Smooth, Chemically Altered Nucleating Platform for Abrupt Performance Enhancement of Ultrathin Cu-Layer-Based Transparent Electrodes.

Rapid advances in flexible optoelectronic devices necessitate the concomitant development of high-performance, cost-efficient, and flexible transparent conductive electrodes (TCEs). This Letter reports an abrupt enhancement in the optoelectronic characteristics of ultrathin Cu-layer-based TCEs via Ar+-mediated modulation of the chemical and physical states of a ZnO support surface. This approach strongly regulates the growth mode for the subsequently deposited Cu layer, in addition to marked alteration to the ZnO/Cu interface states, resulting in exceptional TCE performance in the form of ZnO/Cu/ZnO TCEs. The resultant Haacke figure of merit (T10/Rs) of 0.063 Ω-1, 53% greater than that of the unaltered, otherwise identical structure, corresponds to a record-high value for Cu-layer-based TCEs. Moreover, the enhanced TCE performance in this approach is shown to be highly sustainable under severe simultaneous loadings of electrical, thermal, and mechanical stresses.

Strategy for Fabricating Ultrathin Au Film Electrodes with Ultralow Optoelectrical Losses and High Stability.

A vital objective in the wetting of Au deposited on chemically heterogeneous oxides is to synthesize a completely continuous, highly crystalline, ultrathin-layered geometry with minimized electrical and optical losses. However, no effective solution has been proposed for synthesizing an ideal Au-layered structure. This study presents evidence for the effectiveness of atomic oxygen-mediated growth of such an ideal Au layer by improving Au wetting on ZnO substrates with a substantial reduction in free energy. The unexpected outcome of the atomic oxygen-mediated Au growth can be attributed to the unconventional segregation and incorporation of atomic oxygen along the outermost boundaries of Au nanostructures evolving in the clustering and layering stages. Moreover, the experimental and numerical investigations revealed the spontaneous migration of atomic oxygen from an interstitial oxygen surplus ZnO bulk to the Au-ZnO interface, as well as the segregation (float-out) of the atomic oxygen toward the top Au surfaces. Thus, the implementation of a 4-nm-thick, two-dimensional, quasi-single-crystalline Au layer with a nearly complete crystalline realignment at a mild temperature (570 K) enabled exceptional optoelectrical performance with record-low resistivity (<7.5 × 10-8 Ω·m) and minimal optical loss (∼3.5%) at a wavelength of 700 nm.

Pinhole-free TiO2/Ag(O)/ZnO configuration for flexible perovskite solar cells with ultralow optoelectrical loss.

Perovskite solar cells (PSCs) fabricated on transparent polymer substrates are considered a promising candidate as flexible solar cells that can emulate the advantages of organic solar cells, which exhibit considerable freedom in their device design thanks to their light weight and mechanically flexibility while achieving high photocurrent conversion efficiency, comparable to that of their conventional counterparts fabricated on rigid glasses. However, the full realization of highly efficient, flexible PSCs is largely prevented by technical difficulties in simultaneously attaining a transparent electrode with efficient charge transport to meet the specifications of PSCs. In this study, an effective strategy for resolving this technical issue has been devised by proposing a simple but highly effective technique to fabricate an efficient, multilayer TiO2/Ag(O)/ZnO (TAOZ) configuration. This configuration displays low losses in optical transmittance and electrical conductivity owing to its completely continuous, ultrathin metallic Ag(O) transparent electrode, and any notable current leakage is suppressed by its pinhole-free TiO2 electron transport layer. These features are a direct consequence of the rapid evolution of Ag(O) and TiO2 into ultrathin, completely continuous, pinhole-free layers owing to the dramatically improved wetting of metallic Ag(O) with a minimal dose of oxygen (ca. 3 at%) during sputtering. The TAOZ configuration exhibits an average transmittance of 88.5% in the spectral range of 400-800 nm and a sheet resistance of 8.4 Ω sq-1 while demonstrating superior mechanical flexibility to that of the conventional TiO2 on ITO configuration. The photocurrent conversion efficiency of flexible PSCs is significantly improved by up to 11.2% thanks to an optimum combination of optoelectrical performance and pinhole-free morphologies in the TAOZ configuration.

Nitrogen-Mediated Growth of Silver Nanocrystals to Form UltraThin, High-Purity Silver-Film Electrodes with Broad band Transparency for Solar Cells.

Controlling the shape and crystallography of nanocrystals during the early growth stages of a noble metal layer is important because of its correlation with the final layer morphology and optoelectrical features, but this task is unattainable in vapor deposition processes dominated by artificially uncontrollable thermodynamic free energies. We report on experimental evidence for the controllable evolution of Ag nanocrystals as induced by the addition of nitrogen, presumed to be nonresidual in the Ag lattice given its strong float-out behavior. This atypical formation of energetically stable Ag nanocrystals with significantly improved wetting abilities on a chemically heterogeneous substrate promotes the development of an atomically flat, ultrathin, high-purity Ag layer with a thickness of only 5 nm. This facilitates the fabrication of Ag thin-film electrodes exhibiting highly enhanced optical transparency over a broad spectral range in the visible and near-infrared spectral range. An Ag thin-film electrode with a ZnO/Ag/ZnO configuration exhibits an average transmittance of about 95% in the spectral range of 400-800 nm with a maximum transmittance of over 98% at 580 nm, which is comparable with the best transparency values so far reported for transparent electrodes. This degree of optical transparency provides an excellent chance to improve the photon absorption of photovoltaic devices employing an Ag thin film as their window electrode. This is clearly confirmed by the superior performance of a flexible organic solar cell with a power conversion efficiency of 8.0%, which is far superior to that of the same solar cell using a conventional amorphous indium tin oxide electrode (6.4%).

Ultrathin Silver Film Electrodes with Ultralow Optical and Electrical Losses for Flexible Organic Photovoltaics.

Improving the wetting ability of Ag on chemically heterogeneous oxides is technically important to fabricate ultrathin, continuous films that would facilitate the minimization of optical and electrical losses to develop qualified transparent Ag film electrodes in the state-of-the-art optoelectronic devices. This goal has yet to be attained, however, because conventional techniques to improve wetting of Ag based on heterogeneous metallic wetting layers are restricted by serious optical losses from wetting layers. Herein, we report on a simple and effective technique based on the partial oxidation of Ag nanoclusters in the early stages of Ag growth. This promotes the rapid evolution of the subsequently deposited pure Ag into a completely continuous layer on the ZnO substrate, as verified by experimental and numerical evidence. The improvement in the Ag wetting ability allows the development of a highly transparent, ultrathin (6 nm) Ag continuous film, exhibiting an average optical transmittance of 94% in the spectral range 400-800 nm and a sheet resistance of 12.5 Ω sq-1, which would be well-suited for application to an efficient front window electrode for flexible solar cell devices fabricated on polymer substrates.