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  1. The synthesis of functional graphene nanostructures on Ge(001) provides an attractive route toward integrating graphene-based electronic devices onto complementary metal oxide semiconductor-compatible platforms. In this study, we leverage the phenomenon of the anisotropic growth of graphene nanoribbons from rationally placed graphene nanoseeds and their rotational self-alignment during chemical vapor deposition to synthesize mesoscale graphene nanomeshes over areas spanning several hundred square micrometers. Lithographically patterned nanoseeds are defined on a Ge(001) surface at pitches ranging from 50 to 100 nm, which serve as starting sites for subsequent nanoribbon growth. Rotational self-alignment of the nanoseeds followed by anisotropic growth kinetics causes the resulting nanoribbons to be oriented along each of the equivalent, orthogonal Ge⟨110⟩ directions with equal probability. As the nanoribbons grow, they fuse, creating a continuous nanomesh. In contrast to nanomesh synthesis via top-down approaches, this technique yields nanomeshes with atomically faceted edges and covalently bonded junctions, which are important for maximizing charge transport properties. Additionally, we simulate the electrical characteristics of nanomeshes synthesized from different initial nanoseed-sizes, size-polydispersities, pitches, and device channel lengths to identify a parameter-space for acceptable on/off ratios and on-conductance in semiconductor electronics. The simulations show that decreasing seed diameter and pitch are critical to increasing nanomesh on/off ratio and on-conductance, respectively. With further refinements in lithography, nanomeshes obtained via seeded synthesis and anisotropic growth are likely to have superior electronic properties with tremendous potential in a multitude of applications, such as radio frequency communications, sensing, thin-film electronics, and plasmonics. 
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  2. Remote epitaxy is promising for the synthesis of lattice-mismatched materials, exfoliation of membranes, and reuse of expensive substrates. However, clear experimental evidence of a remote mechanism remains elusive. Alternative mechanisms such as pinhole-seeded epitaxy or van der Waals epitaxy can often explain the resulting films. Here, we show that growth of the Heusler compound GdPtSb on clean graphene/sapphire produces a 30° rotated (R30) superstructure that cannot be explained by pinhole epitaxy. With decreasing temperature, the fraction of this R30 domain increases, compared to the direct epitaxial R0 domain, which can be explained by a competition between remote versus pinhole epitaxy. Careful graphene/substrate annealing and consideration of the relative lattice mismatches are required to obtain epitaxy to the underlying substrate across a series of other Heusler films, including LaPtSb and GdAuGe. The R30 superstructure provides a possible experimental fingerprint of remote epitaxy, since it is inconsistent with the leading alternative mechanisms. 
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  3. Hybrid MBE produces epitaxial SrTiO 3 free-standing nanomembranes using remote epitaxy in an adsorption-controlled manner. 
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  4. Abstract

    Remote epitaxy is a promising approach for synthesizing exfoliatable crystalline membranes and enabling epitaxy of materials with large lattice mismatch. However, the atomic scale mechanisms for remote epitaxy remain unclear. Here we experimentally demonstrate that GaSb films grow on graphene-terminated GaSb (001) via a seeded lateral epitaxy mechanism, in which pinhole defects in the graphene serve as selective nucleation sites, followed by lateral epitaxy and coalescence into a continuous film. Remote interactions are not necessary in order to explain the growth. Importantly, the small size of the pinholes permits exfoliation of continuous, free-standing GaSb membranes. Due to the chemical similarity between GaSb and other III-V materials, we anticipate this mechanism to apply more generally to other materials. By combining molecular beam epitaxy with in-situ electron diffraction and photoemission, plus ex-situ atomic force microscopy and Raman spectroscopy, we track the graphene defect generation and GaSb growth evolution a few monolayers at a time. Our results show that the controlled introduction of nanoscale openings in graphene provides an alternative route towards tuning the growth and properties of 3D epitaxial films and membranes on 2D material masks.

     
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  6. Semiconducting carbon nanotubes promise faster performance and lower power consumption than Si in field-effect transistors (FETs) if they can be aligned in dense arrays. Here, we demonstrate that nanotubes collected at a liquid/liquid interface self-organize to form two-dimensional (2D) nematic liquid crystals that globally align with flow. The 2D liquid crystals are transferred onto substrates in a continuous process generating dense arrays of nanotubes aligned within ±6°, ideal for electronics. Nanotube ordering improves with increasing concentration and decreasing temperature due to the underlying liquid crystal phenomena. The excellent alignment and uniformity of the transferred assemblies enable FETs with exceptional on-state current density averaging 520 μA μm −1 at only −0.6 V, and variation of only 19%. FETs with ion gel top gates demonstrate subthreshold swing as low as 60 mV decade −1 . Deposition across a 10-cm substrate is achieved, evidencing the promise of 2D nanotube liquid crystals for commercial semiconductor electronics. 
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  7. Abstract

    Single-crystalline membranes of functional materials enable the tuning of properties via extreme strain states; however, conventional routes for producing membranes require the use of sacrificial layers and chemical etchants, which can both damage the membrane and limit the ability to make them ultrathin. Here we demonstrate the epitaxial growth of the cubic Heusler compound GdPtSb on graphene-terminated Al2O3substrates. Despite the presence of the graphene interlayer, the Heusler films have epitaxial registry to the underlying sapphire, as revealed by x-ray diffraction, reflection high energy electron diffraction, and transmission electron microscopy. The weak Van der Waals interactions of graphene enable mechanical exfoliation to yield free-standing GdPtSb membranes, which form ripples when transferred to a flexible polymer handle. Whereas unstrained GdPtSb is antiferromagnetic, measurements on rippled membranes show a spontaneous magnetic moment at room temperature, with a saturation magnetization of 5.2 bohr magneton per Gd. First-principles calculations show that the coupling to homogeneous strain is too small to induce ferromagnetism, suggesting a dominant role for strain gradients. Our membranes provide a novel platform for tuning the magnetic properties of intermetallic compounds via strain (piezomagnetism and magnetostriction) and strain gradients (flexomagnetism).

     
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    Single-crystalline membranes of functional materials enable the tuning of properties via extreme strain states; however, conventional routes for producing membranes require the use of sacrificial layers and chemical etchants, which can both damage and limit the ability to make membranes ultrathin. Here we demonstrate the epitaxial growth of cubic and hexagonal Heusler compounds on graphene-terminated Al$_2$O$_3$ substrates. The weak Van der Waals interactions of graphene enable the mechanical exfoliation of LaPtSb and GdPtSb films to yield free-standing membranes. Despite the presence of the graphene interlayer, the Heusler films have epitaxial registry to the underlying sapphire, as revealed by x-ray diffraction, reflection high energy electron diffraction, and transmission electron microscopy. Some films show a uniform in-plane rotation of several degrees with respect to the substrate, which we attribute to a combination of lattice mismatch and weakened Heusler film / sapphire substrate interactions through graphene. The residual resistivity of semi free-standing films on graphene-terminated substrates is similar to the residual resistivity of films grown by direct epitaxy. Our graphene-mediated approach provides a promising platform for tuning the magnetic, topological, and multiferroic properties of Heuslers in a clean, single-crystalline membrane system. 
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