Embedded Oxidized Ag-Pd-Cu Ultrathin Metal Alloy Film Prepared at Low Temperature with Excellent Electronic, Optical, and Mechanical Properties

ACS Appl Mater Interfaces. 2022 Apr 6;14(13):15756-15764. doi: 10.1021/acsami.1c23766. Epub 2022 Mar 22.

Abstract

Most transparent conducting materials are based on Sn:In2O3 (ITO). When applied onto flexible substrates, ITO can be prepared in an oxide-metal-oxide (OMO) configuration, typically ITO/Ag/ITO, where the ductility of the embedded metal layer is intended to reduce the mechanical brittleness and improve the electrical conductivity of the OMO multilayer. Hitherto, the lower limit of the thickness of the Ag layer has been limited by the percolation threshold, which limits the Ag layer to be thicker than ∼10 nm to avoid agglomeration and to ensure conductivity and structural stability. Metal layers of thicknesses below 10 nm are, however, desirable for obtaining OMO coatings with better optical properties. It is known that agglomeration of the metal layer can, to some extent, be suppressed when substituting Ag by an Ag-Pd-Cu (APC) alloy. APC-based OMO films exhibit excellent optical and electrical properties, but still continuous APC films well below 10 nm thickness cannot be achieved. In this work we demonstrate that controlled oxidation of APC results in smooth, ultrathin APC:O continuous coatings (of thickness ∼5 nm) on ITO-coated PET substrates. Moderate oxidation yields superficial PdOx formation, which suppresses Ag agglomeration, while still maintaining excellent conductivity. On the other hand, extensive oxidation of APC leads to extensive Pd oxide nucleation deteriorating the conductivity of the film. The ITO/APC:O/ITO films exhibit low resistivity, attributed to a high Hall mobility associated with suppressed agglomeration, good stability in high humidity/temperature environments, superior transmittance in the visible and infrared region, and excellent mechanical bending properties, thus providing new opportunities for fabricating superior transparent conducting coatings on polymer substrates.

Keywords: Ag−Pd−Cu alloy; OMO structure; magnetron sputtering; transparent conducting materials; ultrathin metal layers.