“…3,4 Therefore, SHG is widely employed to characterise equilibrium and dynamic physical-chemistry processes of all types of interfaces, including buried interfaces, as long as they are accessible by light, with a high sensitivity to layers of adsorbates or contaminants. [12][13][14] The interface-specificity of SHG was first attributed to the discontinuity of the electric field at the interface induced by the non-matching refractive indices, which results in the apparition of an interface quadrupole term in the induced polarisation a ICSM, Univ Montpellier, CEA, CNRS, ENSCM, Marcoule, France. E-mails: yann.foucaud@cea.fr; jean-francois.dufreche@icsm.fr b PASTEUR, Département de Chimie, Ecole normale supérieure, PSL University, Sorbonne Université, CNRS, 75005 Paris, France.…”