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1.
J Am Chem Soc ; 145(50): 27273-27281, 2023 Dec 20.
Artigo em Inglês | MEDLINE | ID: mdl-38065568

RESUMO

Atomically precise Au25 nanoclusters have garnered significant interest in the field of heterogeneous catalysis due to their remarkable activity and selectivity. However, for the extensively studied reaction of low-temperature CO oxidation, their performance has not been competitive compared to other known gold nanocatalysts. To address this, we deposited Au25(SR)18 (R = CH2CH2Ph) nanoclusters onto a manganese oxide support (Au25/MnO2), resulting in a very stable and highly active catalyst. By optimizing the pretreatment temperature, we were able to significantly enhance the performance of the Au25/MnO2 catalyst, which outperformed most other gold catalysts. Impressively, 100% conversion of CO was achieved at temperatures as low as -50 °C, with 50% conversion being reached below -70 °C. Furthermore, the existence of ligands could also influence the negative apparent activation energy observed at intermediate temperatures. Analysis using X-ray photoelectron spectroscopy (XPS), scanning transmission electron microscopy (STEM), and X-ray diffraction (XRD) techniques indicated that the Au25 nanoclusters remained stable on the catalyst surface even after pretreatment at high temperatures. In-situ modulation excitation spectroscopy (MES) spectra also confirmed that the Au cluster was the active site for CO oxidation, highlighting the potential of atomically precise Au25 nanoclusters as primary active sites at very low temperatures.

2.
Nat Mater ; 18(11): 1187-1193, 2019 11.
Artigo em Inglês | MEDLINE | ID: mdl-31501554

RESUMO

While spintronics has traditionally relied on ferromagnetic metals as spin generators and detectors, spin-orbitronics exploits the efficient spin-charge interconversion enabled by spin-orbit coupling in non-magnetic systems. Although the Rashba picture of split parabolic bands is often used to interpret such experiments, it fails to explain the largest conversion effects and their relationship with the electronic structure. Here, we demonstrate a very large spin-to-charge conversion effect in an interface-engineered, high-carrier-density SrTiO3 two-dimensional electron gas and map its gate dependence on the band structure. We show that the conversion process is amplified by enhanced Rashba-like splitting due to orbital mixing and in the vicinity of avoided band crossings with topologically non-trivial order. Our results indicate that oxide two-dimensional electron gases are strong candidates for spin-based information readout in new memory and transistor designs. Our results also emphasize the promise of topology as a new ingredient to expand the scope of complex oxides for spintronics.

3.
Nano Lett ; 19(1): 554-560, 2019 01 09.
Artigo em Inglês | MEDLINE | ID: mdl-30570259

RESUMO

Two-dimensional crystals of semi-metallic van der Waals materials hold much potential for the realization of novel phases, as exemplified by the recent discoveries of a polar metal in few-layer 1T'-WTe2 and of a quantum spin Hall state in monolayers of the same material. Understanding these phases is particularly challenging because little is known from experiments about the momentum space electronic structure of ultrathin crystals. Here, we report direct electronic structure measurements of exfoliated mono-, bi-, and few-layer 1T'-WTe2 by laser-based microfocus angle-resolved photoemission. This is achieved by encapsulating with monolayer graphene a flake of WTe2 comprising regions of different thickness. Our data support the recent identification of a quantum spin Hall state in monolayer 1T'-WTe2 and reveal strong signatures of the broken inversion symmetry in the bilayer. We finally discuss the sensitivity of encapsulated samples to contaminants following exposure to ambient atmosphere.

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