Probing polarization and dielectric function of molecules with higher order harmonics in scattering-near-field scanning optical microscopy
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The idealized system of an atomically flat metallic surface [highly oriented pyrolytic graphite (HOPG)] and an organic monolayer (porphyrin) was used to determine whether the dielectric function and associated properties of thin films can be accessed with scanning-near-field scanning optical microscopy (s-NSOM). Here, we demonstrate the use of harmonics up to fourth order and the polarization dependence of incident light to probe dielectric properties on idealized samples of monolayers of organic molecules on atomically smooth substrates. An analytical treatment of light/sample interaction using the s-NSOM tip was developed in order to quantify the dielectric properties. The theoretical analysis and numerical modeling, as well as experimental data, demonstrate that higher order harmonic scattering can be used to extract the dielectric properties of materials with tens of nanometer spatial resolution. To date, the third harmonic provides the best lateral resolution (∼50 nm) and dielectric constant contrast for a porphyrin film on HOPG. © 2009 American Institute of Physics.
Published Version (Please cite this version)10.1063/1.3245392
Publication InfoNikiforov, MP; Kehr, SC; Park, TH; Milde, P; Zerweck, U; Loppacher, C; ... Bonnell, D (2009). Probing polarization and dielectric function of molecules with higher order harmonics in scattering-near-field scanning optical microscopy. Journal of Applied Physics, 106(11). pp. 114307. 10.1063/1.3245392. Retrieved from https://hdl.handle.net/10161/3353.
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William R. Kenan, Jr. Distinguished Professor of Chemistry
Our research involves the synthesis of compounds, supramolecular assemblies, nano-scale objects, and electronic materials with unusual ground-and excited-state characteristics, and interrogating these structures using state-of-the-art transient optical, spectroscopic, photophysical, and electrochemical methods. Over chemical dimensions that span molecules to materials, we probe experimental and theoretical aspects of charge migration reactions and ultrafast electron transfer processes. Insights