Multicolour single molecule emission and excitation spectroscopy reveals extensive spectral shifts

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Document typeArticle
Defense date2015-07-16
PublisherThe Royal Society of Chemistry
Rights accessOpen Access
European Commission's projectNANOANTENNAS - Nano-Optical Antennas for Tuneable Single Photon Super-Emitters (EC-FP7-247330)
Abstract
We explore the distribution and shape of single molecule spectra at room temperature,
when embedded in a polymer host. Multicolour excitation and emission spectroscopy is
implemented to capture the full inhomogeneous distribution. We observe dramatic
spectral changes in a distribution of single quaterrylene diimide (QDI) molecules
isolated in a PMMA matrix. The molecules are strongly blue shifted with respect to the
ensemble absorption maximum and spread over a staggering 200 nm range. Despite
these strong shifts, the shape of the emission spectra does not differ much between
individual molecules. We demonstrate that a considerable number of molecules may be
invisible in single molecule experiments, as they typically rely on only a single excitation
wavelength, which predetermines which subensemble is probed in the experiment.
Lastly, we make a first step towards single molecule excitation spectroscopy under
ambient conditions, which allows us to determine the spectral range at which individual
molecules absorb light most efficiently. We show how single molecule emission and
excitation spectroscopies can complement each other and a combination of both
techniques can help in understanding the origin of underlaying spectral properties of
individual molecules.
ISSN1359-6640
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