High entropy oxides are a class of materials distinguished by the use of configurational entropy to drive material synthesis. These materials are being examined for their exciting physiochemical properties and hold promise in numerous fields, such as chemical sensing, electronics, and catalysis. Patterning and integration of high entropy materials into devices and platforms can be difficult due to their thermal sensitivity and incompatibility with many conventional thermally-based processing techniques. In this work, we present a laser-based technique, laser-induced thermal voxels, that combines the synthesis and patterning of high entropy oxides into a single process step, thereby allowing patterning of high entropy materials directly onto substrates. As a proof-of-concept, we target the synthesis and patterning of a well-characterized rock salt-phase high entropy oxide, (Mg0.2Co0.2Ni0.2Cu0.2Zn0.2)O, as well as a spinel-phase high entropy oxide, (Mg0.2Ni0.2Co0.2Cu0.2Zn0.2)Cr2O4. We show through electron microscopy and x-ray analysis that the materials created are atomically homogenous and are primarily of the rock salt or spinel phase. These findings show the efficacy of laser induced thermal voxel processing for the synthesis and patterning of high entropy materials and enable new routes for integration of high entropy materials within microscale platform and devices.
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Abstract Hydrophobic hydration, whereby water spontaneously structures around hydrophobic and amphiphilic molecules, plays a key role in the process of surfactant micelle formation and micellar oil solubilization. Using vibrational Raman multivariate curve resolution spectroscopy, we characterized changes in the hydrophobic hydration occurring within nonionic alkylphenol ethoxylate surfactant Tergitol NP‐12 micelles as a function of oil solubilization. We report trends in the changes of hydrophobic hydration depending on the chain length of the oil as well as the presence of a halogen atom in the oil chemical structure. Changes in hydrophobic hydration directly correlate to changes in the physical properties of the micellar solution, including cloud point and micelle hydrodynamic diameter. We compare hydrophobic hydration of Tergitol NP‐12 to nonionic linear alkyl ethoxylate surfactant Makon TD‐12 and ionic sodium dodecyl sulfate and observe similar trends; the molecular structure of the oil has the largest impact on the hydrophobic hydration. We believe these studies contribute to a fundamental understanding of the importance of hydrophobic hydration in surfactant and oil aggregates, especially as it relates to micellar oil solubilization, and provide insight into how the molecular solubilizate can impact micellar structure, size, and stability.
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Abstract An experimental investigation and the optical modeling of the structural coloration produced from total internal reflection interference within 3D microstructures are described. Ray‐tracing simulations coupled with color visualization and spectral analysis techniques are used to model, examine, and rationalize the iridescence generated for a range of microgeometries, including hemicylinders and truncated hemispheres, under varying illumination conditions. An approach to deconstruct the observed iridescence and complex far‐field spectral features into its elementary components and systematically link them to ray trajectories that emanate from the illuminated microstructures is demonstrated. The results are compared with experiments, wherein microstructures are fabricated with methods such as chemical etching, multiphoton lithography, and grayscale lithography. Microstructure arrays patterned on surfaces with varying orientation and size lead to unique color‐traveling optical effects and highlight opportunities for how total internal reflection interference can be used to create customizable reflective iridescence. The findings herein provide a robust conceptual framework for rationalizing this multibounce interference mechanism and establish approaches for characterizing and tailoring the optical and iridescent properties of microstructured surfaces.