Integrating the diverse functionalities of complex oxides into semiconductor [1-7] and flexible [8-12] electronics is a major technological challenge that has motivated extensive work. But despite considerable effort, the structural, chemical, and thermal mismatches between such substrates and complex-oxide materials often yield films with considerably worse crystal quality than that attained on single-crystal perovskite substrates. Alternative strategies for hetero-integration via substrate release and transfer, mimicking the fabrication processes of van-der-Waals heterostructures, [13-15] are just now beginning to yield single-crystal oxide films on arbitrary substrates, [16-21] thus circumventing the constraints of epitaxial growth. Moreover, these detached films no longer experience mechanical constraint from the substrate, giving more flexibility in structural manipulation and heterostructure assembly. Strain control over the lattice structure is particularly impactful in ferroelectrics where the polarization is directly connected to structural distortions. [22,23] In thin films, strain can define the optimal operating temperature regime [24-26] or domain configuration [27-29] that will boost electro-mechanical or thermal functionalities, 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 BaTiO 3 , production of precisely strain-engineered, substratereleased 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 −1 and 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. Perovskite ABO 3 oxides can display an immense number of phases and functions by merely changing the A-and B-site cations. Even within a single chemistry, multiple phases can be in competition, and their stability can be tuned statically by fixing The ORCID identification number(s) for the ...
Surface molecular imprinting, in particular over nanosized support materials, is very suitable for a template of bulky structure like protein. Inspired by the surface template immobilization method reported previously, we herein demonstrate an alternative strategy for enhancing specific recognition of core-shell protein-imprinted nanoparticles through prefunctionalizing the cores with noncovalent template sorption groups. For proof of this concept, silica nanoparticles chosen as the core materials were modified consecutively with 3-aminopropyltrimethoxysilane and maleic anhydride to introduce polymerizable double bonds and terminal carboxyl groups, hence capable of physically adsorbing the print protein. With lysozyme as a template, thin protein-imprinted shells were fabricated according to our newly developed approach for surface protein imprinting over nanoparticles. The rebinding experiments confirmed that the introduction of the carboxyl groups could remarkably improve the imprinting effect in relation to a significantly increased imprinting factor and specific rebinding capacity. Moreover, in contrast to the harsh template removal conditions required for the covalent template coupling approach, the template removal during the imprinted particle synthesis as well as desorption after rebinding could be mildly achieved via washing with salt solution.
Mechanical displacement in commonly used piezoelectric materials is typically restricted to linear or biaxial in nature and to a few percent of the material dimensions. Here, we show that free-standing BaTiO3 membranes exhibit non-conventional electromechanical coupling. Under an external electric field, these superelastic membranes undergo controllable and reversible "sushi-rolling-like" 180° folding-unfolding cycles. This crease-free folding is mediated by charged ferroelectric domains, leading to a giant > 3.8 and 4.6 µm displacements for a 30-nm thick membrane at room temperature and 60 °C, respectively. Further increasing the electric field above the coercive value changes the fold curvature, hence augmenting the effective piezoresponse. Finally, it is found that the membranes fold with increasing temperature followed by complete immobility of the membrane above the Curie temperature, allowing us to model the ferroelectric-domain origin of the effect.The electromechanical power conversion of piezoelectrics is the basis for a broad range of sensing, actuating, and communication technologies, including ultrasound imaging and cellular phones. 1-3 Recent interest in electromechanical energy harvesting 4,5 as well as in flexible electronics for wearable devices, 6,7 nano motors, 8 and medical applications 9-11 raises a need for flexible piezoelectric materials and devices. Modern applications of piezoelectrics hinge on thin films, 12-14 however, the substrate in such geometries is typically rigid, preventing the development of flexible devices. Flexible piezoelectric devices are therefore typically based on either nanowires 4 or on thin-film systems, but with substrates that have been designed especially for such applications. 15,16 Most piezoelectric applications rely on lead-based materials, which exhibit strong piezoelectric coefficients. Nevertheless, the toxicity of these materials is undesirable for environmental considerations, while it also disqualifies them for medical or wearable applications. Likewise, traditional thin-film geometries limit the electromechanical excitation modes. That is, usually, uniaxial electric field results in either parallel or perpendicular uniaxial or biaxial mechanical deformation (or vice versa).Nevertheless, the interest in flexible-electronic technologies raises a need for advanced electromechanical excitation modes, e.g., for motorized devices, including microscale aerial vehicles. 17 Substrate removal for piezoelectric films or membranes augments their functional properties, 18-21 mainly thanks to mechanically-induced ferroic-domain reorganization. 22 However, the preparation of completely stand-alone substrate-free films has remained a challenge. Lu et al. 23 demonstrated lately a general method to prepare oxide materials in the form of membranes, i.e., continuous free-standing thin films with no substrate. More recently, Dong et al. 24 used this method to process BaTiO3 membranes, which is a well-known lead-free piezoelectric and ferroelectric material. This work show...
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