ORCID Profile
0000-0002-9102-6083
Current Organisation
University of Oxford
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Publisher: Elsevier BV
Date: 10-2011
Publisher: Springer Science and Business Media LLC
Date: 10-04-2011
Abstract: Formic acid (HCOOH) has great potential as an in situ source of hydrogen for fuel cells, because it offers high energy density, is non-toxic and can be safely handled in aqueous solution. So far, there has been a lack of solid catalysts that are sufficiently active and/or selective for hydrogen production from formic acid at room temperature. Here, we report that Ag nanoparticles coated with a thin layer of Pd atoms can significantly enhance the production of H₂ from formic acid at ambient temperature. Atom probe tomography confirmed that the nanoparticles have a core-shell configuration, with the shell containing between 1 and 10 layers of Pd atoms. The Pd shell contains terrace sites and is electronically promoted by the Ag core, leading to significantly enhanced catalytic properties. Our nanocatalysts could be used in the development of micro polymer electrolyte membrane fuel cells for portable devices and could also be applied in the promotion of other catalytic reactions under mild conditions.
Publisher: Elsevier BV
Date: 02-2017
Publisher: Springer Science and Business Media LLC
Date: 17-10-2014
Publisher: American Chemical Society (ACS)
Date: 10-02-2012
DOI: 10.1021/JP211687M
Publisher: AIP Publishing
Date: 11-06-2019
DOI: 10.1063/1.5097411
Abstract: We investigate the atomic scale structure of m-plane InGaN quantum wells grown on bulk m-plane GaN templates and reveal that as the indium content increases there is an increased tendency for nonrandom clustering of indium atoms to occur. Based on the atom probe tomography data used to reveal this clustering, we develop a k · p model that takes these features into account and links the observed nanostructure to the optical properties of the quantum wells. The calculations show that electrons and holes tend to colocalize at indium clusters. The transition energies between the electron and hole states are strongly affected by the shape and size of the clusters. Hence, clustering contributes to the very large line widths observed in the experimental low temperature photoluminescence spectra. Also, the emission from m-plane InGaN quantum wells is strongly linearly polarized. Clustering does not alter the theoretically predicted polarization properties, even when the shape of the cluster is strongly asymmetric. Overall, however, we show that the presence of clustering does impact the optical properties, illustrating the importance of careful characterization of the nanoscale structure of m-plane InGaN quantum wells and that atom probe tomography is a useful and important tool to address this problem.
Publisher: Elsevier BV
Date: 05-2016
Publisher: AIP Publishing
Date: 02-05-2016
DOI: 10.1063/1.4948299
Abstract: Atom probe tomography and quantitative scanning transmission electron microscopy are used to assess the composition of non-polar a-plane (11-20) InGaN quantum wells for applications in optoelectronics. The average quantum well composition measured by atom probe tomography and quantitative scanning transmission electron microscopy quantitatively agrees with measurements by X-ray diffraction. Atom probe tomography is further applied to study the distribution of indium atoms in non-polar a-plane (11-20) InGaN quantum wells. An inhomogeneous indium distribution is observed by frequency distribution analysis of the atom probe tomography measurements. The optical properties of non-polar (11-20) InGaN quantum wells with indium compositions varying from 7.9% to 20.6% are studied. In contrast to non-polar m-plane (1-100) InGaN quantum wells, the non-polar a-plane (11-20) InGaN quantum wells emit at longer emission wavelengths at the equivalent indium composition. The non-polar a-plane (11-20) quantum wells also show broader spectral linewidths. The longer emission wavelengths and broader spectral linewidths may be related to the observed inhomogeneous indium distribution.
Publisher: Elsevier BV
Date: 2016
Publisher: Springer Science and Business Media LLC
Date: 2016
DOI: 10.1557/MRS.2015.311
Publisher: American Association for the Advancement of Science (AAAS)
Date: 17-03-2017
Abstract: The design of atomic-scale microstructural traps to limit the diffusion of hydrogen is one key strategy in the development of hydrogen-embrittlement-resistant materials. In the case of bearing steels, an effective trapping mechanism may be the incorporation of finely dispersed V-Mo-Nb carbides in a ferrite matrix. First, we charged a ferritic steel with deuterium by means of electrolytic loading to achieve a high hydrogen concentration. We then immobilized it in the microstructure with a cryogenic transfer protocol before atom probe tomography (APT) analysis. Using APT, we show trapping of hydrogen within the core of these carbides with quantitative composition profiles. Furthermore, with this method the experiment can be feasibly replicated in any APT-equipped laboratory by using a simple cold chain.
Publisher: Maney Publishing
Date: 11-02-2016
Publisher: Elsevier BV
Date: 10-2013
Publisher: Elsevier BV
Date: 03-2016
Publisher: American Chemical Society (ACS)
Date: 31-10-2014
DOI: 10.1021/JP508144Z
Publisher: Oxford University Press (OUP)
Date: 30-04-2015
DOI: 10.1017/S1431927615000422
Abstract: Various practical issues affecting atom probe tomography (APT) analysis of III-nitride semiconductors have been studied as part of an investigation using a c -plane InAlN/GaN heterostructure. Specimen preparation was undertaken using a focused ion beam microscope with a mono-isotopic Ga source. This enabled the unambiguous observation of implantation damage induced by s le preparation. In the reconstructed InAlN layer Ga implantation was demonstrated for the standard “clean-up” voltage (5 kV), but this was significantly reduced by using a lower voltage (e.g., 1 kV). The characteristics of APT data from the desorption maps to the mass spectra and measured chemical compositions were examined within the GaN buffer layer underlying the InAlN layer in both pulsed laser and pulsed voltage modes. The measured Ga content increased monotonically with increasing laser pulse energy and voltage pulse fraction within the examined ranges. The best results were obtained at very low laser energy, with the Ga content close to the expected stoichiometric value for GaN and the associated desorption map showing a clear crystallographic pole structure.
Publisher: American Association for the Advancement of Science (AAAS)
Date: 06-01-2023
Abstract: A potential record of Earth’s magnetic field going back 4.2 billion years (Ga) ago is carried by magnetite inclusions in zircon grains from the Jack Hills. This magnetite may be secondary in nature, however, meaning that the magnetic record is much younger than the zircon crystallization age. Here, we use atom probe tomography to show that Pb-bearing nanoclusters in magnetite-bearing Jack Hills zircons formed during two discrete events at 3.4 and Ga. The older population of clusters contains no detectable Fe, whereas roughly half of the younger population of clusters is Fe bearing. This result shows that the Fe required to form secondary magnetite entered the zircon sometime after 3.4 Ga and that remobilization of Pb and Fe during an annealing event occurred more than 1 Ga after deposition of the Jack Hills sediment at 3 Ga. The ability to date Fe mobility linked to secondary magnetite formation provides new possibilities to improve our knowledge of the Archean geodynamo.
Publisher: Wiley
Date: 07-05-2021
DOI: 10.1111/GGR.12382
Abstract: Hydrous phyllosilicate minerals, including the serpentine subgroup, are likely to be major constituents of material that will be bought back to Earth by missions to Mars and to primitive asteroids Ryugu and Bennu. Small quantities ( 60 g) of micrometre‐sized, internally heterogeneous material will be available for study, requiring minimally destructive techniques. Many conventional methods are unsuitable for phyllosilicates as they are typically finely crystalline and electron beam‐sensitive resulting in amorphisation and dehydration. New tools will be required for nanoscale characterisation of these precious extra‐terrestrial s les. Here we test the effectiveness of atom probe tomography (APT) for this purpose. Using lizardite from the Ronda peridotite, Spain, as a terrestrial analogue, we outline an effective analytical protocol to extract nanoscale chemical and structural measurements of phyllosilicates. The potential of APT is demonstrated by the unexpected finding that the Ronda lizardite contains SiO‐rich nanophases, consistent with opaline silica that formed as a by‐product of the serpentinisation of olivine. Our new APT approach unlocks previously unobservable nanominerals and nanostructures within phyllosilicates owing to resolution limitations of more established imaging techniques. APT will provide unique insights into the processes and products of water/rock interaction on Earth, Mars and primitive asteroids.
Publisher: Elsevier BV
Date: 08-2016
Publisher: Informa UK Limited
Date: 27-04-2016
Publisher: Elsevier BV
Date: 11-2018
Publisher: AIP Publishing
Date: 16-02-2015
DOI: 10.1063/1.4909514
Abstract: Atom probe tomography (APT) has been used to characterize the distribution of In atoms within non-polar a-plane InGaN quantum wells (QWs) grown on a GaN pseudo-substrate produced using epitaxial lateral overgrowth. Application of the focused ion beam microscope enabled APT needles to be prepared from the low defect density regions of the grown s le. A complementary analysis was also undertaken on QWs having comparable In contents grown on polar c-plane s le pseudo-substrates. Both frequency distribution and modified nearest neighbor analyses indicate a statistically non-randomized In distribution in the a-plane QWs, but a random distribution in the c-plane QWs. This work not only provides insights into the structure of non-polar a-plane QWs but also shows that APT is capable of detecting as-grown nanoscale clustering in InGaN and thus validates the reliability of earlier APT analyses of the In distribution in c-plane InGaN QWs which show no such clustering.
Publisher: American Chemical Society (ACS)
Date: 13-08-2012
DOI: 10.1021/JP304359M
Publisher: Elsevier BV
Date: 09-2013
DOI: 10.1016/J.ULTRAMIC.2012.10.012
Abstract: A major practical challenge in heterogeneous catalysis is to minimize the loading of expensive platinum group metals (PGMs) without degrading the overall catalytic efficiency. Gaining a thorough atomic-scale understanding of the chemical/structural changes occurring during catalyst manufacture/operation could potentially enable the design and production of "nano-engineered" catalysts, optimized for cost, stability and performance. In the present study, the oxidation behavior of a Pt-31 at% Pd alloy between 673-1073 K is investigated using atom probe tomography (APT). Over this range of temperatures, three markedly different chemical structures are observed near the surface of the alloy. At 673 K, the surface oxide formed is enriched with Pd, the concentration of which rises further following oxidation at 773 K. During oxidation at 873 K, a thick, stable oxide layer is formed on the surface with a stoichiometry of PdO, beneath which a Pd-depleted (Pt-rich) layer exists. Above 873 K, the surface composition switches to enrichment in Pt, with the Pt content increasing further with increasing oxidation temperature. This treatment suggests a route for tuning the surfaces of Pt-Pd nanoparticles to be either Pd-rich or Pt-rich, simply by adjusting the oxidation temperatures in order to form two different types of core-shell structures. In addition, comparison of the oxidation behavior of Pt-Pd with Pt-Rh and Pd-Rh alloys demonstrates markedly different trends under the same conditions for these three binary alloys.
Publisher: Elsevier BV
Date: 12-2018
Publisher: Elsevier BV
Date: 10-2023
Publisher: Oxford University Press (OUP)
Date: 15-03-2023
Abstract: A large number of atom probe tomography (APT) datasets from past experiments were collected into a database to conduct statistical analyses. An effective way of handling the data is shown, and a study on hydrogen is conducted to illustrate the usefulness of this approach. We propose to handle a large collection of APT spectra as a point cloud and use a city block distance–based metric to measure dissimilarity between spectra. This enables quick and automated searching for spectra by similarity. Since spectra from APT experiments on similar materials are similar, the point cloud of spectra contains clusters. Analysis of these clusters of spectra in this point cloud allows us to infer the s le materials. The behavior of contaminant hydrogen is analyzed and correlated with voltage, electric field, and s le base material. Across several materials, the H2+ /H+ ratio is found to decrease with increasing field, likely an indication of postionization of H2+ ions. The absolute amounts of H2+ and H+ are found to frequently increase throughout APT experiments.
Publisher: Elsevier BV
Date: 08-2020
Publisher: Springer Science and Business Media LLC
Date: 12-07-2016
DOI: 10.1038/SREP25618
Abstract: Understanding the corrosion of uranium is important for its safe, long-term storage. Uranium metal corrodes rapidly in air, but the exact mechanism remains subject to debate. Atom Probe Tomography was used to investigate the surface microstructure of metallic depleted uranium specimens following polishing and exposure to moist air. A complex, corrugated metal-oxide interface was observed, with approximately 60 at.% oxygen content within the oxide. Interestingly, a very thin (~5 nm) interfacial layer of uranium hydride was observed at the oxide-metal interface. Exposure to deuterated water vapour produced an equivalent deuteride signal at the metal-oxide interface, confirming the hydride as originating via the water vapour oxidation mechanism. Hydroxide ions were detected uniformly throughout the oxide, yet showed reduced prominence at the metal interface. These results support a proposed mechanism for the oxidation of uranium in water vapour environments where the transport of hydroxyl species and the formation of hydride are key to understanding the observed behaviour.
Publisher: Springer Science and Business Media LLC
Date: 15-06-2021
DOI: 10.1038/S41377-021-00564-Z
Abstract: We investigated metal-organic vapor phase epitaxy grown (InGa)(AsSb)/GaAs/GaP Stranski–Krastanov quantum dots (QDs) with potential applications in QD-Flash memories by cross-sectional scanning tunneling microscopy (X-STM) and atom probe tomography (APT). The combination of X-STM and APT is a very powerful approach to study semiconductor heterostructures with atomic resolution, which provides detailed structural and compositional information on the system. The rather small QDs are found to be of truncated pyramid shape with a very small top facet and occur in our s le with a very high density of ∼4 × 10 11 cm −2 . APT experiments revealed that the QDs are GaAs rich with smaller amounts of In and Sb. Finite element (FE) simulations are performed using structural data from X-STM to calculate the lattice constant and the outward relaxation of the cleaved surface. The composition of the QDs is estimated by combining the results from X-STM and the FE simulations, yielding ∼In x Ga 1 − x As 1 − y Sb y , where x = 0.25–0.30 and y = 0.10–0.15. Noticeably, the reported composition is in good agreement with the experimental results obtained by APT, previous optical, electrical, and theoretical analysis carried out on this material system. This confirms that the InGaSb and GaAs layers involved in the QD formation have strongly intermixed. A detailed analysis of the QD capping layer shows the segregation of Sb and In from the QD layer, where both APT and X-STM show that the Sb mainly resides outside the QDs proving that Sb has mainly acted as a surfactant during the dot formation. Our structural and compositional analysis provides a valuable insight into this novel QD system and a path for further growth optimization to improve the storage time of the QD-Flash memory devices.
Publisher: American Physical Society (APS)
Date: 10-12-2015
Publisher: Elsevier BV
Date: 05-2022
Publisher: Elsevier BV
Date: 02-2019
Publisher: Oxford University Press (OUP)
Date: 08-2022
DOI: 10.1017/S1431927621012162
Abstract: Cu-doping and crystallographic site occupations within the half-Heusler (HH) TiNiSn, a promising thermoelectric material, have been examined by atom probe tomography. In particular, this investigation aims to better understand the influence of atom probe analysis conditions on the measured chemical composition. Under a voltage-pulsing mode, atomic planes are clearly resolved and suggest an arrangement of elements in-line with the expected HH (F-43m space group) crystal structure. The Cu dopant is also distributed uniformly throughout the bulk material. For operation under laser-pulsed modes, the returned composition is highly dependent on the selected laser energy, with high energies resulting in the measurement of excessively high absolute Ti counts at the expense of Sn and in particular Ni. High laser energies also appear to be correlated with the detection of a high fraction of partial hits, indicating nonideal evaporation behavior. The possible mechanisms for these trends are discussed, along with suggestions for optimal analysis conditions for these and similar thermoelectric materials.
Publisher: Elsevier BV
Date: 12-2015
DOI: 10.1016/J.ULTRAMIC.2015.05.006
Abstract: Whilst atom probe tomography (APT) is a powerful technique with the capacity to gather information containing hundreds of millions of atoms from a single specimen, the ability to effectively use this information creates significant challenges. The main technological bottleneck lies in handling the extremely large amounts of data on spatial-chemical correlations, as well as developing new quantitative computational foundations for image reconstruction that target critical and transformative problems in materials science. The power to explore materials at the atomic scale with the extraordinary level of sensitivity of detection offered by atom probe tomography has not been not fully harnessed due to the challenges of dealing with missing, sparse and often noisy data. Hence there is a profound need to couple the analytical tools to deal with the data challenges with the experimental issues associated with this instrument. In this paper we provide a summary of some key issues associated with the challenges, and solutions to extract or "mine" fundamental materials science information from that data.
Publisher: American Chemical Society (ACS)
Date: 28-01-2014
DOI: 10.1021/CS401117E
Publisher: Elsevier BV
Date: 05-2018
Publisher: Elsevier BV
Date: 08-2015
Publisher: Elsevier BV
Date: 06-2016
Location: United Kingdom of Great Britain and Northern Ireland
No related grants have been discovered for Paul Bagot.