A Comparative Study of Coherent and Action-Detected 2D Electronic Spectroscopies of a Multichromophore Photosynthetic System

[2608.19721] A Comparative Study of Coherent and Action-Detected 2D Electronic Spectroscopies of a Multichromophore Photosynthetic System Skip to main content Search Submit Donate Log in Physics > Chemical Physics arXiv:2608.19721 (physics) [Submitted on 20 Aug 2026 ( v1 ), last revised 27 Aug 2026 (this version, v2)] Title: A Comparative Study of Coherent and Action-Detected 2D Electronic Spectroscopies of a Multichromophore Photosynthetic System Authors: Edoardo Amarotti , Ajeet Kumar , Luca Bolzonello , David Bina , Tõnu Pullerits , Donatas Zigmantas View PDF HTML (experimental) Abstract: Coherent two-dimensional electronic spectroscopy (C-2DES) is a powerful tool for resolving excitonic structure and dynamics in light-harvesting complexes with dense energy-level manifolds. In contrast, action-detected 2DES has seen limited use on such systems, and its capacity to reveal electronic structure and dynamics remains unclear. Here we compare C-2DES and fluorescence-detected 2DES (F-2DES) on the major plant light-harvesting complex (LHCII) at 78 K. C-2DES resolves excitonic features and their spectral evolution, mapping energy-transfer pathways. F-2DES shows strong cross-peaks, but these are largely time-invariant and dominated by incoherent mixing, obscuring the dynamics. C-2DES is therefore preferred for resolving ultrafast energy transfer in light-harvesting complexes and other large interacting networks. Combined, the two measurements directly quantify the suppression of population dynamics by incoherent mixing, confirming that nearly the entire LHCII trimer network contributes. We also identify pulse-shaper nonlinearities in F-2DES as spurious features, highlighting the need for rigorous artifact suppression. Subjects: Chemical Physics (physics.chem-ph) Cite as: arXiv:2608.19721 [physics.chem-ph] (or arXiv:2608.19721v2 [physics.chem-ph] for this version) https://doi.org/10.48550/arXiv.2608.19721 Focus to learn more arXiv-issued DOI via DataCite Submission history From: Edoardo Amarotti [ view email ] [v1] Thu, 20 Aug 2026 07:18:10 UTC (3,079 KB) [v2] Thu, 27 Aug 2026 09:06:14 UTC (3,080 KB) Full-text links: Access Paper: View PDF HTML (experimental) TeX Source view license Current browse context: physics.chem-ph < prev | next > new | recent | 2026-08 Change to browse by: physics References & Citations SciX Google Scholar Semantic Scholar export BibTeX citation Bookmark Bibliographic Tools Bibliographic and Citation Tools Bibliographic Explorer Toggle Bibliographic Explorer ( What is the Explorer? ) Connected Papers Toggle Connected Papers ( What is Connected Papers? ) Litmaps Toggle Litmaps ( What is Litmaps? ) scite.ai Toggle scite Smart Citations ( What are Smart Citations? ) Code, Data, Media Code, Data and Media Associated with this Article alphaXiv Toggle alphaXiv ( What is alphaXiv? ) Links to Code Toggle CatalyzeX Code Finder for Papers ( What is CatalyzeX? ) DagsHub Toggle DagsHub ( What is DagsHub? ) GotitPub Toggle Gotit.pub ( What is GotitPub? ) Huggingface Toggle Hugging Face ( What is Huggingface? ) ScienceCast Toggle ScienceCast ( What is ScienceCast? ) Demos Demos Replicate Toggle Replicate ( What is Replicate? ) Spaces Toggle Hugging Face Spaces ( What is Spaces? ) Spaces Toggle TXYZ.AI ( What is TXYZ.AI? ) Related Papers Recommenders and Search Tools Link to Influence Flower Influence Flower ( What are Influence Flowers? ) Core recommender toggle CORE Recommender ( What is CORE? ) Author Venue Institution Topic About arXivLabs arXivLabs: experimental projects with community collaborators arXivLabs is a framework that allows collaborators to develop and share new arXiv features directly on our website. Both individuals and organizations that work with arXivLabs have embraced and accepted our values of openness, community, excellence, and user data privacy. arXiv is committed to these values and only works with partners that adhere to them. Have an idea for a project that will add value for arXiv's community? Learn more about arXivLabs . Which authors of this paper are endorsers? | Disable MathJax ( What is MathJax? ) We gratefully acknowledge support from our major funders , member institutions , and all contributors. About · Help · Contact · Subscribe · Copyright · Privacy · Accessibility · Operational Status (opens in new tab)

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