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arXiv:2209.02697 · Physical Review Letters

Nonlinear Interferometry for Quantum-Enhanced Measurements of Multiphoton Absorption

S. Panahiyan, Carlos Sánchez Muñoz, Maria V. Chekhova, Frank Schlawin

Published May 19, 2023• 22 citations
arXivHTMLPDF

Abstract

Multiphoton absorption is of vital importance in many spectroscopic, microscopic, or lithographic applications. However, given that it is an inherently weak process, the detection of multiphoton absorption signals typically requires large field intensities, hindering its applicability in many practical situations. In this Letter, we show that placing a multiphoton absorbent inside an imbalanced nonlinear interferometer can enhance the precision of multiphoton cross section estimation with respect to strategies based on photon-number measurements using coherent or even squeezed light directly transmitted through the medium. In particular, the power scaling of the sensitivity with photon flux can be increased by 1 order compared with transmission measurements of the sample with coherent light, such that the measurement precision at any given intensity can be greatly enhanced. Furthermore, we show that this enhanced measurement precision is robust against experimental imperfections leading to photon losses, which usually tend to degrade the detection sensitivity. We trace the origin of this enhancement to an optimal degree of squeezing which has to be generated in a nonlinear SU(1,1) interferometer.

DOI
10.1103/physrevlett.130.203604

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Multiphoton absorption is of vital importance in many spectroscopic, microscopic, or lithographic applications. However, given that it is an inherently weak process, the detection of multiphoton absorption signals typically requires large field intensities, hindering its applicability in many practical situations. In this Letter, we show that placing a multiphoton absorbent inside an imbalanced nonlinear interferometer can enhance the precision of multiphoton cross section estimation with respect to strategies based on photon-number measurements using coherent or even squeezed light directly transmitted through the medium. In particular, the power scaling of the sensitivity with photon flux can be increased by 1 order compared with transmission measurements of the sample with coherent light, such that the measurement precision at any given intensity can be greatly enhanced. Furthermore, we show that this enhanced measurement precision is robust against experimental imperfections leading to photon losses, which usually tend to degrade the detection sensitivity. We trace the origin of this enhancement to an optimal degree of squeezing which has to be generated in a nonlinear SU(1,1) interferometer.
A nonlinear interferometer uses nonlinear elements as beam splitters to split and to recombine optical waves for interference. As a result, the interference fringe size has a nonlinear dependence on the intensity of the field for phase sensing and leads to an enhanced phase signal. In this paper, a practical scheme of nonlinear interferometry for precision phase measurement is analyzed with parametric amplifiers as the nonlinear beam splitters. It is found that the signal due to phase shift is enhanced by a factor of the amplification gain as compared to a linear interferometer with the same phase-sensing light intensity while the quantum noise is kept at the vacuum level, thus, effectively increasing the signal-to-noise ratio (SNR) beyond the standard quantum limit. Furthermore, the scheme is not as sensitive to the detection loss as the linear scheme with a squeezed state for noise reduction. However, losses inside the interferometer limit the enhancement factor in SNR. We apply the concept to a Michelson interferometer but with parametric amplifiers involved for gravitational-wave detection. We find that effective power is increased by the gain of the amplifiers without actually increasing the cycling power inside the interferometer. Furthermore, the full benefits with squeezed input and variational output or the combination of a quantum nondemolition interferometer for sensitivity beyond the standard quantum limit apply here with even better results. Such a nonlinear interferometer will find wide applications in precision measurements.
Multiphoton absorption processes have a nonlinear dependence on the amplitude of the incident optical field, i.e., the number of photons. However, multiphoton absorption is generally weak and multiphoton events occur with extremely low probability. Consequently, it is extremely challenging to engineer quantum nonlinear devices that operate at the single photon level and the majority of quantum technologies have to rely on single photon interactions. Here we demonstrate experimentally and theoretically that exploiting coherent absorption of N=2N=2N=2 NOON states makes it possible to enhance the number of two-photon states that are absorbed by at most a factor of 2 with respect to a linear absorption process. An absorbing metasurface placed inside a Sagnac-style interferometer into which we inject an N=2N=2N=2 NOON state, exhibits two-photon absorption with 40.540.5%40.5 efficiency, close to the theoretical maximum. This high probability of simultaneous absorption of two photons holds the promise for applications in fields that require multiphoton upconversion but are hindered by high peak intensities.
Abstract Recent theoretical and experimental advances have shown that squeezed states of light can be engineered to enhance the resolution of optical measurements. Extending such quantum-enhanced techniques to nonlinear optical processes has therefore attracted considerable interest. In particular, two-photon absorption (TPA), which has wide-ranging applications in physics, chemistry, and biology, has emerged as a promising platform for exploiting these quantum advantages. In this work, we investigate whether and how correlations between light modes can be used to improve optical resolution in TPA. We analyze non-degenerate TPA transmission measurements using two-mode squeezed light and compare different measurement strategies. We find that intensity correlation measurements offer better performance in terms of the achievable estimation error compared to normalized intensity correlations or measurements of the noise reduction factor (NRF). The achievable enhancement from intensity and NRF measurements are degraded by competing photon losses. In contrast, the normalized intensity correlation approach remains robust to loss, albeit at the cost of forfeiting the scaling enhancement at large photon numbers achievable with nonclassical light fields. Thus, we establish a trade-off between robustness to loss and the achievable quantum advantage. We further compute the corresponding Cramér–Rao bound, which sets the ultimate lower limit on the achievable estimation error for the photon-counting-based measurement strategies investigated in this work.
Abstract Nonlinear optics plays a crucial role in science and technology, with applications ranging from spectroscopy to quantum information processing. Therefore, precise estimation of their nonlinear optical parameters is of fundamental importance. Here, we investigate quantum-enhanced sensitivity in the estimation of nonlinear absorption parameters, including saturable absorption (SA) and reverse saturable absorption (RSA). By employing the quantum Fisher information, we quantify the enhancement in sensitivity for estimating transmission ( T ), linear absorption coefficient ( α0\alpha _0α0​ ), saturable intensity ( IsI_sIs​ ), and two-photon absorption coefficient ( β\beta β ) using bright two-mode squeezed states (bTMSS) and applied it to analyze the nonlinear parameters of Pt nanoparticle samples as an example. In addition, we propose an experimental scheme based on an open-aperture Z-scan with bTMSS to realize quantum-enhanced sensitivity. Our findings establish a pathway toward quantum-enhanced estimation of nonlinear optical parameters.
SU(1,1) interferometers, based on nonlinear optical processes, potentially offer better phase sensitivity than traditional instruments. Bright-seeded variants are important for applications with large numbers of photons, yet have remained uncharacterized experimentally, for lack of a real-time technique to measure phase sensitivity. This study uses a direct intensity-detection technique to demonstrate the quantum enhancement of phase sensitivity in real time for a bright-seeded SU(1,1) system, compared to the classical shot-noise limit. It is hoped that these results will promote applications of this class of interferometer in quantum metrology.
Two-photon absorption (TPA) is of fundamental importance in super-resolution imaging and spectroscopy. Its nonlinear character allows for the prospect of using quantum resources, such as entanglement, to improve measurement precision or to gain new information on, e.g., ultrafast molecular dynamics. Here, we establish the metrological properties of nonclassical squeezed light sources for precision measurements of TPA cross sections. We find that the Cram\'er-Rao bound does not provide a fundamental limit for the precision achievable with squeezed states in the limit of very small cross sections. Considering the most relevant measurement strategies---namely, photon-counting and quadrature measurements---we determine the quantum advantage provided by squeezed states as compared to coherent states. We find that squeezed states outperform the precision achievable by coherent states when performing quadrature measurements, which provide improved scaling of the Fisher information with respect to the mean photon number $\ensuremath{\sim}{n}^{4}$. Due to the interplay of the incoherent nature and the nonlinearity of the TPA process, unusual scaling can also be obtained with coherent states, which feature an $\ensuremath{\sim}{n}^{3}$ scaling in both quadrature and photon-counting measurements.