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1.
Adv Sci (Weinh) ; 10(29): e2303028, 2023 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-37607120

RESUMO

Ferroelectrics, due to their polar nature and reversible switching, can be used to dynamically control surface chemistry for catalysis, chemical switching, and other applications such as water splitting. However, this is a complex phenomenon where ferroelectric domain orientation and switching are intimately linked to surface charges. In this work, the temperature-induced domain behavior of ferroelectric-ferroelastic domains in free-standing BaTiO3 films under different gas environments, including vacuum and oxygen-rich, is studied by in situ scanning transmission electron microscopy (STEM). An automated pathway to statistically disentangle and detect domain structure transformations using deep autoencoders, providing a pathway towards real-time analysis is also established. These results show a clear difference in the temperature at which phase transition occurs and the domain behavior between various environments, with a peculiar domain reconfiguration at low temperatures, from a-c to a-a at ≈60 °C. The vacuum environment exhibits a rich domain structure, while under the oxidizing environment, the domain structure is largely suppressed. The direct visualization provided by in situ gas and heating STEM allows to investigate the influence of external variables such as gas, pressure, and temperature, on oxide surfaces in a dynamic manner, providing invaluable insights into the intricate surface-screening mechanisms in ferroelectrics.

2.
J Mater Sci ; 57(34): 16383-16396, 2022.
Artigo em Inglês | MEDLINE | ID: mdl-36101839

RESUMO

In this work, we report an extensive investigation via transmission electron microscopy (TEM) techniques of InGaAs/GaAs pyramidal quantum dots (PQDs), a unique site-controlled family of quantum emitters that have proven to be excellent sources of single and entangled photons. The most striking features of this system, originating from their peculiar fabrication process, include their inherently 3-dimensional nature and their interconnection to a series of nanostructures that are formed alongside them, such as quantum wells and quantum wires. We present structural and chemical data from cross-sectional and plan view samples of both single and stacked PQDs structures. Our findings identify (i) the shape of the dot, being hexagonal and not triangular as previously assumed, (ii) the chemical distribution at the facets and QD area, displaying clear Indium diffusion, and (iii) a near absence of Aluminium (from the AlAs marker) at the bottom of the growth profile. Our results shed light on previously unreported structural and chemical features of PQDs, which is of extreme relevance for further development of this family of quantum emitters. Supplementary Information: The online version contains supplementary material available at 10.1007/s10853-022-07654-2.

3.
JACS Au ; 2(1): 178-187, 2022 Jan 24.
Artigo em Inglês | MEDLINE | ID: mdl-35098234

RESUMO

Spiky/hollow metal nanoparticles have applications across a broad range of fields. However, the current bottom-up methods for producing spiky/hollow metal nanoparticles rely heavily on the use of strongly adsorbing surfactant molecules, which is undesirable because these passivate the product particles' surfaces. Here we report a high-yield surfactant-free synthesis of spiky hollow Au-Ag nanostars (SHAANs). Each SHAAN is composed of >50 spikes attached to a hollow ca. 150 nm diameter cubic core, which makes SHAANs highly plasmonically and catalytically active. Moreover, the surfaces of SHAANs are chemically exposed, which gives them significantly enhanced functionality compared with their surfactant-capped counterparts, as demonstrated in surface-enhanced Raman spectroscopy (SERS) and catalysis. The chemical accessibility of the pristine SHAANs also allows the use of hydroxyethyl cellulose as a weakly bound stabilizing agent. This produces colloidal SHAANs that remain stable for >1 month while retaining the functionalities of the pristine particles and allows even single-particle SERS to be realized.

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