How large is the quantum enhancement of two-photon absorption by time-frequency entanglement of photon pairs?

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

doi:10.1364/optica.426674

Cited by 34 publications

(10 citation statements)

References 11 publications

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“…it creates a molecular excitation, and we have dropped the spatial dependence of the operators. A detailed account for the derivation of the ETPA probability can be found, e.g., in [49,52]. Here, we only present the final result which, neglecting the polarization degrees of freedom at first, reads…”

Section: The Modelmentioning

confidence: 99%

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Polarization-Entangled Two-Photon Absorption in Inhomogeneously Broadened Ensembles

Schlawin

2022

Front. Phys.

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Entangled photons are promising candidates for a variety of novel spectroscopic applications. In this paper, we simulate two-photon absorption (TPA) of entangled photons in a molecular ensemble with inhomogeneous broadening. We compare our results with a homogeneously broadened case and comment on the consequences for the possible quantum enhancement of TPA cross sections. We find that, while there are differences in the TPA cross section, this difference always remains small and of the order unity. We further consider the impact of the polarization degrees of freedom and carry out the orientational average of a model system Hamiltonian. We find that certain molecular geometries can give rise to a substantial polarization dependence of the entangled TPA rate. This effect can increase the TPA cross section by up to a factor of five.

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Section: The Modelmentioning

confidence: 99%

“…In theoretical work, recent analyses predict a very small enhancement of the ETPA cross section due to spectral entanglement [48,49]. The key assumption in these publications is that molecular resonances are broadened much more strongly than their atomic counterparts.…”

Section: Introductionmentioning

confidence: 99%

Polarization-Entangled Two-Photon Absorption in Inhomogeneously Broadened Ensembles

Schlawin

2022

Front. Phys.

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“…These promising features have sparked a lot of interest in two-photon EPPs interaction (EPPI) [6][7][8][9][10]. However, recent studies have shown that, due to the weakness of two-photon interactions and the low EPPs flux in the single-pair regime, EPPI with matter is expected to be around the noise limit of common systems [11][12][13]. This limitation gives rise to a need for improving the employed techniques for EPPI and optimizing the properties of the interaction medium.…”

Section: Introduction Nergy-time Entangled-photon Pairsmentioning

confidence: 99%

Measurement of the Second-Order Polarizability of Silver Nanoparticles With Reference-Free Hyper-Rayleigh Scattering for Entangled Photon Pair Interaction

et al. 2022

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Two-photon interactions of entangled-photon pairs with metallic nanoparticles (NPs) can be enhanced by localized surface-plasmon resonance. Recently, we have described how the properties of this quantum light-matter interaction can be deduced from classical second-harmonic generation measurements performed using a reference-free hyper-Rayleigh scattering method. Herein, we report the results of such classicallight characterization measurements. We obtain a large hyperpolarizability for the NPs, present the dependence of the hyperpolarizability on the NPs' spectral features, and show a dipolar emission pattern for the second-harmonic signal. Our results can be used to optimize entangled-photon pair interactions with metallic NPs to enable first ever detection of this process. Moreover, these results suggest that NPs may be used as source for ultra-broadband entangled-photon pairs through nonphasematched spontaneous parametric down-conversion.

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“…However, the magnitude of this enhancement has been questioned by recent experiments 17−22 and theoretical analysis. 23,24 Entangled two-photon absorption (ETPA) has been applied for electronic state characterization 25,26 but so far has not been demonstrated for detecting electron-nuclear wavepacket dynamics. The passage through conical intersections (CIs) 27 is a ubiquitous example of ultrafast dynamics in molecules.…”

mentioning

confidence: 99%

“…For example, two-photon absorption of time–energy entangled photons contains many nonclassical features and functionalities, − including linear rather than quadratic scaling with the pump intensity, − observing classically forbidden transitions, , suppressing classical one-photon resonant peaks, and manipulating excitation pathways. , A nearly 10 orders of magnitude enhancement of the two-photon absorption rate by entangled photons over classical light at the same photon fluxes has been reported, − thus reducing the risk of photodamage of biological samples. However, the magnitude of this enhancement has been questioned by recent experiments − and theoretical analysis. , …”

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confidence: 99%

Monitoring Wavepacket Dynamics at Conical Intersections by Entangled Two-Photon Absorption

Chen

Mukamel

2022

ACS Photonics

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In this theoretical study, we show how ultrafast electron–nuclear dynamics in a molecule can be monitored by two-photon absorption of time–energy entangled photon pairs generated by spontaneous parametric down-conversion with a narrow-band pump. The dynamics is tracked by a controllable signal-idler delay. Time correlation of the entangled photons enables an ultrafast measurement even with a monochromatic pump. The frequency anticorrelation of the photon pair allows the projection of the intermediate excited-state wavepacket onto an energy-selected vibrational level on a higher-lying electronic state with high energy resolution. Such joint high temporal and energy resolution is not possible with classical light. We demonstrate our scheme for a conical intersection model with four electronic states and two vibrational modes. The ultrafast nuclear wavepacket dynamics around the conical intersection is imprinted onto the time- and frequency-resolved entangled two-photon absorption signals. Electronic population dynamics is obtained by the frequency-integrated signal.

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How large is the quantum enhancement of two-photon absorption by time-frequency entanglement of photon pairs?

Abstract: We present a theoretical proof that the “quantum enhancement” of two-photon absorption, thought to be a means to improve molecular spectroscopy and imaging, is tightly bounded by the physics of photonic entanglement and nonlinear response.

Cited by 34 publications

References 11 publications

Polarization-Entangled Two-Photon Absorption in Inhomogeneously Broadened Ensembles

Polarization-Entangled Two-Photon Absorption in Inhomogeneously Broadened Ensembles

Measurement of the Second-Order Polarizability of Silver Nanoparticles With Reference-Free Hyper-Rayleigh Scattering for Entangled Photon Pair Interaction

Monitoring Wavepacket Dynamics at Conical Intersections by Entangled Two-Photon Absorption

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