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1.
J Phys Chem Lett ; 13(39): 9221-9231, 2022 Oct 06.
Artigo em Inglês | MEDLINE | ID: mdl-36170663

RESUMO

Structural and electronic properties of ultrathin nanocrystals of chalcogenide Bi2(Tex Se1-x)3 were studied. The nanocrystals were formed from the parent compound Bi2Te2Se on as-grown and thermally oxidized Si(100) substrates using Ar-assisted physical vapor deposition, resulting in well-faceted single crystals several quintuple layers thick and a few hundreds nanometers large. The chemical composition and structure of the nanocrystals were analyzed by energy-dispersive X-ray spectroscopy, X-ray photoelectron spectroscopy, electron backscattering, and X-ray diffraction. The electron transport through nanocrystals connected to superconducting Nb electrodes demonstrated Josephson behavior, with the predominance of the topological channels [Stolyarov et al. Commun. Mater., 2020, 1, 38]. The present paper focuses on the effect of the growth conditions on the morphology, structural, and electronic properties of nanocrystals.

2.
Nat Mater ; 21(10): 1165-1174, 2022 10.
Artigo em Inglês | MEDLINE | ID: mdl-35725928

RESUMO

Reversible anionic redox reactions represent a transformational change for creating advanced high-energy-density positive-electrode materials for lithium-ion batteries. The activation mechanism of these reactions is frequently linked to ligand-to-metal charge transfer (LMCT) processes, which have not been fully validated experimentally due to the lack of suitable model materials. Here we show that the activation of anionic redox in cation-disordered rock-salt Li1.17Ti0.58Ni0.25O2 involves a long-lived intermediate Ni3+/4+ species, which can fully evolve to Ni2+ during relaxation. Combining electrochemical analysis and spectroscopic techniques, we quantitatively identified that the reduction of this Ni3+/4+ species goes through a dynamic LMCT process (Ni3+/4+-O2- → Ni2+-On-). Our findings provide experimental validation of previous theoretical hypotheses and help to rationalize several peculiarities associated with anionic redox, such as cationic-anionic redox inversion and voltage hysteresis. This work also provides additional guidance for designing high-capacity electrodes by screening appropriate cationic species for mediating LMCT.


Assuntos
Lítio , Cátions , Eletrodos , Ligantes , Lítio/química , Oxirredução
3.
Adv Sci (Weinh) ; 6(16): 1900435, 2019 Aug 21.
Artigo em Inglês | MEDLINE | ID: mdl-31453063

RESUMO

In this work, a class of metamaterials is proposed on the basis of ferromagnet/superconductor hybridization for applications in magnonics. These metamaterials comprise of a ferromagnetic magnon medium that is coupled inductively to a superconducting periodic microstructure. Spectroscopy of magnetization dynamics in such hybrid evidences formation of areas in the medium with alternating dispersions for spin wave propagation, which is the basic requirement for the development of metamaterials known as magnonic crystals. The spectrum allows for derivation of the impact of the superconducting structure on the dispersion: it takes place due to a diamagnetic response of superconductors on the external and stray magnetic fields. In addition, the spectrum displays a dependence on the superconducting critical state of the structure: the Meissner and the mixed states of a type II superconductor are distinguished. This dependence hints toward nonlinear response of hybrid metamaterials on the magnetic field. Investigation of the spin wave dispersion in hybrid metamaterials shows formation of allowed and forbidden bands for spin wave propagation. The band structures are governed by the geometry of spin wave propagation: in the backward volume geometry the band structure is conventional, while in the surface geometry the band structure is nonreciprocal and is formed by indirect band gaps.

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