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Conference on Lasers and Electro-Optics

Entangled Two-Photon Absorption with Isolated Photon Pairs or Broadband Bright Squeezed Vacuum

Michael G. Raymer, Tiemo S. Landes, Markus Allgaier, Sofiane Merkouche, Andrew H. Marcus, Brian J. Smith

Published Jan 1, 2022• 0 citations
Publisher

Abstract

We present an analytical theoretical model describing two-photon absorption (TPA) driven by spontaneous parametric down conversion (SPDC) or by broadband bright squeezed vacuum (BSV) and identify bounds and discuss contributions of coherent and incoherent processes.
DOI
10.1364/cleo_at.2022.jtu5d.2

Related papers

Theory of two-photon absorption with broadband squeezed vacuum

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We present an analytical quantum theoretic model for nonresonant molecular two-photon absorption (TPA) of broadband, spectrally multimode squeezed vacuum, including low-gain (isolated entangled photon pairs) and high-gain (bright squeezed vacuum or BSV) regimes. The results are relevant to the potential use of entangled-light TPA as a spectroscopic and imaging method. We treat the scenario that the exciting light is spatially single mode and is nonresonant with all intermediate molecular states. In the case of high gain, we find that in the case that the linewidth of the final molecular state is much narrower than the bandwidth of the exciting light, bright squeezed vacuum is found to be equally (but no more) effective in driving TPA as is a quasimonochromatic coherent-state (classical) pulse of the same temporal shape, duration, and mean photon number. Therefore, in this case the sought-for advantage of observing TPA at extremely low optical flux is not provided by broadband bright squeezed vacuum. In the opposite case that the final-state linewidth is much broader than the bandwidth of the BSV exciting light, we show that the TPA rate is proportional to the second-order intensity autocorrelation function at zero time delay ${g}^{(2)}(0)$, as expected. We derive and evaluate formulas describing the transition between these two limiting cases, that is, including the regime where the molecular linewidth and optical bandwidth are comparable, as is often the case in experimental studies. We also show that for ${g}^{(2)}(0)$ to reach the idealized form ${g}^{(2)}(0)=3+1/\overline{n}$, with $\overline{n}$ being the mean number of photons per temporal mode, it is required to compensate the dispersion inherent in the nonlinear-optical crystal used to generate the BSV.

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An investigation of two-photon absorption with entangled photon pairs

Lindsell, Noah

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.

•Aug 1, 2025•1 citation
We present an analytical quantum theoretic model for nonresonant molecular two-photon absorption (TPA) of broadband, spectrally multimode squeezed vacuum, including low-gain (isolated entangled photon pairs) and high-gain (bright squeezed vacuum or BSV) regimes. The results are relevant to the potential use of entangled-light TPA as a spectroscopic and imaging method. We treat the scenario that the exciting light is spatially single mode and is nonresonant with all intermediate molecular states. In the case of high gain, we find that in the case that the linewidth of the final molecular state is much narrower than the bandwidth of the exciting light, bright squeezed vacuum is found to be equally (but no more) effective in driving TPA as is a quasimonochromatic coherent-state (classical) pulse of the same temporal shape, duration, and mean photon number. Therefore, in this case the sought-for advantage of observing TPA at extremely low optical flux is not provided by broadband bright squeezed vacuum. In the opposite case that the final-state linewidth is much broader than the bandwidth of the BSV exciting light, we show that the TPA rate is proportional to the second-order intensity autocorrelation function at zero time delay g(2)(0){g}^{(2)}(0)g(2)(0), as expected. We derive and evaluate formulas describing the transition between these two limiting cases, that is, including the regime where the molecular linewidth and optical bandwidth are comparable, as is often the case in experimental studies. We also show that for g(2)(0){g}^{(2)}(0)g(2)(0) to reach the idealized form g(2)(0)=3+1/n‾{g}^{(2)}(0)=3+1/\overline{n}g(2)(0)=3+1/n, with n‾\overline{n}n being the mean number of photons per temporal mode, it is required to compensate the dispersion inherent in the nonlinear-optical crystal used to generate the BSV.
Two-photon absorption (TPA) and other nonlinear interactions of molecules with time-frequency-entangled photon pairs have been predicted to display a variety of fascinating effects. Therefore, their potential use in practical quantum-enhanced molecular spectroscopy requires close examination. This Tutorial presents a detailed theoretical study of one- and two-photon absorption by molecules, focusing on how to treat the quantum nature of light. We review some basic quantum optics theory and then we review the density-matrix (Liouville) derivation of molecular optical response, emphasizing how to incorporate quantum states of light into the treatment. For illustration, we treat in detail the TPA of photon pairs created by spontaneous parametric down conversion, with an emphasis on how quantum light TPA differs from that with classical light. In particular, we treat the question of how much enhancement of the TPA rate can be achieved using entangled states. This Tutorial includes a review of known theoretical methods and results as well as some extensions, especially the comparison of TPA processes that occur via far-off-resonant intermediate states only and those that involve off-resonant intermediate states by virtue of dephasing processes. A brief discussion of the main challenges facing experimental studies of entangled two-photon absorption is also given.
While two-photon absorption (TPA) and other forms of nonlinear interactions of molecules with isolated time-frequency-entangled photon pairs (EPP) have been predicted to display a variety of fascinating effects, their potential use in practical quantum-enhanced molecular spectroscopy requires close examination. This paper presents a detailed theoretical study of quantum-enhanced TPA by both photon-number correlations and spectral correlations, including an account of the deleterious effects of dispersion. While such correlations in EPP created by spontaneous parametric down conversion can increase the TPA rate significantly in the regime of extremely low optical flux, we find that for typical molecules in solution this regime corresponds to such low TPA event rates as to be unobservable in practice. Our results support the usefulness of EPP spectroscopy in atomic or other narrow-linewidth systems, while questioning the efficacy of such approaches for broadband systems including molecules in solution.
Broadband photon-pairs from a parametric down-conversion (PDC) source are essential for quantum optics experiments in the context of spectroscopy, quantum optical coherence tomography and entangled two-photon absorption [1]–[2]. Entangled two-photon absorption benefits from the ultra-short correlation time of a highly time-frequency entangled photon-pair which increases the absorption cross-section while in spectroscopy, broad spectral coverage in the mid-infrared allows one to enter the regime of life science applications.
The discrepancies between theoretical and experimental results in the process of entangled two-photon absorption (ETPA) are not fully understood. Atomic systems are a promising alternative for investigating this process without the systematic effects present in molecules. We present a theoretical study of the ETPA process in cesium atoms, focusing on the 6S1/2 --> 8S1/2 transition. The ETPA cross section is evaluated both with and without the far-off-resonance (FOR) approximation, including the contributions from intermediate atomic states and decoherence effects. The quantum state of light considered is described by the joint spectral amplitude of photon-pairs produced by the spontaneous parametric down-conversion process. When the FOR approximation is applied, the enhancement factor is constant (36*pi). In contrast, without this approximation the enhancement factor oscillates with the entanglement time, and achieves a maximum value of ~500. These results show the limitations of approximations when calculating the ETPA cross section and contribute to the understanding of the discrepancies between theoretical and experimental values for the ETPA cross section in different samples. The numbers presented in this work can be a starting point for designing experiments aimed at measuring ETPA cross sections in alkali atoms.
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.