title: Immobilization of functional light antenna structures derived from the filamentous green bacterium Chloroflexus aurantiacus.
abstract: The integration of highly efficient, natural photosynthetic light antenna structures into engineered systems while their biophotonic capabilities are maintained has been an elusive goal in the design of biohybrid photonic devices. In this study, we report a novel technique to covalently immobilize nanoscaled bacterial light antenna structures known as chlorosomes from Chloroflexus aurantiacus on both conductive and nonconductive glass while their energy transducing functionality was maintained. Chlorosomes without their reaction centers (RCs) were covalently immobilized on 3-aminoproyltriethoxysilane (APTES) treated surfaces using a glutaraldehyde linker. AFM techniques verified that the chlorosomes maintained their native ellipsoidal ultrastructure upon immobilization. Results from absorbance and fluorescence spectral analysis (where the Stokes shift to 808/810 nm was observed upon 470 nm blue light excitation) in conjunction with confocal microscopy confirm that the functional integrity of immobilized chlorosomes was also preserved. In addition, experiments with electrochemical impedance spectroscopy (EIS) suggested that the presence of chlorosomes in the electrical double layer of the electrode enhanced the electron transfer capacity of the electrochemical cell. Further, chronoamperometric studies suggested that the reduced form of the Bchl- c pigments found within the chlorosome modulate the conduction properties of the electrochemical cell, where the oxidized form of Bchl- c pigments impeded any current transduction at a bias of 0.4 V within the electrochemical cell. The results therefore demonstrate that the intact chlorosomes can be successfully immobilized while their biophotonic transduction capabilities are preserved through the immobilization process. These findings indicate that it is feasible to design biophotonic devices incorporating fully functional light antenna structures, which may offer significant performance enhancements to current silicon-based photonic devices for diverse technological applications ranging from CCD devices used in retinal implants to terrestrial and space fuel cell applications.
authors.affiliation: Harrington Department of Bioengineering, Arizona State University, Tempe, Arizona 85287, USA.
authors.forename: Arati
authors.initials: A
authors.lastname: Sridharan
authors.forename: Jit
authors.initials: J
authors.lastname: Muthuswamy
authors.forename: Jeffrey T
authors.initials: JT
authors.lastname: Labelle
authors.forename: Vincent B
authors.initials: VB
authors.lastname: Pizziconi
mesh_terms: D041861:Chloroflexus / Q000737:chemistry* / Q000648:ultrastructure; D003116:Color; D004563:Electrochemistry; D018625:Microscopy, Atomic Force; D008855:Microscopy, Electron, Scanning; D016877:Oxidants / Q000737:chemistry; D013050:Spectrometry, Fluorescence
chemical_list: D016877:Oxidants