Polycrystalline Ge thin films have recently attracted renewed attention as a material for various electronic and optical devices. However, the difficulty in the Fermi level control of polycrystalline Ge films owing to their high density of defect-induced acceptors has limited their application in the aforementioned devices. Here, we experimentally estimated the origin of acceptor defects by significantly modulating the crystallinity and electrical properties of polycrystalline Ge layers and investigating their correlation. Our proposed linear regression analysis method, which is based on deriving the acceptor levels and their densities from the temperature dependence of the hole concentration, revealed the presence of two different acceptor levels. A systematic analysis of the effects of grain size and post annealing on the hole concentration suggests that deep acceptor levels (53–103 meV) could be attributed to dangling bonds located at grain boundaries, whereas shallow acceptor levels (< 15 meV) could be attributed to vacancies in grains. Thus, this study proposed a machine learning-based simulation method that can be widely applied in the analysis of physical properties, and can provide insights into the understanding and control of acceptor defects in polycrystalline Ge thin films.

Ni-induced layer exchange enabled us to form multilayer graphene (MLG) at 350 °C. The key was to avoid air exposure of sputtered amorphous carbon, which dramatically reduced the layer exchange temperature. Raman spectroscopy, transmission electron microscopy, and scanning electron microscopy showed that the resulting MLG layer had higher uniformity and crystallinity than conventional MLG formed above 600 °C. The electrical conductivity of the 350 °C formed MLG exceeded 500 S cm−1. These findings provide insight into the solid-phase synthesis of MLG from amorphous carbon and open up flexible device applications.

SiGe is a promising anode material for replacing graphite in next generation thin-film batteries owing to its high theoretical charge/discharge capacity. Metal-induced layer exchange (LE) is a unique technique used for the low-temperature synthesis of SiGe layers on arbitrary substrates. Here, we demonstrate the synthesis of Si1−xGex (x = 0–1) layers on plastic films using Al-induced LE. The resulting SiGe layers exhibited high electrical conductivity (up to 1200 S cm−1), reflecting the self-organized doping effect of LE. Moreover, the Si1−xGex layer synthesized by the same process was adopted as the anode for the lithium-ion battery. All Si1−xGex anodes showed clear charge/discharge operation and high coulombic efficiency (≥ 97%) after 100 cycles. While the discharge capacities almost reflected the theoretical values at each x at 0.1 C, the capacity degradation with increasing current rate strongly depended on x. Si-rich samples exhibited high initial capacity and low capacity retention, while Ge-rich samples showed contrasting characteristics. In particular, the Si1−xGex layers with x ≥ 0.8 showed excellent current rate performance owing to their high electrical conductivity and low volume expansion, maintaining a high capacity (> 500 mAh g–1) even at a high current rate (10 C). Thus, we revealed the relationship between SiGe composition and anode characteristics for the SiGe layers formed by LE at low temperatures. These results will pave the way for the next generation of flexible batteries based on SiGe anodes.

Despite its long history, synthesizing n-type polycrystalline Ge layers with high-electron mobility on insulating substrates has been difficult. Based on our recently developed solid-phase crystallization technology, here, we have demonstrated the highest recorded electron mobility (450 cm2 V−1 s−1) for Ge-based polycrystalline thin films on insulating substrates. The underlayer type and small amount of Sn addition were the key parameters controlling both the density and barrier height of the grain boundaries in the P-doped polycrystalline Ge layers. The low growth temperature (≤400 °C) allowed us to develop a GeSn layer on a heat-resistant polyimide film, which exhibited the highest electron mobility (200 cm2 V−1 s−1), as a semiconductor thin film synthesized directly on a flexible substrate. These achievements herald the development of high-performance polycrystalline Ge-based devices on inexpensive glass and flexible plastic substrates.

The carrier mobility of polycrystalline Ge thin-film transistors has significantly improved in recent years, raising hopes for the realization of next-generation electronic devices. Here, we adapted advanced solid-phase crystallization, which achieved the highest hole mobility of the polycrystalline semiconductor layer, to Ge layers doped with n-type impurities (P, As, and Sb). The type and amount of dopants had marked effects on the growth morphology and electrical properties of the Ge layers because they altered the activation energies in crystal growth, dopant activation rates, and grain boundary properties. In particular, P doping was effective in increasing the grain size (25 μm) and lowering the grain boundary barrier height (20 meV), which improved the electron concentration (8.0 × 1018 cm–3) and electron mobility (380 cm2 V–1 s–1) in n-type polycrystalline Ge layers. The electron mobility is greater than that of most semiconductor layers synthesized at low temperatures (≤500 °C) on insulators, and this will pave the way for advanced electronic devices, such as multifunctional displays and three-dimensional large-scale integrated circuits.