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arXiv:1508.00849 · New Journal of Physics

Absorption spectroscopy at the ultimate quantum limit from single-photon states

Rebecca Whittaker, Chris Erven, Alex Neville, M Berry, Jeremy L. O’Brien, Hugo V. Cable, Jonathan C. F. Matthews

Published Dec 21, 2016• 93 citations
arXivHTMLPDF

Abstract

Absorption spectroscopy is routinely used to characterise chemical and biological samples. For the state-of-the-art in laser absorption spectroscopy, precision is theoretically limited by shot-noise due to the fundamental Poisson-distribution of photon number in laser radiation. In practice, the shot-noise limit can only be achieved when all other sources of noise are eliminated. Here, we use wavelength-correlated and tuneable photon pairs to demonstrate how absorption spectroscopy can be performed with precision beyond the shot-noise limit and near the ultimate quantum limit by using the optimal probe for absorption measurement—single photons. We present a practically realisable scheme, which we characterise both the precision and accuracy of by measuring the response of a control feature. We demonstrate that the technique can successfully probe liquid samples and using two spectrally similar types of haemoglobin we show that obtaining a given precision in resolution requires fewer heralded single probe photons compared to using an idealised laser.

DOI
10.1088/1367-2630/aa5512

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Absorption spectroscopy is routinely used to characterise chemical and biological samples. For the state-of-the-art in laser absorption spectroscopy, precision is theoretically limited by shot-noise due to the fundamental Poisson-distribution of photon number in laser radiation. In practice, the shot-noise limit can only be achieved when all other sources of noise are eliminated. Here, we use wavelength-correlated and tuneable photon pairs to demonstrate how absorption spectroscopy can be performed with precision beyond the shot-noise limit and near the ultimate quantum limit by using the optimal probe for absorption measurement—single photons. We present a practically realisable scheme, which we characterise both the precision and accuracy of by measuring the response of a control feature. We demonstrate that the technique can successfully probe liquid samples and using two spectrally similar types of haemoglobin we show that obtaining a given precision in resolution requires fewer heralded single probe photons compared to using an idealised laser.
Absorption measurements are routinely used in science and engineering, it is an exceptionally versatile tool for most applications. For absorption measurements using laser beams of light, the sensitivity is theoretically limited by the shot noise due to the fundamental Poisson distribution of photon number in laser radiation. In practice, the shot-noise limit can only be achieved when all other sources of noise are eliminated. Here, we use bright squeezed light to demonstrate direct absorption measurement can be performed with sensitivity beyond the shot-noise limit. We present a practically realizable scheme, where the bright squeezed light is in the continuous-variable regime generated by the four-wave mixing process in an atomic rubidium vapor. This is a direct sub-shot-noise measurement of absorption, and more than 1 dB quantum advantage for the measurement sensitivity is demonstrated at faint absorption levels. A theoretical model that yields excellent agreements with experimental observations is also provided.
Conventional absorption spectroscopy relies on coherent laser sources, and in turn suffers from the inherent limitation of shot noise, especially in estimating weak absorption. Here, we propose a measurement strategy with correlated photons to determine the weak absorption by distinguishing the output with and without photons, dubbed as the on-off measurement. We demonstrate that absorption spectroscopy that incorporates quantum correlations is capable of estimating weak absorption down to a single-photon level, even in noisy environments, achieving a precision comparable to that obtained through 1000 photons in conventional absorption spectroscopy. Our strategy provides a new method to probe fragile systems with weak absorption, avoiding the occurrence of light-induced damage.
Absorption spectroscopy is one of the most widely used spectroscopic methods. The signal-to-noise ratio in conventional absorption spectroscopy is ultimately limited by the shot noise, which arises from the statistical property of the light used for the measurement. Here we show that the noise in absorption spectra can be suppressed below the shot-noise limit when entangled photon pairs are used for the light source. By combining broadband entangled photon pairs and multichannel detection, we realize the acquisition of sub-shot-noise absorption spectra in the entire visible wavelength. Furthermore, we demonstrate the strength of sub-shot-noise absorption spectroscopy for the identification and quantification of chemical species, which are two primary aims of absorption spectroscopy. For highly diluted binary mixture solutions, sub-shot-noise absorption spectroscopy enables us to determine the concentration of each chemical species with precision beyond the limit of conventional absorption spectroscopy. That is, sub-shot-noise absorption spectroscopy achieves superresolution in concentration measurements.
Absorption measurement is an exceptionally versatile tool for many applications in science and engineering. For absorption measurements using laser beams of light, the sensitivity is theoretically limited by the shot noise due to the fundamental Poisson distribution of the photon number in laser radiation. In practice, the shot-noise limit can only be achieved when all other sources of noise are eliminated. Here, we use seeded squeezed light to demonstrate that direct-absorption measurements can be performed with a sensitivity beyond the shot-noise limit. We present a practically realizable scheme, where intensity-squeezed beams are generated by a seeded four-wave mixing process in an atomic rubidium-vapor cell. More than 1.2 dB quantum advantage for the measurement sensitivity is obtained at faint absorption levels ($\ensuremath{\le}10\mathrm{%}$). We also present a detailed theoretical analysis to show that the observed quantum advantage when corrected for optical loss would be equivalent to 3 dB. Our experiment demonstrates a direct sub-shot-noise measurement of absorption that requires neither homodyne or lock-in nor logic coincidence-detection schemes. It is therefore very applicable in many circumstances where sub-shot-noise-level absorption measurements are highly desirable.
Quantum fluctuations in the intensity of an optical probe is noise which limits measurement precision in absorption spectroscopy. Increased probe power can offer greater precision; however, this strategy is often constrained by sample saturation. Here, we analyze measurement precision for a generalized absorption model in which we account for saturation and explore its effect on both classical and quantum probe performance. We present a classical probe-sample optimization strategy to maximize precision and find that optimal probe powers always fall within the saturation regime. We apply our optimization strategy to two examples, high-precision Doppler broadened thermometry and an absorption spectroscopy measurement of chlorophyll a. We derive a limit on the maximum precision gained from using a nonclassical probe and find a strategy capable of saturating this bound. We evaluate amplitude-squeezed light as a viable experimental probe state and find it capable of providing precision that reaches to within >85>85%>85 of the ultimate quantum limit with currently available technology.