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

TL;DR

This paper presents a non-perturbative theoretical approach to study entangled-photon fields generated by strong pump pulses, revealing nonlinear scaling of two-photon absorption and proposing an experimental scheme to isolate entanglement effects.

Contribution

It introduces a non-perturbative method for analyzing entangled-photon fields under strong pumping and proposes an experimental setup to isolate entanglement contributions in TPA signals.

Findings

TPA signal scales non-linearly with pump intensity.

Increasing pump bandwidth extends the linear scaling regime.

Proposed scheme filters entangled photon contributions in experiments.

Abstract

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.