Frenkel excitons in heat-stressed supramolecular nanocomposites enabled by tunable cage-like scaffolding

Ng, Kara; Webster, Megan; Carbery, William P.; Visaveliya, Nikunjkumar; Gaikwad, Pooja; Jang, Seogjoo J.; Kretzschmar, Ilona; Eisele, Dorthe M.

doi:10.1038/s41557-020-00563-4

Frenkel excitons in heat-stressed supramolecular nanocomposites enabled by tunable cage-like scaffolding

Journal Article · Mon Nov 16 00:00:00 EST 2020 · Nature Chemistry

DOI:https://doi.org/10.1038/s41557-020-00563-4· OSTI ID:1755123

^[1]; Webster, Megan; Carbery, William P.; Visaveliya, Nikunjkumar; Gaikwad, Pooja; ; Kretzschmar, Ilona;

Queens College, City University of New York

Delocalized Frenkel excitons—coherently shared excitations among chromophores—are responsible for the remarkable efficiency of supramolecular light-harvesting assemblies within photosynthetic organisms. The translation of nature’s design principles to applications in optoelectronic devices has been limited by the fragility of the supramolecular structures used and the delicate nature of Frenkel excitons, particularly under mildly changing solvent conditions and elevated temperatures and upon deposition onto solid substrates. Here, we overcome those functionalization barriers through composition of stable supramolecular light-harvesting nanotubes enabled by tunable (~4.3–4.9 nm), uniform (±0.3 nm) cage-like scaffolds. High-resolution cryogenic electron microscopy, combined with scanning electron microscopy, broadband femtosecond transient absorption spectroscopy and near-field scanning optical microscopy revealed that excitons within the cage-like scaffolds are robust, even under extreme heat stress, and control over nanocomposite dimensions is maintained on solid substrates. Our bio-inspired nanocomposites provide a general framework for the development of next-generation organic devices made from stable supramolecular materials.

View Accepted Manuscript (DOE)

Research Organization:: City Univ. of New York (CUNY), NY (United States); The City University of New York, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB)

Grant/Contract Number:: SC0001393; SC0018142

OSTI ID:: 1755123

Alternate ID(s):: OSTI ID: 1991456

Report Number(s):: DOE-Queens-1393-27

Journal Information:: Nature Chemistry, Journal Name: Nature Chemistry Journal Issue: 12 Vol. 12; ISSN 1755-4330

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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