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@PHDTHESIS{Hfig:885908,
author = {Höfig, Henning},
title = {{S}ingle-{M}olecule {C}haracterization of {FRET}-based
{B}iosensors and {D}evelopment of {T}wo-{C}olor
{C}oincidence {D}etection},
volume = {225},
school = {RWTH Aachen},
type = {Dissertation},
address = {Jülich},
publisher = {Forschungszentrum Jülich GmbH Zentralbibliothek, Verlag},
reportid = {FZJ-2020-04172},
isbn = {978-3-95806-502-4},
series = {Schriften des Forschungszentrums Jülich. Reihe
Schlüsseltechnologien / Key Technologies},
pages = {XVIII, 160 S.},
year = {2020},
note = {Dissertation, RWTH Aachen, 2020},
abstract = {Biomolecules often exhibit heterogeneous properties, e. g.
they can exist in different conformational states. Ensemble
measurements provide only averaged values and, hence, cannot
resolve the underlying heterogeneity. In contrast,
single-molecule techniques are based on a
molecule-by-molecule analysis which allows to reveal the
heterogeneity. In this work, two single-molecule methods
based on the confocal detection of fluorescent biomolecules
are presented. First, genetically-encoded FRET-based
biosensors are investigated that utilize Förster resonance
energy transfer (FRET) between two fluorescent proteins as
the sensor signal. FRETbased biosensors have great potential
for applications in biotechnology or diagnostics. Yet, the
development of highly-sensitive sensor constructs is
complicated by the complexity of the sensor design and the
limited information content of the ensemble
characterization. This work presents the experimental
requirements for the single-molecule detection of FRET-based
biosensors followed by a comprehensive single-molecule study
of a set of FRET-based biosensors for the determination of
glucose concentrations. The single-molecule characterization
allows to dissect different parameters that contribute to
the sensor performance and, hence, facilitates a more
targeted sensor design. Furthermore, the effect of
macromolecular crowding on the glucose sensor and two
specific crowding sensor constructs is investigated on the
single-molecule level. In order to elucidate the role of the
fluorescent proteins for the sensor performance, a
dye-labeled analogue of the glucose biosensor is
investigated on the single-molecule level. The small changes
of the FRET signal upon glucose addition in comparison to
the biosensor equipped with fluorescent proteins indicate
the importance of the relative fluorophore orientation for
the FRET signal, that is unique for the employed fluorescent
proteins. The second part of this thesis deals with
two-color coincidence detection (TCCD) which enables to
investigate the binding of two biomolecules that exhibit
fluorescence of two differentcolors. Existing methods
underestimate the coincidence due to an imperfect overlap of
the confocal volumes of the different colors. The
introduction of a brightness gating (BTCCD) for the
single-molecule fluorescence intensity facilitates the
selection of molecule trajectories that transverse both
confocal volumes and, hence, enables quantitative analyses.
The capability ofthe brightness gating is demonstrated by
reproducing the coincidence of various,
dual-labeledreference samples. After a rigorous testing of
the limits of BTCCD, it is applied to FRET-based biosensors
to reveal the donor-only and acceptor-only fractions.
Finally, BTCCD is used tocharacterize protein synthesis in a
cell-free protein synthesis system and to reveal a
previously unrecognized mode of protein translation
initiation in bacteria. The ability of BTCCDto provide
quantitative results in combination with the versatility of
fluorescence assays turns BTCCD into a helpful tool for
further studies of the interaction of biomolecules.},
cin = {IBI-6},
cid = {I:(DE-Juel1)IBI-6-20200312},
pnm = {899 - ohne Topic (POF3-899)},
pid = {G:(DE-HGF)POF3-899},
typ = {PUB:(DE-HGF)3 / PUB:(DE-HGF)11},
urn = {urn:nbn:de:0001-2020120902},
url = {https://juser.fz-juelich.de/record/885908},
}