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.
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.
In this work, we investigate the application of intermodal spontaneous four wave mixing (SFWM) to ghost spectroscopy in the mid-infrared (MIR) spectral region. This technique is of great interest for MIR sensing, being able to overcome the limitations faced by MIR detectors in terms of background noise and dark counts. Through intermodal SFWM in a Silicon-On-Insulator (SOI) waveguide, two temporally correlated photons are generated: using a standard C-band pump, the idler photon is in the near-infrared (NIR) and the signal photon is in the MIR. The integrated source, with a coincidence to accidental ratio (CAR) of 114 ± 4, is used to demonstrate that, in situations of environmental noise, ghost spectroscopy yields advantages with respect to the traditional absorption spectroscopy. The time-energy entanglement of the photon pairs is used to enhance the visibility of the measurement against noisy background conditions and to increase the spectral resolution in the MIR by spectral filtering the NIR photons. Modeling and experimental data support these improvements.
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.
The emissions of two identical spontaneous parametric down-conversion (SPDC) sources pumped coherently, e.g. with the same beam (c.f. Fig. 1(a)), show interference in both, the signal and idler light. This phenomenon results from the indistinguishability of the photon pairs emitted by the identical sources [1]. If a medium between the two SPDC sources absorbs the idler light, the photon pairs from the first and second SPDC source become distinguishable and the interference contrast decreases for both, signal and idler light. By measuring the signal light spectrum in the visible or near-infrared (NIR) range and the corresponding interference contrast, we obtain the information about the idler light absorption of the analyte in the mid-infrared (MIR). Hereby, we enable spectroscopy in the MIR using a standard silicon detector, making detection easier and more efficient than using typical MIR detectors [2].
We introduce an ultrafast, bright, entangled twin-beam source generated by type-0 parametric down-conversion in periodically-poled lithium niobate at MHz repetition rate, with continuously tunable Schmidt number K set by the pump pulse duration. Photon-number statistics characterization via g(2)(0) and singular-value decomposition of the signal spectral density matrix yield K≃1.05 and K≃1.03, respectively, maintained over multiple orders of magnitude in brightness. Group-delay dispersion of the pump drives a continuous transition from single-mode operation to a controlled multimode regime, consistent with the temporal gain window departing from the inverse phase-matching bandwidth. Strong non-degeneracy of the source (signal at 1.37 um, idler at 4.0 um, ∼100 fs duration) decouples a mid-infrared interaction wavelength, which overlaps with molecular vibrational resonances, from a near-infrared detection band, establishing a practical platform for quantum-enhanced metrology, nonlinear interferometry, and mid-infrared spectroscopic sensing. We show that in the bright few-mode limit, the total entanglement resource is clearly separated between modal and occupational degrees of freedom, and that our source allocates up to 95-97% of that resource to the occupational sector.
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.
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.