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1.
Nano Lett ; 24(17): 5110-5116, 2024 May 01.
Artículo en Inglés | MEDLINE | ID: mdl-38624179

RESUMEN

The remarkable development of colloidal nanocrystals with controlled dimensions and surface chemistry has resulted in vast optoelectronic applications. But can they also form a platform for quantum materials, in which electronic coherence is key? Here, we use colloidal, two-dimensional Bi2Se3 crystals, with precise and uniform thickness and finite lateral dimensions in the 100 nm range, to study the evolution of a topological insulator from three to two dimensions. For a thickness of 4-6 quintuple layers, scanning tunneling spectroscopy shows an 8 nm wide, nonscattering state encircling the platelet. We discuss the nature of this edge state with a low-energy continuum model and ab initio GW-Tight Binding theory. Our results also provide an indication of the maximum density of such states on a device.

2.
Chem Mater ; 35(19): 8301-8308, 2023 Oct 10.
Artículo en Inglés | MEDLINE | ID: mdl-37840776

RESUMEN

Cation exchange has become a major postsynthetic tool to obtain nanocrystals with a combination of stoichiometry, size, and shape that is challenging to achieve by direct wet-chemical synthesis. Here, we report on the transformation of highly anisotropic, ultrathin, and planar PbS nanosheets into CdS nanosheets of the same dimensions. We monitor the evolution of the Cd-for-Pb exchange by ex-situ TEM, HAADF-STEM, and EDX. We observe that in the early stages of the exchange the sheets show large in-sheet voids that repair spontaneously upon further exchange and annealing, resulting in ultrathin, planar, and crystalline CdS nanosheets. After cation exchange, the nanosheets show broad sub-band gap luminescence, as often observed in CdS nanocrystals. The photoluminescence excitation spectrum reveals the heavy- and light-hole exciton features, with very strong quantum confinement and large electron-hole Coulomb energy, typical for 2D ultrathin Cd-chalcogenide nanosheets.

3.
Chem Mater ; 33(17): 6853-6859, 2021 Sep 14.
Artículo en Inglés | MEDLINE | ID: mdl-34552306

RESUMEN

The variation in the shape of colloidal semiconductor nanocrystals (NCs) remains intriguing. This interest goes beyond crystallography as the shape of the NC determines its energy levels and optoelectronic properties. While thermodynamic arguments point to a few or just a single shape(s), terminated by the most stable crystal facets, a remarkable variation in NC shape has been reported for many different compounds. For instance, for the well-studied case of CdSe, close-to-spherical quantum dots, rods, two-dimensional nanoplatelets, and quantum rings have been reported. Here, we report how two-dimensional CdSe nanoplatelets reshape into quantum rings. We monitor the reshaping in real time by combining atomically resolved structural characterization with optical absorption and photoluminescence spectroscopy. We observe that CdSe units leave the vertical sides of the edges and recrystallize on the top and bottom edges of the nanoplatelets, resulting in a thickening of the rims. The formation of a central hole, rendering the shape into a ring, only occurs at a more elevated temperature.

4.
J Phys Chem C Nanomater Interfaces ; 123(1): 979-984, 2019 Jan 10.
Artículo en Inglés | MEDLINE | ID: mdl-30873253

RESUMEN

The unusual temperature dependence of exciton emission decay in CsPbX3 perovskite nanocrystals (NCs) attracts considerable attention. Upon cooling, extremely short (sub-ns) lifetimes were observed and were explained by an inverted bright-dark state splitting. Here, we report temperature-dependent exciton lifetimes for CsPbCl3 NCs doped with 0-41% Mn2+. The exciton emission lifetime increases upon cooling from 300 to 75 K. Upon further cooling, a strong and fast sub-ns decay component develops. However, the decay is strongly biexponential and also a weak, slow decay component is observed with a ∼40-50 ns lifetime below 20 K. The slow component has a ∼5-10 times stronger relative intensity in Mn-doped NCs compared to that in undoped CsPbCl3 NCs. The temperature dependence of the slow component resembles that of CdSe and PbSe quantum dots with an activation energy of ∼19 meV for the dark-bright state splitting. Based on our observations, we propose an alternative explanation for the short, sub-ns exciton decay time in CsPbX3 NCs. Slow bright-dark state relaxation at cryogenic temperatures gives rise to almost exclusively bright state emission. Incorporation of Mn2+ or high magnetic fields enhances the bright-dark state relaxation and allows for the observation of the long-lived dark state emission at cryogenic temperatures.

5.
Acta Crystallogr C Struct Chem ; 74(Pt 1): 1-6, 2018 Jan 01.
Artículo en Inglés | MEDLINE | ID: mdl-29303490

RESUMEN

The crystal structure of 5-fluorosalicylic acid is known from the literature [Choudhury & Guru Row (2004). Acta Cryst. E60, o1595-o1597] as crystallizing in the monoclinic crystal system with space-group setting P21/n and with one molecule in the asymmetric unit (polymorph I). We describe here a new polymorph which is again monoclinic but with different unit-cell parameters (polymorph II). Polymorph II has two molecules in the asymmetric unit. Its structure was modelled as a twin, with a pseudo-orthorhombic C-centred twin cell.

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