Regarding crystalline film growth on large lattice-mismatched substrates, there are two primary modes by which thin films grow on a crystal surface or interface. They are Volmer-Weber (VW: island formation) mode and Stranski-Krastanov (SK: layer-plus-island) mode. Since both growth modes end up in the formation of three-dimensional (3D) islands, fabrication of single crystalline films on lattice-mismatched substrates has been challenging. Here, we demonstrate another growth mode, where a buffer layer consisting of 3D islands initially forms and a relaxed two-dimensional (2D) layer subsequently grows on the buffer layer. This 3D-2D mode transition has been realized using impurities. We observed the 3D-2D mode transition for the case of ZnO film growth on 18%-lattice-mismatched sapphire substrates. First, nano-sized 3D islands grow with the help of nitrogen impurities. Then, the islands coalesce to form a 2D layer after cessation of the nitrogen supply, whereupon an increase in the surface energy may provide a driving force for the coalescence. Finally, the films grow in 2D mode, forming atomically flat terraces. We believe that our findings will offer new opportunities for highquality film growth of a wide variety of materials that have no lattice-matched substrates.

We fabricated nanostructured Ge and GeSn films using He radio-frequency magnetron plasma sputtering deposition. Monodisperse amorphous Ge and GeSn nanoparticles of 30–40 nm size were arranged without aggregation by off-axis sputtering deposition in the high He-gas-pressure range of 0.1 Torr. The Ge film porosity was over 30%. We tested the charge/discharge cycle performance of Li-ion batteries with nanostructured Ge and GeSn anodes. The Ge anode with a dispersed arrangement of nanoparticles showed a Li-storage capacity of 565 mAh/g after the 60th cycle. The capacity retention was markedly improved by the addition of 3 at% Sn in Ge anode. The GeSn anode (3 at% Sn) achieved a higher capacity of 1128 mAh/g after 60 cycles with 92% capacity retention. Precise control of the nano-morphology and electrical characteristics by a single step procedure using low temperature plasma is effective for stable cycling of high-capacity Ge anodes.

We present a study on morphological control of nanostructured Ge films by the Ar gas pressure in plasma sputtering deposition. In the low Ar-gas-pressure range, aggregated islands of amorphous grains are formed on the film surface, while in the high-pressure range of 500 mTorr monodisperse nano-grains of about 30 nm in size are orderly arranged without aggregation. The film porosity shows a high value of over 10%. We tested the charge/discharge cycle performance of Li-ion batteries with nanostructured Ge films as anodes. The battery cell with an ordered arrangement structure maintained a high capacity of 434 mAh g−1 after 40 charge/discharge cycles, while that with an aggregated structure exhibited a rapid degradation of capacity to 5.08–183 mAh g−1. An ordered arrangement of Ge nano-grains with a high porosity, which is realized in a simple one-step procedure using high Ar-gas-pressure plasma sputtering, is effective for the stable cycling of high-capacity metal anodes.

The effects of substrates on the growth of sputter-deposited (ZnO) x (InN) 1-x (called "ZION" hereinafter) films have been investigated. We defined the figure of merit (FOM) of ZION films as the reciprocal of the product of full width at half maximum of X-ray rocking curves and root mean square (RMS) roughness. No clear correlation between the FOM and the RMS roughness of the substrates is observed; however, interestingly, a strong correlation between the FOM and the "skewness" of the surface height distribution of the substrates is observed. A possible reason for this is that the existence of a small portion of spikes on the surface, which appear as tiny tails in the distribution but are not reflected in the RMS roughness, limits the migration of adatoms and/or leads to secondary nucleation, degrading the quality of the subsequently grown ZION films. In addition, an atomically flat single-crystalline ZION film is grown on a ZnO template with a small skewness of 0.04.

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