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

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

doi:10.48550/arxiv.2012.06736

Cited by 4 publications

(5 citation statements)

References 11 publications

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“…Some experimental studies [14,15] have reported apparent values of ETPA excitation probabilities that greatly exceed the values predicted here (for example, Eq.142). Other studies have recently found upper bounds on EPTA probabilities that are much smaller and in line with the present predictions [16,17,18], but the final word has yet to be spoken on this question.…”

Section: Summary and Discussionsupporting

confidence: 91%

Entangled two-photon absorption by atoms and molecules: A quantum optics tutorial

Raymer

Landes

Marcus

2021

The Journal of Chemical Physics

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Two-photon absorption (TPA) and other nonlinear interactions of molecules with time-frequencyentangled photon pairs (EPP) has been predicted to display a variety of fascinating effects. Therefore, their potential use in practical quantum-enhanced molecular spectroscopy requires close examination. This paper presents in tutorial style 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, 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.

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Section: Summary and Discussionsupporting

confidence: 91%

Entangled two-photon absorption by atoms and molecules: A quantum optics tutorial

Raymer

Landes

Marcus

2021

The Journal of Chemical Physics

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“…( 8), we can write Eq. (3) as: (9) where in the general case: (10) is the integrated amplitude (antidiagonal projection) for TPA at a particular two-photon detuning x. A graphical interpretation is given in Fig.…”

Section: Theory Of Etpamentioning

confidence: 99%

“…[ 17 ] Other experimental studies place the ETPA cross section many orders of magnitude smaller. [9,11] Without the presence of extremely large values of , two-photon absorption at very low flux levels, where the quantum…”

Section: Introductionmentioning

confidence: 99%

Quantifying the enhancement of two-photon absorption due to spectral-temporal entanglement

Landes¹,

Raymer²,

Allgaier³

et al. 2021

Opt. Express

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When a low flux of time-frequency-entangled photon pairs (EPP) illuminates a twophoton transition, the rate of two-photon absorption (TPA) can be enhanced considerably by the quantum nature of photon number correlations and frequency correlations. We present 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.

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

Cited by 4 publications

References 11 publications

Entangled two-photon absorption by atoms and molecules: A quantum optics tutorial

Entangled two-photon absorption by atoms and molecules: A quantum optics tutorial

Quantifying the enhancement of two-photon absorption due to spectral-temporal entanglement

Quantum metrology of two-photon absorption

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