0000000000961412
AUTHOR
Kate Rodriguez
Observation and analysis of Fano-like lineshapes in the Raman spectra of molecules adsorbed at metal interfaces
Surface enhanced Raman spectra from molecules (bipyridyl ethylene) adsorbed on gold dumbells are observed to become increasingly asymmetric (Fano-like) at higher incident light intensity. The electronic temperature (inferred from the anti-Stokes (AS) electronic Raman signal increases at the same time while no vibrational AS scattering is seen. These observations are analyzed by assuming that the molecule-metal coupling contains an intensity dependent contribution (resulting from light-induced charge transfer transitions as well as renormalization of the molecule metal tunneling barrier). We find that interference between vibrational and electronic inelastic scattering routes is possible in …
Orientation-Dependent Handedness of Chiral Plasmons on Nanosphere Dimers: How to Turn a Right Hand into a Left Hand
Optical activity, which is used as a discriminator of chiral enantiomers, is demonstrated to be orientation dependent on individual, and nominally achiral, plasmonic nanosphere dimers. Through measurements of their giant Raman optical activity, we demonstrate that L/R-handed enantiomers can be continuously turned into their R/L-handed mirror images without passing through an achiral state. The primitive uniaxial multipolar response, with demonstrable broken parity and time reversal symmetry, reproduces the observations as resonant Raman scattering on plasmons that carry angular momentum. The analysis underscores that chirality does not have a quantitative continuous measure and recognizes t…