skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Supramolecular self-assembly of bacteriochlorophyll c molecules in aerosolized droplets to synthesize biomimetic chlorosomes

Journal Article · · Journal of Photochemistry and Photobiology B: Biology
 [1];  [2];  [1];  [1];  [3];  [1];  [4];  [1];  [1]
  1. Washington Univ. in St. Louis, St. Louis, MO (United States)
  2. Washington Univ. in St. Louis, St. Louis, MO (United States); Johns Hopkins Univ., Baltimore, MD (United States)
  3. Washington Univ. in St. Louis, St. Louis, MO (United States); Univ. of California, Berkeley, CA (United States)
  4. Argonne National Lab. (ANL), Lemont, IL (United States)

The unique properties of chlorosomes, arising out of the self-assembled bateriochlorophyll (BChl) c structure, have made them attractive for use in solar cells. In this work, we have demonstrated the self-assembly of BChl c in aerosolized droplets to mimic naturally occurring chlorosomes. We compare two different methods for self-assembly of BChl c, one using a single-solvent and the other using two-solvents, and demonstrate the superiority of the two-solvent method. Results show that the self-assembled BChl c sprayed at different concentrations resulted in a varying red shift of 69-75 nm in absorption spectrum compared to the solution, which has peak at 668 nm corresponding to the monomeric BChl c. The sample fluoresces at 780 nm indicating a quality of self-assembly comparable to that observed in naturally occurring chlorosomes. In order to mimic chlorosomes, solution containing BChl c, BChl a, lipids and carotenes in same proportion as in chlorosomes is sprayed. The resulting self-assembly has an absorption peak at 750 nm, shifted by 82 nm compared to that of monomers and the fluorescence peak at 790 nm. Thus in presence of lipids and carotenes, both the absorption and fluorescence peaks are red shifted. Further, using grazing incidence small angle X-ray scattering (GISAXS), we characterized the deposited films, and the 2D X-ray scattering patterns of sample clearly indicate the distinct lamellar structure as present in chlorosomes. Here, the results of this work provide new insights into self-assembly in aerosolized droplets, which can be used for assembling a wide range of molecules.

Research Organization:
Argonne National Lab. (ANL), Argonne, IL (United States); Energy Frontier Research Centers (EFRC) (United States). Photosynthetic Antenna Research Center (PARC)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC02-06CH11357; SC0001035
OSTI ID:
1464756
Alternate ID(s):
OSTI ID: 1582781
Journal Information:
Journal of Photochemistry and Photobiology B: Biology, Vol. 185, Issue C; ISSN 1011-1344
Publisher:
ElsevierCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 6 works
Citation information provided by
Web of Science

References (31)

Chlorosome antenna complexes from green photosynthetic bacteria journal June 2013
Electrospray-assisted characterization and deposition of chlorosomes to fabricate a biomimetic light-harvesting device journal January 2010
Linker-Free Deposition and Adhesion of Photosystem I onto Nanostructured TiO 2 for Biohybrid Photoelectrochemical Cells journal January 2015
On the way to biomimetic dye aggregate solar cells journal January 2011
Hierarchal Light-Harvesting Aggregates and Their Potential for Solar Energy Applications journal February 2012
Multifunctional Nanoparticles Self-Assembled from Small Organic Building Blocks for Biomedicine journal June 2016
Giant light-harvesting nanoantenna for single-molecule detection in ambient light journal September 2017
Biological Applications of Supramolecular Assemblies Designed for Excitation Energy Transfer journal June 2015
Light-Harvesting Systems Based on Organic Nanocrystals To Mimic Chlorosomes journal January 2016
Anisotropic Organization and Microscopic Manipulation of Self-Assembling Synthetic Porphyrin Microrods That Mimic Chlorosomes: Bacterial Light-Harvesting Systems journal December 2011
Antenna organization in green photosynthetic bacteria. 1. Oligomeric bacteriochlorophyll c as a model for the 740 nm absorbing bacteriochlorophyll c in Chloroflexus aurantiacus chlorosomes journal December 1987
Autocatalyzed Self-Aggregation of (3 R )-[Et,Et]Bacteriochlorophyll c F Molecules in Nonpolar Solvents. Analysis of the Kinetics journal January 2000
The formation and characterization of the in vitro polymeric aggregates of bacteriochlorophyllc homologs fromChlorobium limicola in aqueous suspension in the presence of monogalactosyl diglyceride journal July 1994
Redox effects on the excited-state lifetime in chlorosomes and bacteriochlorophyll c oligomers journal January 1997
Self-aggregates of natural chlorophylls and their synthetic analogues in aqueous media for making light-harvesting systems journal November 2010
Scrambled Self-Assembly of Bacteriochlorophylls c and e in Aqueous Triton X-100 Micelles journal December 2013
Polymer–Chlorosome Nanocomposites Consisting of Non-Native Combinations of Self-Assembling Bacteriochlorophylls journal June 2017
Aerosolized Droplet Mediated Self-Assembly of Photosynthetic Pigment Analogues and Deposition onto Substrates journal January 2014
Effect of Carotenoids and Monogalactosyl Diglyceride on Bacteriochlorophyll c Aggregates in Aqueous Buffer: Implications for the Self-assembly of Chlorosomes¶ journal January 2004
A new bacteriochlorophyll a-protein complex associated with chlorosomes of green sulfur bacteria journal January 1986
De novo synthesis and properties of analogues of the self-assembling chlorosomal bacteriochlorophylls journal January 2011
Isolation and characterization of cytoplasmic membranes and chlorosomes from the green bacterium Chloroflexus aurantiacus. journal January 1982
Electrospraying of conducting liquids for monodisperse aerosol generation in the 4 nm to 1.8 μm diameter range journal September 1995
Electrospray of ionic precursor solutions to synthesize iron oxide nanoparticles: Modified scaling law journal February 2007
Effect of Carotenoid Biosynthesis Inhibition on the Chlorosome Organization in Chlorobium phaeobacteroides Strain CL1401 journal June 2000
Characterization and deposition of various light-harvesting antenna complexes by electrospray atomization journal September 2012
Structural Analysis of Block Copolymer Thin Films with Grazing Incidence Small-Angle X-ray Scattering journal May 2005
Multiple-scaled polymer surfaces investigated with micro-focus grazing-incidence small-angle X-ray scattering journal March 2003
Alternating syn-anti bacteriochlorophylls form concentric helical nanotubes in chlorosomes journal May 2009
X-Ray Scattering and Electron Cryomicroscopy Study on the Effect of Carotenoid Biosynthesis to the Structure of Chlorobium tepidum Chlorosomes journal July 2007
Lamellar Organization of Pigments in Chlorosomes, the Light Harvesting Complexes of Green Photosynthetic Bacteria journal August 2004

Cited By (1)

Using the Endogenous CRISPR-Cas System of Heliobacterium modesticaldum To Delete the Photochemical Reaction Center Core Subunit Gene journal September 2019