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arXiv:2512.19261 · Physical Review A

Limitations of Entangled Two-Photon Absorption detection

René Pollmann, Franz Roeder, Christine Silberhorn, Benjamin Brecht

quant-phphysics.opticsSubmitted Dec 22, 2025• Announced Dec 23, 2025• 0 citations
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Abstract

We introduce a method for determining the sensitivity of any given Entangled Two-Photon Absorption (ETPA) measurement. By modeling all signal and noise contributions to the measurement, we derive a single numerical value that describes the sensitivity of the ETPA measurement in Göppert-Mayer units. This allows us to directly compare vastly different experimental approaches and, determine whether ETPA will be detectable under the given conditions. Therefore, we can quantify the effect of any change to a given experimental apparatus and identify the ideal optimization pathway.

DOI
10.1103/qpb1-hk5l
Comments
9 pages, 3 figures

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We introduce a method for determining the sensitivity of any given Entangled Two-Photon Absorption (ETPA) measurement. By modeling all signal and noise contributions to the measurement, we derive a single numerical value that describes the sensitivity of the ETPA measurement in Göppert-Mayer units. This allows us to directly compare vastly different experimental approaches and, determine whether ETPA will be detectable under the given conditions. Therefore, we can quantify the effect of any change to a given experimental apparatus and identify the ideal optimization pathway.
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.
Recently, different experimental methods to investigate the entangled two-photon absorption (ETPA) process in a variety of materials have been reported. The present work reports on a different approach on which the ETPA process is detected based on the changes induced on the Hong-Ou-Mandel (HOM) interferogram of two photons produced by a spontaneous parametric down conversion (SPDC) Type-II process. Using an organic solution of the laser dye Rhodamine B as a model, it is demonstrated that ETPA at 800nm can be monitored by the changes in the temporal-width and visibility of the HOM interferogram produced by the photons at a beam splitter after interacting with the sample. Additionally, we present a detail model in which the sample is modeled as a filtering function which fullfills the energy conservation conditions required by ETPA, allowing to explain the experimental observations with excellent agreement. We believe that this work represents a new perspective to study the ETPA process, by using an ultra-sensitive quantum interference technique and a detailed mathematical model of the process.
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 obtained by a number of groups. In this work, we provide a thorough experimental study of ETPA in the organic molecules Rhodamine B (RhB) and zinc tetraphenylporphirin (ZnTPP). Our contribution is 3-fold: first, we reproduce previous results from other groups; second, we on the one hand determine the effects of different temporal correlations─introduced as a controllable temporal delay between the signal and idler photons to be absorbed─on the strength of the ETPA signal, and on the other hand, we introduce two concurrent and equivalent detection systems with and without the sample in place as a useful experimental check; third, we introduce, and apply to our data, a novel method to quantify the ETPA rate based on taking into account the full photon-pair behavior rather than focusing on singles or coincidence counts independently. Through this experimental setup we find that, surprisingly, the purported ETPA signal is not suppressed for a temporal delay much greater than the characteristic photon-pair temporal correlation time. While our results reproduce the previous findings from other authors, our full analysis indicates that the signal observed is not actually due to ETPA but simply to linear losses. Interestingly, for higher RhB concentrations, we find a two-photon signal that, contrary to expectations, likewise does not correspond to ETPA.
Multiphoton absorption of entangled photons offers ways for obtaining unique information about chemical and biological processes. Measurements with entangled photons may enable sensing biological signatures with high selectivity and at very low light levels to protect against photodamage. In this paper, we present a theoretical and experimental study of the excitation wavelength dependence of the entangled two-photon absorption (ETPA) process in a molecular system, which provides insights into how entanglement affects molecular spectra. We demonstrate that the ETPA excitation spectrum can be different from that of classical TPA as well as that for one-photon resonant absorption (OPA) with photons of doubled frequency. These results are modeled by assuming the ETPA cross-section is governed by a two-photon excited state radiative linewidth rather than by electron-phonon interactions, and this leads to excitation spectra that match the observed results. Further, we find that the two-photon-allowed states with highest TPA and ETPA intensities have high electronic entanglements, with ETPA especially favoring states with the longest radiative lifetimes. These results provide concepts for the development of quantum light-based spectroscopy and microscopy that will lead to much higher efficiency of ETPA sensors and low-intensity detection schemes.
Recent investigations suggest that the use of non-classical states of light, such as entangled photon pairs, may open new and exciting avenues in experimental two-photon absorption spectroscopy. Despite several experimental studies of entangled two-photon absorption (eTPA), there is still a heated debate on whether eTPA has truly been observed. This interesting debate has arisen, mainly because it has been recently argued that single-photon-loss mechanisms, such as scattering or hot-band absorption may mimic the expected entangled-photon linear absorption behavior. In this work, we focus on transmission measurements of eTPA, and explore three different two-photon quantum interferometers in the context of assessing eTPA. We demonstrate that the so-called N00N-state configuration is the only one amongst those considered insensitive to linear (single-photon) losses. Remarkably, our results show that N00N states may become a potentially powerful tool for quantum spectroscopy, and place them as a strong candidate for the certification of eTPA in an arbitrary sample.