Pump-intensity-scaling of Two-Photon-Absorption and Photon Statistics of Entangled-Photon Fields

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Hauptverfasser: Jadoun, Deependra, Harbola, Upendra, Chernyak, Vladimir Y., Mukamel, Shaul
Format: Preprint
Veröffentlicht: 2025
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author Jadoun, Deependra
Harbola, Upendra
Chernyak, Vladimir Y.
Mukamel, Shaul
author_facet Jadoun, Deependra
Harbola, Upendra
Chernyak, Vladimir Y.
Mukamel, Shaul
contents We use a non-perturbative theoretical approach to the parametric down-conversion (PDC) process, which generates entangled-photon field for an arbitrarily strong pump-pulse. This approach can be used to evaluate multi-point field correlation functions to compute nonlinear spectroscopic signals induced by a strong pump. The entangled-photon statistics is studied using Glauber's $g^{(2)}$ function, which helps understand the significance of the photon entanglement-time and the pump-pulse intensity on spectroscopic signals. Under the non-perturbative treatment of the entangled field, the two-photon absorption (TPA) signal shows linear to strongly non-linear growth with the pump intensity, rather than linear to quadratic scaling reported previously. An increase in the range of pump intensity for the linear scaling is observed as the pump band-width is increased. We propose an experimental scheme that can select contributions to the TPA signal that arise solely from interactions with the entangled photons, and filter out unentangled photon contributions, which are dominant at higher pump intensities, paving a way to explore the entanglement effects at higher intensities.
format Preprint
id arxiv_https___arxiv_org_abs_2502_09848
institution arXiv
publishDate 2025
record_format arxiv
spellingShingle Pump-intensity-scaling of Two-Photon-Absorption and Photon Statistics of Entangled-Photon Fields
Jadoun, Deependra
Harbola, Upendra
Chernyak, Vladimir Y.
Mukamel, Shaul
Chemical Physics
We use a non-perturbative theoretical approach to the parametric down-conversion (PDC) process, which generates entangled-photon field for an arbitrarily strong pump-pulse. This approach can be used to evaluate multi-point field correlation functions to compute nonlinear spectroscopic signals induced by a strong pump. The entangled-photon statistics is studied using Glauber's $g^{(2)}$ function, which helps understand the significance of the photon entanglement-time and the pump-pulse intensity on spectroscopic signals. Under the non-perturbative treatment of the entangled field, the two-photon absorption (TPA) signal shows linear to strongly non-linear growth with the pump intensity, rather than linear to quadratic scaling reported previously. An increase in the range of pump intensity for the linear scaling is observed as the pump band-width is increased. We propose an experimental scheme that can select contributions to the TPA signal that arise solely from interactions with the entangled photons, and filter out unentangled photon contributions, which are dominant at higher pump intensities, paving a way to explore the entanglement effects at higher intensities.
title Pump-intensity-scaling of Two-Photon-Absorption and Photon Statistics of Entangled-Photon Fields
topic Chemical Physics
url https://arxiv.org/abs/2502.09848