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Register a new userTwo-photon absorption of time-frequency-entangled photon pairs by molecules: the roles of photon-number correlations and spectral correlations
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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.
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Entangled photon pairs have been promised to deliver a substantial quantum advantage for two-photon absorption spectroscopy. However, recent work has challenged the previously reported magnitude of quantum enhancement in two-photon absorption. Here, we present an experimental comparison of sum-frequency generation and molecular absorption, each driven by isolated photon pairs. We establish an upper bound on the enhancement for entangled-two-photon absorption in Rhodamine-6G, which lies well below previously reported values.
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.
Two-photon absorption (TPA) and other nonlinear interactions of molecules with time-frequency-entangled photon pairs (EPP) has been predicted to display a variety of fascinating effects. Therefore, their potential use in practical quantum-enhanced molecular spectroscopy requires close examination. This paper presents in tutorial style a detailed theoretical study of one- and two-photon absorption by molecules, focusing on how to treat the quantum nature of light. We review some basic quantum optics theory, then we review the density-matrix (Liouville) derivation of molecular optical response, emphasizing how to incorporate quantum states of light into the treatment. For illustration we treat in detail the TPA of photon pairs created by spontaneous parametric down conversion, with an emphasis on how quantum light TPA differs from that with classical light. In particular, we treat the question of how much enhancement of the TPA rate can be achieved using entangled states. The paper includes review of known theoretical methods and results, as well as some extensions, especially the comparison of TPA processes that occur via far-off-resonant intermediate states only and those that involve off-resonant intermediate state by virtue of dephasing processes. A brief discussion of the main challenges facing experimental studies of entangled TPA is also given.
A theory of correlations between N photons of given frequencies and detected at given time delays is presented. These correlation functions are usually too cumbersome to be computed explicitly. We show that they are obtained exactly through intensity correlations between two-level sensors in the limit of their vanishing coupling to the system. This allows the computation of correlation functions hitherto unreachable. The uncertainties in time and frequency of the detection, which are necessary variables to describe the system, are intrinsic to the theory. We illustrate the formalism with the Jaynes--Cummings model, showing how correlations of various peaks at zero or finite time delays bring new insights into the dynamics of open quantum systems.
Photonic time-frequency entanglement is a promising resource for quantum information processing technologies. We investigate swapping of continuous-variable entanglement in the time-frequency degree of freedom using three-wave mixing in the low-gain regime with the aim of producing heralded biphoton states with high purity and low multi-pair probability. Heralding is achieved by combining one photon from each of two biphoton sources via sum-frequency generation to create a herald photon. We present a realistic model with pulsed pumps, investigate the effects of resolving the frequency of the herald photon, and find that frequency-resolving measurement of the herald photon is necessary to produce high-purity biphotons. We also find a trade-off between the rate of successful entanglement swapping and both the purity and quantified entanglement resource (negativity) of the heralded biphoton state.
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