Exploring fast proton transfer events associated with lateral proton diffusion on the surface of membranes.
excited-state proton transfer
lipid vesicles
molecular dynamics
photoacid
proton diffusion
Journal
Proceedings of the National Academy of Sciences of the United States of America
ISSN: 1091-6490
Titre abrégé: Proc Natl Acad Sci U S A
Pays: United States
ID NLM: 7505876
Informations de publication
Date de publication:
12 02 2019
12 02 2019
Historique:
pubmed:
27
1
2019
medline:
27
1
2019
entrez:
26
1
2019
Statut:
ppublish
Résumé
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.
Identifiants
pubmed: 30679274
pii: 1812351116
doi: 10.1073/pnas.1812351116
pmc: PMC6377470
doi:
Types de publication
Journal Article
Research Support, Non-U.S. Gov't
Langues
eng
Pagination
2443-2451Déclaration de conflit d'intérêts
The authors declare no conflict of interest.
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