Molecular mechanism of charge inversion revealed by polar orientation of interfacial water molecules: A heterodyne-detected vibrational sum frequency generation study

The Journal of Chemical Physics
Matthew M SartinTahei Tahara

Abstract

"Charge inversion" is a phenomenon in which multivalent counterions overcompensate for interfacial charges and invert the sign of the net charge near a surface. This phenomenon is believed to be relevant to biologically important processes such as DNA condensation, and hence it has attracted much attention. We investigated the polar orientation of interfacial water molecules at two different negatively charged interfaces in the absence and presence of La3+ using heterodyne-detected vibrational sum frequency generation spectroscopy, which can directly determine the up/down orientation of interfacial molecules. It was found that the orientations of water molecules at a bio-relevant phospholipid interface change from the hydrogen-up to the hydrogen-down with the addition of 10 µM La3+. This change of water orientation indicates that the net charge at the phospholipid interface is inverted by adsorption of La3+ to the phosphate headgroup. By contrast, at an alkylsulfate interface, the majority of the interfacial water molecules remain hydrogen-up orientated even in the presence of 25 mM La3+, indicating that the sulfate headgroup is still solvated by up-oriented water. The observed headgroup specificity suggests that charge inversi...Continue Reading

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Citations

Apr 22, 2019·The Journal of Chemical Physics·Adelina Voukadinova, Dirk Gillespie
Jun 27, 2020·Scientific Reports·Madeleine R FriesFrank Schreiber
Jul 20, 2021·Journal of Physics. Condensed Matter : an Institute of Physics Journal·Yuki Uematsu
Aug 10, 2019·Langmuir : the ACS Journal of Surfaces and Colloids·Manuela E RichertBjörn Braunschweig
Nov 3, 2021·The Journal of Physical Chemistry Letters·Carolyn J MollHuib J Bakker
Jan 21, 2022·The Journal of Physical Chemistry Letters·Kenneth D JuddPaul S Cremer

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