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arXiv:2009.12026 · Physical Review Letters

Entanglement-Assisted Absorption Spectroscopy

Haowei Shi, Zheshen Zhang, Stefano Pirandola, Quntao Zhuang

Published Oct 28, 2020• 49 citations
arXivHTMLPDF

Abstract

Spectroscopy is an important tool for probing the properties of materials, chemicals, and biological samples. We design a practical transmitter-receiver system that exploits entanglement to achieve a provable quantum advantage over all spectroscopic schemes based on classical sources. To probe the absorption spectra, modeled as a pattern of transmissivities among different frequency modes, we employ broadband signal-idler pairs in two-mode squeezed vacuum states. At the receiver side, we apply photodetection after optical parametric amplification. Finally, we perform a maximum likelihood decision test on the measurement results, achieving an error probability orders of magnitude lower than the optimum classical systems in various examples, including "wine tasting" and "drug testing" where real molecules are considered. In detecting the presence of an absorption line, our quantum scheme achieves the optimum performance allowed by quantum mechanics. The quantum advantage in our system is robust against noise and loss, which makes near-term experimental demonstration possible.

DOI
10.1103/physrevlett.125.180502

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Spectroscopy is an important tool for probing the properties of materials, chemicals, and biological samples. We design a practical transmitter-receiver system that exploits entanglement to achieve a provable quantum advantage over all spectroscopic schemes based on classical sources. To probe the absorption spectra, modeled as a pattern of transmissivities among different frequency modes, we employ broadband signal-idler pairs in two-mode squeezed vacuum states. At the receiver side, we apply photodetection after optical parametric amplification. Finally, we perform a maximum likelihood decision test on the measurement results, achieving an error probability orders of magnitude lower than the optimum classical systems in various examples, including "wine tasting" and "drug testing" where real molecules are considered. In detecting the presence of an absorption line, our quantum scheme achieves the optimum performance allowed by quantum mechanics. The quantum advantage in our system is robust against noise and loss, which makes near-term experimental demonstration possible.
Absorption spectroscopy has long been hailed as an absolute necessity for detecting the properties of complex chemical and biological samples. While conventional spectroscopy using classical light is severely limited by shot noise and lacks robustness against experimental imperfections, quantum light offers an avenue to perform absorption spectroscopy with provable advantages in the technical operations and the measurement precision. Here, we present an experimental approach to implement entanglement-based absorption spectroscopy with the assistance of Hong-Ou-Mandel interference. Since the temporal interference fringe is determined by the spectrum pattern, a maximum-likelihood decision is sufficient for revealing the relevant quantum information about the absorptive properties of the test samples. These experimental results may significantly facilitate the use of quantum interferometric spectroscopy to practical applications, which may be particularly relevant for photon-sensitive biological and chemical samples.
Abstract Dual-comb interferometry harnesses the interference of two laser frequency combs to provide unprecedented capability in spectroscopy applications. In the past decade, the state-of-the-art systems have reached a point where the signal-to-noise ratio per unit acquisition time is fundamentally limited by shot noise from vacuum fluctuations. To address the issue, we propose an entanglement-enhanced dual-comb spectroscopy protocol that leverages quantum resources to significantly improve the signal-to-noise ratio performance. To analyze the performance of real systems, we develop a quantum model of dual-comb spectroscopy that takes practical noises into consideration. Based on this model, we propose quantum combs with side-band entanglement around each comb lines to suppress the shot noise in heterodyne detection. Our results show significant quantum advantages in the uW to mW power range, making this technique particularly attractive for biological and chemical sensing applications. Furthermore, the quantum comb can be engineered using nonlinear optics and promises near-term experimentation.
Quantum spectroscopy seeks to probe chemical systems using nonclassical light, which has properties that are qualitatively and quantitatively different than conventional light sources. One promising technique uses intensity-correlated twin beams of light to reduce the noise sources inherent to absorption spectroscopy. However, measurements of the phase shift imparted by the chemical sample, which provides complementary information to the absorption, continue to be a challenge. Here, we propose and demonstrate a scheme using entangled photon pairs that can simultaneously measure both the absorption and phase shift of a sample with extremely low optical intensities and with relatively fast few-minute acquisition times. This method combines the previous use of intensity correlations with a broadband quantum interferometer utilizing two-photon interference to measure the complete linear optical response of the sample. Our work shows that precise measurements of absorption can also be made phase-sensitive using suitable choices of probe beam and detection scheme. This enables a new class of quantum spectroscopy schemes which measure absorption and phase with a single probe. Our technique is relevant to the characterization of a wide array of chemical and biological samples, such as quantum dots and organic fluorophores, and may be useful for spectroscopic measurements that are otherwise constrained in intensity.
Absorption spectroscopy identifies molecules by detecting frequency-dependent optical loss, and its fundamental limit is a quantum channel-discrimination problem. In this work, we develop a general framework for characterizing the ultimate quantum limit of molecular absorption spectroscopy without collective measurements: we formulate it as an asymmetric quantum hypothesis testing task between different absorption channels. Using a semidefinite-programming formulation, we construct optimal probe states and compare them with coherent-state photon counting, Fock states, and two-mode squeezed vacuum probes. We introduce a random-loss channel model for imperfectly known background transmission, reflecting the fact that a blank experiment need not return all incident photons due to scattering, solvent absorption, or collection losses. Our results show that optimized non-classical probes can substantially outperform conventional laser spectroscopy, and that the advantage is robust to realistic baseline random loss. % In multi-frequency spectroscopy, the optimization also determines how photons should be allocated across absorption lines, revealing an additional resource-allocation advantage beyond single-mode state engineering. We illustrate our framework using infrared detection of 4-nitrophenol against chemically relevant comparison molecules, showing how quantum channel-discrimination methods provide constructive performance limits for molecular spectroscopy under realistic photon constraints.
The most important problem of spectroscopic chiral analysis is the enantioselective effects of the light-molecule interactions are inherently weak and severely reduced by the environment noises. Enormous efforts had been spent to overcome this problem by enhancing the symmetry break in the light-molecule interactions or reducing the environment noises. Here, we propose an alternative way to solve this problem by using frequency-entangled two-photon pairs as probe signals and detecting them in coincidence, i.e., using quantum chiral spectroscopy. For this purpose, we develop the theory of entanglement-assisted quantum chiral spectroscopy. Our results show that the quantum spectra of the left- and right-handed molecules are always distinguishable by suitably configuring the frequency-entangled two-photon pairs. In contrast, the classical spectra of the two enantiomers, where the broadband signal photon is frequency-uncorrelated with the idle one, become indistinguishable in the strong dissipation region. This offers our quantum chiral spectroscopy a great advantage over the classical chiral spectroscopy. Our work opens up an exciting area that exploring profound advantages of the quantum spectroscopy in chiral analysis.