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Physical Review A

Limitations in fluorescence-detected entangled two-photon-absorption experiments: Exploring the low- to high-gain squeezing regimes

Tiemo S. Landes, Brian J. Smith, Michael G. Raymer

Published Sep 9, 2024• 28 citations
Publisher

Abstract

The authors present an experimental study of entangled two-photon absorption in solvated rhodamine 6G, providing strong evidence that the orders-of-magnitude increases in two-photon-absorption efficiency by using entangled light reported in previous studies cannot be explained by the community's current understanding of the process. Thus, the sought-after advantages of using two-photon absorption of time-frequency-entangled photon pairs as a practical tool for enhancing molecular spectroscopy and biological imaging remains elusive.

DOI
10.1103/physreva.110.033708

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The authors present an experimental study of entangled two-photon absorption in solvated rhodamine 6G, providing strong evidence that the orders-of-magnitude increases in two-photon-absorption efficiency by using entangled light reported in previous studies cannot be explained by the community's current understanding of the process. Thus, the sought-after advantages of using two-photon absorption of time-frequency-entangled photon pairs as a practical tool for enhancing molecular spectroscopy and biological imaging remains elusive.
We closely replicated and extended a recent experiment ("Spatial properties of entangled two-photon absorption," Phys. Rev. Lett. 129, 183601, 2022) that reportedly observed enhancement of two-photon absorption rates in molecular samples by using time-frequency-entangled photon pairs, and we found that in the low-flux regime, where such enhancement is theoretically predicted in-principle, the two-photon fluorescence signal is below detection threshold using current state-of-the-art methods. The results are important in the context of efforts to enable quantum-enhanced molecular spectroscopy and imaging at ultra-low optical flux. Using an optical parametric down-conversion photon-pair source that can be varied from the low-gain spontaneous regime to the high-gain squeezing regime, we observed two-photon-induced fluorescence in the high-gain regime but in the low-gain regime any fluorescence was below detection threshold. We supplemented the molecular fluorescence experiments with a study of nonlinear-optical sum-frequency generation, for which we are able to observe the low-to-high-gain crossover, thereby verifying our theoretical models and experimental techniques. The observed rates (or lack thereof) in both experiments are consistent with theoretical predictions and with our previous experiments, and indicate that time-frequency photon entanglement does not provide a practical means to enhance in-solution molecular two-photon fluorescence spectroscopy or imaging with current techniques.
Entangled photon pairs have 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. We present a measurement of molecular absorption driven by isolated photon pairs using sum-frequency generation in a nonlinear optical crystal as a calibration device. We thereby establish an upper bound on the enhancement for entangled two-photon absorption in Rhodamine 6G, which lies well below previously reported values.
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.
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.
Excitation with entangled photon pairs may lead to an increase in the efficiency of two-photon absorption at low photon flux. The corresponding process, entangled two-photon absorption (E2PA), has been investigated in numerous theoretical and experimental studies. However, significant ambiguity and inconsistency remain in the literature about the absolute values of E2PA cross sections. Here, we use a fluorescence-based registration scheme to experimentally determine upper bounds on the cross sections for six fluorophores. These bounds are up to 4 orders of magnitude lower than the smallest published cross section. For two samples that have been studied by others, Rhodamine 6G and 9R-S, we measure upper bounds 4 and 5 orders of magnitude lower than the previously reported cross sections.