Soft-landing of mass-selected ions is a powerful tool for precisely-controlled preparation of cluster-based interfaces. We have developed a high-intensity electrospray ionization source that delivers nanoamperes of mass-selected cluster ions onto surfaces. This capability allows us to efficiently populate two- and three-dimensional (2D and 3D) interfaces with cluster ions. We are particularly interested in studying the deposition of stable anionic species, which efficiently retain their ionic charge on surfaces. Although it is generally assumed that charging of the surface should prevent ions from reaching the deposition substrate, we observe a steady increase in the deposition rate with ion exposure. <i>In situ</i> surface characterization using infrared spectroscopy indicates a gradual accumulation of hydrocarbons during anion deposition. We demonstrate that co-adsorption of neutral molecules stabilizes the charged layer and results in formation of either solid- or liquid-like layers with bulk properties strongly dependent on the soft-landed anion, co-adsorbed neutral, and surface. Furthermore, we demonstrate that anion deposition is an effective tool for populating 2D and 3D interfaces with redox-active clusters. This capability is particularly important for the controlled preparation of high-performance electrode-electrolyte interfaces for applications in supercapacitors and alkali ion batteries.

High-coverage deposition of mass-selected cluster anions: Fundamentals and applications

256th National Meeting (2018)

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