Browsing by Author "Olson, Jana M."

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    Circular Differential Scattering of Single Chiral Self-Assembled Gold Nanorod Dimers
    (American Chemical Society, 2015) Wang, Lin-Yung; Smith, Kyle W.; Dominiquez-Medina, Sergio; Moody, Nicole; Olson, Jana M.; Zhang, Huanan; Chang, Wei-Shun; Kotov, Nicholas; Link, Stephan; Laboratory for Nanophotonics
    Circular dichroism spectroscopy is essential for structural characterization of proteins and chiral nanomaterials. Chiral structures from plasmonic materials have extraordinary strong circular dichroism effects compared to their molecular counterparts. While being extensively investigated, the comprehensive account of circular dichroism effects consistent with other plasmonic phenomena is still missing. Here we investigated the circular differential scattering of a simple chiral plasmonic system, a twisted side-by-side Au nanorod dimer, using single-particle circular dichroism spectroscopy complimented with electromagnetic simulations. This approach enabled us to quantify the effects of structural symmetry breaking, namely, size-mismatch between the constituent Au nanorods and large twist angles on the resulting circular differential scattering spectrum. Our results demonstrate that, if only scattering is considered as measured by dark-field spectroscopy, a homodimer of Au nanorods with similar sizes produces a circular differential scattering line shape that is different from the bisignate response of the corresponding conventional CD spectrum, which measures extinction, that is, the sum of scattering and absorption. On the other hand, symmetry breaking in a heterodimer with Au nanorods with different sizes yields a bisignate circular differential scattering line shape. In addition, we provide a general method for correcting linear dichroism artifacts arising from slightly elliptically polarized light in a typical dark-field microscope, as is necessary especially when measuring highly anisotropic nanostructures, such as side-by-side nanorods. This work lays the foundation for understanding absorption and scattering contributions to the CD line shape of single chiroplasmonic nanostructures free from ensemble-averaging, especially important for self-assembled chiral nanostructures that usually exist as both enantiomers.
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    Patterning of supported gold monolayers via chemical lift-off lithography
    (Beilstein, 2017) Slaughter, Liane S.; Cheung, Kevin M.; Kaappa, Sami; Cao, Huan H.; Yang, Qing; Young, Thomas D.; Serino, Andrew C.; Malola, Sami; Olson, Jana M.; Link, Stephan; Häkkinen, Hannu; Andrews, Anne M.; Weiss, Paul S.
    The supported monolayer of Au that accompanies alkanethiolate molecules removed by polymer stamps during chemical lift-off lithography is a scarcely studied hybrid material. We show that these Au–alkanethiolate layers on poly(dimethylsiloxane) (PDMS) are transparent, functional, hybrid interfaces that can be patterned over nanometer, micrometer, and millimeter length scales. Unlike other ultrathin Au films and nanoparticles, lifted-off Au–alkanethiolate thin films lack a measurable optical signature. We therefore devised fabrication, characterization, and simulation strategies by which to interrogate the nanoscale structure, chemical functionality, stoichiometry, and spectral signature of the supported Au–thiolate layers. The patterning of these layers laterally encodes their functionality, as demonstrated by a fluorescence-based approach that relies on dye-labeled complementary DNA hybridization. Supported thin Au films can be patterned via features on PDMS stamps (controlled contact), using patterned Au substrates prior to lift-off (e.g., selective wet etching), or by patterning alkanethiols on Au substrates to be reactive in selected regions but not others (controlled reactivity). In all cases, the regions containing Au–alkanethiolate layers have a sub-nanometer apparent height, which was found to be consistent with molecular dynamics simulations that predicted the removal of no more than 1.5 Au atoms per thiol, thus presenting a monolayer-like structure.
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    Plasmonic Polymers Unraveled Through Single Particle Spectroscopy
    (Royal Society of Chemistry, 2014) Slaughter, Liane S.; Wang, Lin-Yung; Willingham, Britain A.; Olson, Jana M.; Swanglap, Pattanawit; Dominguez-Medina, Sergio; Link, Stephan; Laboratory for Nanophotonics
    Plasmonic polymers are quasi one-dimensional assemblies of nanoparticles whose optical responses are governed by near-field coupling of localized surface plasmons. Through single particle extinction spectroscopy correlated with electron microscopy, we reveal the effect of the composition of the repeat unit, the chain length, and extent of disorder on the energies, intensities, and line shapes of the collective resonances of individual plasmonic polymers constructed from three different sizes of gold nanoparticles. Our combined experiment and theoretical analysis focuses on the superradiant plasmon mode, which results from the most attractive interactions along the nanoparticle chain and yields the lowest energy resonance in the spectrum. This superradiant mode redshifts with increasing chain length until an infinite chain limit, where additional increases in chain length cause negligible change in the energy of the superradiant mode. We find that, among plasmonic polymers of equal width comprising nanoparticles with different sizes, the onset of the infinite chain limit and its associated energy are dictated by the number of repeat units and not the overall length, of the polymer. The intensities and linewidths of the superradiant mode relative to higher energy resonances, however, differ as the size and number of nanoparticles are varied in the plasmonic polymers studied here. These findings provide general guidelines for engineering the energies, intensities, and line shapes of the collective optical response of plasmonic polymers constructed from nanoparticles with sizes ranging from a few tens to one hundred nanometers.