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Civil War Book Review

Witnessing Entangled Two-Photon Absorption via Quantum Interferometry

Áulide Martínez-Tapia, Samuel Corona-Aquino, Freiman Triana-Arango, Chenglong You, Rui‐Bo Jin, Omar S. Magaña‐Loaiza, Shi‐Hai Dong, Alfred B. U’Ren, Roberto de J. León‐Montiel

Published Jan 1, 2023• 0 citations
Publisher

Abstract

We demonstrate that a two-photon, N00N-state interferometer is insensitive to linear (single-photon) losses, and thus capable to unequivocally certify entangled two-photon absorption (eTPA) in arbitrary-sample transmission-based absorption measurements.
DOI
10.1364/cleo_fs.2023.fw4j.2

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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.
Recent investigations have suggested 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 recently been 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 among those considered insensitive to linear (single-photon) losses. Remarkably, our results show that N00N states may become a potentially powerful tool for quantum spectroscopy, placing them as a strong candidate for the certification of eTPA in an arbitrary sample.
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.
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.