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arXiv:2302.02846 · Physical Review A

Enhancement of broadband entangled two-photon absorption by resonant spectral phase flips

Baihong Li, Holger Friedrich Hofmann

Published Jul 14, 2023• 6 citations
arXivHTMLPDF

Abstract

Broadband energy-time entanglement can be used to enhance the rate of two-photon absorption (TPA) by combining a precise two-photon resonance with a very short coincidence time. Because of this short coincidence time, broadband TPA is not sensitive to the spectrum of intermediate levels, making it the optimal choice when the intermediate transitions are entirely virtual. In the case of distinct intermediate resonances, it is possible to enhance TPA by introducing a phase dispersion that matches the intermediate resonances. Here, we consider the effects of a phase flip in the single photon spectrum, where the phases of all frequencies above a certain frequency are shifted by half a wavelength relative to the frequencies below this frequency. The frequency at which the phase is flipped can then be scanned to reveal the position of intermediate resonances. We find that a resonant phase flip maximizes the contributions of the asymmetric imaginary part of the dispersion that characterizes a typical resonance, resulting in a considerable enhancement of the TPA rate. Due to the bosonic symmetry of TPA, the enhancement is strongest when the resonance occurs when the frequency difference of the two photons is much higher than the linewidth of the resonance. Our results indicate that broadband entangled TPA with spectral phase flips may be suitable for phase-sensitive spectroscopy at the lower end of the spectrum where direct photon detection is difficult.

DOI
10.1103/physreva.108.013706

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Broadband energy-time entanglement can be used to enhance the rate of two-photon absorption (TPA) by combining a precise two-photon resonance with a very short coincidence time. Because of this short coincidence time, broadband TPA is not sensitive to the spectrum of intermediate levels, making it the optimal choice when the intermediate transitions are entirely virtual. In the case of distinct intermediate resonances, it is possible to enhance TPA by introducing a phase dispersion that matches the intermediate resonances. Here, we consider the effects of a phase flip in the single photon spectrum, where the phases of all frequencies above a certain frequency are shifted by half a wavelength relative to the frequencies below this frequency. The frequency at which the phase is flipped can then be scanned to reveal the position of intermediate resonances. We find that a resonant phase flip maximizes the contributions of the asymmetric imaginary part of the dispersion that characterizes a typical resonance, resulting in a considerable enhancement of the TPA rate. Due to the bosonic symmetry of TPA, the enhancement is strongest when the resonance occurs when the frequency difference of the two photons is much higher than the linewidth of the resonance. Our results indicate that broadband entangled TPA with spectral phase flips may be suitable for phase-sensitive spectroscopy at the lower end of the spectrum where direct photon detection is difficult.
It is well known that energy-time entanglement can enhance two-photon absorption (TPA) by simultaneously optimizing the two-photon resonance and the coincidence rate of photons at the absorber. However, the precise relation between entanglement and the TPA rate depends on the coherences of intermediate states involved in the transition, making it a rather challenging task to identify universal features of TPA processes. In the present paper, we show that the theory can be simplified greatly by separating the two-photon resonance from the temporal dynamics of the intermediate levels. The result is a description of the role of entanglement in the TPA process by a one-dimensional coherence in the Hilbert space defined by the arrival-time difference of the two photons. Transformation into the frequency-difference basis results in Kramers-Kronig relations for the TPA process, separating off-resonant contributions of virtual levels from resonant contributions. In particular, it can be shown that off-resonant contributions are insensitive to the frequencies of the associated virtual states, indicating that virtual-state spectroscopy of levels above the final two-photon excited state is not possible.
Energy-time entanglement can enhance two photon absorption by combining a precise two photon resonance with temporal correlations between the arrival times of the two photons. In general, the optimal timing of photon arrival is determined by the dynamics of the system between the initial and the final excitations. In this presentation, we show that the optimal timing of photon arrival corresponds to a specific phase dispersion in the frequency difference of the two photons. The absorption cross-section of energy-time entangled photons can be enhanced beyond the rate observed for optimal photon coincidence by adjusting the phase dispersion of one of the photons to match the optimal characteristics. We determine the maximal enhancement factor as a function of the bandwidth of the intermediate states and their detuning relative to the average photon frequency. Significant additional enhancements can be achieved when the bandwidth of the intermediate states is very narrow.
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.
When a low flux of time-frequency-entangled photon pairs (EPP) illuminates a two-photon transition, the rate of two-photon absorption (TPA) can be enhanced considerably by the quantum nature of photon number correlations and frequency correlations. We use a quantum-theoretic derivation of entangled TPA (ETPA) and calculate an upper bound on the amount of quantum enhancement that is possible in such systems. The derived bounds indicate that in order to observe ETPA the experiments would need to operate at a combination of significantly higher rates of EPP illumination, molecular concentrations, and conventional TPA cross sections than are achieved in typical experiments.
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.
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.