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Realizing laterally continuous ultra‐thin gold films on transparent substrates is a challenge of significant technological importance. In the present work, formation of ultra‐thin gold films on fused silica is studied, demonstrating how suppression of island formation and reduction of plasmonic absorption can be achieved by treating substrates with (3‐mercaptopropyl) trimethoxysilane prior to deposition. Void‐free films with deposition thickness as low as 5.4 nm are realized and remain structurally stable at room temperature. Based on detailed structural analysis of the films by specular and diffuse X‐ray reflectivity measurements, it is shown that optical transmission properties of continuous ultra‐thin films can be accounted for using the bulk dielectric function of gold. However, it is important to take into account the non‐abrupt transition zone between the metal and the surrounding dielectrics, which extends through several lattice constants for the laterally continuous ultra‐thin films (film thickness below 10 nm). This results in a significant reduction of optical transmission, as compared to the case of abrupt interfaces. These findings imply that the atomic‐scale interface structure plays an important role when continuous ultra‐thin films are considered, e.g., as semi‐transparent electrical contacts, since optical transmission deviates significantly from the theoretical predictions for ideal films.

Optical and Structural Properties of Ultra‐thin Gold Films