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Nonlinear Frequency Generation and Conversion: Materials and Devices

Mid-infrared coincidence measurements based on intracavity frequency conversion

Sara Piccione, Mattia Mancinelli, Alessandro Trenti, Giorgio Fontana, Peter Tidemand‐Lichtenberg, Christian Pedersen, Jeppe Seidelin Dam, Lorenzo Pavesi

Published Feb 15, 2018• 1 citation
Publisher

Abstract

In the last years, the Mid Infrared (MIR) spectral region has attracted the attention of many areas of science and technology, opening the way to important applications, such as molecular imaging, remote sensing, free- space communication and environmental monitoring. However, the development of new sources of light, such as quantum cascade laser, was not followed by an adequate improvement in the MIR detection system, able to exceed the current challenges. Here we demonstrate the single-photon counting capability of a new detection system, based on efficient up-converter modules, by proving the correlated nature of twin photons pairs at about 3.1μm, opening the way to the extension of quantum optics experiments in the MIR.

DOI
10.1117/12.2305713

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In the last years, the Mid Infrared (MIR) spectral region has attracted the attention of many areas of science and technology, opening the way to important applications, such as molecular imaging, remote sensing, free- space communication and environmental monitoring. However, the development of new sources of light, such as quantum cascade laser, was not followed by an adequate improvement in the MIR detection system, able to exceed the current challenges. Here we demonstrate the single-photon counting capability of a new detection system, based on efficient up-converter modules, by proving the correlated nature of twin photons pairs at about 3.1μm, opening the way to the extension of quantum optics experiments in the MIR.
Quantum measurements using single-photon detectors are opening interesting new perspectives in diverse fields such as remote sensing, quantum cryptography and quantum computing. A particularly demanding class of applications relies on the simultaneous detection of correlated single photons. In the visible and near infrared wavelength ranges suitable single-photon detectors do exist. However, low detector quantum efficiency or excessive noise has hampered their mid-infrared (MIR) counterpart. Fast and highly efficient single-photon detectors are thus highly sought after for MIR applications. Here we pave the way to quantum measurements in the MIR by the demonstration of a room temperature coincidence measurement with non-degenerate twin photons at about 3.1 μm. The experiment is based on the spectral translation of MIR radiation into the visible region, by means of efficient up-converter modules. The up-converted pairs are then detected with low-noise silicon avalanche photodiodes without the need for cryogenic cooling.
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) 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.
Frequency-correlated light offers a route to mid-infrared (MIR) spectroscopy without direct spectral detection in the MIR. Previous MIR ghost spectroscopy has mainly relied on low-gain spontaneous parametric down-conversion (SPDC) and photon-pair coincidence measurements, where the limited photon flux has restricted acquisition times to longer than one minute. Here, we demonstrate ghost infrared spectroscopy using bright twin beams generated by high-gain parametric down-conversion (PDC). High-gain PDC amplifies vacuum fluctuations, producing a different pair of frequency-correlated random spectra in each pump pulse. This pulse-resolved stochastic emission is naturally matched to time-stretch detection, which records the spectrum of the correlated near-infrared telecom signal for every pulse, while the MIR idler is measured by bucket detection. Consequently, each pump pulse yields one paired projection measurement comprising a spectrally resolved reference and the corresponding bucket value. We reconstruct the transmission spectrum of a structured optical filter and the molecular vibrational absorption spectrum of liquid benzene near 3.3 um with millisecond-scale acquisition, in good agreement with Fourier-transform infrared spectroscopy. This reduces the acquisition time by four to five orders of magnitude compared with previous MIR ghost spectroscopy demonstrations. These results transform ghost spectroscopy from coincidence-based photon counting to high-flux analog correlation spectroscopy, establishing a practical architecture for high-speed computational infrared spectroscopy driven by a narrowband semiconductor laser.
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.
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.