期刊
NANO LETTERS
卷 17, 期 5, 页码 3215-3224出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.7b00804
关键词
Cooperative effect; pi-pi interaction; transfer integral; molecular electronics; nanoelectrochemistry; coupled quantum dot
类别
资金
- Marie Curie ITN Grants
- EU-FP7 Nano-microwave project
- iSwitch (GA) [642196]
- Renatech (the French national nanofabrication network)
- Equipex Excelsior
- Interuniversity Attraction Pole program of the Belgian Federal Science Policy Office [PAI 7/05]
- Belgian National Fund for Scientific Research (FNRS)
The pi-pi interactions between organic molecules are among the most important parameters for optimizing the transport and optical properties of organic transistors, light-emitting diodes, and (bio-) molecular devices. Despite substantial theoretical progress, direct experimental measurement of the pi-pi electronic coupling energy parameter t has remained an old challenge due to molecular structural variability and the large number of parameters that affect the charge transport. Here, we propose a study of pi-pi interactions from electrochemical and current measurements on a large array of ferrocene-thiolated gold nanocrystals. We confirm the theoretical prediction that t can be assessed from a statistical analysis of current histograms. The extracted value of t 35 meV is in the expected range based on our density functional theory analysis. Furthermore, the t distribution is not necessarily Gaussian and could be used as an ultrasensitive technique to assess intermolecular distance fluctuation at the subangstrom level. The present work establishes a direct bridge between quantum chemistry, electrochemistry, organic electronics, and mesoscopic physics, all of which were used to discuss results and perspectives in a quantitative manner.
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