The photoelectrochemical (PEC) properties of a Cu(In,Ga)Se2 (CIGS) photocathode covered with reduced graphene oxide (rGO) as a catalyst binder for solar‐driven hydrogen evolution are reported. Chemically reduced rGO with various concentrations is deposited as an adhesive interlayer between CIGS/CdS and Pt. PEC characteristics of the CIGS/CdS/rGO/Pt are improved compared to the photocathode without rGO due to enhancement of charge transfer via efficient lateral distribution of photogenerated electrons by conductive rGO to the Pt. More importantly, the introduction of rGO to the CIGS photocathode significantly enhances the PEC stability; in the absence of rGO, a rapid loss of PEC stability is observed in 2.5 h, while the optimal rGO increases the PEC stability of the CIGS photocathode for more than 7 h. Chemical and structural characterizations show that the loss of the Pt catalyst is one of the main reasons for the lack of long‐term PEC stability; the introduction of rGO, which acts as a binder to the Pt catalysts by providing anchoring sites in the rGO, results in complete conservation of the Pt and hence much enhanced stability. Multiple functionality of rGO as an adhesive interlayer, an efficient charge transport layer, a diffusion barrier, and protection layer is demonstrated.

By introducing ZnS between Cu(In, Ga)(S,Se) 2 (CIGS) and the CdS, we greatly improved the photoelectrochemical (PEC) performance of the CIGS photocathode for hydrogen evolution. Chemical and structural analysis reveals that the enhanced performance is due to additional band bending driven by in-diffusion of Zn into the CIGS and suppression of nonradiative recombination. The improved onset potential of CIGS photocathode was exploited by building a tandem device with a perovskite absorber for bias-free water splitting. A PEC device with a solar-to-hydrogen conversion efficiency exceeding 9% (the highest among PEC cells including a CIGS photocathode) with a stable operation of 6.5 h is demonstrated.

Tungsten has been commonly used for fine interconnects due to its good gap-filling characteristics in 3D molds, such as trench patterns. However, tungsten shows high deposition stress. This causes mold distortion because tungsten has low ad-atom mobility, and diffusion-driven relaxation does not occur. To reduce tungsten's deposition stress, the shape of the nuclei can be controlled, which is an effective way to suppress the mechanical deformation caused by the formation of a grain boundary between free surfaces during the coalescence stage. In this study, elliptical tungsten nuclei with various aspect ratios, which suppress coalescence in the early stage of deposition, were proposed to reduce the deposition stress. Stress was calculated using the finite element method (FEM) in the range of 0.5 to 8 radius ratios of the tungsten nuclei. The bending of the trench mold was calculated due to tungsten stress and additional coalescence between films during the filling process. As a result, the wider the elliptical nucleus was, the lower the film stress, and mold bending between line patterns was also reduced. The defects in the depth and width of the periodic trench influenced the mold bending in the early growth stage and the stage of coalescence between films, respectively.