Journal
ACS NANO
Volume 7, Issue 6, Pages 5391-5401Publisher
AMER CHEMICAL SOC
DOI: 10.1021/nn401321k
Keywords
break junction; molecular bridge; charge transport; dephasing; nucleic acids
Categories
Funding
- National Science Foundation [CHE 1057953, CHE 0809838, CHE 1059037, CHE 1057981]
- Goldblatt Fellowship
- Direct For Mathematical & Physical Scien
- Division Of Chemistry [1057953, 1059037, 1057981] Funding Source: National Science Foundation
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This study examines quantitative correlations between molecular conductances and standard electrochemical rate constants for alkanes and peptide nucleic acid (PNA) oligomers as a function of the length, structure, and charge transport mechanism. The experimental data show a power-law relationship between conductances and charge transfer rates within a given class of molecules with the same bridge chemistry, and a lack of correlation when a more diverse group of molecules is compared, in contrast with some theoretical predictions. Surprisingly, the PNA duplexes exhibit the lowest charge-transfer rates and the highest molecular conductances. The nonlinear rate-conductance relationships for structures with the same bridging chemistries are attributed to differences in the charge-mediation characteristics of the molecular bridge, energy barrier shifts and electronic dephasing, in the two different experimental settings.
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