Related papers: Photonic entanglement enhanced multidimensional spectroscopy for probing exciton correlations: theory and applications to photosynthetic aggregates

Photonic entanglement enhanced multidimensional spectroscopy for probing exciton correlations: theory and applications to photosynthetic aggregates

URL: http://arxiv.org/abs/2602.05080v1
Date: Wed, 04 Feb 2026 21:56:46 GMT
Title: Photonic entanglement enhanced multidimensional spectroscopy for probing exciton correlations: theory and applications to photosynthetic aggregates
Authors: Arunangshu Debnath, Shaul Mukamel,
Abstract summary: We propose an entangled photon pair-enhanced multidimensional spectroscopic technique.<n>It is sensitive to exciton-exciton interactions and correlations at the ultrafast timescale.<n>These insights can be used to explore multi-exciton dynamics using multiphoton entanglement.
Score: 0.0
License: http://creativecommons.org/licenses/by-nc-nd/4.0/
Abstract: Nonlinear spectroscopic techniques using entangled photon pairs provide an opportunity to exploit non-classical correlations encoded in two-photon wavefunctions to manipulate two-exciton wavefunctions. We propose an entangled photon pair-enhanced multidimensional spectroscopic technique which is sensitive to exciton-exciton interactions and correlations at the ultrafast timescale. Simulations for a dissipative photosynthetic aggregate reveal the superior ability of entangled photon pairs, compared to both transform-limited and frequency-chirped laser pulses, to manipulate excited-state absorption pathways. The corresponding spectral features in the two-dimensional spectrogram are interpreted in terms of one- and two-exciton resonances. The signal scales linearly with the incoming intensity of the photon sources. It is argued that classifying these resonances using entangled photon source at the perturbative limit allow for probing exciton correlations at the natural energy scale. These insights can be used to explore multi-exciton dynamics using multiphoton entanglement.

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