Surface-enhanced Raman scattering is a powerful approach to detect molecules at very low concentrations, even up to the single-molecule level. One important aspect of the materials used in such a technique is how much the signal is intensified, quantified by the enhancement factor (EF). Herein we obtained the EFs for gold nanoparticle dimers of 60 and 80 nm diameter, respectively, self-assembled using DNA origami nanotriangles. Cy5 and TAMRA were used as surface-enhanced Raman scattering (SERS) probes, which enable the observation of individual nanoparticles and dimers. EF distributions are determined at four distinct wavelengths based on the measurements of around 1000 individual dimer structures. The obtained results show that the EFs for the dimeric assemblies follow a log-normal distribution and are in the range of 106 at 633 nm and that the contribution of the molecular resonance effect to the EF is around 2, also showing that the plasmonic resonance is the main source of the observed signal. To support our studies, FDTD simulations of the nanoparticle’s electromagnetic field enhancement has been carried out, as well as calculations of the resonance Raman spectra of the dyes using DFT. We observe a very close agreement between the experimental EF distribution and the simulated values.
Porous, layered materials containing sp2-hybridized carbon and nitrogen atoms, offer through their tunable properties, a versatile route towards tailormade catalysts for electrochemistry and photochemistry. A key molecule interacting with these...
Recently,
Nocera and co-workers (J. Am. Chem. Soc.
2018, 140, 13711) demonstrated that
triaryl borate Lewis acids facilitate the direct electrochemical reduction
of triphenylphosphine oxide (TPPO) to triphenylphosphine (TPP). In
the present contribution, we report a quantum chemical study unravelling
details of the reaction, which also supports the proposed EC
r
EC
i
mechanism. Alternative
electrochemical routes to TPPO reduction facilitated by other Lewis
acids (CH3
+),
or by photocatalysis at semiconductor surfaces, are also briefly discussed.
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