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arXiv:2608.27157

Franson-Interferometric Bounds on Entangled Two-Photon Absorption

Albin Hedse, Sankaran Ramesh, Luis Matheis, Sebastian Gstir, A. Wacker, Gregor Weihs, Robert Keil, Qi Shi, Amitav Sahu, Tõnu Pullerits

Published Aug 27, 2026• 0 citations
arXivHTMLPDF

Abstract

Entangled photons offer quantum correlations with no classical analogue. In entangled pair two-photon absorption (ETPA), absorption rate is predicted to scale linearly rather than quadratically with photon flux, promising molecular excitation at fluxes far below the classical threshold. Reported ETPA cross sections nevertheless vary widely across experiments, largely since the observable, the differential of the transmitted flux or weak fluorescence, is difficult to separate from scattering and linear losses. We present a method which uses Franson interference to study entangled two-photon absorption through delay-dependent coincidence measurements on dye molecules. Applying the method to Rhodamine 6G, we observe a small asymmetry in the Franson interference envelope and obtain a model-derived effective cross section of approximately 2.1 E(-21) centimeter squared for Rhodamine 6G. However, the estimated systematic uncertainty does not allow a definitive ETPA assignment. Instead, the experiment establishes a quantitative bound on the ETPA response and provides a background-free benchmark for future measurements.

DOI
10.48550/arxiv.2608.27157

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Entangled photons offer quantum correlations with no classical analogue. In entangled pair two-photon absorption (ETPA), absorption rate is predicted to scale linearly rather than quadratically with photon flux, promising molecular excitation at fluxes far below the classical threshold. Reported ETPA cross sections nevertheless vary widely across experiments, largely since the observable, the differential of the transmitted flux or weak fluorescence, is difficult to separate from scattering and linear losses. We present a method which uses Franson interference to study entangled two-photon absorption through delay-dependent coincidence measurements on dye molecules. Applying the method to Rhodamine 6G, we observe a small asymmetry in the Franson interference envelope and obtain a model-derived effective cross section of approximately 2.1 E(-21) centimeter squared for Rhodamine 6G. However, the estimated systematic uncertainty does not allow a definitive ETPA assignment. Instead, the experiment establishes a quantitative bound on the ETPA response and provides a background-free benchmark for future measurements.
Nonlinear spectroscopy and microscopy techniques are ubiquitous in a wide range of applications across physics and biology. However, these usually rely on high-powered pulsed laser systems. A promising alternative is to exploit entangled two-photon absorption (ETPA), which can lead to tens of orders of magnitude lower incident fluxes than in conventional two-photon absorption schemes. However, the role of different entangled degrees of freedom in ETPA was unclear following recent experimental studies, when compared to earlier theoretical works. Here, we first demonstrate a linear dependence of the ETPA rate with the photon-pair rate, a clear signature of ETPA, and estimate the values for the concentration-dependent ETPA cross section for Rhodamine 6G. We then investigate the signature of energy-time entanglement and polarization dependence in the ETPA fluorescence rate and demonstrate a strong dependence of the signal on the interphoton delay that reflects the coherence time of the entangled two-photon wave packet.
We experimentally study entangled two-photon absorption in rhodamine 6G as a function of the spatial properties of a high flux of broadband entangled photon pairs. We first demonstrate a key signature dependence of the entangled two-photon absorption rate on the type of entangled pair flux attenuation: linear, when the laser pump power is attenuated, and quadratic, when the pair flux itself experiences linear loss. We then perform a fluorescence-based Z-scan measurement to study the influence of beam waist size on the entangled two-photon absorption process and compare this to classical single- and two-photon absorption processes. We demonstrate that the entangled two-photon absorption shares a beam waist dependence similar to that of classical two-photon absorption. This result presents an additional argument for the wide range of contrasting values of quoted entangled two-photon absorption cross sections of dyes in literature.
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Entangled two-photon absorption (ETPA) could form the basis of nonlinear quantum spectroscopy at very low photon fluxes, since, at sufficiently low photon fluxes, ETPA scales linearly with the photon flux. When different pairs start to overlap temporally, accidental coincidences are thought to give rise to a "classical" quadratic scaling that dominates the signal at large photon fluxes and, thus, recovers a supposedly classical regime, where any quantum advantage is thought to be lost. Here, we scrutinize this assumption and demonstrate that quantum-enhanced absorption cross sections can persist even for very large photon numbers. To this end, we use a minimal model for quantum light, which can interpolate continuously between the entangled pair and a high-photon-flux limit, to analytically derive ETPA cross sections and the intensity crossover regime. We investigate the interplay between spectral and spatial degrees of freedom and how linewidth broadening of the sample impacts the experimentally achievable enhancement.
The phenomenon of Entangled Two-Photon Absorption (ETPA) presents a persistent controversy in the literature, evidenced by a wide disparity in the reported values for the σEσ_EσE​ cross-sections. Much of this discrepancy is attributed to the difficulty in discriminating ETPA from various background processes that can mimic its signal, such as linear absorption or scattering. Given this need to certify the presence of ETPA unequivocally, this work introduces a key strategy to isolate the ETPA contribution through its spectral signature. This involves modeling the molecule as a two-photon notch filter and inducing a controlled asymmetric overlap with the joint spectral intensity (JSI) of the incident photons. This asymmetry is used to generate a measurable distortion in the transmitted JSI, and, complementarily, as a reduction in the visibility of the Hong-Ou-Mandel (HOM) dip. To ensure the experimental feasibility of this technique, a comprehensive analysis of the experimental conditions required for its detection is presented, establishing the absorption efficiency limits that must be overcome given the constraints of entangled-photon-pair flux and detector noise. A preliminary experiment addressing the ETPA detection limits using the standard RhB dye is presented.
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.