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arXiv:2209.15628 · Physical Review Letters

Quantum-Enhanced Absorption Spectroscopy with Bright Squeezed Frequency Combs

Alexandre Belsley

Published Mar 28, 2023• 25 citations
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Abstract

Absorption spectroscopy is a widely used technique that permits the detection and characterization of gas species at low concentrations. We propose a sensing strategy combining the advantages of frequency modulation spectroscopy with the reduced noise properties accessible by squeezing the probe state. A homodyne detection scheme allows the simultaneous measurement of the absorption at multiple frequencies and is robust against dispersion across the absorption profile. We predict a significant enhancement of the signal-to-noise ratio that scales exponentially with the squeezing factor. An order of magnitude improvement beyond the standard quantum limit is possible with state-of-the-art squeezing levels facilitating high precision gas sensing.

DOI
10.1103/physrevlett.130.133602

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Absorption spectroscopy is a widely used technique that permits the detection and characterization of gas species at low concentrations. We propose a sensing strategy combining the advantages of frequency modulation spectroscopy with the reduced noise properties accessible by squeezing the probe state. A homodyne detection scheme allows the simultaneous measurement of the absorption at multiple frequencies and is robust against dispersion across the absorption profile. We predict a significant enhancement of the signal-to-noise ratio that scales exponentially with the squeezing factor. An order of magnitude improvement beyond the standard quantum limit is possible with state-of-the-art squeezing levels facilitating high precision gas sensing.
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Optical frequency combs have enabled distinct advantages in broadband, high-resolution spectroscopy and precision interferometry. However, quantum mechanics ultimately limits the metrological precision achievable with laser frequency combs. Quantum squeezing has led to substantial measurement improvements with continuous wave lasers, but experiments demonstrating metrological advantage with squeezed combs are less developed. Using the Kerr effect in nonlinear optical fiber, a 1-gigahertz frequency comb centered at 1560 nanometers is amplitude-squeezed by >3 decibels (dB) over a 2.5-terahertz bandwidth. Dual-comb interferometry yields mode-resolved spectroscopy of hydrogen sulfide gas with a signal-to-noise ratio nearly 3 dB beyond the shot-noise limit. The quantum noise reduction leads to a twofold quantum speedup in the determination of gas concentration, with implications for high-speed measurements of multiple species in dynamic chemical environments.
Precision molecular spectroscopy provides a sensitive detection method for ultralight bosonic dark matter. This wavelike dark matter couples to the Standard Model fundamental constants, modulates the frequencies of the molecular transitions and of the resonances of the optical cavities, and brings oscillations in the laser absorption spectroscopy signals. Spectroscopy experiments with differential detection methods approach the fundamental limitation imposed by quantum noise in photodetection. The use of squeezed light in spectroscopy is addressed here to circumvent this limitation. An experimental setup is proposed for the interrogation of an acetylene transition at 1542 nm with a bright squeezed light field and a homodyne detection scheme. This approach enables measurements using the squeezed quadrature, ensures broadband sensitivity, demonstrates robustness to moderate losses, and provides improved constraints for the couplings of the ultralight bosonic dark matter to the Standard Model in the radiofrequency range.
In this article, we present a novel spectroscopy technique that improves the signal-to-shot-noise ratio without the need to increase the laser power. Detrimental effects by technical noise sources are avoided by frequency-modulation techniques (frequency up-shifting). Superimposing the signal on non-classical states of light leads to a reduced quantum noise floor. Our method reveals in a proof-of-concept experiment small signals at Hz to kHz frequencies even below the shot noise limit. Our theoretical calculations fully support our experimental findings. The proposed technique is interesting for applications such as high-precision cavity spectroscopy, e.g., for explosive trace gas detection where the specific gas might set an upper limit for the laser power employed.
Optical frequency combs have emerged as a cornerstone for a wide range of areas, including spectroscopy, ranging, optical clocks, time and frequency transfer, waveform synthesis, and communications. However, quantum-mechanical fluctuations of the optical carrier impose fundamental performance limits on the precision of classical optical frequency combs, particularly in their use for interferometry and spectroscopy. Entanglement, as a quintessential quantum resource, allows for surpassing the fundamental limits of classical systems. Here, we introduce entanglement into the realm of optical frequency combs, formulating entangled dual-comb spectroscopy (EDCS) that surmounts the fundamental limits of classical DCS. EDCS capitalizes on tailored entangled structures across the frequency comb, enabling simultaneous detection of all comb lines below the standard quantum limit of classical DCS. Applying EDCS in gas detection, we achieve a 2.6-dB enhancement in signal-to-noise ratio and a 1.7-fold reduction in integration time over classical DCS, rendering EDCS particularly suited for dynamic chemical and biological sensing, where fast, precise measurements subject to power constraints are required. EDCS opens a new avenue for exploiting quantum frequency combs, underscoring their prospects in a plethora of applications in precision metrology, spectroscopy, and timekeeping.