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Heterogeneous integration of two-dimensional materials and the conventional semiconductor has opened opportunities for next-generation semiconductor devices and their processing. Heterogeneous integration has been studied for economical manufacturing by substrate recycling and novel functionalities by a combination of incommensurate materials. However, utilizing the integration requires controlling locations of the integrated architectures. Here, we show area-selective deposition (ASD) of germanium on the graphene/MoS2 stack. Ge nucleation precisely occurred on the surfaces of the patterned graphene/MoS2 stack via dipole engineering. In this study, the growth temperature of ASD of Ge was significantly lower than that based on precursor desorption on SiO2. The first-principles calculations revealed that Ge deposited by ASD on the graphene/MoS2 stack was not affected by charge transfer. This work provides a viable way to utilize atomically thin materials for next-generation semiconductor devices, which can be applicable for “Beyond Moore” and “More Moore” approaches.

Abstract Remote epitaxy has opened novel opportunities for advanced manufacturing and heterogeneous integration of two-dimensional (2D) materials and conventional (3D) materials. The lattice transparency as the fundamental principle of remote epitaxy has been studied and challenged by recent observations defying the concept. Understanding remote epitaxy requires an integrated approach of theoretical modeling and experimental validation at multi-scales because the phenomenon includes remote interactions of atoms across an atomically thin material and a few van der Waals gaps. The roles of atomically thin 2D material for the nucleation and growth of a 3D material have not been integrated into a framework of remote epitaxy research. Here, we summarize studies of remote epitaxy mechanisms with a comparison to other epitaxy techniques. In the end, we suggest the crucial topics of remote epitaxy research for basic science and applications. Graphical Abstract

Growing three-dimensional (3D) materials on two-dimensional (2D) van der Waals surface has shown its effectiveness in overcoming materials incompatibility for stacking transferrable membranes toward advanced device manufacturing. Herein, we demonstrate that the nucleation of hexagonal germanium (Ge) grains within a continuous crystalline film, which has been unfeasible through traditional epitaxy techniques, is realized by chemical vapor deposition on top of n-type monolayer molybdenum disulfide (MoS2) substrates. Suggested by quantum molecular dynamics calculation, the hexagonal Ge nucleation is thermodynamically preferable to cubic Ge when growing on monolayer MoS2 with sulfur vacancies. The strained hexagonal Ge grains have been confirmed by transmission electron microscopy analyses from both real space and reciprocal space. Scanning probe microscopy shows that the hexagonal Ge film possesses higher reflectivity in infrared spectral range, implying a higher carrier concentration resulted from the narrower band gap, as compared to cubic Ge.

Abstract The discovery of topological Hall effect (THE) has important implications for next‐generation high‐density nonvolatile memories, energy‐efficient nanoelectronics, and spintronic devices. Both real‐space topological spin configurations and two anomalous Hall effects (AHE) with opposite polarity due to two magnetic phases have been proposed for THE‐like feature in SrRuO3 (SRO) films. In this work, SRO thin films with and without THE‐like features are systematically Investigated to decipher the origin of the THE feature. Magnetic measurement reveals the coexistence of two magnetic phases of different coercivity (Hc) in both the films, but the hump feature cannot be explained by the two channel AHE model based on these two magnetic phases. In fact, the AHE is mainly governed by the magnetic phase with higher Hc. A diffusive Berry phase transition model is proposed to explain the THE feature. The coexistence of two Berry phases with opposite signs over a narrow temperature range in the high Hc magnetic phase can explain the THE like feature. Such a coexistence of two Berry phases is due to the strong local structural tilt and microstructure variation in the thinner films. This work provides an insight between structure/micro structure and THE like features in SRO epitaxial thin films.

Abstract Transition metal oxides exhibit a plethora of electrical and magnetic properties described by their order parameters. In particular, ferroic orderings offer access to a rich spectrum of fundamental physics phenomena, in addition to a range of technological applications. The heterogeneous integration of ferroelectric and ferromagnetic materials is a fruitful way to design multiferroic oxides. The realization of freestanding heterogeneous membranes of multiferroic oxides is highly desirable. In this study, epitaxial BaTiO3/La0.7Sr0.3MnO3 freestanding bilayer membranes are fabricated using pulsed laser epitaxy. The membrane displays ferroelectricity and ferromagnetism above room temperature accompanying the finite magnetoelectric coupling constant. This study reveals that a freestanding heterostructure can be used to manipulate the structural and emergent properties of the membrane. In the absence of the strain caused by the substrate, the change in orbital occupancy of the magnetic layer leads to the reorientation of the magnetic easy‐axis, that is, perpendicular magnetic anisotropy. These results of designing multiferroic oxide membranes open new avenues to integrate such flexible membranes for electronic applications.

Abstract We report on morphology-controlled remote epitaxy via hydrothermal growth of ZnO micro- and nanostructure crystals on graphene-coated GaN substrate. The morphology control is achieved to grow diverse morphologies of ZnO from nanowire to microdisk by changing additives of wet chemical solution at a fixed nutrient concentration. Although the growth of ZnO is carried out on poly-domain graphene-coated GaN substrate, the direction of hexagonal sidewall facet of ZnO is homogeneous over the whole ZnO-grown area on graphene/GaN because of strong remote epitaxial relation between ZnO and GaN across graphene. Atomic-resolution transmission electron microscopy corroborates the remote epitaxial relation. The non-covalent interface is applied to mechanically lift off the overlayer of ZnO crystals via a thermal release tape. The mechanism of facet-selective morphology control of ZnO is discussed in terms of electrostatic interaction between nutrient solution and facet surface passivated with functional groups derived from the chemical additives.

Realizing a tubular conduction channel within a one-dimensional core–shell nanowire (NW) enables better understanding of quantum phenomena and exploration of electronic device applications. Herein, we report the growth of a SiGe(P)/Si core/shell NW heterostructure using a chemical vapor deposition coupled with vapor–liquid–solid growth mechanism. The entire NW heterostructure behaves as a p-type semiconductor, which demonstrates that the high-density carriers are confined within the 4 nm-thick Si shell and form a tubular conduction channel. These findings are confirmed by both calculations and the gate-dependent current–voltage (Id–Vg) characteristics. Atomic resolution microscopic analyses suggest a coherent epitaxial core/shell interface where strain is released by forming dislocations along the axial direction of the NW heterostructure. Additional surface passivation achieved via growing a SiGe(P)/Si/SiGe core/multishell NW heterostructure suggests potential strategies to enhance the tubular carrier density, which could be further modified by improving multishell crystallinity and structural design.

Abstract A variety of mechanisms are reported to play critical roles in contributing to the high carrier/electron mobility in oxide/SrTiO3 (STO) heterostructures. By using La0.95Sr0.05TiO3 (LSTO) epitaxially grown on different single crystal substrates (such as STO, GdScO3, LaAlO3, (LaAlO3)0.3(Sr2AlTaO6)0.7, and CeO2 buffered STO) as the model systems, the formation of a conducting substrate surface layer (CSSL) on STO substrate is shown at relatively low growth temperature and high oxygen pressure (725 °C, 5 × 10–4 Torr), which contributes to the enhanced conductivity of the LSTO/STO heterostructures. Different from the conventional oxygen vacancy model, this work reveals that the formation of the CSSL occurs when growing an oxide layer (LSTO in this case) on STO, while neither annealing nor the growth of an Au layer alone at the exact same growth condition generates the CSSL in STO. It demonstrates that the oxide layer actively pulls oxygen from STO substrate at given growth conditions, leading to the formation of the CSSL. The observations emphasize the oxygen transfer across film/substrate interface during the synthesis of oxide heterostructures playing a critical role in functional properties.

In this work, we employ an atomic force microscopy-based technique, Kelvin probe force microscopy, to analyze heterogeneities of four different 2D/3D Ge/MoS2 heterostructures with Ge chemical vapor deposition (CVD) time. High-contrast spatially resolved contact potential difference (CPD) maps reveal the evolution of the samples by Ge deposition. The CPD map in an as-prepared sample does not display any heterogeneity, but CPD contrasts along the grain boundaries are obviously noticed as Ge is deposited on MoS2. With a sufficiently long Ge CVD deposition time, strong grain-to-grain CPD variations over the 2D/3D heterostructures are observed. The results show the variations of the work function from grain to grain that are attributed to the strain induced by the Ge island formation on the cracked MoS2 initiated by sulfur vacancies.