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1.
J Chem Phys ; 151(8): 084701, 2019 Aug 28.
Artigo em Inglês | MEDLINE | ID: mdl-31470698

RESUMO

Photo-luminescence (P-L) intermittency (or blinking) in semiconductor nanocrystals (NCs), a phenomenon ubiquitous to single-emitters, is generally considered to be temporally random intensity fluctuations between "bright" ("On") and "dark" ("Off") states. However, individual quantum-dots (QDs) rarely exhibit such telegraphic signals, and yet, a vast majority of single-NC blinking data are analyzed using a single fixed threshold which generates binary trajectories. Furthermore, while blinking dynamics can vary dramatically over NCs in the ensemble, the extent of diversity in the exponents (mOn/Off) of single-particle On-/Off-time distributions (P(tOn/Off)), often used to validate mechanistic models of blinking, remains unclear due to a lack of statistically relevant data sets. Here, we subclassify an ensemble of QDs based on the emissivity of each emitter and subsequently compare the (sub)ensembles' behaviors. To achieve this, we analyzed a large number (>1000) of blinking trajectories for a model system, Mn+2 doped ZnCdS QDs, which exhibits diverse blinking dynamics. An intensity histogram dependent thresholding method allowed us to construct distributions of relevant blinking parameters (such as mOn/Off). Interestingly, we find that single QD P(tOn/Off)s follow either truncated power law or power law, and their relative proportion varies over subpopulations. Our results reveal a remarkable variation in mOn/Off amongst as well as within subensembles, which implies multiple blinking mechanisms being operational amongst various QDs. We further show that the mOn/Off obtained via cumulative single-particle P(tOn/Off) is distinct from the weighted mean value of all single-particle mOn/Off, evidence for the lack of ergodicity. Thus, investigation and analyses of a large number of QDs, albeit for a limited time span of a few decades, are crucial to characterize the spatial heterogeneity in possible blinking mechanisms.

2.
ACS Catal ; 7(7): 4248-4252, 2017 Jul 07.
Artigo em Inglês | MEDLINE | ID: mdl-28713643

RESUMO

Molecular-sized micropores of ZSM-5 zeolite catalysts provide spatial restrictions around catalytic sites that allow for shape-selective catalysis. However, the fact that ZSM-5 has two main pore systems with different geometries is relatively unexploited as a potential source of additional shape selectivity. Here, we use confocal laser-scanning microscopy to show that by changing the polarity of the solvent, the acid-catalyzed furfuryl alcohol oligomerization can be directed to selectively occur within either of two locations in the microporous network. This finding is confirmed for H-ZSM-5 particles with different Si/Al ratios and indicates a general trend for shape-selective catalytic reactions.

3.
Chem Commun (Camb) ; 52(23): 4353-6, 2016 Mar 21.
Artigo em Inglês | MEDLINE | ID: mdl-26924607

RESUMO

We demonstrate the coexistence of Eu(2+) and Eu(3+) in corundum and bixbyite-type colloidal In2O3 nanocrystals. The emission properties of dopants in both oxidation states are determined by their interaction with native defects, and are dramatically different in the two nanocrystal phases. This difference arises from the smaller nanocrystal size and higher defect density in metastable corundum-type nanocrystals.


Assuntos
Európio/química , Índio/química , Nanopartículas , Luminescência , Microscopia Eletrônica de Transmissão
4.
Phys Rev Lett ; 110(26): 267401, 2013 Jun 28.
Artigo em Inglês | MEDLINE | ID: mdl-23848921

RESUMO

Extensively studied Mn-doped semiconductor nanocrystals have invariably exhibited photoluminescence over a narrow energy window of width ≤150 meV in the orange-red region and a surprisingly large spectral width (≥180 meV), contrary to its presumed atomic-like origin. Carrying out emission measurements on individual single nanocrystals and supported by ab initio calculations, we show that Mn PL emission, in fact, can (i) vary over a much wider range (∼370 meV) covering the deep green--deep red region and (ii) exhibit widths substantially lower (∼60-75 meV) than reported so far, opening newer application possibilities and requiring a fundamental shift in our perception of the emission from Mn-doped semiconductor nanocrystals.

5.
J Phys Chem Lett ; 2(11): 1241-7, 2011 Jun 02.
Artigo em Inglês | MEDLINE | ID: mdl-26295417

RESUMO

The intrinsic spectral line widths of defect-related transitions in quantum-confined semiconductor nanocrystals are often difficult to estimate using ensemble measurements because the extent of inhomogeneous broadening due to particle size distributions is not known precisely. To address this problem, we performed spectrally resolved photoluminescence (PL) microscopy of individual ZnO NC by directly populating the defects states using low-energy laser excitation. The temporal evolution of PL intensities shows discrete blinking behaviors, suggesting that the NCs are detected near single-particle levels. The transition energies of individual NCs are found to fluctuate around their mean position (2.25 eV) by ∼0.130 eV, which is attributed to particle size distribution and defects densities associated with each NC. The spectral line width associated with defect emission envelope of ZnO NCs is found to be inherently broad (200-400 meV), which further establishes the presence of multiple closely spaced defect energy levels within every ZnO NC.

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