Growth of low-density vertical quantum dot molecules with control in energy emission

This article is distributed under the terms of the Creative Commons Attribution Noncommercial License.-- This article is part of the series 8th International Workshop on Epitaxial Semiconductors on Patterned Substrates and Novel Index Surfaces.

Size-filtering effects by stacking InAs/InP (001) self-assembled quantum wires into multilayers

Multilayer structure containing vertically stacked InAs/InP self-assembled quantum wires have been successfully grown by molecular-beam epitaxy. The influence of the InP spacer layer thickness on the structural and optical properties of the wire superlattice has been studied by means of transmission electron microscopy and photoluminescence. The coherent propagation of the strain field in the sample with a 5-nm-thick spacer determines by a size filtering effect a good homogeneity and uniformity of the wire stacks, and hence a good optical quality. The exciton recombination dynamics in the wire superlattice cannot be related to thermal escape of carriers out to the barriers, as occurs in sin…

Solution-Processed Ni-Based Nanocomposite Electrocatalysts: An Approach to Highly Efficient Electrochemical Water Splitting

In this study, we report an up-scalable and low-cost solution-processed method to in situ synthesize an earth-abundant non-stoichiometric NiOx-based electrocatalytic film for water oxidation. The catalytic activity was found to be inversely proportional to the baking temperature, which varied from 50 to 500 °C. We found the formation of a hybrid nanocomposite thin film of NiOx nanocrystals (<2 nm size) inside an acetate-based organic matrix at low temperatures (<200 °C). The defective and short-range structural order of the NiOx-based nanocomposite electrocatalysts, compatible with lattice stress, low electrical conductivity, and high density of catalytically active surface species, and hig…

CVD synthesis of carbon spheres using NiFe-LDHs as catalytic precursors: structural, electrochemical and magnetoresistive properties

The gram-scale synthesis of carbon spheres with a diameter of ca. 740 nm has been achieved by means of a chemical vapour deposition method using NiFe-layered double hydroxides as a solid catalytic precursor. The presence of the catalyst (FeNi3) allows controlling the final size distribution, resulting in a monodisperse sample. Their structural properties exhibited a high degree of graphitization according to their ID/IG ratio. In addition, their morphological features were unveiled by FIB-SEM and HRTEM, showing that they are formed by solid inner cores, and presenting labile chain-like structures due to accretion procedures. The solution and posterior sonication of the samples in toluene ga…

Structural and chemical characterization of CdSe-ZnS core-shell quantum dots

Abstract The structural and compositional properties of CdSe-ZnS core-shell quantum dots (QDs) with a sub-nm shell thickness are analyzed at the atomic scale using electron microscopy. QDs with both wurtzite and zinc blende crystal structures, as well as intermixing of the two structures and stacking faults, are observed. High-angle annular dark-field scanning transmission electron microscopy suggests the presence of a lower atomic number epitaxial shell of irregular thickness around a CdSe core. The presence of a shell is confirmed using energy dispersive X-ray spectroscopy. Despite the thickness irregularities, the optical properties of the particles, such as photoluminescence and quantum…

Size self-filtering effect in vertical stacks of InAs/InP self-assembled quantum wires

3 páginas, 2 figuras.-- PACS: 73.21.Hb; 78.55.Cr; 78.67.Lt.-- Proceedings of the International Conference on Superlattices, Nano-structures and Nano-devices ICSNN 2002.

Impact of Noah-LSM Parameterizations on WRF Mesoscale Simulations: Case Study of Prevailing Summer Atmospheric Conditions over a Typical Semi-Arid Region in Eastern Spain

The current study evaluates the ability of the Weather Research and Forecasting Model (WRF) to forecast surface energy fluxes over a region in Eastern Spain. Focusing on the sensitivity of the model to Land Surface Model (LSM) parameterizations, we compare the simulations provided by the original Noah LSM and the Noah LSM with multiple physics options (Noah-MP). Furthermore, we assess the WRF sensitivity to different Noah-MP physics schemes, namely the calculation of canopy stomatal resistance (OPT_CRS), the soil moisture factor for stomatal resistance (OPT_BTR), and the surface layer drag coefficient (OPT_SFC). It has been found that these physics options strongly affect the energy partiti…

Heterometallic Titanium–Organic Frameworks by Metal-Induced Dynamic Topological Transformations

Reticular chemistry has boosted the design of thousands of metal and covalent organic frameworks for unlimited chemical compositions, structures, and sizable porosities. The ability to generate porous materials at will on the basis of geometrical design concepts is responsible for the rapid growth of the field and the increasing number of applications derived. Despite their promising features, the synthesis of targeted homo- and heterometallic titanium–organic frameworks amenable to these principles is relentlessly limited by the high reactivity of this metal in solution that impedes the controlled assembly of titanium molecular clusters. We describe an unprecedented methodology for the syn…

Production of nanometer-size GaAs nanocristals by nanosecond laser ablation in liquid.

This paper reports the formation and characterization of spherical GaAs quantum dots obtained by nanosecond pulsed laser ablation in a liquid (ethanol or methanol). The produced bare GaAs nanoparticles demonstrate rather narrow size distribution which depends on the applied laser power density (from 4.25 to 13.9 J/cm 2 in our experiments) and is as low as 2.5 nm for the highest power used. The absolute value of the average diameter also decreases significantly, from 13.7 to 8.7 nm, as the laser power increases in this interval. Due to the narrow nanoparticle size dispersion achieved at the highest laser powers two absorption band edges are clearly distinguishable at about 1.72 and 3.15 eV w…

Morphological evolution of InAs/InP quantum wires through aberration-corrected scanning transmission electron microscopy

Evolution of the size, shape and composition of self-assembled InAs/InP quantum wires through the Stranski–Krastanov transition has been determined by aberration-corrected Z-contrast imaging. High resolution compositional maps of the wires in the initial, intermediate and final formation stages are presented. (001) is the main facet at their very initial stage of formation, which is gradually reduced in favour of {114} or {118}, ending with the formation of mature quantum wires with {114} facets. Significant changes in wire dimensions are measured when varying slightly the amount of InAs deposited. These results are used as input parameters to build three-dimensional models that allow calcu…

Charge transfer interactions in self-assembled single walled carbon nanotubes/Dawson–Wells polyoxometalate hybrids

We demonstrate the success in self-assembling pyrene-modified Dawson–Wells-type polyoxometalates (POMs) with single walled carbon nanotubes (SWCNTs) by means of π–π interactions. In this context, the immobilization of POMs onto SWCNTs is corroborated by aberration-corrected high-resolution electron microscopy, thermogravimetric analysis, and Raman spectroscopy. From steady-state and time-resolved photophysical techniques we derived evidence for mutual interactions between SWCNTs and POMs in the excited states. The latter are the inception to a charge transfer from the SWCNTs to the POMs. Our results corroborate the suitability of POM–SWCNTs assemblies for photoactive molecular devices.

Structural quality of CH3NH3PbI3 perovskites for photovoltaic applications analyzed by electron microscopy techniques

Au–NiOx nanocomposite for hot electron-assisted plasmonic photocatalysis

Nanocomposites of metal–oxide semiconductors containing Au nanoparticles are emerging multifunctional materials for sunlight-driven highly efficient photocatalysis. Here we report a solution-processed nanocomposite synthesis of Au–NiOx nanocomposite films by slot-die coating and plotter printing in a straightforward in situ synthesis approach. Our study demonstrated a significantly enhanced photocatalytic decomposition reaction of MO upon exposure of Au–NiOx films to a sunlight simulator. The excellent photocatalytic activity is ascribed to the generation of hot carriers after LSPR excitation in Au NPs. Suitable band alignment between the valence band of NiOx and the Fermi level of Au NPs l…

High spatial resolution mapping of individual and collective localized surface plasmon resonance modes of silver nanoparticle aggregates: correlation to optical measurements

Non-isolated nanoparticles show a plasmonic response that is governed by the localized surface plasmon resonance (LSPR) collective modes created by the nanoparticle aggregates. The individual and collective LSPR modes of silver nanoparticle aggregated by covalent binding by means of bifunctional molecular linkers are described in this study. Individual contributions to the collective modes are investigated at nanometer scale by means of energy-filtering transmission electron microscopy and compared to ultraviolet–visible spectroscopy. It is found that the aspect ratio and the shape of the clusters are the two main contributors to the low-energy collective modes.

Purcell Enhancement and Wavelength Shift of Emitted Light by CsPbI3 Perovskite Nanocrystals Coupled to Hyperbolic Metamaterials

Manipulation of the exciton emission rate in nanocrystals of lead halide perovskites (LHPs) was demonstrated by means of coupling of excitons with a hyperbolic metamaterial (HMM) consisting of alternating thin metal (Ag) and dielectric (LiF) layers. Such a coupling is found to induce an increase of the exciton radiative recombination rate by more than a factor of three due to the Purcell effect when the distance between the quantum emitter and HMM is nominally as small as 10 nm, which coincides well with the results of our theoretical analysis. Besides, an effect of the coupling-induced long wavelength shift of the exciton emission spectrum is detected and modeled. These results can be of i…

Novel Method of Preparation of Gold-Nanoparticle-Doped TiO2 and SiO2 Plasmonic Thin Films: Optical Characterization and Comparison with Maxwell-Garnett Modeling

SiO2 and TiO2 thin films with gold nanoparticles (NPs) are of particular interest as photovoltaic materials. A novel method for the preparation of spin-coated SiO2–Au and TiO2–Au nanocomposites is presented. This fast and inexpensive method, which includes three separate stages, is based on the in situ synthesis of both the metal-oxide matrix and the Au NPs during a baking process at relatively low temperature. It allows the formation of nanocomposite thin films with a higher concentration of Au NPs than other methods. High-resolution transmission electron microscopy studies revealed a homogeneous distribution of NPs over the film volume along with their narrow size distribution. The optica…

Inhibition of light emission from the metastable tetragonal phase at low temperatures in island-like films of lead iodide perovskites

Photonic applications based on halide perovskites, namely CH3NH3PbI3 (MAPbI3), have recently attracted remarkable attention due to the high efficiencies reported for photovoltaic and light emitting devices. Despite these outstanding results, there are many temperature-, laser excitation power-, and morphology-dependent phenomena that require further research to be completely understood. In this work, we have investigated in detail the nature of exciton optical transitions and recombination dynamics below and above the orthorhombic/tetragonal ('O'-/'T'-) temperature phase transition (∼150 K) depending on the material continuity (continuous-like) or discontinuity (island-like) in MAPbI3 films…

Structural characterization of bulk and nanoparticle lead halide perovskite thin films by (S)TEM techniques.

Lead halide (APbX3) perovskites, in polycrystalline thin films but also perovskite nanoparticles (NPs) has demonstrated excellent performance to implement a new generation of photovoltaic and photonic devices. The structural characterization of APbX3 thin films using (scanning) transmission electron microscopy ((S)TEM) techniques can provide valuable information that can be used to understand and model their optoelectronic performance and device properties. However, since APbX3 perovskites are soft materials, their characterization using (S)TEM is challenging. Here, we study and compare the structural properties of two different metal halide APbX3 perovskite thin films: bulk CH3NH3PbI3 prep…

Small-pore driven high capacitance in a hierarchical carbon via carbonization of Ni-MOF-74 at low temperatures

A hierarchical porous carbon prepared via direct carbonization of Ni-MOF-74 loaded with furfuryl alcohol at 450 °C displays high specific capacitance in comparison with other MOF-derived carbons as a result of the formation of micropores smaller than 1 nm.

Mapping the plasmonic response of gold nanoparticles embedded in TiO2thin films

We present the mapping of the plasmonic properties of gold nanoparticles that are embedded in a TiO2 thin film deposited over two different substrates, glass and silicon. An improved electron energy-loss spectroscopy (EELS) imaging technique was used to extract plasmon maps with nanometre resolution. Several representative cases of randomly dispersed NPs have been examined to carefully evaluate surrounding effects on the optical response of such nanostructured material. Data were compared to analytical calculations and showed good agreement. These results validate previous structural and far-field optical results and provide a clear description of the optical phenomena that take place at a …

Size control of InAs∕InP(001) quantum wires by tailoring P∕As exchange

The size and emission wavelength of self-assembled InAs∕InP(001) quantum wires (QWrs) is affected by the P∕As exchange process. In this work, we demonstrate by in situ stress measurements that P∕As exchange at the InAs∕InP interface depends on the surface reconstruction of the InAs starting surface and its immediate evolution when the arsenic cell is closed. Accordingly, the amount of InP grown on InAs by P∕As exchange increases with substrate temperature in a steplike way. These results allow us to engineer the size of the QWr for emission at 1.3 and 1.55 μm at room temperature by selecting the range of substrate temperatures in which the InP cap layer is grown.

CCDC 1965235: Experimental Crystal Structure Determination

Related Article: Natalia M. Padial, Bel��n Lerma-Berlanga, Neyvis Almora-Barrios, Javier Castells-Gil, Iv��n da Silva, Mar����a de la Mata, Sergio I. Molina, Jes��s Hern��ndez-Saz, Ana E. Platero-Prats, Sergio Tatay, Carlos Mart����-Gastaldo|2019|J.Am.Chem.Soc.|142|6638|doi:10.1021/jacs.0c00117