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Polymer–Chlorosome Nanocomposites Consisting of Non-Native Combinations of Self-Assembling Bacteriochlorophylls
journal contribution
posted on 2017-06-06, 00:00 authored by Gregory
S. Orf, Aaron M. Collins, Dariusz M. Niedzwiedzki, Marcus Tank, Vera Thiel, Adam Kell, Donald A. Bryant, Gabriel A. Montaño, Robert E. BlankenshipChlorosomes
are one of the characteristic light-harvesting antennas
from green sulfur bacteria. These complexes represent a unique paradigm:
self-assembly of bacteriochlorophyll pigments within a lipid monolayer
without the influence of protein. Because of their large size and
reduced complexity, they have been targeted as models for the development
of bioinspired light-harvesting arrays. We report the production of
biohybrid light-harvesting nanocomposites mimicking chlorosomes, composed
of amphiphilic diblock copolymer membrane bodies that incorporate
thousands of natural self-assembling bacteriochlorophyll molecules
derived from green sulfur bacteria. The driving force behind the assembly
of these polymer–chlorosome nanocomposites is the transfer
of the mixed raw materials from the organic to the aqueous phase.
We incorporated up to five different self-assembling pigment types
into single nanocomposites that mimic chlorosome morphology. We establish
that the copolymer-BChl self-assembly process works smoothly even
when non-native combinations of BChl homologues are included. Spectroscopic
characterization revealed that the different types of self-assembling
pigments participate in ultrafast energy transfer, expanding beyond
single chromophore constraints of the natural chlorosome system. This
study further demonstrates the utility of flexible short-chain, diblock
copolymers for building scalable, tunable light-harvesting arrays
for technological use and allows for an in vitro analysis of the flexibility
of natural self-assembling chromophores in unique and controlled combinations.
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Keywords
Self-Assembling Bacteriochlorophylls Chlorosomesself-assembling bacteriochlorophyll moleculescombinationchromophoreself-assembling pigment typeschlorosomebiohybrid light-harvesting nanocompositesbioinspired light-harvesting arraystunable light-harvesting arraysamphiphilic diblock copolymer membrane bodiessulfur bacteriacopolymer-BChl self-assembly process worksultrafast energy transfer
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