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At least 55 records · Page 3

Cathodoluminescence and transmission electron microscopy study of dark line defects in thick In(0.2)Ga(0.8)As/GaAs multiple quantum wells

TEM and cathodoluminescence (CL) imaging and spectroscopy have been performed on In(0.2)Ga(0.8)As/GaAs MQW structures. Cross-sectional and plan-view TEM demonstrates that misfit dislocations (MDs) are confined to the MQW-to-GaAs interfacial regions. The observed large variation in the exciton luminescence intensity is interpreted as due to the presence of nonradiative recombination centers spread homogeneously in the MQW region away from interface MDs. These nonradiative recombination centers compete with exciton and midgap radiative centers at wavelengths of 950 nm and 1000-1600 nm, respectively, resulting in spatiallty correlated dark line defects for all CL imaging wavelengths.

Rich, D. H.↗

Dependence of the cathodoluminescence of diamond films on deposition temperature

The deposition temperature dependence of the cathodoluminescence (CL) of diamond thin films grown by microwave-plasma-assisted chemical vapor deposition has been investigated. Depositions were made in the temperature range of 400 to 750 C at a pressure of 10 Torr, with a gas mixture of 5 percent CH4 and 5 percent O2 in hydrogen. The intensity of the luminescent peak at 430 nm was used as a measure of diamond quality for the film. This peak was found to be a maximum above 600 C. Examination of the intensities of CL emissions associated with nitrogen and silicon impurities at 530, 560, and 740 nm indicate incorporation of these impurities is more efficient at temperatures above 600 C. Film quality was thus found to be an optimization of competing mechanisms, i.e., improvement of diamond quality as evidenced by the intensity of the 430 nm peak, with the apparent activation of impurities and vacancy defects at elevated temperatures.

Shing, Y. H.↗

Cathodoluminescence properties of components in enstatite chondrites

As a group, the enstatite chondrites are notable by the extremely low FeO content of most of their silicates. This property predisposes many of these materials to emit Cathodoluminescence (CL). Since examination of the CL properties of meteoritic components in ordinary and carbonaceous chondrites have proven to be a useful technique, we have initiated a survey of the enstatite chondrites in order to better characterize the chemical and physical properties of their luminescing phases. Because of the diversity encountered in this study, it is first necessary to describe the number and types of materials observed to emit CL in these meteorites. Two CL techniques were used. First, the initial survey work was conducted at low magnification using a Nuclide (now MAAS) Luminoscope mounted to a Wild MP binocular microscope equipped for photomicroscopy. The beam conditions used were 14 +/- KeV and 7 +/- 1 milliamps, with the beam focussed to the diameter of the field of view of the microscope at 20x (appox. 1.25 cm). Photomosaics were produced for each section using Ecktar 1000 film and an exposure time of 15 to 30 seconds. Second, high magnification (400x) photos were obtained of individual components of interest by mounting a 35mm camera to the optical system of the Cameca Camebax microprobe located at the Johnson Space Center. Beam conditions used were 15 KeV and 600 nA. Ecktar 1000 film was also used, but exposure times of 6 minutes were necessary to produce a useful image. The components in E chondrites that produce CL can be divided into four broad categories. These are clasts and aggregates, chondrules, matrix components, and refractory objects. Components in each category are discussed.

Dehart, John M.↗

Cathodoluminescence observations of in situ aqueous destruction of chondrules in the Murchison CM chondrite

A low-power cathodoluminescence (CL) mosaic of a 1x2 cm section of the Murchison CM chondrite contains chondrules of two types: one contains olivines with red CL and is thought to be the equivalent of group A chondrules of Sears et.; and one without observable CL, which is probably equivalent to their group B chondrules. Both types of chondrule contain dust mantles with a characteristic uniform red CL due to very fine-grained forsterites, but the mantles of group A chondrules have a complex internal structure and are much thicker than the relatively thin rims on the group B chondrules. The variety of internal textures and the progressive integration of the objects with the surrounding matrix suggests to us that these features are large group A chondrules in the process of being destroyed by aqueous alteration. Prior to aqueous alteration, group A chondrules in CM chondrites were larger than group B chondrules, which is contrary to the situation in ordinary chondrites and were apparently destroyed more rapidly than group B chondrules by aqueous alteration.

Sears, Derek W. G.↗

Two chondrule groups each with distinctive rims in Murchison recognized by cathodoluminescence

Two groups of chondrules in the Murchison CM chondrite, which have previously been identified on the basis of FeO in the chondrule grains, are readily identified from cathodoluminescence (CL) and belong to those of the ordinary chondrite group A and B chondrules of Sears et al. (1992a). All chondrules are surrounded by fine-grained rims containing forsterite with bright red CL, but on group A chondrules an outer thin rim grades into a much thicker rim, with a lower density of forsterite grains, which in turn grades into the central chondrule. Group B chondrules have only the thin outer rim with a high density of small forsterite grains. This is the first time an unequivocal correlation has been observed between chondrule rim thickness and the composition of the object on which the rim is located. We suggest that while all objects in the meteorite (group B chondrules, refractory inclusions, mineral and chondrule fragments, clasts) acquired a very thin rim during processing in a wet regolith, the thick rims on group A chondrules were formed by aqueous alteration of precursor metal- and sulfide-rich rims which are a characteristic of group A chondrules in ordinary chondrites.

Sears, Derek W. G.↗

Pyroxene structures, cathodoluminescence and the thermal history of the enstatite chondrites

In order to explore the thermal history of enstatite chondrites, we examined the cathodoluminescence (CL) and thermoluminescence (TL) properties of 15 EH chondrites and 21 EL chondrites, including all available petrographic types, both textural types 3-6 and mineralogical types alpha-delta. The CL properties of EL3(alpha) and EH3(alpha) chondrites are similar. Enstatite grains high in Mn and other transition metals display red CL, while enstatite with low concentrations of these elements show blue CL. A few enstatite grains with greater than 5 wt% FeO display no CL. In contrast, the luminescent properties of the metamorphosed EH chondrites are very different from those of metamorphosed EL chondrites. While the enstatites in metamorphosed EH chondrites display predominantly blue CL, the enstatites in metamorphosed EL chondrites display a distinctive magenta CL with blue and red peaks of approximately equal intensity in their spectra. The TL sensitivities of the enstatite chondrites correlate with the intensity of the blue CL and, unlike other meteorite classes, are not simply related to metamorphism. The different luminescent properties of metamorphosed EH and EL chondrites cannot readily be attributed to compositional differences. But x-ray diffraction data suggests that the enstatite in EH5(gamma),(delta) chondrites is predominantly disordered orthopyroxene, while enstatite in EL6(beta) chondrites is predominantly ordered orthopyroxene. The difference in thermal history of metamorphosed EL and EH chondrites is so marked that the use of single 'petrographic' types is misleading, and separate textural and mineralogical types are preferable. Our data confirm earlier suggestions that metamorphosed EH chondrites underwent relatively rapid cooling, and the metamorphosed EL chondrites cooled more slowly and experienced prolonged heating in the orthopyroxene field.

Zhang, Yanhong↗

Cathodoluminescent Source of Intense White Light

The device described exploits cathodoluminescence to generate intense light in the visible and near-infrared regions of the spectrum. In this device, the material to be excited to luminescence is a layer of quartz or alumina powder on an electrically conductive plate exposed to a low-pressure plasma discharge. The plate is electrically biased positively to collect electron current.

Foster, John E.↗

Nanoscale optical tomography with cathodoluminescence spectroscopy

In one aspect, a cathodoluminescence (CL) spectroscopic tomography device includes a sample stage to support a sample. An electron beam source scans an electron beam over the sample to yield light emission by the sample. A reflective element directs the light emission by the sample to a light detector. A controller controls operation of the sample stage, the electron beam source, and the light detector. In one aspect, a CL spectroscopic tomography device includes an electron beam source which directs an electron beam at an object to yield an emission by the object. A detector detects the emission. A controller receives information from the detector related to the detected emission. The controller derives a two-dimensional (2D) CL map from the information related to the detected emission, and derives a three-dimensional (3D) CL tomogram from the 2D CL map.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Unraveling sources of emission heterogeneity in Silicon Vacancy color centers with cryo-cathodoluminescence microscopy

Diamond color centers have proven to be versatile quantum emitters and exquisite sensors of stress, temperature, electric and magnetic fields, and biochemical processes. Among color centers, the silicon-vacancy (SiV - ) defect exhibits high brightness, minimal phonon coupling, narrow optical linewidths, and high degrees of photon indistinguishability. Yet the creation of reliable and scalable SiV - -based color centers has been hampered by heterogeneous emission, theorized to originate from surface imperfections, crystal lattice strain, defect symmetry, or other lattice impurities. Here, we advance high-resolution cryo-electron microscopy combined with cathodolumines cence spectroscopy and 4D scanning transmission electron microscopy (STEM) to elucidate the structural sources of heterogeneity in SiV - emission from nanodiamond with sub-nanometer-scale resolution. Our diamond nanoparticles are grown directly on TEM membranes from molecular-level seedings, representing the natural formation conditions of color centers in diamond. We show that individual subcrystallites within a single nanodiamond exhibit distinct zero-phonon line (ZPL) energies and differences in brightness that can vary by 0.1 meV in energy and over 70% in brightness. These changes are correlated with the atomic-scale lattice structure. We find that ZPL blue shifts result from tensile strain, while ZPL red shifts are due to compressive strain. We also find that distinct crystallites host distinct densities of SiV - emitters and that grain boundaries impact SiV - emission significantly. Finally, we interrogate nanodiamonds as small as 40 nm in diameter and show that these diamonds exhibit no spatial change to their ZPL energy. Our work provides a foundation for atomic-scale structure-emission correlation, e.g., of single atomic defects in a range of quantum and two-dimensional materials.

36 MATERIALS SCIENCE↗

Low temperature annealing and cathodoluminescence studies of type 1 chondrule compositions

Preliminary results indicate that the yellow luminescing mesostases in type I chondrules can be altered by the effects of the low level thermal metamorphism. Although heat alone was insufficient to alter the CL, reheating for geologically relevant periods could have the same results as we obtained in a second series of experiments with water present. It is known that both water and solutions of sodium metasilicate greatly accelerate the devitrification of glasses. The results of the experiments that will be repeated should further clarify how the CL changes with increased thermal alteration.

Dehart, John M.↗

Near-field imaging of plasmonic nanopatch antennas with integrated semiconductor quantum dots

Plasmonic nanopatch antennas that incorporate dielectric gaps hundreds of picometers to several nanometers thick have drawn increasing attention over the past decade because they confine electromagnetic fields to grossly sub-diffraction-limited volumes. Substantial control over the optical properties of excitons and color centers confined within these plasmonic cavities has already been demonstrated with far-field optical spectroscopies, but near-field optical spectroscopies are essential for an improved understanding of the plasmon–emitter interaction at the nanoscale. Here, we characterize the intensity and phase-resolved plasmonic response of isolated nanopatch antennas by cathodoluminescence microscopy. Furthermore, we explore the distinction between optical and electron beam spectroscopies of coupled plasmon–exciton heterostructures to identify constraints and opportunities for future nanoscale characterization and control of hybrid nanophotonic structures. While we observe substantial Purcell enhancement in time-resolved photoluminescence spectroscopies, negligible Purcell enhancement is observed in cathodoluminescence spectroscopies of hybrid nanophotonic structures. The substantial differences in measured Purcell enhancement for electron beam and laser excitation can be understood as a result of the different selection rules for these complementary experiments. Overall, these results provide a fundamentally new understanding of near-field plasmon–exciton interactions in nanopatch antennas, which is essential for myriad emerging quantum photonic devices.

36 MATERIALS SCIENCE↗

Green-emitting cubic GaN/In 0.16 Ga 0.84 N/GaN quantum well with 32% internal quantum efficiency at room temperature

Structural and optical properties of a green-emitting cubic (i.e., zinc blende) GaN/In 0.16 Ga 0.84 N/GaN single quantum well structure are reported. The active layer is grown on a phase-pure (i.e., 100%) cubic GaN enabled on a 1 × 1 cm 2 U-grooved silicon (100) through aspect ratio phase trapping. Energy dispersive x-ray spectroscopy combined with room temperature cathodoluminescence reveals 522 nm green light emission at room temperature with only 16.0% ± 1.6% of indium content, which is ~30% less than the amount of indium needed in a traditional green-emitting hexagonal (i.e., wurtzite) well. Temperature-dependent behavior of the green emission, such as activation energy, s-shaped peak energy shift, and linewidth, is reported. Cathodoluminescence at 8 and 300 K reveals an internal quantum efficiency of 32.0% ± 0.6%, which is higher than any reported value for cubic wells. Altogether, phase-pure cubic active layers on phase transition cubic GaN are shown to be promising for green and longer wavelength emitters.

42 ENGINEERING↗

Closed-loop electron-beam-induced spectroscopy and nanofabrication around individual quantum emitters

Color centers in diamond play a central role in the development of quantum photonic technologies, and their importance is only expected to grow in the near future. For many quantum applications, high collection efficiency from individual emitters is required, but the refractive index mismatch between diamond and air limits the optimal collection efficiency with conventional diamond device geometries. While different out-coupling methods with near-unity efficiency exist, many have yet to be realized due to current limitations in nanofabrication methods, especially for mechanically hard materials like diamond. Here, we leverage electron-beam-induced etching to modify Sn-implanted diamond quantum microchiplets containing integrated waveguides with a width and thickness of 280 nm and 200 nm, respectively. This approach allows for simultaneous high-resolution imaging and modification of the host matrix with an open geometry and direct writing. When coupled with the cathodoluminescence signal generated from the electron–emitter interactions, we can monitor the enhancement of the quantum emitters in real-time with nanoscale spatial resolution. The operando cathodoluminescence measurement and fabrication around single photon emitters demonstrated here provide a new foundation for the potential control of emitter–cavity interactions in integrated quantum photonics.

36 MATERIALS SCIENCE↗

Formation of wide-blocky calcite veins by extreme growth competition

Liassic limestones on the coast of Somerset in the UK contain dense arrays of calcite microveins with a common, but poorly understood microstructure, characterized by laterally wide crystals that form bridges across the vein. We investigated the mechanisms of formation and evolution of these ‘wide-blocky’ vein microstructures using a combination of high-resolution analytical methods, including virtual petrography, optical cathodoluminescence and scanning electron microscopy techniques (e.g. energy-dispersive X-ray spectrometry, back-scattered electron imaging, cathodoluminescence and electron back-scattered diffraction), laboratory experiments and multiphase field modelling. Our results indicate that the studied veins formed in open, fluid-filled fractures, each in a single opening and sealing episode. As shown by the optical and electron back-scattered diffraction images, the vein crystals grew epitaxially on grains of the wall rock and we hypothesize that their growth rates differed depending on whether the crystals were on a wall rock grain substrate that fractured intergranularly (slow growth rates) or transgranularly (rapid growth rates). Our multiphase field models support this hypothesis, showing that wide, blocky crystals only form where there are significant differences in the growth rate and are dependent on the type of seed grain. These results provide strong evidence for extreme growth competition, a process that we propose controls vein-filling in many micritic carbonate reservoirs, as well as demonstrate that the characteristics of the fracture wall can affect the filling processes in syntaxial veins. Supplementary material: The description and images of the studied thin sections are available at https://doi.org/10.6084/m9.figshare.c.5172371 . High-resolution optical microscopy mosaics (under plane-polarized- and crossed polarized light) of the thin section collection in PetroScan file format are available on request from the authors.

Geology↗

Electron Beam Induced Luminescence of SiO2 Optical Coatings

Optical coatings of disordered thin film SiO,/SiO, samples undergoing electron beam bombardment exhibited a cathodoluminescence effect. Measurements were made of the absolute illuminance and emission spectra as functions of incident electron energy (0.2 keV to 30 keV). flux (approx. 0.1 nA/sq cm to > 100 nA/sq cm) and power (<50 nW/sq cm to > 3mW/sq cm) for coatings (approx.60 nm to approx.200 nm thick) on reflective metal substrates over a range of sample temperatures (approx.40 K to approx.400 K) and emission wavelengths (approx.260 nm to approx.5000 nm). Illuminance reached a plateau saturation intensity I(sub sat) approx. 10(exp -4)W/sq cm. scaling as [I(sub mc)/(I + I(sub mc)/I(sub sat)] as incident power I(sub mc) approached I(sub sat). Well below I(sub sat), illuminance scaled linearly with incident power for lower-energy non-penetrating radiation that deposited all of its energy in the dielectric film. At higher incident energies (> 1-5 keV) electrons penetrate the dielectric, depositing only a fraction of their energy in the dielectric film, where deposited energy scales as the ratio of film thickness to penetration range. Since electron range exhibits a peak below approx. 1 keV, the illuminance decreased with increasing energy for penetrating radiation. The temperature dependence of the illuminance. in general, increased with decreasing temperature. Changes in apparent color with temperature were also observed. Four bands in the UV/VIS/NIR range from 300 nm to 1000 nm were observed in spectral measurements; no significant luminescence was detected in a range from approx. 1000 nm to approx. 5000 nm. These different bands either increased or decreased in intensity and shifted slightly in energy with decreasing temperature. Our measurements are explained in terms of simple disordered band theory models based on atomic-scale stochastic transport of electrons in highly disordered insulating materials. The theoretical models provide a fundamental basis for understanding the dependence of cathodoluminescence on irradiation time, incident flux and energy. and sample thickness and temperature. The observed luminescence occurs when an incident high energy electron excites a valence band electron into the conduction band. Following the excitation. a complex series of transitions take place between the extended conduction states and the long-lived localized trapped states (or chromophores) associated with structural or compositional defects in the dielectric materials. Thc transport equations and models of thc spatial and energy distribution of the trapped states below the mobility edge, their occupancy, and transitions provide microscopic scale insights into this macroscopic phenomenon. Our observations and theoretical models are also compared with similar previous room temperature studies of similar SiO2 films.

Dennison, J. R.↗

Lithium Spatial Distribution and Split-Off Electronic Bands at Nanoscale V 2 O 5 /LiPON Interfaces

A combination of depth-resolved cathodoluminescence spectroscopy (DRCLS) and X-ray photoemission depth profiling (XPS) measured the pronounced changes in both the electronic density of states and lithium composition near the nanoscale LixV2O5/LiPON interface. DRCLS studies of electrochemically lithiated bare V2O5 and the sputterdeposited V2O5 plus LiPON overlayer electrochemically lithiated in stages both showed that in the bulk the luminescence intensity of the “split-off” hybridized bonding density of states was anticorrelated with XPSmeasured Li content, decreasing as the Li content increased. However, the LiPON overlayer was found to modify the band structure of the underlying LixV2O5 (LVO) to a depth of at least 30 nm beneath the V2O5 interface. DRCLS spectra near the electrochemically lithiated LiPON/ LVO interface showed a significant intensity of the split-off band, implying a low Li content. However, XPS depth profiling revealed a pronounced negative gradient of Li extending from a maximum Li content at the intimate LiPON boundary to its lowest content of ∼30 nm into the V2O5 in the same region, indicating a strong interaction between band structure and Li electrochemical potential near this heterojunction. These results provide evidence for substantial effects on the local band structure near an electrolyte/cathode interface and insights into the electrochemical interface behavior of solid-state batteries in general.

25 ENERGY STORAGE↗

Lateral Integration of SnS and GeSe van der Waals Semiconductors: Interface Formation, Electronic Structure, and Nanoscale Optoelectronics

The emergence of atomically thin crystals has allowed extending materials integration to lateral heterostructures where different 2D materials are covalently connected in the plane. The concept of lateral heterostructures can be generalized to thicker layered crystals, provided that a suitably faceted seed crystal presents edges to which a compatible second van der Waals material can be attached layer by layer. Here, we examine the possibility of integrating multilayer crystals of the group IV monochalcogenides SnS and GeSe, which have the same crystal structure, small lattice mismatch, and similar bandgaps. In a two-step growth process, lateral epitaxy of GeSe on the sidewalls of multilayer SnS flakes (obtained by vapor transport of a SnS 2 precursor on graphite) yields heterostructures of laterally stitched crystalline GeSe and SnS without any detectable vertical overgrowth of the SnS seeds and with sharp lateral interfaces. Combined cathodoluminescence spectroscopy and ab initio calculations show the effects of small band offsets on carrier transport and radiative recombination near the interface. Further, the results demonstrate the possibility of forming atomically connected lateral interfaces across many van der Waals layers, which is promising for manipulating optoelectronics, photonics, and for managing charge- and thermal transport.

2D layered crystals↗