Exploring fast proton transfer events associated with lateral proton diffusion on the surface of membranes
Amdursky, N., Lin, Y., Aho, N., & Groenhof, G. (2019). Exploring fast proton transfer events associated with lateral proton diffusion on the surface of membranes. Proceedings of the National Academy of Sciences, 116(7), 2443-2451. https://doi.org/10.1073/pnas.1812351116
Published inProceedings of the National Academy of Sciences
© National Academy of Sciences, 2019.
Proton diffusion (PD) across biological membranes is a fundamental process in many biological systems, and much experimental and theoretical effort has been employed for deciphering it. Here, we report on a spectroscopic probe, which can be tightly tethered to the membrane, for following fast (nanosecond) proton transfer events on the surface of membranes. Our probe is composed of a photoacid that serves as our light-induced proton source for the initiation of the PD process. We use our probe to follow PD, and its pH dependence, on the surface of lipid vesicles composed of a zwitterionic headgroup, a negative headgroup, a headgroup that is composed only from the negative phosphate group, or a positive headgroup without the phosphate group. We reveal that the PD kinetic parameters are highly sensitive to the nature of the lipid headgroup, ranging from a fast lateral diffusion at some membranes to the escape of protons from surface to bulk (and vice versa) at others. By referring to existing theoretical models for membrane PD, we found that while some of our results confirm the quasi-equilibrium model, other results are in line with the nonequilibrium model. ...
PublisherNational Academy of Sciences
Publication in research information system
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Related funder(s)Academy of Finland
Funding program(s)Academy Project, AoF
Additional information about fundingWe thank D. Huppert and N. Agmon for fruitful discussions. G.G. and N. Aho thank the CSC – IT Center for Science (Espoo, Finland) for computational resources. N. Amdursky received financial support from the Chaya Career Advancement Chair, the Russel Berrie Nanotechnology Institute, and the Grand Technion Energy Program, and G.G. and N. Aho were supported by the Academy of Finland (Grant 311031).
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