Theoretical Contributions to CaSTL Science: Explaining Experiment with Theory

One of the main goals of the CaSTL center is to explore chemistry at the space-time limit. Researchers in the center have developed many new and exciting experimental techniques that produce rich chemical information. The Schatz group has been working to connect theory with CaSTL experiments using a variety of analytic, electronic structure, and electrodynamic theories.

Nonlinear optical properties of gold nanocrescent arrays studied by second harmonic spectroscopy

In recent advancement of nonlinear plasmonics and metamaterials, significant near-field enhancement by localized surface plasmon resonance (LSPR) of noble metal nanostructure array plays a key role. It is important to better understand the fundamental relationship between LSPR and the induced nonlinear polarization. In this talk, we will discuss the second-order nonlinear optical properties of plasmonic gold nanocrescent array whose LSPR can be selectively excited by tuning the wavelength and polarization of incident electric field.

Optical activity and controllable chiro-optical handedness of symmetric and asymmetric dimer nanocrescents

Asymmetric dimer nanocrescents fabricated using copper mask nanosphere template lithography elicit giant circular dichroism (CD) responses. Chiro-optical activity, commonly used to distinguish between molecular chiral enantiomers, illustrates light-matter interactions that depend dramatically on plasmonic structural characteristics. Dimer nanocrescents exhibit enhanced chiro-optical activity and switches in CD handedness relative to tilt.

ALD-Functionalized Plasmonic Nantennas: A Platform towards Time-Resolved Single-Molecule Studies of Photocatalysis

In the recent push toward single molecule spectroscopy and photochemistry, plasmonic nanostructures have emerged as an attractive and experimentally tractable design. The primary enhancement mechanism of the so-called “nantennas” arises from their ability to couple far-field radiation with molecular receivers, by confining the light in nm-scale junctions (“hotspots”). This small spatial confinement of radiation leads to enhancement factors large enough as to allow for single molecule detection.

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