Beyond the Gouy-Chapman Model with Heterodyne-Detected Second Harmonic Generation

Paul E. Ohno, Hanbyul Chang, Austin P. Spencer, Yangdongling Liu, Mavis D. Boamah, Hong Fei Wang, Franz M. Geiger*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

61 Scopus citations


We report ionic strength-dependent phase shifts in second harmonic generation (SHG) signals from charged interfaces that verify a recent model in which dispersion between the fundamental and second harmonic beams modulates observed signal intensities. We show how phase information can be used to unambiguously separate the χ(2) and interfacial potential-dependent χ(3) terms that contribute to the total signal and provide a path to test primitive ion models and mean field theories for the electrical double layer with experiments to which theory must conform. Finally, we demonstrate the new method on supported lipid bilayers and comment on the ability of our new instrument to identify hyper-Rayleigh scattering contributions to common homodyne SHG measurements in reflection geometries.

Original languageEnglish (US)
Pages (from-to)2328-2334
Number of pages7
JournalJournal of Physical Chemistry Letters
Issue number10
StatePublished - May 16 2019

ASJC Scopus subject areas

  • General Materials Science
  • Physical and Theoretical Chemistry


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