MyJournals Home  

RSS FeedsMolecules, Vol. 27, Pages 755: Suppression of Charge Recombination by Auxiliary Atoms in Photoinduced Charge Separation Dynamics with Mn Oxides: A Theoretical Study (Molecules)

 
 

24 january 2022 13:59:41

 
Molecules, Vol. 27, Pages 755: Suppression of Charge Recombination by Auxiliary Atoms in Photoinduced Charge Separation Dynamics with Mn Oxides: A Theoretical Study (Molecules)
 


Charge separation is one of the most crucial processes in photochemical dynamics of energy conversion, widely observed ranging from water splitting in photosystem II (PSII) of plants to photoinduced oxidation reduction processes. Several basic principles, with respect to charge separation, are known, each of which suffers inherent charge recombination channels that suppress the separation efficiency. We found a charge separation mechanism in the photoinduced excited-state proton transfer dynamics from Mn oxides to organic acceptors. This mechanism is referred to as coupled proton and electron wave-packet transfer (CPEWT), which is essentially a synchronous transfer of electron wave-packets and protons through mutually different spatial channels to separated destinations passing through nonadiabatic regions, such as conical intersections, and avoided crossings. CPEWT also applies to collision-induced ground-state water splitting dynamics catalyzed by Mn4CaO5 cluster. For the present photoinduced charge separation dynamics by Mn oxides, we identified a dynamical mechanism of charge recombination. It takes place by passing across nonadiabatic regions, which are different from those for charge separations and lead to the excited states of the initial state before photoabsorption. This article is an overview of our work on photoinduced charge separation and associated charge recombination with an additional study. After reviewing the basic mechanisms of charge separation and recombination, we herein studied substituent effects on the suppression of such charge recombination by doping auxiliary atoms. Our illustrative systems are X–Mn(OH)2 tied to N-methylformamidine, with X=OH, Be(OH)3, Mg(OH)3, Ca(OH)3, Sr(OH)3 along with Al(OH)4 and Zn(OH)3. We found that the competence of suppression of charge recombination depends significantly on the substituents. The present study should serve as a useful guiding principle in designing the relevant photocatalysts.


 
143 viewsCategory: Biochemistry, Chemistry, Molecular Biology
 
Molecules, Vol. 27, Pages 758: Metal Complexes—A Promising Approach to Target Biofilm Associated Infections (Molecules)
Molecules, Vol. 27, Pages 759: Investigation of Nonlinear Optical Modulation Characteristics of MXene VCrC for Pulsed Lasers (Molecules)
 
 
blog comments powered by Disqus


MyJournals.org
The latest issues of all your favorite science journals on one page

Username:
Password:

Register | Retrieve

Search:

Molecular Biology


Copyright © 2008 - 2024 Indigonet Services B.V.. Contact: Tim Hulsen. Read here our privacy notice.
Other websites of Indigonet Services B.V.: Nieuws Vacatures News Tweets Nachrichten