Artificial light-harvesting systems (ALHSs), which are closely related to Förster resonance energy transfer (FRET), are among the most attractive scientific topics during the past few decades. Specifically, binary ALHSs that are composed of a fluid donor and acceptor have a simplified composition and high number density of the donor units. However, largely due to the difficulty in obtaining a fluid donor, investigation of these systems is still quite limited, especially for the ionic systems. Herein, we report a new type of binary ALHS using an ionic naphthalimide (NPI) derivative as a donor, which shows greatly improved photoluminescence for its bicontinuous liquid structure. When blending with an acceptor such as rhodamine 6G or -4-[4-(dimethylamino)styryl]-methylpyridinium iodide, efficient FRET was confirmed by both experimental results and molecular dynamics simulations, with an energy transfer efficiency up to ∼90%. Tunable color, including white-light emission, was achieved by tuning the acceptor/donor ratio, opening the door for a variety of applications such as light-emitting diodes and photoluminescent inks.
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http://dx.doi.org/10.1021/acs.jpclett.2c02314 | DOI Listing |
ACS Catal
December 2024
Institute of Systems, Molecular and Integrative Biology, University of Liverpool, Liverpool L69 7ZB, U.K.
Synthetic photobiocatalysts are promising catalysts for valuable chemical transformations by harnessing solar energy inspired by natural photosynthesis. However, the synergistic integration of all of the components for efficient light harvesting, cascade electron transfer, and efficient biocatalytic reactions presents a formidable challenge. In particular, replicating intricate multiscale hierarchical assembly and functional segregation involved in natural photosystems, such as photosystems I and II, remains particularly demanding within artificial structures.
View Article and Find Full Text PDFJ Phys Chem B
December 2024
Dipartimento di Biotecnologie, Chimica e Farmacia, Università degli Studi di Siena, Via A. Moro 2, Siena 53100, Italy.
The functional units of natural photosynthetic systems control the process of converting sunlight into chemical energy. In this article, we explore a series of chemically and structurally modified bacteriochlorophyll and chlorophyll pigments through computational chemistry to evaluate their electronic spectroscopy properties. More specifically, we use multiconfigurational and time-dependent density functional theory methods, along with molecular dynamics simulations, to compute the models' energetics both in an implicit and explicit solvent environment.
View Article and Find Full Text PDFChem Sci
December 2024
Department of Chemistry, University of Warwick Coventry CV4 7AL UK
Self-assembling cyclic peptide nanotubes are fascinating supramolecular systems with promising potential for various applications, such as drug delivery, transmembrane ionic channels, and artificial light-harvesting systems. In this study, we present novel pH-responsive nanotubes based on asymmetric cyclic peptide-polymer conjugates. The pH response is introduced by a tertiary amine-based polymer, poly(dimethylamino ethyl methacrylate) (pDMAEMA) or poly(diethylamino ethyl methacrylate) (pDEAEMA) which is protonated at low pH.
View Article and Find Full Text PDFPlant Cell Environ
December 2024
Copernicus Institute for Sustainable Development, Utrecht University, Utrecht, Netherlands.
Leaf photosynthesis models are used extensively in photosynthesis research and are embedded in many larger scale models. Typical photosynthesis models simplify light intensity as the integrated intensity over the 400-700 nm waveband (photosynthetic active radiation, PAR). However, far-red light (700-750 nm, FR) also drives photosynthesis when supplied in addition to light within the PAR spectrum.
View Article and Find Full Text PDFJ Integr Plant Biol
December 2024
Key Laboratory of Photobiology, Photosynthesis Research Center, Institute of Botany, Chinese Academy of Sciences, Beijing, 100093, China.
Diatoms rely on fucoxanthin chlorophyll a/c-binding proteins (FCPs) for light harvesting and energy quenching under marine environments. Here we report two cryo-electron microscopic structures of photosystem I (PSI) with either 13 or five fucoxanthin chlorophyll a/c-binding protein Is (FCPIs) at 2.78 and 3.
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