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  Two-photon absorption cross sections of pulsed entangled beams

Schlawin, F. (2024). Two-photon absorption cross sections of pulsed entangled beams. The Journal of Chemical Physics, 160(14): 144117. doi:10.1063/5.0196817.

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144117_1_5.0196817.pdf (Verlagsversion), 6MB
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https://doi.org/10.1063/5.0196817 (Verlagsversion)
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https://arxiv.org/abs/2312.00167 (Preprint)
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 Urheber:
Schlawin, F.1, 2, 3, Autor           
Affiliations:
1Condensed Matter Dynamics Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society, ou_1938285              
2University of Hamburg, ou_persistent22              
3The Hamburg Centre for Ultrafast Imaging, ou_persistent22              

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 Zusammenfassung: Entangled two-photon absorption (ETPA) could form the basis of nonlinear quantum spectroscopy at very low photon fluxes, since, at sufficiently low photon fluxes, ETPA scales linearly with the photon flux. When different pairs start to overlap temporally, accidental coincidences are thought to give rise to a “classical” quadratic scaling that dominates the signal at large photon fluxes and, thus, recovers a supposedly classical regime, where any quantum advantage is thought to be lost. Here, we scrutinize this assumption and demonstrate that quantum-enhanced absorption cross sections can persist even for very large photon numbers. To this end, we use a minimal model for quantum light, which can interpolate continuously between the entangled pair and a high-photon-flux limit, to analytically derive ETPA cross sections and the intensity crossover regime. We investigate the interplay between spectral and spatial degrees of freedom and how linewidth broadening of the sample impacts the experimentally achievable enhancement.

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Sprache(n): eng - English
 Datum: 2024-01-092024-03-242024-04-152024-04-14
 Publikationsstatus: Erschienen
 Seiten: -
 Ort, Verlag, Ausgabe: -
 Inhaltsverzeichnis: -
 Art der Begutachtung: Expertenbegutachtung
 Identifikatoren: DOI: 10.1063/5.0196817
arXiv: 2312.00167
 Art des Abschluß: -

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Projektname : I would like to thank Dr. Shahram Panahiyan for his helpful feedback on the manuscript and acknowledge the support from the Cluster of Excellence Advanced Imaging of Matter of the Deutsche Forschungsgemeinschaft (DFG)—EXC 2056—Project No. 390715994.
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Titel: The Journal of Chemical Physics
  Kurztitel : J. Chem. Phys.
Genre der Quelle: Zeitschrift
 Urheber:
Affiliations:
Ort, Verlag, Ausgabe: Woodbury, N.Y. : American Institute of Physics
Seiten: - Band / Heft: 160 (14) Artikelnummer: 144117 Start- / Endseite: - Identifikator: ISSN: 0021-9606
CoNE: https://pure.mpg.de/cone/journals/resource/954922836226