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Bressan, Giovanni 
ORCID: https://orcid.org/0000-0001-7801-8495, Chambrier, Isabelle, Cammidge, Andrew N. ORCID: https://orcid.org/0000-0001-7912-4310 and Meech, Stephen R. ORCID: https://orcid.org/0000-0001-5561-2782
(2025)
Symmetry-breaking charge-separation in a subphthalocyanine dimer resolved by two-dimensional electronic spectroscopy.
The Journal of Physical Chemistry C.
ISSN 1932-7447
Abstract
Understanding the role of structural and environmental dynamics in the excited state properties of strongly coupled chromophores is of paramount importance in molecular photonics. Ultrafast, coherent, and multidimensional spectroscopies have been utilized to investigate such dynamics in the simplest model system, the molecular dimer. Here, we present a half-broadband two-dimensional electronic spectroscopy (HB2DES) study of the previously reported ultrafast symmetry-breaking charge separation (SB-CS) in the subphthalocyanine oxo-bridged homodimer μOSubPc2. Electronic structure calculations and 2D cross-peaks reveal the dimer’s excitonic structure, while ultrafast evolution of the multidimensional spectra unveils subtle features of structural relaxation, solvation dynamics, and inhomogeneous broadening in the SB-CS. Analysis of coherently excited vibrational motions reveals dimer-specific low-frequency Raman active modes coupled to higher-frequency vibrations localized on the SubPc cores. Finally, beatmap amplitude distributions characteristic of excitonic dimers with multiple bright states are reported and analyzed.
| Item Type: | Article |
|---|---|
| Additional Information: | Funding information: Engineering and Physical Sciences Research Council under award no. EP/V00817X/1. G.B. is grateful to the Leverhulme Trust for funding him through an Early Career Fellowship (Grant no. ECF-2023-195). |
| Uncontrolled Keywords: | photochemistry,ultrafast spectroscopy,ultrafast dynamics,excitonic coupling,subphthalocyanines |
| Faculty \ School: | Faculty of Science > School of Chemistry, Pharmacy and Pharmacology Faculty of Science > School of Chemistry (former - to 2024) |
| UEA Research Groups: | Faculty of Science > Research Groups > Centre for Photonics and Quantum Science Faculty of Science > Research Groups > Chemistry of Light and Energy |
| Related URLs: | |
| Depositing User: | LivePure Connector |
| Date Deposited: | 14 Jan 2025 01:00 |
| Last Modified: | 14 Jan 2025 01:00 |
| URI: | https://ueaeprints.uea.ac.uk/id/eprint/98199 |
| DOI: | 10.1021/acs.jpcc.4c07588 |
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