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It has been generally accepted that there are significant quadrupolar andbulk contributions to the second harmonic generation (SHG) reflected from theneat air/water interface, as well as common liquid interfaces. Because therehas been no general methodology to determine the quadrupolar and bulkcontributions to the SHG signal from a liquid interface, this conclusion wasreached based on the following two experimental phenomena. Namely, the brokenof the macroscopic Kleinman symmetry, and the significant temperaturedependence of the SHG signal from the neat air/water interface. However,because sum frequency generation vibrational spectroscopy (SFG-VS) measurementof the neat air/water interface observed no apparent temperature dependence,the temperature dependence in the SHG measurement has been reexamined andproven to be an experimental artifact. Here we present a complete microscopicanalysis of the susceptibility tensors of the air/water interface, and showthat dipolar contribution alone can be used to address the issue of broken ofthe macroscopic Kleinman symmetry at the neat air/water interface. Using thisanalysis, the orientation of the water molecules at the interface can beobtained, and it is consistent with the measurement from SFG-VS. Therefore, thekey rationales to conclude significantly quadrupolar and bulk contributions tothe SHG signal of the neat air/water interface can no longer be considered asvalid as before. This new understanding of the air/water interface can shedlight on our understanding of the nonlinear optical responses from othermolecular interfaces as well

journal of chemical physics online/the journal of chemical physics/journal of chemical physics

Reconsideration of second-harmonic generation from isotropic liquid interface: Broken Kleinman symmetry of neat air/water interface from dipolar contribution