Ultrafast charge separation and charge stabilization in axially linked ‘tetrathiafulvalene–aluminum(iii) porphyrin–gold(iii) porphyrin’ reaction center mimics

2015 ◽  
Vol 17 (39) ◽  
pp. 26346-26358 ◽  
Author(s):  
Prashanth K. Poddutoori ◽  
Gary N. Lim ◽  
Serguei Vassiliev ◽  
Francis D'Souza

Sequential electron transfer leading to charge stabilization in newly synthesized vertically aligned ‘tetrathiafulvalene–aluminum(iii) porphyrin–gold(iii) porphyrin’ supramolecular triads is reported.

Nanoscale ◽  
2015 ◽  
Vol 7 (15) ◽  
pp. 6813-6826 ◽  
Author(s):  
Chandra B. KC ◽  
Gary N. Lim ◽  
Francis D'Souza

Charge stabilization as a result of electron transfer followed by a hole-shift mechanism is demonstrated in a supramolecular multi-modular donor–acceptor assembly.


2007 ◽  
Vol 111 (29) ◽  
pp. 11123-11130 ◽  
Author(s):  
Francis D'Souza ◽  
Suresh Gadde ◽  
Amy L. Schumacher ◽  
Melvin E. Zandler ◽  
Atula S. D. Sandanayaka ◽  
...  

Nanoscale ◽  
2018 ◽  
Vol 10 (44) ◽  
pp. 20723-20739 ◽  
Author(s):  
Niloofar Zarrabi ◽  
Christopher O. Obondi ◽  
Gary N. Lim ◽  
Sairaman Seetharaman ◽  
Benjamin G. Boe ◽  
...  

Three, broad band capturing, vertically aligned reaction center models have been constructed using aluminum(iii) porphyrin.


2021 ◽  
Author(s):  
Somen Mandal ◽  
Nadav Amdursky ◽  
Nandan Ghorai ◽  
Hirendra N. Ghosh ◽  
SOUMYADIP BHUNIA

Electron transfer (ET) across proteins is ubiquitous in nature, such as the notable photosynthesis example, where light-induced charge separation takes place within the reaction center, followed by sequential ET via...


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.


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