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Abstract Determining suitable dopants with optimized doping concentration is critical to design efficient water splitting photocatalysts. However, there is currently a lack of fundamental knowledge to guide this process. Herein, we examine the impact of Al3+, Mg2+, and Ga3+on the photocatalytic performance of SrTiO3and propose a defect compensation model to understand the doping effect. Doped SrTiO3crystals were grown hydrothermally and treated in molten SrCl2. The hydrogen production rates from 50 catalysts produced in this way were measured with a high‐throughput parallelized and automated photochemical reactor (PAPCR). The investigation revealed that all three dopants significantly enhance the photocatalytic reactivity. According to Brouwer diagrams computed using available reaction constants, the optimum reactivity is achieved when the concentration of acceptor dopants fully compensates the oxygen vacancy donors. The improved reactivity can be attributed to the reduction in free electron concentration, resulting in a space charge layer that is 1000 times longer. Consequently, this situation enhances the number of photogenerated charge carriers capable of being separated by the band bending and transported to the surface.more » « lessFree, publicly-accessible full text available October 9, 2026
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In modern machine learning systems, distributed algorithms are deployed across applications to ensure data privacy and optimal utilization of computational resources. This work offers a fresh perspective to model, analyze, and design distributed optimization algorithms through the lens of stochastic multi-rate feedback control. We show that a substantial class of distributed algorithms—including popular Gradient Tracking for decentralized learning, and FedPD and Scaffold for federated learning—can be modeled as a certain discrete-time stochastic feedback-control system, possibly with multiple sampling rates. This key observation allows us to develop a generic framework to analyze the convergence of the entire algorithm class. It also enables one to easily add desirable features such as differential privacy guarantees, or to deal with practical settings such as partial agent participation, communication compression, and imperfect communication in algorithm design and analysis.more » « less
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Summary Tfap2b, a pivotal transcription factor, plays critical roles within neural crest cells and their derived lineage. To unravel the intricate lineage dynamics and contribution of these Tfap2b+ cells during craniofacial development, we established aTfap2b‐CreERT2knock‐in transgenic mouse line using the CRISPR‐Cas9‐mediated homologous direct repair. By breeding with tdTomato reporter mice and initiating Cre activity through tamoxifen induction at distinct developmental time points, we show theTfap2blineage within the key neural crest‐derived domains, such as the facial mesenchyme, midbrain, cerebellum, spinal cord, and limbs. Notably, the migratory neurons stemming from the dorsal root ganglia are visible subsequent to Cre activity initiated at E8.5. Intriguingly, Tfap2b+ cells, serving as the progenitors for limb development, show activity predominantly commencing at E10.5. Across the mouse craniofacial landscape, Tfap2b exhibits a widespread presence throughout the facial organs. Here we validate its role as a marker of progenitors in tooth development and have confirmed that this process initiates from E12.5. Our study not only validates theTfap2b‐CreERT2transgenic line, but also provides a powerful tool for lineage tracing and genetic targeting ofTfap2b‐expressing cells and their progenitor in a temporally and spatially regulated manner during the intricate process of development and organogenesis.more » « less
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Abstract BaTiO3heated in an excess of SrCl2at 1150 °C converts to SrTiO3through an ion exchange reaction. The SrTiO3synthesized by ion exchange produces hydrogen from pH 7 water at a rate more than twice that of conventional SrTiO3treated identically. The apparent quantum yield for hydrogen production in pure water of the ion exchanged SrTiO3is 11.4% under 380 nm illumination. The catalyst resulting from ion‐exchange differs from conventional SrTiO3by having ≈2% residual Ba, inhomogeneous Cl‐doping at a concentration less than 1%, Kirkendall voids in the centers of particles that result from the unequal rates of Sr and Ba diffusion together with the transport of Ti and O, and nanoscale regions near the surface that have lattice spacings consistent with the Sr‐excess phase Sr2TiO4. The increased photochemical efficiency of this nonequilibrium structure is most likely related to the Sr‐excess, which is known to compensate donor defects that can act as charge traps and recombination centers.more » « less
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