Antenna-Enhanced Fluorescence Correlation Spectroscopy Resolves Calcium-Mediated Lipid-Lipid Interactions

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Block, Stephan,1978Freie Universität Berlin,Chalmers tekniska högskola,Chalmers University of Technology (author)

Antenna-Enhanced Fluorescence Correlation Spectroscopy Resolves Calcium-Mediated Lipid-Lipid Interactions

Article/chapterEnglish2018

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2018-03-12
American Chemical Society (ACS),2018

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LIBRIS-ID:oai:research.chalmers.se:72563643-be5a-4ca0-ab53-82bb245d2b61
https://research.chalmers.se/publication/502970URI
https://doi.org/10.1021/acsnano.7b07854DOI

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Language:English
Summary in:English

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Fluorescence correlation spectroscopy (FCS) has provided a wealth of information on the composition, structure, and dynamics of cell membranes. However, it has proved challenging to reach the spatial resolution required to resolve biophysical interactions at the nanometer scale relevant to many crucial membrane processes. In this work, we form artificial cell membranes on dimeric, nanoplasmonic antennas, which shrink the FCS probe volume down to the ∼20 nm length scale. By analyzing the autocorrelation functions associated with the fluorescence bursts from individual fluorescently tagged lipids moving through the antenna "hotspots", we show that the confinement of the optical readout volume below the diffraction limit allows the temporal resolution of FCS to be increased by up to 3 orders of magnitude. Employing this high spatial and temporal resolution to probe diffusion dynamics of individual dye-conjugated lipids, we further show that lipid molecules diffuse either as single entities or as pairs in the presence of calcium ions. Removal of calcium ions by addition of the chelator EDTA almost completely removes the complex contribution, in agreement with previous theoretical predications on the role of calcium ions in mediating transient interactions between zwitterionic lipids. We envision that antenna-enhanced FCS with single-molecule burst analysis will enable resolving a broad range of challenging membrane biophysics questions, such as stimuli-induced lipid clustering and membrane protein dynamics.

Subject headings and genre

NATURVETENSKAP Kemi Fysikalisk kemi hsv//swe
NATURAL SCIENCES Chemical Sciences Physical Chemistry hsv//eng
NATURVETENSKAP Fysik Atom- och molekylfysik och optik hsv//swe
NATURAL SCIENCES Physical Sciences Atom and Molecular Physics and Optics hsv//eng
NATURVETENSKAP Fysik Annan fysik hsv//swe
NATURAL SCIENCES Physical Sciences Other Physics Topics hsv//eng
single-molecule fluorescence correlation spectroscopy
hotspot
lipid complexes
lipid mobility
nanoplasmonics

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Acimovic, Srdjan,1982Chalmers tekniska högskola,Chalmers University of Technology(Swepub:cth)acimovic (author)
Odebo Länk, Nils,1988Chalmers tekniska högskola,Chalmers University of Technology(Swepub:cth)odebo (author)
Käll, Mikael,1963Chalmers tekniska högskola,Chalmers University of Technology(Swepub:cth)kall (author)
Höök, Fredrik,1966Chalmers tekniska högskola,Chalmers University of Technology(Swepub:cth)fredrikh (author)
Freie Universität BerlinChalmers tekniska högskola (creator_code:org_t)

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In:ACS Nano: American Chemical Society (ACS)12:4, s. 3272-32791936-086X1936-0851

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