scholarly journals Photo-Induced Electron Transfer from Dye or Quantum Dot to TiO2 Nanoparticles at Single Molecule Level

Author(s):  
King-Chuen Lin ◽  
Chun-Li Chang
2020 ◽  
Vol 73 (8) ◽  
pp. 699
Author(s):  
Rosalind P. Cox ◽  
Saman Sandanayake ◽  
Steven J. Langford ◽  
Toby D. M. Bell

Electron transfer (ET) is a key chemical reaction in nature and has been extensively studied in bulk systems, but remains challenging to investigate at the single-molecule level. A previously reported naphthalene diimide (NDI)-based system (Higginbotham et al., Chem. Commun. 2013, 49, 5061–5063) displays delayed fluorescence with good quantum yield (~0.5) and long-lived (nanoseconds) prompt and delayed fluorescence lifetimes, providing an opportunity to interrogate the underlying ET processes in single molecules. Time-resolved single-molecule fluorescence measurements enabled forward and reverse ET rate constants to be calculated for 45 individual molecules embedded in poly(methylmethacrylate) (PMMA) film. Interpretation of the results within the framework of Marcus–Hush theory for ET demonstrates that variation in both the electronic coupling and the driving force for ET is occurring from molecule to molecule within the PMMA film and over time for individual molecules.


2003 ◽  
Vol 115 (35) ◽  
pp. 4341-4346 ◽  
Author(s):  
Roel Gronheid ◽  
Alina Stefan ◽  
Mircea Cotlet ◽  
Johan Hofkens ◽  
Jianqiag Qu ◽  
...  

2019 ◽  
Vol 116 (9) ◽  
pp. 3407-3412 ◽  
Author(s):  
Yueqi Li ◽  
Hui Wang ◽  
Zixiao Wang ◽  
Yanjun Qiao ◽  
Jens Ulstrup ◽  
...  

Electron transfer reactions can now be followed at the single-molecule level, but the connection between the microscopic and macroscopic data remains to be understood. By monitoring the conductance of a single molecule, we show that the individual electron transfer reaction events are stochastic and manifested as large conductance fluctuations. The fluctuation probability follows first-order kinetics with potential dependent rate constants described by the Butler–Volmer relation. Ensemble averaging of many individual reaction events leads to a deterministic dependence of the conductance on the external electrochemical potential that follows the Nernst equation. This study discloses a systematic transition from stochastic kinetics of individual reaction events to deterministic thermodynamics of ensemble averages and provides insights into electron transfer processes of small systems, consisting of a single molecule or a small number of molecules.


2003 ◽  
Vol 15 (18) ◽  
pp. S1873-S1890 ◽  
Author(s):  
Jingdong Zhang ◽  
Mikala Grubb ◽  
Allan G Hansen ◽  
Alexander M Kuznetsov ◽  
Anja Boisen ◽  
...  

2013 ◽  
Vol 2013 ◽  
pp. 1-9 ◽  
Author(s):  
Mette Eriksen ◽  
Peter Horvath ◽  
Michael A. Sørensen ◽  
Szabolcs Semsey ◽  
Lene B. Oddershede ◽  
...  

To perform single-molecule studies of the T7RNA polymerase, it is crucial to visualize an individual T7RNA polymerase, for example, through a fluorescent signal. We present a novel complex combining two different molecular functions, an active T7RNA polymerase and a highly luminescent nanoparticle, a quantum dot. The complex has the advantage of both constituents: the complex can traffic along DNA and simultaneously be visualized, both at the ensemble and at the single-molecule level. The labeling was mediated through anin vivobiotinylation of a His-tagged T7RNA polymerase and subsequent binding of a streptavidin-coated quantum dot. Our technique allows for easy purification of the quantum dot labeled T7RNA polymerases from the reactants. Also, the conjugation does not alter the functionality of the polymerase; it retains the ability to bind and transcribe.


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