The nanometer-scale sensitivity of electromagnetic plasmon coupling allows the translation of minute morphological changes in nanostructures into macroscopic optical signals. We demonstrate here a ...widefield spectral analysis of 40 nm diameter gold nanoparticle (AuNP) dimers, linked by a short DNA double strand, using a low-cost color CCD camera and allowing a quantitative estimation of interparticle distances in a 3-20 nm range. This analysis can be extended to lower spacings and a parallel monitoring of dimer orientations by performing a simple polarization analysis. Our measurement approach is calibrated against confocal scattering spectroscopy using AuNP dimers that are distorted from a stretched geometry at low ionic strength to touching particles at high salt concentrations. We then apply it to identify dimers featuring two different conformations of the same DNA template and discuss the parallel colorimetric sensing of short sequence-specific DNA single strands using dynamic plasmon rulers.
We produce gold nanoparticle dimers with a surface-to-surface distance that varies reversibly by a factor of 3 when hybridizing or removing a single target DNA strand. The dimers are built on one DNA ...template that features a stem-loop enabling the interparticle distance change. Using electrophoresis, we reach 90% sample purities and demonstrate that this chemical process is reversible in solution at room temperature for a low molar excess of the target DNA strand. The kinetics of the reaction is asymmetric due to steric hindrance in the stem-loop opening process. Furthermore, a statistical analysis of cryo-electron microscopy measurements allows us to provide the first quantitative analysis of distance changes in chemically switchable nanoparticle assemblies.
We demonstrate that symmetric or asymmetric gold nanoparticle dimers with substantial scattering cross sections and plasmon coupling can be produced with a perfectly controlled chemical environment ...and a high purity using a single DNA linker as short as 7 nm. A statistical analysis of the optical properties and morphology of single dimers is performed using darkfield and cryo-electron microscopies. These results, correlated to Mie theory calculations, indicate that the particle dimers are stretched in water by electrostatic interactions.
A photon interacts efficiently with an atom when its frequency corresponds exactly to the energy between two eigenstates. But at the nanoscale, homogeneous and inhomogeneous broadenings strongly ...hinder the ability of solid-state systems to absorb, scatter or emit light. By compensating the impedance mismatch between visible wavelengths and nanometre-sized objects, optical antennas can enhance light-matter interactions over a broad frequency range. Here we use a DNA template to introduce a single dye molecule in gold particle dimers that act as antennas for light with spontaneous emission rates enhanced by up to two orders of magnitude and single photon emission statistics. Quantitative agreement between measured rate enhancements and theoretical calculations indicate a nanometre control over the emitter-particle position while 10 billion copies of the target geometry are synthesized in parallel. Optical antennas can thus tune efficiently the photo-physical properties of nano-objects by precisely engineering their electromagnetic environment.
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