Signature of the surface hydrated proton and associated restructuring of water at model membrane interfaces: a vibrational sum frequency generation study

Abstract

Hydrated proton at membrane interfaces plays an important role in the bioenergetic process of almost all organisms. Herein, the signature of the hydrated proton at membrane interfaces has been investigated by measuring the vibrational sum frequency generated (VSFG) spectra of negatively charged and zwitterionic lipids in the presence of different concentrations of acids. The addition of acids decreases the intensity of the OH stretch of the VSFG signal of water present at the negatively charged and zwitterionic lipids along with the enhanced intensity of the broad VSFG signal in the range of 2500–2800 cm⁻¹. The enhanced intensity of the broad continuum observed in the range of 2500–2800 cm⁻¹ has been assigned to the signature of the hydrated proton at the lipid interfaces. The decrease in the VSFG signal of the OH stretch of water along with the appearance of the broad signal suggests that the hydrated proton exists in the vicinity of the lipid interfaces and restructures the interaction between the interfacial water molecules.