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This study uses a novel surface engineering approach to demonstrate the influence of organic functional group substitutions on molecular electronic properties. Specifically, bilayered organic monomolecular systems immobilized on an inorganic electrode as the charge‐injecting components of organic electronic devices are compared. Recent literature reports demonstrate that structural modification in functional monolayers have unpredictable effects on their electronic properties. These studies indicate that the structure most certainly plays an important role, but its effect on the molecular resistance is diminished due to differences in other monolayer parameters. It is demonstrated that a separate control over the monolayer geometry and its chemical structure is required in order to observe predictable structure‐property relations. Here, bilayered molecular interfaces, comprising inert and functional layers whose properties can be independently controlled, are formed. It is shown that 1) the charge transfer through the bilayered system is sensitive to small structural molecular changes; 2) that it can be controlled and predicted by controlling the electron‐withdrawing or donating nature of the organic moiety; and 3) that the differences in the charge transfer dynamics of two bilayered systems can be visualized via patterned electroluminescence.

We report a new protocol for the preparation of shape-controlled multicomponent particles comprising metallic (Au and Ti), magnetic (Ni), and oxide (SiO2, TiO2) layers. Our method allows for a precise control over the composition, shape, and size and permits fabrication of nonsymmetrical particles, whose opposite sides can be orthogonally functionalized using well-established organosilanes and thiol chemistries. Because of their unique geometries and surface chemistries, these colloids represent ideal materials with which to study nonsymmetrical self-assembly at the meso- and microscales.

A. A. Shestopalov and co‐workers demonstrate in article 1300109 the influence of functional group substitution on the molecular resistance in ordered and functional self‐assembled monolayers on indium tin oxide. By independently controlling the geometry and chemistry of the monolayers, the charge transfer through the monolayers can be controlled with the electron‐withdrawing or donating functional groups, and the differences in the charge transfer dynamics can be visualized via patterned electroluminescence using traditional organic light emitting diodes.