Prominent Signatures of Energy Transfer in Action-Detected Spectra of a Cyanobacterial Photosynthetic Protein

Fuente: arXiv
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Autori principali: Ghosh, Sayan, Sahu, Amitav, Gonzalez-Migoni, Stephanie, Jansen, Thomas L. C., Tiwari, Vivek
Natura: Preprint
Pubblicazione: 2026
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author Ghosh, Sayan
Sahu, Amitav
Gonzalez-Migoni, Stephanie
Jansen, Thomas L. C.
Tiwari, Vivek
author_facet Ghosh, Sayan
Sahu, Amitav
Gonzalez-Migoni, Stephanie
Jansen, Thomas L. C.
Tiwari, Vivek
contents Action-detected two-dimensional electronic spectroscopy (A-2DES) could potentially be a versatile chemical tool with applicability across a range of photophysical observables such as photocurrent, photoionization, or fluorescence. However, a prominent absence of excited state energy/charge transfer dynamics signals in archetypal photosynthetic proteins has suggested severe limitations of A-2DES in probing large aggregates where sensitivity to excited state dynamics is proposed to go down as 1/N, where N is the aggregate size. We report measurements of energy transfer dynamics in a cyanobacterial protein through both conventional and fluorescence 2DES (F-2DES), where the dynamics reported by F-2DES is quite prominent and comparable to that measured by conventional 2DES. Analysis of our experiments combined with coarse-grained simulations of the spectra suggest that the 1/N limit argument, which assumes infinitely fast intra-exciton manifold equilibration, is modified in case of cyanobacterial proteins because of slow annihilation. Our results suggest that action detection may in fact be well-suited to probe exciton diffusion across weakly coupled systems.
format Preprint
id arxiv_https___arxiv_org_abs_2604_25105
institution arXiv
publishDate 2026
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spellingShingle Prominent Signatures of Energy Transfer in Action-Detected Spectra of a Cyanobacterial Photosynthetic Protein
Ghosh, Sayan
Sahu, Amitav
Gonzalez-Migoni, Stephanie
Jansen, Thomas L. C.
Tiwari, Vivek
Chemical Physics
Action-detected two-dimensional electronic spectroscopy (A-2DES) could potentially be a versatile chemical tool with applicability across a range of photophysical observables such as photocurrent, photoionization, or fluorescence. However, a prominent absence of excited state energy/charge transfer dynamics signals in archetypal photosynthetic proteins has suggested severe limitations of A-2DES in probing large aggregates where sensitivity to excited state dynamics is proposed to go down as 1/N, where N is the aggregate size. We report measurements of energy transfer dynamics in a cyanobacterial protein through both conventional and fluorescence 2DES (F-2DES), where the dynamics reported by F-2DES is quite prominent and comparable to that measured by conventional 2DES. Analysis of our experiments combined with coarse-grained simulations of the spectra suggest that the 1/N limit argument, which assumes infinitely fast intra-exciton manifold equilibration, is modified in case of cyanobacterial proteins because of slow annihilation. Our results suggest that action detection may in fact be well-suited to probe exciton diffusion across weakly coupled systems.
title Prominent Signatures of Energy Transfer in Action-Detected Spectra of a Cyanobacterial Photosynthetic Protein
topic Chemical Physics
url https://arxiv.org/abs/2604.25105