Probing polarization and dielectric function of molecules with higher order harmonics in scattering-near-field scanning optical microscopy
Abstract
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.
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https://hdl.handle.net/10161/3353Published Version (Please cite this version)
10.1063/1.3245392Publication Info
Nikiforov, 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.This is constructed from limited available data and may be imprecise. To cite this
article, please review & use the official citation provided by the journal.
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Show full item recordScholars@Duke
Michael J. Therien
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

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