Tuning the Fermi energy of silicon through doping leads to alignment of silicon bands with the redox active sites of photosystem I. Integrating photosystem I films with p-doped silicon results in the highest reported photocurrent enhancement for a biohybrid electrode based on photosystem I.
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http://dx.doi.org/10.1002/adma.201202794 | DOI Listing |
J Chem Theory Comput
December 2024
Department of Chemistry and Biochemistry, Kent State University, Kent, Ohio 44242, United States.
A density functional theory framework is developed to study electronic excited states affected by an anisotropic dielectric environment. In particular, an anisotropic dielectric screened range-separated hybrid (SRSH[r]) functional is defined and combined with an anisotropic polarizable continuum model (PCM) implemented through a generalized Poisson equation solver. We develop the SRSH-PCM(r) approach and use it to quantify the effect of anisotropy on an excited charge transfer (CT) state energy.
View Article and Find Full Text PDFNanoscale Adv
January 2024
Department of Chemical and Biomolecular Engineering, Vanderbilt University Nashville Tennessee 37235-1604 USA
Photosystem I (PSI) is an intrinsically photoactive multi-subunit protein that is found in higher order photosynthetic organisms. PSI is a promising candidate for renewable biohybrid energy applications due to its abundance in nature and its high quantum yield. To utilize PSI's light-responsive properties and to overcome its innate electrically insulating nature, the protein can be paired with a biologically compatible conducting polymer that carries charge at appropriate energy levels, allowing excited PSI electrons to travel within a composite network upon light excitation.
View Article and Find Full Text PDFPhotosynth Res
December 2024
Molecular Biophysics and Integrated Bioimaging Division, Lawrence Berkeley National Laboratory, University of California, Berkeley, CA, 94720, USA.
Organic bilayers or amorphous silica films of a few nanometer thickness featuring embedded molecular wires offer opportunities for chemically separating while at the same time electronically connecting photo- or electrocatalytic components. Such ultrathin membranes enable the integration of components for which direct coupling is not sufficiently efficient or stable. Photoelectrocatalytic systems for the generation or utilization of renewable energy are among the most prominent ones for which ultrathin separation layers open up new approaches for component integration for improving efficiency.
View Article and Find Full Text PDFNanoscale Adv
September 2023
Department of Chemical and Biomolecular Engineering, Vanderbilt University Nashville TN 37235-1604 USA
The combination of conducting polymers with electro- and photoactive proteins into thin films holds promise for advanced energy conversion materials and devices. The emerging field of protein electronics requires conductive soft materials in a composite with electrically insulating proteins. The electropolymerization of pyrrole through voids in a drop-casted photosystem I (PSI) multilayer film enables the straightforward fabrication of photoactive and conductive biohybrid films.
View Article and Find Full Text PDFPhotosynth Res
March 2023
Department of Chemical and Biomolecular Engineering, Vanderbilt University, Nashville, TN, 37235-1604, USA.
One of the main barriers to making efficient Photosystem I-based biohybrid solar cells is the need for an electrochemical pathway to facilitate electron transfer between the P reaction center of Photosystem I and an electrode. To this end, nature provides inspiration in the form of cytochrome c, a natural electron donor to the P site. Its natural ability to access the P binding pocket and reduce the reaction center can be mimicked by employing cytochrome c, which has a similar protein structure and redox chemistry while also being compatible with a variety of electrode surfaces.
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