Two-photon absorption of time-frequency-entangled photon pairs by molecules: the roles of photon-number correlations and spectral correlations

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

doi:10.48550/arxiv.2012.05375

Cited by 7 publications

(17 citation statements)

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“…Most theoretical work on ETPA had neglected to account for the rate at which signal can be obtained in different regimes with regards to flux, optical pulse duration, and the amount of time-frequency entanglement. Recent calculations cast doubt over previously published experimental results and thus prompt further investigation into the magnitude of TPA enhancement through the use of EPP [13]. That treatment em-phasizes the separate roles played by spectral correlations and by photon-number correlations.…”

Section: Introductionmentioning

confidence: 93%

“…The advantage provided by photon-number correlations is operable only in the limit of extremely low photon flux where signals are practically unobservable below common detection thresholds. It has been predicted that the quantum enhancement factor (QEF ) for broadband transitions only depends on EPP bandwdith B and photon flux F , QEF ≈ B/F [13]. While the enhancement can be several orders of magnitude, it is predicted to be insufficient for observing TPA-induced fluorescence at typical EPP flux.…”

Section: Introductionmentioning

confidence: 99%

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Experimental feasibility of molecular two-photon absorption with isolated time-frequency-entangled photon pairs

Landes,

Allgaier,

Merkouche

et al. 2020

Preprint

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Entangled photon pairs have been promised to deliver a substantial quantum advantage for twophoton absorption spectroscopy. However, recent work has challenged the previously reported magnitude of quantum enhancement in two-photon absorption. Here, we present an experimental comparison of sum-frequency generation and molecular absorption, each driven by isolated photon pairs. We establish an upper bound on the enhancement for entangled-two-photon absorption in Rhodamine-6G, which lies well below previously reported values.

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Section: Introductionmentioning

confidence: 93%

Section: Introductionmentioning

confidence: 99%

Experimental feasibility of molecular two-photon absorption with isolated time-frequency-entangled photon pairs

Landes,

Allgaier,

Merkouche

et al. 2020

Preprint

Self Cite

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“…3,4 In addition to this absorption efficiency enhancement from the photon statistics, further enhancement is possible from the spectral shape and bandwidth of the frequency anticorrelated photon pairs. 5,6 Whether these mechanisms can provide a practical advantage for E2PA in molecules is still unclear.…”

Section: Introductionmentioning

confidence: 99%

Hot-Band Absorption Can Mimic Entangled Two-Photon Absorption

Mikhaylov¹,

Wilson²,

Parzuchowski³

et al. 2021

Preprint

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It has been proposed that entangled two-photon absorption (E2PA) can be observed with up to 10 orders of magnitude lower photon flux than its classical counterpart.However, there is a significant controversy regarding the magnitude of this quantum enhancement in excitation efficiency. We investigated the fluorescence signals from Rhodamine 6G and LDS798 excited with a CW laser or an entangled photon pair source at ≈1060 nm. We observed a signal that originates from hot-band absorption (HBA), which is one-photon absorption from thermally-populated vibrational levels of the ground electronic state. This mechanism, which has not been previously discussed in the context of E2PA, produces a signal with a linear power dependence, as would be expected for entangled two-photon excited fluorescence (E2PEF). For the typical conditions under which E2PEF measurements are performed, contributions from the HBA process could lead to a several orders-of-magnitude overestimate of the quantum advantage for excitation efficiency.

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“…Future research should extend these results to the multimode regime, where in addition to the photon statistics considered in this work time-energy entanglement provides an additional resource, whose impact on TPA measurements is the subject of an intense current debate [57][58][59][60].…”

Section: Absorbance Classical Fisher Informationmentioning

confidence: 97%

Quantum metrology of two-photon absorption

Muñoz

Frascella

Schlawin

2021

Phys. Rev. Research

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Two-photon absorption (TPA) is of fundamental importance in super-resolution imaging and spectroscopy. Its nonlinear character allows for the prospect of using quantum resources, such as entanglement, to improve measurement precision or to gain new information on, e.g., ultrafast molecular dynamics. Here, we establish the metrological properties of nonclassical squeezed light sources for precision measurements of TPA cross sections. We find that there is no fundamental limit for the precision achievable with squeezed states in the limit of very small cross sections. Considering the most relevant measurement strategies-namely photon counting and quadrature measurements-we determine the quantum advantage provided by squeezed states as compared to coherent states. We find that squeezed states outperform the precision achievable by coherent states when performing quadrature measurements, which provide improved scaling of the Fisher information with respect to the mean photon number ∼ n 4 . Due to the interplay of the incoherent nature and the nonlinearity of the TPA process, unusual scaling can also be obtained with coherent states, which feature a ∼ n 3 scaling in both quadrature and photon-counting measurements.

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Two-photon absorption of time-frequency-entangled photon pairs by molecules: the roles of photon-number correlations and spectral correlations

Cited by 7 publications

References 0 publications

Experimental feasibility of molecular two-photon absorption with isolated time-frequency-entangled photon pairs

Experimental feasibility of molecular two-photon absorption with isolated time-frequency-entangled photon pairs

Hot-Band Absorption Can Mimic Entangled Two-Photon Absorption

Quantum metrology of two-photon absorption

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