Aerosolized droplet mediated self-assembly of photosynthetic pigment analogues and deposition onto substrates

Vivek B. Shah, Pratim Biswas

Research output: Contribution to journalArticlepeer-review

17 Scopus citations

Abstract

Self-assembled photosynthetic molecules have a high extinction coefficient and a broad absorption in the infrared region, and these properties can be used to improve the efficiency of solar cells. We have developed a single-step method for the self-assembly of synthetic chlorin molecules (analogues of native bacteriochlorophylls) in aerosolized droplets, containing a single solvent and two solvents, to synthesize biomimetic light-harvesting structures. In the single-solvent approach, assembly is promoted by a concentration-driven process due to evaporation of the solvent. The peak absorbance of Zn(II) 3-(1-hydroxyethyl)-10-phenyl-131-oxophorbine (1) in methanol shifted from 646 nm to 725 nm (∼80 nm shift) after assembly, which is comparable to the shift observed in the naturally occurring assembly of bacteriochlorophyll c. Although assembly is thermodynamically favorable, the kinetics of self-assembly play an important role, and this was demonstrated by varying the initial concentration of the pigment monomer. To overcome kinetic limitations, a two-solvent approach using a volatile solvent (tetrahydrofuran) in which the dye is soluble and a less volatile solvent (ethanol) in which the dye is sparingly soluble was demonstrated to be effective. The effect of molecular structure is demonstrated by spraying the sterically hindered Zn(II) 3-(1-hydroxyethyl)-10- mesityl-131-oxophorbine (2), which is an analogue of 1, under similar conditions. The results illustrate a valuable and facile aerosol-based method for the formation of films of supramolecular assemblies.

Original languageEnglish (US)
Pages (from-to)1429-1438
Number of pages10
JournalACS Nano
Volume8
Issue number2
DOIs
StatePublished - Feb 25 2014
Externally publishedYes

Keywords

  • aerosol route
  • bacteriochlorophyll analogues
  • chlorin
  • photosynthetic antenna
  • supramolecular self-assembly

ASJC Scopus subject areas

  • Materials Science(all)
  • Engineering(all)
  • Physics and Astronomy(all)

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