Browsing by Author "Carter, Emily A."

Now showing 1 - 2 of 2
  • Thumbnail Image
    Item
    Plasmon damping depends on the chemical nature of the nanoparticle interface
    (AAAS, 2019) Foerster, Benjamin; Spata, Vincent A.; Carter, Emily A.; Sönnichsen, Carsten; Link, Stephan
    The chemical nature of surface adsorbates affects the localized surface plasmon resonance of metal nanoparticles. However, classical electromagnetic simulations are blind to this effect, whereas experiments are typically plagued by ensemble averaging that also includes size and shape variations. In this work, we are able to isolate the contribution of surface adsorbates to the plasmon resonance by carefully selecting adsorbate isomers, using single-particle spectroscopy to obtain homogeneous linewidths, and comparing experimental results to high-level quantum mechanical calculations based on embedded correlated wavefunction theory. Our approach allows us to indisputably show that nanoparticle plasmons are influenced by the chemical nature of the adsorbates 1,7-dicarbadodecaborane(12)-1-thiol (M1) and 1,7-dicarbadodecaborane(12)-9-thiol (M9). These surface adsorbates induce inside the metal electric dipoles that act as additional scattering centers for plasmon dephasing. In contrast, charge transfer from the plasmon to adsorbates—the most widely suggested mechanism to date—does not play a role here.
  • Thumbnail Image
    Item
    Plasmonic Photocatalysis of Nitrous Oxide into N2 and O2 Using Aluminum–Iridium Antenna–Reactor Nanoparticles
    (American Chemical Society, 2019) Swearer, Dayne F.; Robatjazi, Hossein; Martirez, John Mark P.; Zhang, Ming; Zhou, Linan; Carter, Emily A.; Nordlander, Peter; Halas, Naomi J.; Laboratory for Nanophotonics
    Photocatalysis with optically active “plasmonic” nanoparticles is a growing field in heterogeneous catalysis, with the potential for substantially increasing efficiencies and selectivities of chemical reactions. Here, the decomposition of nitrous oxide (N2O), a potent anthropogenic greenhouse gas, on illuminated aluminum–iridium (Al–Ir) antenna–reactor plasmonic photocatalysts is reported. Under resonant illumination conditions, N2 and O2 are the only observable decomposition products, avoiding the problematic generation of NOx species observed using other approaches. Because no appreciable change to the apparent activation energy was observed under illumination, the primary reaction enhancement mechanism for Al–Ir is likely due to photothermal heating rather than plasmon-induced hot-carrier contributions. This light-based approach can induce autocatalysis for rapid N2O conversion, a process with highly promising potential for applications in N2O abatement technologies, satellite propulsion, or emergency life-support systems in space stations and submarines.