期刊
JOURNAL OF CHEMICAL PHYSICS
卷 149, 期 2, 页码 -出版社
AMER INST PHYSICS
DOI: 10.1063/1.5036656
关键词
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资金
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-SC0016353]
- Army Research Office (ARO-MURI) Award [W911NF1210420]
- Office of Naval Research Award [N00014-17-1-2609, N00014-13-1-0664, N00014-15-1-2830]
- Skoltech Award [1911/R]
- Koch Institute Support (core) from the National Cancer Institute [P30-CA14051]
- Center for Excitonics, an Energy Frontier Research Center - U.S. Department of Energy, Office of Science, and Office of Basic Energy Sciences [DE-SC0001088]
- Biophysical Instrumentation Facility for the Study of Complex Macromolecular Systems [NSF-0070319]
- U.S. Department of Energy (DOE) [DE-SC0016353] Funding Source: U.S. Department of Energy (DOE)
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. 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. Published by AIP Publishing.
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