Building artificial neurons and synapses is key to achieving the promise of energy efficiency and acceleration envisioned for brain-inspired information processing. Emulating the spiking behavior of biological neurons in physical materials requires precise programming of conductance nonlinearities. Strong correlated solid-state compounds exhibit pronounced nonlinearities such as metal-insulator transitions arising from dynamic electron-electron and electron-lattice interactions.
View Article and Find Full Text PDFJ Phys Chem C Nanomater Interfaces
October 2024
Nucleation particles, solid phases dispersed throughout a medium to decrease the energy barrier for solidification or other reversible phase transitions, are generally selected on the basis of structural or interfacial energy considerations between the host phase and the solid phase that is crystallizing. However, the existence of chemical reactions between the nucleation particles and the host phase can obscure these underlying relationships, thereby complicating the process of selection of active nucleation particle phases. Here, we reveal the origin of nucleation activity of barium-based nucleation particles in the salt hydrate calcium chloride hexahydrate (CCH), a candidate for near room temperature thermal energy storage.
View Article and Find Full Text PDFAny electrical signal propagating in a metallic conductor loses amplitude due to the natural resistance of the metal. Compensating for such losses presently requires repeatedly breaking the conductor and interposing amplifiers that consume and regenerate the signal. This century-old primitive severely constrains the design and performance of modern interconnect-dense chips.
View Article and Find Full Text PDFWe present soft-template encapsulation of salt hydrate phase change materials (PCMs) using modified silica particles to both stabilize emulsions and serve as initiators for organocatalyzed photoredox ATRP. The resulting core-shell structures have high core loading and are robust to thermal cycling. Critically, this strategy eliminates the need for a reagent in the core phase, thus preserving purity, and offers the ability to tailor shell composition for desired applications.
View Article and Find Full Text PDFStoichiometric salt hydrates can be inexpensive and provide higher volumetric energy density relative to other near-room-temperature phase change materials (PCMs), but few salt hydrates exhibit congruent melting behavior between 0 and 30 °C. Eutectic salt hydrates offer a strategy to design bespoke PCMs with tailored application-specific eutectic melting temperatures. However, the general solidification behavior and stability of eutectic salt hydrate systems remain unclear, as metastable solidification in eutectic salt hydrates may introduce opportunities for phase segregation.
View Article and Find Full Text PDFOne of the challenges preventing wide use of inorganic salt hydrate phase change materials (PCMs) is their low viscosity above their melting point, leading to leakage, phase segregation, and separation from heat exchanger surfaces in thermal management applications. The development of a broad strategy for using polymers that provide tunable, temperature-reversible shape stabilization of a variety of salt hydrates by using the lowest possible polymer concentrations is hindered by differences in solubility and gelation behavior of polymers with change in the type of ion. This work addressed the challenge of creating robust, temperature-responsive shape-stabilizing polymer gels (i.
View Article and Find Full Text PDFCurrent thermally conductive and electrically insulating insulation systems are struggling to meet the needs of modern electronics due to increasing heat generation and power densities. Little research has focused on creating insulation systems that excel at both dissipating heat and withstanding high voltages (i.e.
View Article and Find Full Text PDFIn this work, we developed a method using precession electron diffraction data to map the residual elastic strain at the nano-scale. The diffraction pattern of each pixel was first collected and denoised. Template matching was then applied using the center spot as the mask to identify the positions of the diffraction disks.
View Article and Find Full Text PDFFuture-generation neuromorphic computing seeks to overcome the limitations of von Neumann architectures by colocating logic and memory functions, thereby emulating the function of neurons and synapses in the human brain. Despite remarkable demonstrations of high-fidelity neuronal emulation, the predictive design of neuromorphic circuits starting from knowledge of material transformations remains challenging. VO is an attractive candidate since it manifests a near-room-temperature, discontinuous, and hysteretic metal-insulator transition.
View Article and Find Full Text PDFJ Colloid Interface Sci
December 2022
Hypothesis: Encapsulation of ionic liquids (ILs) and phase change materials (PCMs) can overcome limitations associated with bulk materials, e.g., slow mass transfer rates, high viscosities, or susceptibility to external environment.
View Article and Find Full Text PDFThe metal-to-insulator transition of VO underpins applications in thermochromics, neuromorphic computing, and infrared vision. Ge alloying is shown to elevate the transition temperature by promoting V-V dimerization, thereby expanding the stability of the monoclinic phase to higher temperatures. By suppressing the propensity for oxygen vacancy formation, Ge alloying renders the hysteresis of the transition exquisitely sensitive to oxygen stoichiometry.
View Article and Find Full Text PDFACS Appl Mater Interfaces
April 2021
In an effort to protect metal substrates from extreme heat, polymer-clay multilayer thin films are studied as expendable thermal barrier coatings. Nanocomposite films with a thickness ranging from 2 to 35 μm were deposited on steel plates and exposed to the flame from a butane torch. The 35 μm coating, composed of 14 deposited bilayers of tris(hydroxymethyl)aminomethane (THAM)-buffered polyethylenimine (PEI) and vermiculite clay (VMT), decreased the maximum temperature observed on the back side of a 0.
View Article and Find Full Text PDFTransformations between different atomic configurations of a material oftentimes bring about dramatic changes in functional properties as a result of the simultaneous alteration of both atomistic and electronic structure. Transformation barriers between polytypes can be tuned through compositional modification, generally in an immutable manner. Continuous, stimulus-driven modulation of phase stabilities remains a significant challenge.
View Article and Find Full Text PDFThe development of neuromorphic computing architectures based on two terminal filamentary resistance switching devices is limited in part by the high degree of variability in resistance states and switching voltages. Because of the large role filament shape plays in directing thermal and electric fields around the filament (and thus switching parameters), unambiguous knowledge of filament morphology resulting from direct characterization of filament shape is essential to solve critical ongoing challenges of device switching variability. Here, we have utilized a conductive atomic force microscopy scalpel technique to simultaneously scribe through a polycrystalline dielectric layer in formed Cu/HfO/p+Si electrochemical metallization cell devices.
View Article and Find Full Text PDFA plant-derived lignin polymer has been sought-after as a low-cost carbon fiber (CF) precursor, but the underlying mechanisms defining CF performances are still elusive. This study revealed that both the electroconductive and mechanical performances of lignin-based CF were synergistically improved by enhancing the microstructures through modifying the lignin chemistry, which paved a pathway to holistically improve the lignin CF quality.
View Article and Find Full Text PDFThe design of multifunctional alloys with multiple chemical components requires controllable synthesis approaches. Physical vapor deposition techniques, which result in thin films (<1 μm), have previously been demonstrated for micromechanical devices and metallic combinatorial libraries. However, this approach deviates from bulk-like properties due to the residual stress derived in thin films and is limited by total film thickness.
View Article and Find Full Text PDFVariability remains the principal concern for commercialization of HfO2 based resistance switching devices. Here, we investigate the role of thermal processing conditions on internal structure of atomic layer deposited HfO2 thin films, and the impact of that structure on filament forming kinetics of p+ Si/HfO2/Cu and TiN/HfO2/Cu devices. Regardless of bias polarity or electrode metal, filament formation times are at least one order of magnitude shorter in polycrystalline than in amorphous films, which we attribute to the presence of fast ion migration along grain boundaries.
View Article and Find Full Text PDFIn this paper, we report on n-alkyl phosphonic acid (PA) self-assembled monolayer (SAM)/hafnium oxide (HfO(2)) hybrid dielectrics utilizing the advantages of SAMs for control over the dielectric/semiconductor interface with those of high-k metal oxides for low-voltage organic thin film transistors (OTFTs). By systematically varying the number of carbon atoms of the n-alkyl PA SAM from six to eighteen on HfO(2) with stable and low leakage current density, we observe how the structural nature of the SAM affects the thin-film crystal structure and morphology, and subsequent device performance of low-voltage pentacene based OTFTs. We find that two primary structural factors of the SAM play a critical role in optimizing the device electrical characteristics, namely, the order/disorder of the SAM and its physical thickness.
View Article and Find Full Text PDFCoherent carbon cryogel-ammonia borane (C-AB) nanocomposites were synthesized, and improved H2 storage properties are reported. Porous carbon cryogels were impregnated with AB in tetrahydrofuran solution at 25 degrees C under argon; 30% of the carbon cryogel pore volume was filled to produce a 24 wt % C-AB nanocomposite. Nitrogen sorption isotherms, X-ray diffraction, differential scanning calorimetry, differential thermal/thermal gravimetric analyses, mass spectrometry, and 11B NMR were used to characterize the coherent C-AB nanocomposites.
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