Abstract
The second-order nonlinear susceptibility, which is the source of the sum frequency generation (SFG) spectrum, for the vapor−water interface is calculated by molecular dynamics simulation based on the time correlation formula. The calculated susceptibility well reproduces that of the recent phase-sensitive SFG experiment (Ji et al. Phys. Rev. Lett. 2008, 100, 096102), including the positive imaginary part in the 3000−3200 cm−1 region, which is a controversial problem in the assignment. It is found that this positive part of the imaginary susceptibility is induced by the intermolecular orientational correlation at the interface through the anisotropic local field.
Talk to us
Join us for a 30 min session where you can share your feedback and ask us any queries you have
Schedule a callDisclaimer: All third-party content on this website/platform is and will remain the property of their respective owners and is provided on "as is" basis without any warranties, express or implied. Use of third-party content does not indicate any affiliation, sponsorship with or endorsement by them. Any references to third-party content is to identify the corresponding services and shall be considered fair use under The CopyrightLaw.
