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arXiv:2208.11387 · Civil War Book Review

Witnessing Entangled Two-Photon Absorption via Quantum Interferometry

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

Published Aug 24, 2022• 0 citations
arXivHTMLPDF

Abstract

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.

DOI
10.48550/arxiv.2208.11387

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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.
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.
The application of quantum states of light such as entangled photons, for example, created by parametric down conversion, has experienced tremendous progress in the almost 40 years since their first experimental realization. Initially, they were employed in the investigation of the foundations of quantum physics, such as the violation of Bell's inequalities and studies of quantum entanglement. They later emerged as basic platforms for quantum communication protocols and, in the recent experiments on single-photon interactions, in photonic quantum computation. These applications aim at the controlled manipulation of the photonic degrees of freedom, and therefore rely on simple models of matter, where the analysis is simpler. Furthermore, quantum imaging with entangled light can achieve enhanced resolution, and quantum metrology can overcome the shot noise limit for classical light. This Account focuses on an entirely different emerging class of applications using quantum light as a powerful spectroscopic tool to reveal novel information about complex molecules. These applications utilize two appealing properties of quantum light: its distinct intensity fluctuations and its nonclassical bandwidth properties. These give rise to new and surprising behavior of nonlinear optical signals. Nonclassical intensity fluctuations can enhance nonlinear optical signals relative to linear absorption. For instance, the two-photon absorption of entangled photon pairs scales linearly (rather than quadratically) in the photon flux, just like a single photon absorption. This enables nonlinear quantum spectroscopy of photosensitive, for example, biological, samples at low light intensities. We will discuss how the two-photon absorption cross section becomes a function of the photonic quantum state, which can be manipulated by properties of the entangled photon pairs. In addition, the quantum correlations in entangled photon states further influence the nonlinear signals in a variety of ways. Apart from affecting the signal's scaling with intensity, they also constitute an entirely new approach to shaping and controlling excitation pathways in molecular aggregates in a way that cannot be achieved with shaped classical pulses. This is because between the two absorption events in entangled two-photon absorption, the light and material system are entangled. Classical constraints for the simultaneous time and frequency resolution can thus be circumvented, since the two are not Fourier conjugates. Here we review the simplest manifestation of quantum light spectroscopy, two-photon absorption spectroscopy with entangled photons. This will allow us to discuss exemplarily the impact of quantum properties of light on a nonlinear optical signal and explore the opportunities for future applications.
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.
Recently different experimental schemes have been proposed to study the elusive phenomenon of entangled two-photon absorption (ETPA) in nonlinear materials. The attempts to detect ETPA using transmission-based schemes have led to results whose validity is currently under debate because the ETPA signal can be corrupted or emulated by artifacts associated with linear optical losses. The present work addresses the issue of linear losses and the corresponding artifacts in transmission-based ETPA experiments through a new approach that exploits the properties of a Hong-Ou-Mandel (HOM) interferogram. Here, we analyze solutions of rhodamine B (RhB), commonly used as a model of a nonlinear medium in ETPA studies. Then, by using the HOM interferometer as a sensing device, we first demonstrate the equivalence of the standard transmission vs pump power ETPA experiments, presented in many reports, with our novel approach of transmission vs two-photon temporal delay. Second, a detailed study of the effects of optical losses, unrelated to ETPA, over the HOM interferogram is carried out by: (1) characterizing RhB in solutions prepared with different solvents and (2) considering scattering losses introduced by silica nanoparticles used as a controlled linear loss mechanism. Our results clearly expose the deleterious effects of linear optical losses over the ETPA signal when standard transmission experiments are employed and show how, by using the HOM interferogram as a sensing device, it is possible to detect the presence of such losses. Finally, once we showed that the HOM interferogram discriminates properly linear losses, our study also reveals that under the specific experimental conditions considered here, which are the same as those employed in many reported works, the ETPA was not unequivocally detected.
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.