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Intercalation-type metal oxides are promising negative electrode materials for safe rechargeable lithium-ion batteries due to the reduced risk of Li plating at low voltages. Nevertheless, their lower energy and power density along with cycling instability remain bottlenecks for their implementation, especially for fast-charging applications. Here, we report a nanostructured rock-salt Nb2O5 electrode formed through an amorphous-to-crystalline transformation during repeated electrochemical cycling with Li+. This electrode can reversibly cycle three lithiums per Nb2O5, corresponding to a capacity of 269 mAh g-1 at 20 mA g-1, and retains a capacity of 191 mAh g-1 at a high rate of 1 A g-1. It exhibits superb cycling stability with a capacity of 225 mAh g-1 at 200 mA g-1 for 400 cycles, and a Coulombic efficiency of 99.93%. We attribute the enhanced performance to the cubic rock-salt framework, which promotes low-energy migration paths. Our work suggests that inducing crystallization of amorphous nanomaterials through electrochemical cycling is a promising avenue for creating unconventional high-performance metal oxide electrode materials.
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Actinide-based compounds exhibit unique physics due to the presence of 5f electrons, and serve in many cases as important technological materials. Targeted thin film synthesis of actinide materials has been successful in generating high-purity specimens in which to study individual physical phenomena. These films have enabled the study of the unique electron configuration, strong mass renormalization, and nuclear decay in actinide metals and compounds. The growth of these films, as well as their thermophysical, magnetic, and topological properties, have been studied in a range of chemistries, albeit far fewer than most classes of thin film systems. This relative scarcity is the result of limited source material availability and safety constraints associated with the handling of radioactive materials. Here, we review recent work on the synthesis and characterization of actinide-based thin films in detail, describing both synthesis methods and modeling techniques for these materials. We review reports on pyrometallurgical, solution-based, and vapor deposition methods. We highlight the current state-of-the-art in order to construct a path forward to higher quality actinide thin films and heterostructure devices.
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In this paper, ordered TiO2 nanotubes were grown on a Ti substrate via electrochemical anodization and subsequently annealed at 450 °C for 4 h under various atmospheres to create different point defects. Oxygen-deficient environments such as Ar and N2 were used to develop oxygen vacancies, while a water vapor (WV) atmosphere was used to generate titanium vacancies. Computational models by density functional theory predicted that the presence of oxygen vacancies would cause electronic conductivity to increase, while the presence of Ti vacancies could lead to decreased conductivity. The predictions were confirmed by two-point electrical conductivity measurements and Mott-Schottky analysis. Raman spectroscopy was also conducted to confirm the presence of defects. The annealed samples were then evaluated as anodes in lithium-ion batteries. The oxygen-deficient samples had an improvement in capacity by 10% and 25% for Ar- and N2-treated samples, respectively, while the WV-treated sample displayed a capacity increase of 24% compared to the stoichiometric control sample (annealed in O2). Electrochemical impedance spectroscopy studies revealed that the WV-treated sample's increased capacity was a consequence of its higher Li diffusivity. The results suggest that balanced electrical and ionic conductivity in nanostructured metal oxide anodes can be tuned through defect generation using heat treatments in various atmospheres for improved electrochemical properties.
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In this letter, we report on quantum light emission from bulk AlInAs grown on InP(111) substrates. We observe indium rich clusters in the bulk Al0.48In0.52As (AlInAs), resulting in quantum dot-like energetic traps for charge carriers, which are confirmed via cross-sectional scanning tunnelling microscopy (XSTM) measurements and 6-band k·p simulations. We observe quantum dot (QD)-like emission signals, which appear as sharp lines in our photoluminescence spectra at near infrared wavelengths around 860 nm, and with linewidths as narrow as 50 µeV. We demonstrate the capability of this new material system to act as an emitter of pure single photons as we extract g(2)-values as low as gcw(2)(0)=0.05-0.05+0.17 for continuous wave (cw) excitation and gpulsed, corr.(2)=0.24±0.02 for pulsed excitation.
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We use thin tensile-strained AlAs layers to manage compressive strain in stacked layers of InAs/AlAsSb quantum dots (QDs). The AlAs layers allow us to reduce residual strain in the QD stacks, suppressing strain-related defects. AlAs layers 2.4 monolayers thick are sufficient to balance the strain in the structures studied, in agreement with theory. Strain balancing improves material quality and helps increase QD uniformity by preventing strain accumulation and ensuring that each layer of InAs experiences the same strain. Stacks of 30 layers of strain-balanced QDs exhibit carrier lifetimes as long as 9.7 ns. QD uniformity is further enhanced by vertical ABAB ordering of the dots in successive layers. Strain compensated InAs/AlAsSb QD stacks show great promise for intermediate band solar cell applications.
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We demonstrate the ability to tailor self-assembled growth of In0.5Ga0.5As quantum dots (QDs) on GaSb(111)A surfaces by molecular beam epitaxy. Spontaneous formation via the Volmer-Weber growth mode produces QDs with excellent structural and optical quality. By harnessing tensile strain to reduce their band gap energy, these QDs are characterized by light emission that extends into the midwave infrared wavelength range of 3.2-3.9 µm (0.318-0.388 eV). As we increase QD size, we can tune the band alignment from type-III to type-II, where light emission occurs due to interband recombination between quantum confined electrons in the InGaAs QDs and holes in the GaSb barriers. Of particular interest is an unusual blue-shift in emission wavelength with increasing QD size, which we attribute to the incorporation of Sb into the InGaAs QDs from the GaSb barriers. By expanding this approach to produce tensile-strained QDs from other narrow band gap semiconductors, we anticipate the development of a range of highly tunable mid-infrared light sources.
RESUMO
Driven by tensile strain, GaAs quantum dots (QDs) self-assemble on In0.52Al0.48As(111)A surfaces lattice-matched to InP substrates. In this study, we show that the tensile-strained self-assembly process for these GaAs(111)A QDs unexpectedly deviates from the well-known Stranski-Krastanov (SK) growth mode. Traditionally, QDs formed via the SK growth mode form on top of a flat wetting layer (WL) whose thickness is fixed. The inability to tune WL thickness has inhibited researchers' attempts to fully control QD-WL interactions in these hybrid 0D-2D quantum systems. In contrast, using microscopy, spectroscopy, and computational modeling, we demonstrate that for GaAs(111)A QDs, we can continually increase WL thickness with increasing GaAs deposition, even after the tensile-strained QDs (TSQDs) have begun to form. This anomalous SK behavior enables simultaneous tuning of both TSQD size and WL thickness. No such departure from the canonical SK growth regime has been reported previously. As such, we can now modify QD-WL interactions, with future benefits that include more precise control of TSQD band structure for infrared optoelectronics and quantum optics applications.
RESUMO
Self-assembled quantum dots (SAQDs) grown under biaxial tension could enable novel devices by taking advantage of the strong band gap reduction induced by tensile strain. Tensile SAQDs with low optical transition energies could find application in the technologically important area of mid-infrared optoelectronics. In the case of Ge, biaxial tension can even cause a highly desirable crossover from an indirect- to a direct-gap band structure. However, the inability to grow tensile SAQDs without dislocations has impeded progress in these directions. In this article, we demonstrate a method to grow dislocation-free, tensile SAQDs by employing the unique strain relief mechanisms of (110)-oriented surfaces. As a model system, we show that tensile GaAs SAQDs form spontaneously, controllably, and without dislocations on InAlAs(110) surfaces. The tensile strain reduces the band gap in GaAs SAQDs by ~40%, leading to robust type-I quantum confinement and photoluminescence at energies lower than that of bulk GaAs. This method can be extended to other zinc blende and diamond cubic materials to form novel optoelectronic devices based on tensile SAQDs.