Molecular model of J-aggregated pseudoisocyanine fibers

Bricker, William P.; Banal, James L.; Stone, Matthew B.; Bathe, Mark

doi:10.1063/1.5036656

Title: Molecular model of J-aggregated pseudoisocyanine fibers

Journal Article · Fri Jul 13 00:00:00 EDT 2018 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/1.5036656· OSTI ID:1512946

^[1];

^[1]; Stone, Matthew B. ^[1]; Bathe, Mark ^[1]

Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)

Aggregated cyanines form ordered supramolecular structures with the potential to transport energy efficiently over long distances, a hallmark of photosynthetic light-harvesting complexes. In concentrated aqueous solution, pseudoisocyanine (PIC) spontaneously forms fibers with a chiral J-band red-shifted 1600 cm^-1 from the monomeric 0–0 transition. A cryogenic transmission electron microscopy analysis of these fibers show an average fiber width of 2.89 nm, although the molecular-level structure of the aggregate is currently unknown. To determine a molecular model for these PIC fibers, the calculated spectra and dynamics using a Frenkel exciton model are compared to experiment. A chiral aggregate model in which the PIC monomers are neither parallel nor orthogonal to the long axis of the fiber is shown to replicate the experimental spectra most closely. This model can be physically realized by the sequential binding of PIC dimers and monomers to the ends of the fiber. Furthermore, these insights into the molecular aggregation model for aqueous PIC can also be applied to other similar cyanine-based supramolecular complexes with the potential for long-range energy transport, a key building block for the rational design of novel excitonic systems

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Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Center for Excitonics (CE); Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0001088; SC0016353

OSTI ID:: 1512946

Alternate ID(s):: OSTI ID: 1460131

Journal Information:: Journal of Chemical Physics, Vol. 149, Issue 2; ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 11 works

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