Impurity spectroscopy at its ultimate limit: relation between bulk spectrum, inhomogeneous broadening, and local disorder by spectroscopy of (nearly) all individual dopant molecules in solids

Titelangaben

Naumov, Andrei V. ; Gorshelev, Aleksey A. ; Vainer, Yury G. ; Kador, Lothar ; Köhler, Jürgen:
Impurity spectroscopy at its ultimate limit: relation between bulk spectrum, inhomogeneous broadening, and local disorder by spectroscopy of (nearly) all individual dopant molecules in solids.
In: Physical Chemistry Chemical Physics. Bd. 13 (2011) Heft 5 . - S. 1734-1742.
ISSN 1463-9076
DOI der Verlagsversion: https://doi.org/10.1039/c0cp01689f

Volltext

Format: PDF Name: c0cp01689f.pdf Version: Veröffentlichte Version Verfügbar mit der Lizenz Deutsches Urheberrecht. Dieser Beitrag ist mit Zustimmung des Rechteinhabers aufgrund einer (DFG-geförderten) Allianz- bzw. Nationallizenz frei zugänglich. Das Dokument darf zum eigenen Gebrauch kostenfrei genutzt werden. Darüber hinaus bedürfen die Vervielfältigung, Bearbeitung, Verbreitung und jede Art der Verwertung der schriftlichen Zustimmung des jeweiligen Rechteinhabers.

Download (2MB)

Abstract

We present a technique for the measurement of the low-temperature fluorescence excitation spectra and imaging of a substantial fraction of all single chromophore molecules (hundreds of thousands and even more) embedded in solid bulk samples as nanometre-sized probes. An important feature of our experimental studies is that the full information about the lateral coordinates and spectral parameters of all individual molecules is stored for detailed analysis. This method enables us to study a bulk sample in a broad spectral region with ultimate sensitivity, combining excellent statistical accuracy and the capability of detecting rare events. From the raw data we determined the distributions of several parameters of the chromophore spectra and their variations across the inhomogeneous absorption band, including the frequencies of the electronic zero-phonon lines, their spectral linewidths, and fluorescence count rates. Relationships between these distributions and the disorder of the matrix were established for the examples of two polycrystalline solids with very different properties, n-hexadecane and o-dichlorobenzene, and the amorphous polymer polyisobutylene. We also found spatially inhomogeneous distributions of some parameters.