A new protein-based approach has been developed for the construction of light-harvesting systems through self-assembly. The building blocks were prepared by attaching fluorescent chromophores to cysteine residues introduced on tobacco mosaic virus coat protein monomers. When placed under the appropriate buffer conditions, these conjugates could be assembled into stacks of disks or into rods that reached hundreds of nanometers in length. Characterization of the system using fluorescence spectroscopy indicated that efficient energy transfer could be achieved from large numbers of donor chromophores to a single acceptor. Energy transfer is proposed to occur through direct donor-acceptor interactions, although degenerate donor-to-donor transfer events are also possible. Three-chromophore systems were also prepared to achieve broad spectrum light collection with over 90% overall efficiency. Through the combination of self-organizing biological structures and synthetic building blocks, a highly tunable new method has emerged for the construction of photovoltaic device components.
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http://dx.doi.org/10.1021/ja063887t | DOI Listing |
Angew Chem Int Ed Engl
January 2025
University of Science and Technology Beijing, School of Chemistry and Biological Engineering, CHINA.
Designing and realizing new topologies represent one of the most important ways toward developing new structures and functionalities for molecule-based frameworks including SOFs, MOFs, and COFs. Herein, Aldol condensation between 5,10,15,20-tetrayl(tetrakis(([1,1':3',1''-terphenyl]-4,4''-dicarbaldehyde)))-porphyrin (TTEP) and 2,4,6-trimethyl-1,3,5-triazine (TMT) affords the vinylene-linked 3D covalent organic framework Por-COF-cya. Powder X-ray diffraction (PXRD) in combination with structural simulation reveals its high crystalline structure with an unprecedented cya topology in the molecule-based frameworks reported thus far.
View Article and Find Full Text PDFJ Chem Phys
January 2025
Department of Physics, University of Pretoria, 0002 Pretoria, South Africa.
Much can be learned about molecular aggregates by modeling their fluorescence-type spectra. In this study, we systematically describe the accuracy of various methods for simulating fluorescence-type linear spectra in a dimer system with a complex system-environment interaction, which serves as a model for various molecular aggregates, including most photosynthetic light-harvesting complexes (LHCs). We consider the approximate full cumulant expansion (FCE), complex time-dependent Redfield (ctR), time-independent Redfield, and modified Redfield methods and calculate their accuracy as a function of the site energy gap and coupling, excitonic energy gap, and dipole factor (i.
View Article and Find Full Text PDFMacromol Rapid Commun
January 2025
School of Chemistry and Chemical Engineering, Nantong University, Nantong, 226019, China.
A novel aggregation-induced emission (AIE)-based artificial light-harvesting system (LHS) is successfully assembled via the host-guest interaction of bis-naphthylacrylonitrile derivative (BND), water-soluble pillar[5]arene (WP5), and sulforhodamine 101 (SR101). After host-guest assembly, the formed WP5⊃BND complexes spontaneously self-aggregated into WP5⊃BND nanoparticles (donors) and SR101 (acceptors) is introduced into WP5⊃BND to fabricate WP5⊃BND-SR101 LHS. Through the investigation of energy transfer between donors and acceptors, the artificial light-harvesting processes are certified in WP5⊃BND-SR101 LHS and the absolute fluorescence quantum yields (Φ) are significantly improved from 8.
View Article and Find Full Text PDFACS Nano
January 2025
Sauvage Laboratory for Smart Materials, School of Materials Science and Engineering, Harbin Institute of Technology (Shenzhen), Shenzhen 518055, China.
With the potential to surpass the Shockley-Queisser (S-Q) limitation for solar energy conversion, the bulk photovoltaic (BPV) effect, which is induced by the broken inversion symmetry of the lattice, presents prospects for future light-harvesting technologies. However, the development of BPV is largely limited by the low solar spectrum conversion efficiency of existing noncentrosymmetric materials with wide band gaps. This study reports that the strain-induced reduction of inversion symmetry can enhance the second-order nonlinear susceptibility (χ) of SnPSe crystals by an order of magnitude, which contributes to an extremely high value of 1.
View Article and Find Full Text PDFACS Omega
December 2024
Department of Physics and Beijing Key Laboratory of Optoelectronic Functional Materials and Micro-Nano Devices, Renmin University of China, Beijing 100872, China.
Photosynthesis in nature begins with light harvesting. The special pigment-protein complex converts sunlight into electron excitation that is transmitted to the reaction center, which triggers charge separation. Evidence shows that quantum coherence between electron excited states is important in the excitation energy transfer process.
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