-infrared band with quantum correlation preservation. Via the group delay of fiber, the MIR spectral information within a 1.18-micrometer bandwidth of 2.76 to 3.94 micrometers is then successfully projected to arrival times of correlated photon pairs. Under the conditions of 6.4 × 10 6 photons per second illumination, the transmission spectra of polymers with single-photon sensitivity are demonstrated using single-pixel detectors. The developed approach circumvents scanning and frequency selection instability, which stands out for its inherent compatibility for evolving environments and scalability for various wavelengths. Because of its high sensitivity and robustness, characterization of biochemical samples and weak measurement of quantum systems are possible to foresee.
Ultrasensitive spectroscopy is an essential component in mid-infrared (MIR) technology. However, the drawbacks of MIR detectors pose challenges to robust MIR spectroscopy at the single-photon level. We propose an MIR single-photon frequency upconversion spectroscopy nonlocally mapping the MIR information to the time domain. Broadband MIR photons from spontaneous parametric downconversion are frequency-upconverted to the near-infrared band with quantum correlation preservation. Via the group delay of fiber, the MIR spectral information within a 1.18-micrometer bandwidth of 2.76 to 3.94 micrometers is then successfully projected to arrival times of correlated photon pairs. Under the conditions of 6.4 × 10 6 photons per second illumination, the transmission spectra of polymers with single-photon sensitivity are demonstrated using single-pixel detectors. The developed approach circumvents scanning and frequency selection instability, which stands out for its inherent compatibility for evolving environments and scalability for various wavelengths. Because of its high sensitivity and robustness, characterization of biochemical samples and weak measurement of quantum systems are possible to foresee.
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.
Mid-infrared (MIR) detection remains challenging due to limited detector sensitivity and strong background noise. Frequency up-conversion enables MIR detection with visible-range detectors but suffers from limited robustness and additional noise generated in the nonlinear process. We demonstrate a quantum-enhanced MIR frequency up-conversion detection system that generates strongly non-degenerate, time-correlated photon pairs via spontaneous parametric down-conversion and detects MIR photons under severe loss and noise. With a 62 dB transmission loss and background noise 28 times higher than the detected signal, the quantum signal-to-noise ratio substantially surpasses that of classical photon counting. The system achieves stable signal retrieval under unpredictable noise fluctuations, highlighting its robustness in dynamically varying environments. These results establish a basis for practical sensing and imaging applications of quantum-enhanced MIR detection.
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.
Mid-infrared (MIR) imaging plays a pivotal role in chemical sensing, biomedicine, and material analysis, yet its further development is fundamentally constrained by limited room-temperature sensitivity and the lack of efficient multidimensional light-field control. In recent years, frequency upconversion imaging has emerged as a rapidly advancing approach that translates MIR signals to the visible or near-infrared domain, enabling high-sensitivity detection with mature, low-noise photonic platforms. More importantly, by engineering the pump field in nonlinear frequency conversion processes, a multidimensional imaging framework has been established, enabling indirect, all-optical encoding and retrieval of multiple degrees of freedom—including amplitude, phase, spectrum, time, and polarization—of MIR light fields. This paradigm shifts complex light-field manipulation from the MIR to technologically mature short-wavelength regimes, overcoming intrinsic limitations of conventional approaches. In this review, we systematically summarize the principles, architectures, and representative methodologies of MIR upconversion multidimensional imaging, and outline future directions toward high-sensitivity, high-dimensional, and integrated imaging systems, with implications extending to broader photonic and information processing domains.
We report an experimental demonstration of wavelength variable generation and detection of photon pairs in the visible and mid-infrared (MIR) regions over a wide spectral range of 2–5 µm via spontaneous parametric downconversion. Despite the recent increase in interest in such a photon-pair source, there have been few detailed evaluations of emitted photons generated via the downconversion process in the low gain regime, due to the lack of suitable single-photon detectors. By changing the angle of the nonlinear crystal, we continuously tune the phase-matching condition and generate photon pairs as signal photons in the wavelength range of 600–965 nm and idler photons in the wavelength range of 1186–4694 nm. We evaluate the generated photon pairs using single and coincidence counts by superconducting nanowire single-photon detectors up to a wavelength of 2 µm and detect the intensity using an InSb detector with a lock-in detection system up to 5 µm. From this analysis, a pair generation rate of 10 5 s − 1 per mW of pump power is experimentally obtained for this wavelength range. This work provides a basis for the realization of applications such as heralded MIR single-photon sources, infrared imaging, and infrared spectroscopy based on quantum technologies in the MIR region.
Plasmonic nanostructures offer a prominent foundation for plasmon sensing owing to their capacity to confine light within nanoscale regions and enhance the intensity of the local electromagnetic field. Nevertheless, the development of plasmonic sensors that operate in the midinfrared (MIR) region still presents a notable obstacle, primarily due to the limited detection sensitivity of commercial MIR detectors. To break this bottleneck, we demonstrate the characterization of the plasmonic nanostructures' MIR spectral response using a time-stretched quantum spectroscopy with frequency upconversion. Quantum spectroscopy of correlated photon pairs offers a novel approach to overcome the limitations associated with the detection sensitivity of localized surface plasmon resonances (LSPRs), particularly under conditions of excessive noise. This scheme not only extends the application of quantum spectroscopy for the plasmonic nanostructures to the MIR regions, but also circumvents the necessity of employing various types of MIR detectors. In addition, by wavelength-to-time mapping and using a single-pixel detector to obtain the MIR spectral response of a plasmonic sample, nonlocal time stretching significantly increases system stability and efficiently reduces the measurement time under a low-light-level illumination. With an integration time of 600 s, time-stretched quantum spectroscopy demonstrates a detection sensitivity of 0.22 photons per pulse. The outcomes of our research pave the way for the realization of enhanced detection sensitivity in the investigation of plasmonic nanostructures in the MIR range.