scholarly journals Local water sensing: water exchange in bacterial photosynthetic reaction centers embedded in a trehalose glass studied using multiresonance EPR

2017 ◽  
Vol 19 (41) ◽  
pp. 28388-28400 ◽  
Author(s):  
Anna Nalepa ◽  
Marco Malferrari ◽  
Wolfgang Lubitz ◽  
Giovanni Venturoli ◽  
Klaus Möbius ◽  
...  

Pulsed EPR spectroscopies and isotope labeled water are applied to detect and quantify the local water in a bacterial reaction center embedded into a trehalose glass.

2021 ◽  
Vol 12 (1) ◽  
Author(s):  
Yin Song ◽  
Riley Sechrist ◽  
Hoang H. Nguyen ◽  
William Johnson ◽  
Darius Abramavicius ◽  
...  

AbstractPhotochemical reaction centers are the engines that drive photosynthesis. The reaction center from heliobacteria (HbRC) has been proposed to most closely resemble the common ancestor of photosynthetic reaction centers, motivating a detailed understanding of its structure-function relationship. The recent elucidation of the HbRC crystal structure motivates advanced spectroscopic studies of its excitonic structure and charge separation mechanism. We perform multispectral two-dimensional electronic spectroscopy of the HbRC and corresponding numerical simulations, resolving the electronic structure and testing and refining recent excitonic models. Through extensive examination of the kinetic data by lifetime density analysis and global target analysis, we reveal that charge separation proceeds via a single pathway in which the distinct A0 chlorophyll a pigment is the primary electron acceptor. In addition, we find strong delocalization of the charge separation intermediate. Our findings have general implications for the understanding of photosynthetic charge separation mechanisms, and how they might be tuned to achieve different functional goals.


2021 ◽  
Author(s):  
Yin Song ◽  
Riley Sechrist ◽  
Hoang Huy Nguyen ◽  
William Johnson ◽  
Darius Abramavičius ◽  
...  

<p>Photochemical reaction centers are the engines that drive photosynthesis. The reaction center from heliobacteria (HbRC) has been proposed to most closely resemble the common ancestor of photosynthetic reaction centers, motivating a detailed understanding of its structure-function relationship. The recent elucidation of the HbRC crystal structure motivates advanced spectroscopic studies of its excitonic structure and charge separation mechanism. We perform multispectral two-dimensional electronic spectroscopy of the HbRC and corresponding numerical simulations, resolving the electronic structure and testing and refining recent excitonic models. Through extensive examination of the kinetic data by lifetime density analysis and global target analysis, we reveal that charge separation proceeds via a single pathway in which the distinct A<sub>0 </sub>chlorophyll <i>a</i> pigment is the primary electron acceptor. In addition, we find strong delocalization of the initial excited state and charge separation intermediate. Our findings have general implications for the understanding of photosynthetic charge separation mechanisms, and how they might be tuned to achieve different functional goals.</p>


1996 ◽  
Vol 100 (12) ◽  
pp. 2036-2040 ◽  
Author(s):  
F. Lendzian ◽  
J. Rautter ◽  
H. Käß ◽  
A. Gardine ◽  
W. Lubitz

1998 ◽  
Vol 283 (1-2) ◽  
pp. 51-60 ◽  
Author(s):  
Gerd Kothe ◽  
Michael Bechtold ◽  
Gerhard Link ◽  
Ernst Ohmes ◽  
Jörg-Ulrich Weidner

2017 ◽  
Vol 114 (15) ◽  
pp. 3837-3842 ◽  
Author(s):  
Emiliano Altamura ◽  
Francesco Milano ◽  
Roberto R. Tangorra ◽  
Massimo Trotta ◽  
Omar Hassan Omar ◽  
...  

Photosynthesis is responsible for the photochemical conversion of light into the chemical energy that fuels the planet Earth. The photochemical core of this process in all photosynthetic organisms is a transmembrane protein called the reaction center. In purple photosynthetic bacteria a simple version of this photoenzyme catalyzes the reduction of a quinone molecule, accompanied by the uptake of two protons from the cytoplasm. This results in the establishment of a proton concentration gradient across the lipid membrane, which can be ultimately harnessed to synthesize ATP. Herein we show that synthetic protocells, based on giant lipid vesicles embedding an oriented population of reaction centers, are capable of generating a photoinduced proton gradient across the membrane. Under continuous illumination, the protocells generate a gradient of 0.061 pH units per min, equivalent to a proton motive force of 3.6 mV⋅min−1. Remarkably, the facile reconstitution of the photosynthetic reaction center in the artificial lipid membrane, obtained by the droplet transfer method, paves the way for the construction of novel and more functional protocells for synthetic biology.


1990 ◽  
Vol 218 ◽  
Author(s):  
Devens Gust ◽  
Thomas A. Moore ◽  
Ana L. Moore

AbstractThe photosynthetic reaction centers of plants and bacteria are photovoltaic devices on the molecular scale which convert light energy into chemical potential energy in the form of long-lived, energetic charge separated states. It is now possible to prepare synthetic multicomponent molecules which mimic important aspects of this process. For example, one of the keys to reaction center function is a multistep electron transfer strategy. In this paper, two general types of multistep electron transfer, sequential and parallel, are described and illustrated with several synthetic triad and pentad molecules.


2005 ◽  
Vol 69 (6) ◽  
pp. 1130-1136 ◽  
Author(s):  
Masayuki KOBAYASHI ◽  
Yoichiro FUJIOKA ◽  
Takayuki MORI ◽  
Minoru TERASHIMA ◽  
Hiroaki SUZUKI ◽  
...  

2021 ◽  
Author(s):  
Yin Song ◽  
Riley Sechrist ◽  
Hoang Huy Nguyen ◽  
William Johnson ◽  
Darius Abramavičius ◽  
...  

<p>Photochemical reaction centers are the engines that drive photosynthesis. The reaction center from heliobacteria (HbRC) has been proposed to most closely resemble the common ancestor of photosynthetic reaction centers, motivating a detailed understanding of its structure-function relationship. The recent elucidation of the HbRC crystal structure motivates advanced spectroscopic studies of its excitonic structure and charge separation mechanism. We perform multispectral two-dimensional electronic spectroscopy of the HbRC and corresponding numerical simulations, resolving the electronic structure and testing and refining recent excitonic models. Through extensive examination of the kinetic data by lifetime density analysis and global target analysis, we reveal that charge separation proceeds via a single pathway in which the distinct A<sub>0 </sub>chlorophyll <i>a</i> pigment is the primary electron acceptor. In addition, we find strong delocalization of the initial excited state and charge separation intermediate. Our findings have general implications for the understanding of photosynthetic charge separation mechanisms, and how they might be tuned to achieve different functional goals.</p>


2012 ◽  
Vol 16 (05n06) ◽  
pp. 626-632 ◽  
Author(s):  
Nguyen Thi Viet Thanh ◽  
Thorsten Könekamp ◽  
Daniela Hanke ◽  
Franziska Löwer ◽  
Tobias Borrmann ◽  
...  

Special pair chlorophylls arranged in a cofacial dimeric structure play an important role in the initial step of light induced electron transfer of photosynthetic reaction centers of bacteria and plants. For mimicking the natural photosynthetic reaction center we aimed on synthesis of an artificial special pair 13 constructed from two chlorin subunits 5a, b and a rigid biphenylene spacer moiety 11. Due to the reduced C2h symmetry of the chlorin units compared with so far used D4h porphyrins and due to the rigid spacer a cofacial dimer of defined symmetry and distance was obtained.


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