A New Imaginary Term in the Second-Order Nonlinear Susceptibility from Charged Interfaces

نویسندگان

چکیده

Nonresonant second harmonic generation (SHG) phase and amplitude measurements obtained from the silica-water interface at varying pH values an ionic strength of 0.5 M point to existence a nonlinear susceptibility term, which we call ?X(3), that is associated with 90° shift. Including this contribution in model for total effective second-order produces reasonable estimates interfacial potentials susceptibilities when ?X(3) ? 1.5?water(3). A without term containing only traditional ?(2) ?(3) terms cannot recapitulate experimental data. The new also provides demonstrated utility distinguishing apparent differences electrolyte NaCl versus MgSO4, pointing possibility using heterodyne-detected SHG investigate ion specificity processes.

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ژورنال

عنوان ژورنال: Journal of Physical Chemistry Letters

سال: 2021

ISSN: ['1948-7185']

DOI: https://doi.org/10.1021/acs.jpclett.1c01103