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  1. Abstract

    Tuning the properties of a pair of entangled electron and hole in a light-induced exciton is a fundamentally intriguing inquiry for quantum science. Here, using semiconducting hybrid perovskite as an exploratory platform, we discover that Nd2+-doped CH3NH3PbI3(MAPbI3) perovskite exhibits a Kondo-like exciton-spin interaction under cryogenic and photoexcitation conditions. The feedback to such interaction between excitons in perovskite and the localized spins in Nd2+is observed as notably prolonged carrier lifetimes measured by time-resolved photoluminescence, ~10 times to that of pristine MAPbI3without Nd2+dopant. From a mechanistic standpoint, such extended charge separation states are the consequence of the trap state enabled by the antiferromagnetic exchange interaction between the light-induced exciton and the localized 4 fspins of the Nd2+in the proximity. Importantly, this Kondo-like exciton-spin interaction can be modulated by either increasing Nd2+doping concentration that enhances the coupling between the exciton and Nd2+4 fspins as evidenced by elongated carrier lifetime, or by using an external magnetic field that can nullify the spin-dependent exchange interaction therein due to the unified orientations of Nd2+spin angular momentum, thereby leading to exciton recombination at the dynamics comparable to pristine MAPbI3.

     
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  2. Free, publicly-accessible full text available November 22, 2024
  3. FeCrAl alloys are promising candidates to replace Zr alloys as fuel cladding materials in nuclear light-water reactors. Grain refinement has been indicated to improve irradiation resistance. To enhance corrosion resistance as well, the effects of grain refinement on steam corrosion behavior were investigated in this work. Samples of Kanthal D alloy (Fe-21Cr-5Al) with two different grain sizes (coarse-grained and ultrafine-grained) were exposed to steam at 1200 °C for 2 hrs. Results indicate improved steam corrosion resistance in ultrafine-grained Kanthal D with formation of a thinner protective Al oxide layer and the presence of a thin underlying Cr oxide layer. 
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    Free, publicly-accessible full text available January 1, 2025
  4. Free, publicly-accessible full text available October 11, 2024
  5. Abstract Image Advances in the synthesis and self-assembly of nanocrystals have enabled researchers to create a plethora of different nanoparticle superlattices. But while many superlattices with complex types of translational order have been realized, rotational order of nanoparticle building blocks within the lattice is more difficult to achieve. Self-assembled superstructures with atomically coherent nanocrystal lattices, which are desirable due to their exceptional electronic and optical properties, have been fabricated only for a few selected systems. Here, we combine experiments with molecular dynamics (MD) simulations to study the self-assembly of heterostructural nanocrystals (HNCs), consisting of a near-spherical quantum dot (QD) host decorated with a small number of epitaxially grown gold nanocrystal (Au NC) “patches”. Self-assembly of these HNCs results in face-centered-cubic (fcc) superlattices with well-defined orientational relationships between the atomic lattices of both QD hosts and Au patches. MD simulations indicate that the observed dual atomic coherence is linked to the number, size, and relative positions of gold patches. This study provides a strategy for the design and fabrication of NC superlattices with large structural complexity and delicate orientational order. 
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  6. Abstract

    Using microwave irradiation, PtCo alloy nanoparticles were deposited within a few minutes on COOH‐functionalized MWCNT supports. The obtained catalysts were used for selective hydrogenation of cinnamaldehyde, a reaction whose products are widely used in various fields. In the selective cinnamaldehyde hydrogenation to cinnamyl alcohol, microwave‐prepared catalysts (generically, PtxCoy‐MW) outperformed a catalyst prepared by the conventional method (Pt1Co2‐con). The highest selective hydrogenation to cinnamyl alcohol, 89%, was obtained using Pt1Co2‐MW, while Pt1Co2‐con showed a selectivity of 76%. Characterization results confirmed that the microwave prepared samples had a stronger interaction between Pt and Co than that in the Pt1Co2‐con sample. The alloyed Co altered the electronic structure of Pt, leading to favorable adsorption of the C=O bond by the lone‐pair electrons of its oxygen atom. Moreover, the Pt1Co2‐MW sample showed neglectable change in catalytic performance (e. g., cinnamaldehyde conversion and selective hydrogenation to cinnamyl alcohol) during recycling experiments.

     
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  7. Metal nanoparticles of multi-principal element alloys (MPEA) with a single crystalline phase have been synthesized by flash heating/cooling of nanosized metals encapsulated in micelle vesicles dispersed in an oil phase (e.g., cyclohexane). Flash heating is realized by selective absorption of a microwave pulse in metals to rapidly heat metals into uniform melts. The oil phase barely absorbs microwave and maintains the low temperature, which can rapidly quench the high-temperature metal melts to enable the flash cooling process. The precursor ions of four metals, including Au, Pt, Pd, and Cu, can be simultaneously reduced by hydrazine in the aqueous solution encapsulated in the micelle vesicles. The resulting metals efficiently absorb microwave energy to locally reach a temperature high enough to melt themselves into a uniform mixture. The duration of microwave pulse is crucial to ensure the reduced metals mix uniformly, while the temperature of oil phase is still low to rapidly quench the metals and freeze the single-phase crystalline lattices in alloy nanoparticles. The microwave-enabled flash heating/cooling provides a new method to synthesize single-phase MPEA nanoparticles of many metal combinations when the appropriate water-in-oil micelle systems and the appropriate reduction reactions of metal precursors are available. 
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