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  1. Abstract

    Designing highly active and robust catalysts for the oxygen evolution reaction is key to improving the overall efficiency of the water splitting reaction. It has been previously demonstrated that evaporation induced self‐assembly (EISA) can be used to synthesize highly porous and high surface area cerate‐based fluorite nanocatalysts, and that substitution of Ce with 50% rare earth (RE) cations significantly improves electrocatalyst activity. Herein, the defect structure of the best performing nanocatalyst in the series are further explored, Nd2Ce2O7, with a combination of neutron diffraction and neutron pair distribution function analysis. It is found that Nd3 +cation substitution for Ce in the CeO2fluorite lattice introduces higher levels of oxygen Frenkel defects and induces a partially reduced RE1.5Ce1.5O5 +xphase with oxygen vacancy ordering. Significantly, it is demonstrated that the concentration of oxygen Frenkel defects and improved electrocatalytic activity can be further enhanced by increasing the compositional complexity (number of RE cations involved) in the substitution. The resulting novel compositionally‐complex fluorite– (La0.2Pr0.2Nd0.2Tb0.2Dy0.2)2Ce2O7is shown to display a low OER overpotential of 210 mV at a current density of 10 mAcm−2in 1M KOH, and excellent cycling stability. It is suggested that increasing the compositional complexity of fluorite nanocatalysts expands the ability to tailor catalyst design.

     
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    Free, publicly-accessible full text available March 14, 2025
  2. Free, publicly-accessible full text available October 6, 2024
  3. Free, publicly-accessible full text available July 1, 2024
  4. Abstract

    At elevated temperatures SnSe is reported to undergo a structural transition from the low symmetry orthorhombic GeS-type to a higher symmetry orthorhombic TlI-type. Although increasing symmetry should likewise increase lattice thermal conductivity, many experiments on single crystals and polycrystalline materials indicate that this is not the case. Here we present temperature dependent analysis of time-of-flight (TOF) neutron total scattering data in combination with theoretical modeling to probe the local to long-range evolution of the structure. We report that while SnSe is well characterized on average within the high symmetry space group above the transition, over length scales of a few unit cells SnSe remains better characterized in the low symmetry GeS-type space group. Our finding from robust modeling provides further insight into the curious case of a dynamic order-disorder phase transition in SnSe, a model consistent with the soft-phonon picture of the high thermoelectric power above the phase transition.

     
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  5. Polar nanoregions (PNRs) are believed to play a decisive role in the local and macroscopic polarization in relaxor ferroelectrics. The limited microscopic understanding of the structure and dynamics of PNRs hampers the rational design of new lead-free materials. Here, the local structure of A-site disordered Bi 0.5 K 0.5 TiO 3 (BKT) is investigated using synchrotron x-ray and neutron pair distribution function (PDF) analysis and density functional theory (DFT) optimized special quasirandom structures (SQSs). DFT-relaxed SQS with a 4 × 4 × 4 supercell size can reproduce the experimental PDFs of disordered BKT, as well as the partial PDFs and total polarization, with comparable results to those reported from a combined analysis of x-ray and neutron PDF data with large-box reverse Monte Carlo methods. We find that small Bi 3+ -rich polar clusters are likely to be the microscopic origin of relaxor behavior in disordered BKT, and that the existence of large polar nanoregions (PNRs) is not necessary to explain the relaxor properties. Our results also highlight the great potential of the SQS approach to gain a nanoscale-to-microscopic understanding of other relaxor solid solutions. 
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  6. Training deep learning (DL) models in the cloud has become a norm. With the emergence of serverless computing and its benefits of true pay-as-you-go pricing and scalability, systems researchers have recently started to provide support for serverless-based training. However, the ability to train DL models on serverless platforms is hindered by the resource limitations of today's serverless infrastructure and DL models' explosive requirement for memory and bandwidth. This paper describes FuncPipe, a novel pipelined training framework specifically designed for serverless platforms that enable fast and low-cost training of DL models. FuncPipe is designed with the key insight that model partitioning can be leveraged to bridge both memory and bandwidth gaps between the capacity of serverless functions and the requirement of DL training. Conceptually simple, we have to answer several design questions, including how to partition the model, configure each serverless function, and exploit each function's uplink/downlink bandwidth. In particular, we tailor a micro-batch scheduling policy for the serverless environment, which serves as the basis for the subsequent optimization. Our Mixed-Integer Quadratic Programming formulation automatically and simultaneously configures serverless resources and partitions models to fit within the resource constraints. Lastly, we improve the bandwidth efficiency of storage-based synchronization with a novel pipelined scatter-reduce algorithm. We implement FuncPipe on two popular cloud serverless platforms and show that it achieves 7%-77% cost savings and 1.3X-2.2X speedup compared to state-of-the-art serverless-based frameworks. 
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  7. Abstract

    We performed a rigorous reverberation-mapping analysis of the broad-line region (BLR) in a highly accreting (L/LEdd= 0.74–3.4) active galactic nucleus, Markarian 142 (Mrk 142), for the first time using concurrent observations of the inner accretion disk and the BLR to determine a time lag for the Hβλ4861 emission relative to the ultraviolet (UV) continuum variations. We used continuum data taken with the Niel Gehrels Swift Observatory in theUVW2 band, and the Las Cumbres Observatory, Dan Zowada Memorial Observatory, and Liverpool Telescope in thegband, as part of the broader Mrk 142 multiwavelength monitoring campaign in 2019. We obtained new spectroscopic observations covering the Hβbroad emission line in the optical from the Gemini North Telescope and the Lijiang 2.4 m Telescope for a total of 102 epochs (over a period of 8 months) contemporaneous to the continuum data. Our primary result states a UV-to-Hβtime lag of8.680.72+0.75days in Mrk 142 obtained from light-curve analysis with a Python-based running optimal average algorithm. We placed our new measurements for Mrk 142 on the optical and UV radius–luminosity relations for NGC 5548 to understand the nature of the continuum driver. The positions of Mrk 142 on the scaling relations suggest that UV is closer to the “true” driving continuum than the optical. Furthermore, we obtainlog(M/M)= 6.32 ± 0.29 assuming UV as the primary driving continuum.

     
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  8. Steady-state fluorescence spectroscopy has a central role not only for sensing applications, but also in biophysics and imaging. Light switching probes, such as ruthenium dipyridophenazine complexes, have been used to study complex systems such as DNA, RNA, and amyloid fibrils. Nonetheless, steady-state spectroscopy is limited in the kind of information it can provide. In this paper, we use time-resolved spectroscopy for studying binding interactions between amyloid-β fibrillar structures and photoluminescent ligands. Using time-resolved spectroscopy, we demonstrate that ruthenium complexes with a pyrazino phenanthroline derivative can bind to two distinct binding sites on the surface of fibrillar amyloid-β, in contrast with previous studies using steady-state photoluminescence spectroscopy, which only identified one binding site for similar compounds. The second elusive binding site is revealed when deconvoluting the signals from the time-resolved decay traces, allowing the determination of dissociation constants of 3 and 2.2 μM. Molecular dynamic simulations agree with two binding sites on the surface of amyloid-β fibrils. Time-resolved spectroscopy was also used to monitor the aggregation of amyloid-β in real-time. In addition, we show that common polypyridine complexes can bind to amyloid-β also at two different binding sites. Information on how molecules bind to amyloid proteins is important to understand their toxicity and to design potential drugs that bind and quench their deleterious effects. The additional information contained in time-resolved spectroscopy provides a powerful tool not only for studying excited state dynamics but also for sensing and revealing important information about the system including hidden binding sites. 
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  9. The Ruddlesden–Popper (RP) layered perovskite structure is of great interest due to its inherent tunability, and the emergence and growth of the compositionally complex oxide (CCO) concept endows the RP family with further possibilities. Here, a comprehensive assessment of thermodynamic stabilization, local order/disorder, and lattice distortion was performed in the first two reported examples of lanthanum-deficient Lan+1BnO3n+1 (n = 1, B = Mg, Co, Ni, Cu, Zn) obtained via various processing conditions. Chemical short-range order (CSRO) at the B-site and the controllable excess interstitial oxygen (δ) in RP-CCOs are uncovered by neutron pair distribution function analysis. Reverse Monte Carlo analysis of the data, Metropolis Monte Carlo simulations, and extended x-ray absorption fine structure analysis implies a modest degree of magnetic element segregation on the local scale. Further, ab initio molecular dynamics simulations results obtained from special quasirandom structure disagree with experimentally observed CSRO but confirm Jahn–Teller distortion of CuO6 octahedra. These findings highlight potential opportunities to control local order/disorder and excess interstitial oxygen in layered RP-CCOs and demonstrate a high degree of freedom for tailoring application-specific properties. They also suggest a need for expansion of theoretical and data modeling approaches in order to meet the innate challenges of CCO and related high-entropy phases.

     
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