Effect of Hydrogen Bonding on the Rotational and Translational Dynamics of a Headgroup-Bound Chromophore in Bilayer Lipid Membranes

Greiner, Aaron J.; Pillman, Heather A.; Worden, R. Mark; Blanchard, G. J.; Ofoli, Robert Y.

doi:10.1021/jp9057862

Cited by 15 publications

(15 citation statements)

References 57 publications

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“…To explore lifetime shortening of NBD due to the depth-specific quenching in a quantitative way, we subjected all the decay curves to deconvolution analysis. It has been reported previously that an NBD probe attached to lipids or proteins reveals multiexponentional fluorescence decays in heterogeneous membrane environment (Posokhov and Ladokhin 2006); (Mukherjee et al 2004); (Loura and Ramalho 2007); (Greiner et al 2009). The best fits to all the NBD decays were obtained using a sum of two exponentials.…”

Section: Resultsmentioning

confidence: 99%

“…Among a variety of fluorescent lipids, NBD-functionalized phospholipids have been widely utilized as fluorescent analogues of native lipids to measure membrane polarity (Chattopadhyay and London 1988); (Chattopadhyay and Mukherjee 1999b), hydrogen-bonding (Greiner et al 2009), lateral diffusion (Shrive et al 1996) as well as lipid heterogeneity (Armstrong et al 2003); (Pucadyil et al 2007); (Vaish and Sanyal 2011). Lipids and cholesterol analogues labeled with an NBD fluorophore have also been used to detect the presence of lipid domains in cell membranes (Stubbs et al 1989).…”

Section: Introductionmentioning

confidence: 99%

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Calibration of Distribution Analysis of the Depth of Membrane Penetration Using Simulations and Depth-Dependent Fluorescence Quenching

2014

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Determination of the depth of membrane penetration provides important information for studies of membrane protein folding and protein-lipid interactions. Here we use a combination of molecular dynamics (MD) simulations and depth-dependent fluorescence quenching to calibrate the methodology for extracting quantitative information on membrane penetration. In order to investigate the immersion depth of the fluorescent label in lipid bilayer, we studied 7-nitrobenz-2-oxa-1,3-diazole (NBD) attached to the lipid headgroup in NBD-PE incorporated into POPC bilayer. The immersion depth of NBD was estimated by measuring steady-state and time-resolved fluorescence quenching with spin-labeled lipids co-incorporated into lipid vesicles. Six different spin-labeled lipids were utilized: one with headgroup-attached Tempo probe (Tempo-PC) and five with acyl-chain-labeled n-Doxyl moieties (n-Doxyl-PC where n is a chain labeling position equal to 5, 7, 10, 12, and 14, respectively). The Stern-Volmer analysis revealed that NBD quenching in membranes occurs by both static and dynamic collisional quenching processes. Using the methodology of Distribution Analysis, the immersion depth and the apparent half-width of the transversal distributions of the NBD moiety were estimated to be 14.9 Å and 6.7 Å from the bilayer center. This position is independently validated by atomistic MD simulations of NBD-PE lipids in a POPC bilayer (14.4 Å). In addition, we demonstrate that MD simulations of the transverse overlap integrals between dye and quencher distributions can be used for proper analysis of the depth-dependent quenching profile. Finally, we illustrate the application of this methodology by determining membrane penetration of site-selectively labeled mutants of diphtheria toxin T-domain.

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Section: Resultsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Calibration of Distribution Analysis of the Depth of Membrane Penetration Using Simulations and Depth-Dependent Fluorescence Quenching

2014

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“…Time-resolved fluorescence decays were recorded using the time-correlated single photon counting (TCSPC) method. [72][73][74][75][76] Data analysis was carried via commercial software provided by Horiba Instruments.…”

Section: Experimental and Theoretical Methodsmentioning

confidence: 99%

The Effect of Intermolecular Hydrogen Bonding on the Fluorescence of a Bimetallic Platinum Complex

et al. 2010

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The bimetallic platinum complexes are known as unique building blocks and arewidely utilized in the coordination-driven self-assembly of functionalized supramolecular metallacycles. Hence, photophysical study of the bimetallic platinum complexes will be very helpful for the understanding on the optical properties and further applications of coordination-driven self-assembled supramolecular metallacycles. Herein, we report steady-state and time-resolved spectroscopic experiments as well as quantum chemistry calculations to investigate the significant intermolecular hydrogen bonding effects on the intramolecular charge transfer (ICT) fluorescence of a bimetallic platinum compound 4,4'-bis(trans-Pt(PEt(3))(2)OTf)benzophenone 3 in solution. We demonstrated that the fluorescent state of compound 3 can be assigned as a metal-to-ligand charge transfer (MLCT) state. Moreover, it was observed that the formation of intermolecular hydrogen bonds can effectively lengthen the fluorescence lifetime of 3 in alcoholic solvents compared with that in hexane solvent. At the same time, the electronically excited states of 3 in solution are definitely changed by intermolecular hydrogen bonding interactions. As a consequence, we propose a new fluorescence modulation mechanism by hydrogen bonding to explain different fluorescence emissions of 3 in hydrogen-bonding solvents and nonhydrogen-bonding solvents.

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“…This has also been found in related membrane composition where DOPG likely interacts with neighboring lipid molecules by hydrogen bonding. This hydrogen bonding is between glycerol moiety of DOPG and the phosphate oxygen of the neighboring phospholipid which leads to ordering of the membrane (Greiner et al, 2009). The early membrane binding of A-40 could be predominantly driven by the lipid packing defects and the limiting bulk peptide concentration; however, the polar interactions should be essential for the stabilization of the interactions.…”

Section: Introductionmentioning

confidence: 99%

In vitro reconstitution demonstrates the amyloid-beta mediated myelin membrane deformation

Tiwari

Pradhan

Sannigrahi

et al. 2021

Preprint

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Amyloid-beta (Ab) aggregation mediated neuronal membrane deformation, although poorly understood, is implicated in Alzheimer's Disease (AD). Particularly, whether Ab aggregation can induce neuronal demyelination remains unknown. Here we show that Aβ-40 binds and induces extensive tubulation in the myelin membrane in vitro. The binding of Aβ-40 depends predominantly on the lipid packing defect densities and electrostatic interactions and results in rigidification of the myelin membrane in the early time scales. Furthermore, elongation of Aβ-40 into higher oligomeric and fibrillar species leads to eventual fluidization of the myelin membrane followed by extensive membrane tubulation observed in the late phase. Taken together, our results capture mechanistic insights into snapshots of temporal dynamics of Aβ-40- myelin membrane interaction and demonstrate how short timescale, local phenomena of binding, and fibril mediated load generation manifests into long timescale, global phenomena of myelin tubulation and demonstrates the ability of Aβ-40 to demyelinate.

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Effect of Hydrogen Bonding on the Rotational and Translational Dynamics of a Headgroup-Bound Chromophore in Bilayer Lipid Membranes

Cited by 15 publications

References 57 publications

Calibration of Distribution Analysis of the Depth of Membrane Penetration Using Simulations and Depth-Dependent Fluorescence Quenching

Calibration of Distribution Analysis of the Depth of Membrane Penetration Using Simulations and Depth-Dependent Fluorescence Quenching

The Effect of Intermolecular Hydrogen Bonding on the Fluorescence of a Bimetallic Platinum Complex

In vitro reconstitution demonstrates the amyloid-beta mediated myelin membrane deformation

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