Science Advances

Supplementary Materials

This PDF file includes:

  • section S1. Brewster angle microscopy
  • section S2. Sigmoidal fits
  • section S3. SFG data analysis
  • section S4. SFG experiments with different electrolytes in the subphase
  • section S5. Calculation of interference between χ(2) and χ(3) terms
  • section S6. SFG experiments measured with ppp and pss polarization combination
  • section S7. SFG experiments of different lipid mixtures, different layer preparation, and isotopic dilution of the subphase
  • section S8. SFG experiments with different lipid surface area per molecule and Brewster angle microscopy measurement
  • section S9. SFG experiments of lipid mixtures on pure D2O
  • section S10. SFG experiments with NaSCN in the subphase
  • section S11. Supplementary information to MD simulations and additional MD simulations
  • section S12. Calculation of another orientational metric
  • section S13. Calculation of charge condensation
  • table S1. Signals frequencies (ω), widths (2Γ), and their corresponding molecular vibrations and the nonresonant amplitudes and the amplitudes of all resonances of the SFG spectra of the D2O-lipid interface with a varying ratio of DPTAP/DPPG at the surface and 10 mM NaCl in the subphase.
  • table S2. Peak position (ω), width (2Γ), and assignment to the corresponding molecular vibrations and nonresonant and resonant amplitudes for the SFG spectra of the D2O-DPTAP interface with 10-μm NaSCN in the subphase.
  • table S3. Frequency (ω), area (A), phase (ϕ), and width (2Γ) of the χ(2) and χ(3) contributions for the lineshape calculation.
  • fig. S1. Electrolyte-dependent saturation of water alignment.
  • fig. S2. Effect of interference between χ(2) and χ(3) terms.
  • fig. S3. SFG spectra of the lipid mixtures at different polarization combinations.
  • fig. S4. Polarization-dependent saturation of water alignment.
  • fig. S5. Systematic investigation of the water alignment saturation effect.
  • fig. S6. Surface area dependence of the saturation of the water alignment.
  • fig. S7. Brewster angle microscopy images of different lipid layers.
  • fig. S8. Influence of salt on the water alignment saturation effect.
  • fig. S9. SFG spectra of the lipid mixtures with NaSCN in the subphase.
  • fig. S10. Counterion concentration–dependent MD simulations.
  • fig. S11. Calculation of another orientational metric from MD simulations.
  • fig. S12. Critical charge density for charge condensation.
  • References (59–69)

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