8 research outputs found

    Preprocess dependence of optical properties of ensembles and single siphonaxanthin-containing major antenna from the marine green alga Codium fragile

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    The siphonaxanthin-siphonein-Chl-a/b-protein (SCP) is the light-harvesting complex of the marine alga Codium fragile. Its structure resembles that of the major light-harvesting complexes of higher plants, LHC II, yet it features a reversed Chl a:Chl b ratio and it accommodates other variants of carotenoids. We have recorded the fluorescence emission spectra and fluorescence lifetimes from ensembles and single SCP complexes for three different scenarios of handling the samples. While the data obtained from ensembles of SCP complexes yield equivalent results, those obtained from single SCP complexes featured significant differences as a function of the sample history. We ascribe this discrepancy to the different excitation intensities that have been used for ensemble and single complex spectroscopy, and conclude that the SCP complexes undergo an aging process during storage. This process is manifested as a lowering of energetic barriers within the protein, enabling thermal activation of conformational changes at room temperature. This in turn leads to the preferential population of a red-shifted state that features a significant decrease of the fluorescence lifetime

    Metal-Enhanced Fluorescence of Chlorophylls in Single Light-Harvesting Complexes

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    Ensemble and single-molecule spectroscopy demonstrates that both emission and absorption of peridinin−chlorophyll−protein photosynthetic antennae can be largely enhanced through plasmonic interactions. We find up to 18-fold increase of the chlorophyll fluorescence for complexes placed near a silver metal layer. This enhancement, which leaves no measurable effects on the protein structure, is observed when exciting either chlorophyll or carotenoid and is attributed predominantly to an increase of the excitation rate in the antenna. The enhancement mechanism comes from plasmon-induced amplification of electromagnetic fields inside the complex. This result is an important step toward applying plasmonic nanostructures for controlling the optical response of complex biomolecules and improving the design and functioning of artificial light-harvesting systems

    Absorption Enhancement in Peridinin–Chlorophyll–Protein Light-Harvesting Complexes Coupled to Semicontinuous Silver Film

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    We report on experimental and theoretical studies of plasmon-induced effects in a hybrid nanostructure composed of light-harvesting complexes and metallic nanoparticles in the form of semicontinuous silver film. The results of continuous-wave and time-resolved spectroscopy indicate that absorption of the light-harvesting complexes is strongly enhanced upon coupling with the metallic film spaced by 25 nm of a dielectric silica layer. This conclusion is corroborated by modeling, which confirms the morphology of the silver island film

    Energy Transfer in Reconstituted Peridinin-Chlorophyll-Protein Complexes: Ensemble and Single-Molecule Spectroscopy Studies

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    We combine ensemble and single-molecule spectroscopy to gain insight into the energy transfer between chlorophylls (Chls) in peridinin-chlorophyll-protein (PCP) complexes reconstituted with Chl a, Chl b, as well as both Chl a and Chl b. The main focus is the heterochlorophyllous system (Chl a/b-N-PCP), and reference information essential to interpret experimental observations is obtained from homochlorophyllous complexes. Energy transfer between Chls in Chl a/b-N-PCP takes place from Chl b to Chl a and also from Chl a to Chl b with comparable Förster energy transfer rates of 0.0324 and 0.0215 ps−1, respectively. Monte Carlo simulations yield the ratio of 39:61 for the excitation distribution between Chl a and Chl b, which is larger than the equilibrium distribution of 34:66. An average Chl a/Chl b fluorescence intensity ratio of 66:34 is measured, however, for single Chl a/b-N-PCP complexes excited into the peridinin (Per) absorption. This difference is attributed to almost three times more efficient energy transfer from Per to Chl a than to Chl b. The results indicate also that due to bilateral energy transfer, the Chl system equilibrates only partially during the excited state lifetimes

    Evaluating Provitamin A Carotenoids and Polar Metabolite Compositions during the Ripening Stages of the Agung Semeru Banana (Musa paradisiaca L. AAB)

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    Banana cultivars that are rich in provitamin A carotenoids and other nutrients may offer a potential food source to help alleviate vitamin A deficiencies, particularly in developing countries. The local plantain type banana, Agung Semeru (Musa paradisiaca L.), was investigated, in order to analyse the changes in the compositions of the provitamin A carotenoids and metabolite compounds, including the amino acids, organic acids, and sugars, during the ripening stage as this banana is widely processed for food products in either the unripe, ripe, or overripe stages. The bananas that had reached the desired ripening stages were subjected to high-performance liquid chromatography (HPLC) analysis, and the results indicated that the total provitamin A carotenoid concentrations ranged between 4748.83 μg/100 g dry weight (dw) and 7330.40 μg/100 g dw, with the highest level of vitamin A activity at 457.33±5.18 μg retinol activity equivalents (RAE)/100 g dw. Compared to the Cavendish variety, which is consumed worldwide, the Agung Semeru banana had vitamin A activity that was 40 to 90 times higher, dependent on the stage of ripening. The breakdown of the starch during the ripening stages resulted in an increase of its sugar compounds, such as sucrose, fructose, and glucose, as well as its dominant organic acids, such as malic acid, oxalic acid, and citric acid, which were observed using gas chromatography-mass spectrometry (GC-MS) during the ripening stages. The findings of this study show that the Agung Semeru banana is a promising fruit that could be widely produced as a nutritional and energy food resource, due to its high levels of vitamin A activity and sugars

    The light intensity under which cells are grown controls the type of peripheral light-harvesting complexes that are assembled in a purple photosynthetic bacterium

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    The differing composition of LH2 (peripheral light-harvesting) complexes present in Rhodopseudomonas palustris 2.1.6 have been investigated when cells are grown under progressively decreasing light intensity. Detailed analysis of their absorption spectra reveals that there must be more than two types of LH2 complexes present. Purified HL (high-light) and LL (low-light) LH2 complexes have mixed apoprotein compositions. The HL complexes contain PucAB(a) and PucAB(b) apoproteins. The LL complexes contain PucAB(a), PucAB(d) and PucB(b)-only apoproteins. This mixed apoprotein composition can explain their resonance Raman spectra. Crystallographic studies and molecular sieve chromatography suggest that both the HL and the LL complexes are nonameric. Furthermore, the electron-density maps do not support the existence of an additional Bchl (bacteriochlorophyll) molecule; rather the density is attributed to the N-termini of the alpha-polypeptide
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