2D Electronic Spectroscopy Reveals Excitonic Structure in the Baseplate of a Chlorosome

Vácha, František; Pšenčı́k, Jakub; Zigmantas, Donatas

doi:10.1021/jz5005279

Cited by 26 publications

(33 citation statements)

References 40 publications

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“…Excitation energy cascades have been described for the light-harvesting pigment-protein complexes of photosynthetic bacteria [1][2][3] and plants [4,5] with femtosecond temporal resolution. On the other hand, excitation energy transfer mechanisms in light-harvesting complexes from diatoms attracted considerably less attention.…”

Section: Introductionmentioning

confidence: 99%

“…Coherent two-dimensional (2D) electronic spectroscopy (ES) provides a wealth of information about the energy and charge transfer dynamics, exciton diffusion and relaxation in molecular systems [1,2,4,5,[17][18][19][20]3,21,22]. In the 2D ES the temporal and spectral resolutions are not related [23], providing a huge advantage over the pumpprobe techniques.…”

Section: Introductionmentioning

confidence: 99%

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Mapping energy transfer channels in fucoxanthin–chlorophyll protein complex

Gelžinis

Butkus

Songaila

et al. 2015

Biochimica et Biophysica Acta (BBA) - Bioenergetics

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Fucoxanthin-chlorophyll protein (FCP) is the key molecular complex performing the light-harvesting function in diatoms, which, being a major group of algae, are responsible for up to one quarter of the total primary production on Earth. These photosynthetic organisms contain an unusually large amount of the carotenoid fucoxanthin, which absorbs the light in the blue-green spectral region and transfers the captured excitation energy to the FCP-bound chlorophylls. Due to the large number of fucoxanthins, the excitation energy transfer cascades in these complexes are particularly tangled. In this work we present the two-color two-dimensional electronic spectroscopy experiments on FCP. Analysis of the data using the modified decay associated spectra permits a detailed mapping of the excitation frequency dependent energy transfer flow with a femtosecond time resolution.

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Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Mapping energy transfer channels in fucoxanthin–chlorophyll protein complex

Gelžinis

Butkus

Songaila

et al. 2015

Biochimica et Biophysica Acta (BBA) - Bioenergetics

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“…In the experiments we performed, the fluorescence of BChl a in the baseplate could not be separated from the fluorescence of BChl a in the FMO complex and the cores of RCs. This is in agreement with the observation that the distributions of energy levels in all these three LH complexes are highly overlapping (Dostál et al 2014), despite the fact that the fluorescence maxima for baseplate, FMO complex, and RC core differ: ~810, ~825 and ~835 nm respectively (Francke et al 1996;Pšenčík et al 2003;Hohmann-Marriott and Blankenship 2007;Orf et al 2014).…”

Section: Chaptersupporting

confidence: 91%

“…The size of the chlorosome together with the very high pigment concentration is apparently essential for efficient photon gathering at low-light conditions. However, efficient energy transfer of the formed excitations to the RCs is also crucial and that is why the overall arrangement of the photosynthetic apparatus together with the baseplate they exhibit highly overlapping spectra (Dostál et al 2014).…”

Section: Chaptermentioning

confidence: 99%

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Studying photosynthetic antenna complexes in vivo and in vitro using time-resolved fluorescence spectroscopy

Choubeh

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Chapter 1 Introduction 7 Chapter 2 Picosecond excitation energy transfer of allophycocyanin studied in solution and in crystals 33 Chapter 3 State transitions in the cyanobacterium Synechococcus elongatus 7942 involve reversible quenching of the photosystem II core 57 Chapter 4 Light harvesting dynamics in desert crust cyanobacteria: Changes in aggregation state as a mechanism for modulating energy transfer 93 Chapter 5 Efficiency of excitation-energy trapping in the reaction center of the low-light adapted green photosynthetic bacterium Chlorobaculum tepidum 129 Chapter 6 General discussion 163 Chapter 7 Summary 175 Acknowledgements 179 Photosynthesis, cyanobacteria, and state transitions Photosynthetic organisms convert light energy into chemical energy to sustain their metabolism, but which can also be used by other living organisms. Photosynthetic reactions are divided into light-dependent and light-independent reactions (Blankenship 2008a). Plants and cyanobacteria produce Adenosine Triphosphate (ATP) and reduced nicotinamide adenine dinucleotide phosphate (NADPH) during the light-dependent reactions. In the light-independent reactions, ATP and NADPH are used to fix carbon dioxide into carbohydrates. The light-dependent reactions start with the absorption of light by the photosynthetic antennas. Cyanobacteria use phycobilisomes (PBSs) and photosystems I and II (PSI and PSII) to absorb light (Figure 1). PBSs are the main light-harvesting antennas in cyanobacteria which mainly absorb green-orange light. They are composed of rodlike proteins and core proteins. (MacColl 2004; Mirkovic et al. 2016). The rods are built of C-phycocyanins (CPCs) and in various organisms they also have phycoerythrins (PEs). The rods are attached to allophycocyanins (APCs), which contain APC trimers and three other protein-pigments, namely LCM, β 16 , and α B. The excitation energy absorbed by PEs and PCs travels along the rods and reaches APCs, which are attached to the rods by linker proteins, and from there it is delivered in cyan. The dotted line separates one monomer. The codes in the protein data bank are 1jbo (CPC) and 4rmp (APC). PSII is another multi-subunit complex present in cyanobacteria, which is generally believed to form dimers in vivo (Nelson and Ben-Shem 2004; Nickelsen and Rengstl 2013; Zlenko et al. 2017) (Figure 3). The PSII reaction center complex largely consists of two proteins, D1 and D2 and binds six chlorophylls a, two pheophytins a a, two pheophytin and two quinone molecules as described as follows. PD1 and PD2, which are Chls a, are shown in red and blue and next to them are two other Chls a in green, which are called ChlD1 and ChlD2. The pheophytin molecules (PheD1 and PheD2) are represented in black and the quinones in purple. The bottom of the figure shows two different pathways that result in the same chargeseparated state. Only one branch is active in charge separation. The star shows the excited state and the rectangles show the charge-separated states. it takes up one proton from the stroma (two in t...

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Exciton Transport in Molecular Aggregates – From Natural Antennas to Synthetic Chromophore Systems

Brixner

Hildner

Köhler

et al. 2017

Advanced Energy Materials

302

301

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The transport of excitation energy in molecular aggregates is of crucial importance for the function of organic optoelectronic devices and next‐generation solar cells. First, this review summarizes the theoretical background of the nature of the electronically excited states of molecular aggregates. For these systems, the electronic interaction between the monomers leads to the formation of exciton states. This goes along with a shift of the excitation energies and a redistribution of the oscillator strength with respect to the monomers. Next, a brief overview is provided over experimental techniques that allow to study the properties of excitons in molecular aggregates. This includes single‐molecule spectroscopy, coherent two‐dimensional (2D) spectroscopy, and single‐molecule coherent spectroscopy. Finally, examples of molecular aggregates spanning the range from natural systems that act in photosynthesis as light‐harvesting antennas to artificial aggregates built from synthetic chromophores are illustrated.

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2D Electronic Spectroscopy Reveals Excitonic Structure in the Baseplate of a Chlorosome

Cited by 26 publications

References 40 publications

Mapping energy transfer channels in fucoxanthin–chlorophyll protein complex

Mapping energy transfer channels in fucoxanthin–chlorophyll protein complex

Studying photosynthetic antenna complexes in vivo and in vitro using time-resolved fluorescence spectroscopy

Exciton Transport in Molecular Aggregates – From Natural Antennas to Synthetic Chromophore Systems

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