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  1. In nature, structural and functional materials often form programmed three-dimensional (3D) assembly to perform daily functions, inspiring researchers to engineer multifunctional 3D structures. Despite much progress, a general method to fabricate and assemble a broad range of materials into functional 3D objects remains limited. Herein, to bridge the gap, we demonstrate a freeform multimaterial assembly process (FMAP) by integrating 3D printing (fused filament fabrication (FFF), direct ink writing (DIW)) with freeform laser induction (FLI). 3D printing performs the 3D structural material assembly, while FLI fabricates the functional materials in predesigned 3D space by synergistic, programmed control. This paper showcases the versatility of FMAP in spatially fabricating various types of functional materials (metals, semiconductors) within 3D structures for applications in crossbar circuits for LED display, a strain sensor for multifunctional springs and haptic manipulators, a UV sensor, a 3D electromagnet as a magnetic encoder, capacitive sensors for human machine interface, and an integrated microfluidic reactor with a built-in Joule heater for nanomaterial synthesis. This success underscores the potential of FMAP to redefine 3D printing and FLI for programmed multimaterial assembly.

     
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    Free, publicly-accessible full text available December 1, 2025
  2. While electrical poling of organic ferroelectrics has been shown to improve device properties, there are challenges in visualizing accompanying structural changes. We observe poling induced changes in ferroelectric domains by applying differential phase contrast (DPC) imaging in the scanning transmission electron microscope, a method that has been used to observe spatial distributions of electromagnetic fields at the atomic scale. In this work, we obtain DPC images from unpoled and electrically poled polyvinylidene fluoride trifluorethylene films and compare their performance in polymer thin film transistors. The vertically poled films show uniform domains throughout the bulk compared to the unpoled film with a significantly higher magnitude of the overall polarization. Thin film transistors comprising a donor–acceptor copolymer as the active semiconductor layer show improved performance with the vertically poled ferroelectric dielectric film compared with the unpoled ferroelectric dielectric film. A poling field of 80–100 MV/m for the dielectric layer yields the best performing transistors; higher than 100 MV/m is seen to degrade the transistor performance. The results are consistent with a reduction in deleterious charge carrier scattering from ferroelectric domain boundaries or interfacial dipoles arising from electrical poling.

     
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    Free, publicly-accessible full text available April 8, 2025
  3. Free, publicly-accessible full text available December 27, 2024
  4. We report the growth of epitaxial wurtzite AlScN thin films on Si (111) substrates with a wide range of Sc concentrations using ultra-high vacuum reactive sputtering. Sc alloying in AlN enhances piezoelectricity and induces ferroelectricity, and epitaxial thin films facilitate systematic structure-based investigations of this important and emerging class of materials. Two main effects are observed as a function of increasing Sc concentration. First, increasing crystalline disorder is observed together with a structural transition from wurtzite to rocksalt at ∼30 at% Sc. Second, nanoscale compositional segregation consistent with spinodal decomposition occurs at intermediate compositions, before the wurtzite to rocksalt phase boundary is reached. Lamellar features arising from composition fluctuations are correlated with polarization domains in AlScN, suggesting that composition segregation can influence ferroelectric properties. The present results provide a route to the creation of single crystal AlScN films on Si (111), as well as a means for self-assembled composition modulation. 
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  5. Core–shell Ge/GeSn nanowires provide a route to dislocation-free single crystal germanium-tin alloys with desirable light emission properties because the Ge core acts as an elastically compliant substrate during misfitting GeSn shell growth. However, the uniformity of tin incorporation during reduced pressure chemical vapor deposition may be limited by the kinetics of mass transfer to the shell during GeSn growth. The balance between Sn precursor flux and available surfaces for GeSn nucleation and growth determines whether defects are formed and their type. On the one hand, when the Sn precursor delivery is insufficient, local variations in Sn arrival rate at the nanowire surfaces during GeSn growth produce asymmetries in shell growth that induce wire bending. This inhomogeneous elastic dilatation due to the varying composition occurs via deposition of Sn-poor regions on some of the {112} sidewall facets of the nanowires. On the other hand, when the available nanowire surface area is insufficient to accommodate the arriving Sn precursor flux, Sn-rich precipitate formation results. Between these two extremes, there exists a regime of growth conditions and nanowire densities that permits defect-free GeSn shell growth. 
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  6. Solar water splitting using photoelectrochemical cells (PEC's) is a promising pathway toward clean and sustainable storage of renewable energy. Practical realization of solar-driven synthesis of hydrogen and oxygen integrating light absorption and electrolysis of water has been challenging because of (1) the limited stability of good photovoltaic materials under the required electrochemical conditions, and (2) photovoltaic efficiency losses due to light absorption by catalysts, the electrolyte, and generated bubbles, or reflection at their various interfaces. Herein, we evaluate a novel integrated solar water splitting architecture using efficient silicon heterojunction photovoltaic cells that avoids such losses and exhibits a solar-to-hydrogen (STH) efficiency in excess of 10%. Series-connected silicon Heterojunction with Intrinsic Thin layer (HIT) cells generate sufficient photovoltage for unassisted water splitting, with one of the cells acting as the photocathode. Platinum is deposited on the back (dark) junction of this HIT cell as the catalyst for the hydrogen evolution reaction (HER). The photocathode is protected from corrosion by a TiO 2 layer deposited by atomic layer deposition (ALD) interposed between the HIT cell and the Pt, enabling stable operation for >120 hours. Combined with oxygen evolution reaction (OER) catalysts deposited on a porous metal dark anode, these PEC's achieve stable water splitting with a record high STH efficiency for an integrated silicon photosynthesis device. 
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