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Excitation energy transfer in the far-red absorbing violaxanthin/vaucheriaxanthin chlorophyll a complex from the eustigmatophyte alga FP5
摘要： This work highlights spectroscopic investigations on a new representative of photosynthetic antenna complexes in the LHC family, a putative violaxanthin/vaucheriaxanthin chlorophyll a (VCP) antenna complex from a freshwater Eustigmatophyte alga FP5. A representative VCP-like complex, named as VCP-B3 was studied with both static and time-resolved spectroscopies with the aim of obtaining a deeper understanding of excitation energy migration within the pigment array of the complex. Compared to other VCP representatives, the absorption spectrum of the VCP-B3 is strongly altered in the range of the chlorophyll a Qy band, and is substantially red-shifted with the longest wavelength absorption band at 707 nm at 77 K. VCP-B3 shows a moderate xanthophyll-to-chlorophyll a efficiency of excitation energy transfer in the 50–60% range, 20–30% lower from comparable VCP complexes from other organisms. Transient absorption studies accompanied by detailed data fitting and simulations support the idea that the xanthophylls that occupy the central part of the complex, complementary to luteins in the LHCII, are violaxanthins. Target analysis suggests that the primary route of xanthophyll-to-chlorophyll a energy transfer occurs via the xanthophyll S1 state.
关键词： Chlorophyll a,Light-harvesting complex,Transient absorption,Violaxanthin,Photosynthesis,Vaucheriaxanthin
更新于2025-11-19 16:46:39
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Unravelling the effect of charge dynamics at the plasmonic metal/semiconductor interface for CO2 photoreduction
摘要： Sunlight plays a critical role in the development of emerging sustainable energy conversion and storage technologies. Light-induced CO2 reduction by artificial photosynthesis is one of the cornerstones to produce renewable fuels and environmentally friendly chemicals. Interface interactions between plasmonic metal nanoparticles and semiconductors exhibit improved photoactivities under a wide range of the solar spectrum. However, the photo-induced charge transfer processes and their influence on photocatalysis with these materials are still under debate, mainly due to the complexity of the involved routes occurring at different timescales. Here, we use a combination of advanced in situ and time-resolved spectroscopies covering different timescales, combined with theoretical calculations, to unravel the overall mechanism of photocatalytic CO2 reduction by Ag/TiO2 catalysts. Our findings provide evidence of the key factors determining the enhancement of photoactivity under ultraviolet and visible irradiation, which have important implications for the design of solar energy conversion materials.
关键词： Ag/TiO2 catalysts,photocatalysis,plasmonic metal nanoparticles,sustainable energy,solar energy conversion,artificial photosynthesis
更新于2025-10-22 19:40:53
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Quantumness in light harvesting is determined by vibrational dynamics
摘要： We demonstrate for the multi-level spin-boson (MLSB) Hamiltonian, typically used to describe biological light-harvesting, that the distinction between quantum and classical dynamics is determined entirely by the thermal environment. In particular, any MLSB model featuring classical interactions with a classical bath is exactly equivalent in its absorption and energy transfer dynamics to a classical model involving coupled harmonic oscillators. This result holds in the linear response regime for both pulsed and incoherent excitation. In the biological context, this finding highlights the centrality of vibrational dynamics in determining the 'quantumness' of photosynthetic light-harvesting, particularly in the creation of the photosynthetic energy funnel where excitation energy concentrates near the reaction center via a series of downhill energy transfer events. These findings support the idea that this energy funnel is exclusively quantum-mechanical in origin, although it need not rely on entanglement.
关键词： vibrational dynamics,energy transfer,photosynthesis,quantumness,light harvesting,spin-boson model
更新于2025-09-23 15:23:52
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[IEEE IGARSS 2018 - 2018 IEEE International Geoscience and Remote Sensing Symposium - Valencia (2018.7.22-2018.7.27)] IGARSS 2018 - 2018 IEEE International Geoscience and Remote Sensing Symposium - Imaging Spectrometry and Fluorometry in Support of Flex: What Can We Learn from Multi-Scale Experiments?
摘要： In advance of the FLEX mission, experimental studies are needed to better understand the factors driving Solar-Induced Fluorescence (SIF) emission from vegetation across different temporal and spatial scales. Here, we present findings from boreal (evergreen and deciduous) forest trees and Midwestern (annual) crops, illustrating effects of seasonal downregulation and drought on the fluorescence signals. Further work is needed to develop defensible, quantitative fluorescence measurements, and to partition the drivers of the fluorescence signals into effects of structure and physiology.
关键词： chlorophyll fluorescence (SIF, Fs),stress,photosynthesis,drought,temperature,chlorophyll/carotenoid pigments
更新于2025-09-23 15:23:52
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Electronic Structure of Chlorophyll a Solution Investigated by Photoelectron Yield Spectroscopy
摘要： Various bio-related processes are driven by electron transfer reactions. Therefore the electronic structures of bio-molecules in their living environment are keys of their functionalities. One significant example photosynthesis which has attracted much attention due to urgent necessity of clean energy source. In this study, we carried out photoelectron yield spectroscopy (PYS) measurements to demonstrate the electronic structures of oligomerizedChl-a molecules, which is known as an essential reaction center of the photosystem in general green plants, under the atmospheric environment. The ionization energies of the Chl-a aggregates are successfully derived.
关键词： Photoelectron Yield Spectroscopy,Polarization energy,Light harvesting antenna,Photosynthesis,Photosystem,Electronic structure,Ionization energy,Reaction center,Chlorophyll a
更新于2025-09-23 15:23:52
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Artificial Mn4Ca-cluster with Exchangeable Solvent Molecules Mimicking the Oxygen-Evolving Center in Photosynthesis
摘要： The natural Mn4Ca-cluster in photosystem II serves as a blueprint to develop artificial water-splitting catalysts in artificial photosynthesis. Although significant advances have recently been achieved, it remains great challenges to prepare robust artificial Mn4Ca-cluster to precisely mimic the structure and function of the biological catalyst in the laboratory. Here, we report the isolation and structural characterization of two Mn4CaO4-complexes from polar solvents acetonitrile or N, N-dimethylformamide, which closely mimics the two water molecules on calcium ion, as well as, the oxidation states of the four manganese ions and the main geometric structure of the natural Mn4Ca-cluster. These new artificial Mn4Ca-complexes provide important chemical clues to understand the structure and mechanism of its biological paragon.
关键词： heterometallic complexes,photosynthesis,bioinorganic chemistry,water splitting,manganese
更新于2025-09-23 15:23:52
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Conjugated donor-acceptor polymer photocatalysts with electron-output “tentacles” for efficient hydrogen evolution
摘要： The tunable structures and versatile properties for conjugated polymers (CPs) make them viable as a molecular platform for photocatalytic water splitting. Normally, structure design of polymer photocatalyst is focus on tuning its optical band structure or charge-separation ability, the importance of electron-output ability in photocatalytic process is always ignored. This study demonstrates a molecular engineering strategy by introducing an electron-output “tentacle” site, i.e. dibenzothiophene-S,S-dioxide (FSO) unit, into the polymer backbone to construct a series of donor-acceptor type conjugated polymer photocatalysts for efficient hydrogen evolution, which not only results in optimized light absorption ability and excellent exciton-separation, but also leads to the efficient electron-output ability. Detailed DFT calculations further theoretically confirm the vital role of FSO unit as an electron-output “tentacle” site.
关键词： Conjugated polymer,Electron-output “tentacles”,Artificial photosynthesis,Hydrogen evolution,Photocatalysis
更新于2025-09-23 15:23:52
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Artificial Photosynthesis for Carbon Dioxide Reduction and Conversion
摘要： In recent years, solar fuel or chemical production based on the photoreduction or fixation of CO2, the so-called “artificial photosynthesis” has received considerable attention. Thus, the development of an effective catalyst for the conversion of CO2 to useful organic molecules is desirable. Biocatalysts for CO2 reduction and conversion are useful catalyst for the artificial photosynthesis system. In this review, two types of artificial photosynthesis systems for CO2 reduction and conversion consisting of the visible-light sensitizer and biocatalyst are introduced. One is the artificial photosynthesis with visible-light sensitizer and biocatalyst for CO2 photoreduction to formic acid or methanol. The other one is the artificial photosynthesis with visible-light sensitizer, and novel electron carrier molecule and biocatalyst for the carbon-carbon bond formation from CO2 as a feedstock.
关键词： carbon-carbon bond formation,artificial photosynthesis,biocatalyst,CO2 reduction and conversion
更新于2025-09-23 15:23:52
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Normalization of <sup>11</sup> C-autoradiographic images for semi-quantitative analysis of woody tissue photosynthesis
摘要： To understand plant survival and mortality during drought it is important to gain better insights into the different mechanisms contributing to both the carbon budget and the hydraulic functioning of plants. However, the role of internally transported carbon dioxide (CO2) in xylem together with related woody tissue photosynthesis is often neglected. Trees contain large amounts of CO2 (often between 3 and 10%, and sometimes exceeding 20%), which is substantially higher than the atmospheric CO2 concentration (c. 0.04%). It is known that a portion of this locally respired CO2 escapes to the atmosphere during transport and that photosynthetic active cells in woody tissues or leaves can fix another portion. A new approach for direct visualization of woody tissue (stem) photosynthesis is presented in this study and using a radioactive 11C-tracer and autoradiographic imaging. To allow semi-quantitative comparison of woody tissue photosynthesis between different branches, a normalization method is required. We developed such a normalization technique by taking into account: (i) the radioactivity at the start of the experiment; (ii) the labeling time; (iii) the start and (iv) duration of exposure of the branch to the autoradiographic phosphor screen. In addition to these time-related parameters, we also accounted for total transpiration during the labeling experiment.
关键词： biomedical imaging,woody tissue photosynthesis,positron autoradiography
更新于2025-09-23 15:22:29
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Structure and binding efficiency relations of QB site inhibitors of photosynthetic reaction centres*
摘要： Many herbicides employed in agriculture and also some antibiotics bind to a specific site of the reaction centre protein (RC) blocking the photosynthetic electron transport. Crystal structures showed that all these compounds bind at the secondary ubiquinone (QB) site albeit to slightly different places. Different herbicide molecules have different binding affinities (evaluated as inhibition constants, KI, and binding enthalpy values, ?Hbind). The action of inhibitors depends on the following parameters: (i) herbicide molecular structure; (ii) interactions between herbicide and quinone binding site; (iii) protein environment. In our investigations KI and ?Hbind were determined for several inhibitors. Bound herbicide structures were optimized and their intramolecular charge distributions were calculated. Experimental and calculated data were compared to those available from databank crystal structures. We can state that the herbicide inhibition efficiency depends on steric and electronic factors, i.e. geometry of binding with the protein and molecular charge distribution, respectively. Apolar bulky groups on N-7 atom of the inhibitor molecule (like t-buthyl in terbutryn) are preferable for establishing stronger interactions with QB site, while such substituents are not recommended on N-8. The N-4,7,8 nitrogen atoms maintain a larger electron density so that more effective H-bonds are formed between the inhibitor and the surrounding amino acids of the protein.
关键词： Herbicides,Bacterial reaction centers,Photosynthesis,Molecular modeling
更新于2025-09-23 15:22:29