Over the last 50 years entangled photon pairs have received attention for use in lowering the flux in two-photon absorption imaging and spectroscopy. Despite this, evidence for entangled two-photon absorption (ETPA) effects remain highly debated, especially at low-fluxes. Here, we structure the transverse spatial correlations of entangled photon pairs to evidence signs of ETPA at room-temperature in organic and inorganic chromophores, in the low-flux regime. We demonstrate our scheme to be robust to common artifacts that have previously hampered detection of ETPA such as linear absorption and background fluorescence, and show that ETPA scales with transverse correlation area and chromophore two-photon cross-sections. Our results present a step towards verifying ETPA and experimentally exploring entangled light-matter interactions.
Over the last 50 years entangled photon pairs have received attention for use in lowering the flux in two-photon absorption imaging and spectroscopy. Despite this, evidence for entangled two-photon absorption (ETPA) effects remain highly debated, especially at low-fluxes. Here, we structure the transverse spatial correlations of entangled photon pairs to evidence signs of ETPA at room-temperature in organic and inorganic chromophores, in the low-flux regime. We demonstrate our scheme to be robust to common artifacts that have previously hampered detection of ETPA such as linear absorption and background fluorescence, and show that ETPA scales with transverse correlation area and chromophore two-photon cross-sections. Our results present a step towards verifying ETPA and experimentally exploring entangled light-matter interactions.
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.
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.
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.
We present an ongoing experiment to investigate the potential enhancement of the two-photon absorption (TPA) rate of an atom using time–frequency-entangled photon pairs, a process known as entangled two-photon absorption (ETPA). There has been significant debate in the literature regarding the existence and magnitude of such enhancement. Previous studies have primarily focused on ETPA in molecular fluorophores, which are relevant for biological imaging applications but typically exhibit relatively low two-photon cross sections, often not exceeding 10⁻⁵⁰ cm⁴s/photon. In this work, we sacrifice broad applicability for experimental practicality, and instead probe ETPA in rubidium vapor, which has a comparatively large two-photon cross section (∼10⁻¹⁸ cm⁴s/photon) relative to most molecular fluorophores used in prior studies. We have developed and characterized an entangled photon-pair source, and have observed two-photon absorption in rubidium vapor. We have also reproduced previous theoretical models of ETPA. Preliminary results are presented, along with a discussion of the future direction of the experiment.
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.
The Two-photon absorption processes (TPA) is of great interest due to its variety of technical applications. Two-photon transitions can be excited using light with different statistical properties, such as laser light (coherent light), pseudo-thermal light and entangled photons-pairs (ETPA). For a TPA process driven with entangled photons (ETPA), a linear dependence of the signal with the photon flux has been theoretically predicted and experimentally demonstrated by various groups. The main motivation for studying ETPA relies on the capability of inducing TPA with a low photon flux. This is advantageous to analyze, among other things, biological samples with a reduced probability of destroying them in the process. However, ETPA experiments developed to date raise many questions regarding the difficulty of isolating a signal in organic molecules. One of the main problems in these experiments is the difficulty to study independently all the systematic effects due to the complex structure of organic molecules. An alternative to clarify the origin of the signal is to study the ETPA process in atomic systems. In this case, the possibility to excite narrow band transitions with tunable single frequency lasers can provide a clear signature of the ETPA process. To achieve this objective, the first step consists of understanding TPA with coherent light, or classical TPA, and measuring the corresponding cross-section in atomic systems. Once the classical regime is characterized, the ETPA process can be studied considering decoherence effects and coherence between intermediate states. For this, the ETPA cross section must be calculated and measured. In this work we present a theoretical calculation of the ETPA transition probability and cross-section with the density operator formalism for the transition 62S1/2 →82S1/2. The theoretical results will be complemented with an experiment with atomic Cesium based in a coincidence detection scheme.