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Register a new userQuantifying the enhancement of two-photon absorption due to spectral-temporal entanglement
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When a low flux of time-frequency-entangled photon pairs (EPP) illuminates a two-photon transition, the rate of two-photon absorption (TPA) can be enhanced considerably by the quantum nature of photon number correlations and frequency correlations. We present a quantum-theoretic derivation of entangled TPA (ETPA) and calculate an upper bound on the amount of quantum enhancement that is possible in such systems. The derived bounds indicate that in order to observe ETPA the experiments would need to operate at a combination of significantly higher rates of EPP illumination, molecular concentrations, and conventional TPA cross sections than are achieved in typical experiments.
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Entangled two-photon absorption (ETPA) has recently become a topic of lively debate, mainly due to the apparent inconsistencies in the experimentally-reported ETPA cross sections of organic molecules. In this work, we provide a thorough experimental study of ETPA in the organic molecules Rhodamine B (RhB) and Zinc Tetraphenylporphirin (ZnTPP). The goal of this contribution is twofold: on one hand, it seeks to reproduce the results of previous experimental reports and, on the other, it aims to determine the effects of different temporal correlations -- introduced as a controllable time-delay between the photons to be absorbed -- on the strength of the ETPA signal. In our experiment, the samples are excited by entangled pairs produced by type-I SPDC, with a spectral distribution centered at 810 nm. Surprisingly, and contrary to what was expected, the time delay did not produce in our experiments any systematic change in the cross-sections when monitoring the ETPA signal using a transmission measurement scheme. As a plausible cause of this unexpected result, we argue that the photon-pair flux, typically-used in these experiments, is not sufficient to promote the two-photon absorption process in these molecules. This suggests that the actual absorption cross-section values are lower than those previously reported, and therefore do not lead to a measurable ETPA effect for the transmission method.
It is well known that energy-time entanglement can enhance two photon absorption (TPA) by simultaneously optimizing the two photon resonance and the coincidence rate of photons at the absorber. However, the precise relation between entanglement and the TPA rate depends on the coherences of intermediate states involved in the transition, making it a rather challenging task to identify universal features of TPA processes. In the present paper, we show that the theory can be simplified greatly by separating the two photon resonance from the temporal dynamics of the intermediate levels. The result is a description of the role of entanglement in the TPA process by a one-dimensional coherence in the Hilbert space defined by the arrival time difference of the two photons. Transformation into the frequency difference basis results in Kramers-Kronig relations for the TPA process, separating off-resonant contributions of virtual levels from resonant contributions. In particular, it can be shown that off-resonant contributions are insensitive to the frequencies of the associated virtual states, indicating that virtual-state spectroscopy of levels above the final two photon excited state is not possible.
Marine microorganisms often reach high swimming speeds, either to take advantage of evanescent nutrient patches or to beat Brownian forces. Since this implies that a sizable part of their energetic budget must be allocated to motion, it is reasonable to assume that some fast-swimming microorganisms may increase their nutrient intake by increasing their speed v. We formulate a model to investigate this hypothesis and its consequences, finding the steady state solutions and analyzing their stability. Surprisingly, we find that even modest increases in nutrient absorption may lead to a significant increase of the microbial speed. In fact, evaluations obtained using realistic parameter values for bacteria indicate that the speed increase due to the enhanced nutrient absorption may be quite large.
While two-photon absorption (TPA) and other forms of nonlinear interactions of molecules with isolated time-frequency-entangled photon pairs (EPP) have been predicted to display a variety of fascinating effects, their potential use in practical quantum-enhanced molecular spectroscopy requires close examination. This paper presents a detailed theoretical study of quantum-enhanced TPA by both photon-number correlations and spectral correlations, including an account of the deleterious effects of dispersion. While such correlations in EPP created by spontaneous parametric down conversion can increase the TPA rate significantly in the regime of extremely low optical flux, we find that for typical molecules in solution this regime corresponds to such low TPA event rates as to be unobservable in practice. Our results support the usefulness of EPP spectroscopy in atomic or other narrow-linewidth systems, while questioning the efficacy of such approaches for broadband systems including molecules in solution.
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 there is no 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 $sim n^4$. 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 a $sim n^3$ scaling in both quadrature and photon-counting measurements.
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