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1. Epitaxy and Exfoliation of Free-Standing Heusler Membranes Using a Graphene Interlayer

   https://doi.org/arXiv200610100D  

   Du, Dongxue ; Manzo, Sebastian ; Zhang, Chenyu ; Saraswat, Vivek ; Arnold, Michael S ; Voyles, Paul M ; Kawasaki, Jason K ( January 2020 , ArXivorg)

   null (Ed.)

   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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2. Strain and strain gradient engineering in membranes of quantum materials

   https://doi.org/10.1063/5.0146553  

   Du, Dongxue ; Hu, Jiamian ; Kawasaki, Jason K. ( April 2023 , Applied Physics Letters)

   Strain is powerful for discovery and manipulation of new phases of matter; however, elastic strains accessible to epitaxial films and bulk crystals are typically limited to small ( < 2 %), uniform, and often discrete values. This Perspective highlights emerging directions for strain and strain gradient engineering in free-standing single-crystalline membranes of quantum materials. Membranes enable large ( ∼ 10 %), continuously tunable strains and strain gradients via bending and rippling. Moreover, strain gradients break inversion symmetry to activate polar distortions, ferroelectricity, chiral spin textures, superconductivity, and topological states. Recent advances in membrane synthesis by remote epitaxy and sacrificial etch layers enable extreme strains in transition metal oxides, intermetallics, and Heusler compounds, expanding beyond the natively van der Waals (vdW) materials like graphene. We highlight emerging opportunities and challenges for strain and strain gradient engineering in membranes of non-vdW materials. 

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3. Pinhole-seeded lateral epitaxy and exfoliation of GaSb films on graphene-terminated surfaces

   https://doi.org/10.1038/s41467-022-31610-y  

   Manzo, Sebastian ; Strohbeen, Patrick J. ; Lim, Zheng Hui ; Saraswat, Vivek ; Du, Dongxue ; Xu, Shining ; Pokharel, Nikhil ; Mawst, Luke J. ; Arnold, Michael S. ; Kawasaki, Jason K. ( July 2022 , Nature Communications)

   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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4. Crystal Symmetry Engineering in Epitaxial Perovskite Superlattices

   https://doi.org/10.1002/adfm.202106466  

   Ding, Xiang ; Yang, Baishun ; Leng, Huaqian ; Jang, Jae Hyuch ; Zhao, Junrui ; Zhang, Chao ; Zhang, Sa ; Cao, Guixin ; Zhang, Ji ; Mishra, Rohan ; et al ( August 2021 , Advanced Functional Materials)

   Interface plays a critical role in determining the physical properties and device performance of heterostructures. Traditionally, lattice mismatch, resulting from the different lattice constants of the heterostructure, can induce epitaxial strain. Over past decades, strain engineering has been demonstrated as a useful strategy to manipulate the functionalities of the interface. However, mismatch of crystal symmetry at the interface is relatively less studied due to the difficulty of atomically structural characterization, particularly for the epitaxy of low symmetry correlated materials on the high symmetry substrates. Overlooking those phenomena restrict the understanding of the intrinsic properties of the as‐ determined heterostructure, resulting in some long‐standing debates including the origin of magnetic and ferroelectric dead layers. Here, perovskite LaCoO₃‐SrTiO₃superlattice (SL) is used as a model system to show that the crystal symmetry effect can be isolated by the existing interface strain. Combining the state‐of‐art diffraction and electron microscopy, it is found that the symmetry mismatch of LaCoO₃‐SrTiO₃SL can be tuned by manipulating the SrTiO₃layer thickness to artificially control the magnetic properties. The work suggests that crystal symmetry mismatch can also be designed and engineered to act as an effective strategy to generate functional properties of perovskite oxides.

    

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5. Beyond Substrates: Strain Engineering of Ferroelectric Membranes

   https://doi.org/10.1002/adma.202003780  

   Pesquera, David ; Parsonnet, Eric ; Qualls, Alexander ; Xu, Ruijuan ; Gubser, Andrew J. ; Kim, Jieun ; Jiang, Yizhe ; Velarde, Gabriel ; Huang, Yen‐Lin ; Hwang, Harold Y. ; et al ( September 2020 , Advanced Materials)

   Strain engineering in perovskite oxides provides for dramatic control over material structure, phase, and properties, but is restricted by the discrete strain states produced by available high‐quality substrates. Here, using the ferroelectric BaTiO₃, production of precisely strain‐engineered, substrate‐released nanoscale membranes is demonstrated via an epitaxial lift‐off process that allows the high crystalline quality of films grown on substrates to be replicated. In turn, fine structural tuning is achieved using interlayer stress in symmetric trilayer oxide‐metal/ferroelectric/oxide‐metal structures fabricated from the released membranes. In devices integrated on silicon, the interlayer stress provides deterministic control of ordering temperature (from 75 to 425 °C) and releasing the substrate clamping is shown to dramatically impact ferroelectric switching and domain dynamics (including reducing coercive fields to <10 kV cm⁻¹and improving switching times to <5 ns for a 20 µm diameter capacitor in a 100‐nm‐thick film). In devices integrated on flexible polymers, enhanced room‐temperature dielectric permittivity with large mechanical tunability (a 90% change upon ±0.1% strain application) is demonstrated. This approach paves the way toward the fabrication of ultrafast CMOS‐compatible ferroelectric memories and ultrasensitive flexible nanosensor devices, and it may also be leveraged for the stabilization of novel phases and functionalities not achievable via direct epitaxial growth.

    

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