arXiv subjects

Leigh T. Stephenson

Publications and source records attributed to Leigh T. Stephenson.

28 records · Page 2Linked to original sources

arXiv2020

Enabling near-atomic-scale analysis of frozen water

Transmission electron microscopy has undergone a revolution in recent years with the possibility to perform routine cryo-imaging of biological materials and (bio)chemical systems, as well as the possibility to image liquids via dedicated reaction cells or graphene-sandwiching. These approaches however typically require imaging a large number of specimens and reconstructing an average representation and often lack analytical capabilities. Here, using atom probe tomography we provide atom-by-atom analyses of frozen liquids and analytical sub-nanometre three dimensional reconstructions. The analyzed ice is in contact with, and embedded within, nanoporous gold (NPG). We report the first such data on 2-3 microns thick layers of ice formed from both high purity deuterated water and a solution of 50mM NaCl in high purity deuterated water. We present a specimen preparation strategy that uses a NPG film and, additionally, we report on an analysis of the interface between nanoporous gold and frozen salt water solution with an apparent trend in the Na and Cl concentrations across the interface. We explore a range of experimental parameters to show that the atom probe analyses of bulk aqueous specimens come with their own special challenges and discuss physical processes that may produce the observed phenomena. Our study demonstrates the viability of using frozen water as a carrier for near-atomic scale analysis of objects in solution by atom probe tomography.

cond-mat.mtrl-sci↗

arXiv2019

Imaging individual solute atoms at crystalline imperfections in metals

Directly imaging all atoms constituting a material and, maybe more importantly, crystalline defects that dictate materials' properties, remains a formidable challenge. Here, we propose a new approach to chemistry-sensitive field-ion microscopy (FIM) combining contrast interpretation from density-functional theory (DFT) and elemental identification enabled by time-of-flight mass-spectrometry and data mining. Analytical-FIM has true atomic resolution and we demonstrate how the technique can reveal the presence of individual solute atoms at specific positions in the microstructure. The performance of this new technique is showcased in revealing individual Re atoms at crystalline defects formed in Ni during creep deformation. The atomistic details offered by A-FIM allowed us to directly compare our results with simulations, and to tackle a long-standing question of how Re extends lifetime of Ni-based superalloys in service at high-temperature.

cond-mat.mtrl-sci↗

arXiv2019

Quantification challenges for atom probe tomography of hydrogen and deuterium in Zircaloy-4

Analysis and understanding of the role of hydrogen in metals is a significant challenge for the future of materials science, and this is a clear objective of recent work in the atom probe tomography (APT) community. Isotopic marking by deuteration has often been proposed as the preferred route to enable quantification of hydrogen by APT. Zircaloy-4 was charged electrochemically with hydrogen and deuterium under the same conditions to form large hydrides and deuterides. Our results from a Zr hydride and a Zr deuteride highlight challenges associated to accurate quantification of hydrogen and deuterium, in particular associated to the overlap of peaks at low mass-to-charge ratio and of hydrogen/deuterium containing molecular ions. We discuss possible ways to ensure that appropriate information is extracted from APT analysis of hydrogen in a zirconium alloy systems that is important for nuclear power.

cond-mat.mtrl-sci↗

arXiv2018

Atomic-scale investigation of hydrogen distribution in a Ti-Mo alloy

Ingress of hydrogen is often linked to catastrophic failure of Ti-alloys. Here, we quantify the hydrogen distribution in fully \b{eta} and α+\b{eta} Ti-Mo alloys by using atom probe tomography. Hydrogen does not segregate at grain boundaries in the fully \b{eta} sample but segregates at some α/\b{eta} phase boundaries with a composition exceeding 20 at.% in the α+\b{eta} sample. No stable hydrides were observed in either sample. The hydrogen concentration in \b{eta} phases linearly decreases from ~13 at. % to ~4 at. % with increasing Mo-content, which is ascribed to the suppression of hydrogen uptake by Mo addition.

cond-mat.mtrl-sci↗

arXiv2018

The Laplace project: an integrated suite for correlative atom probe tomography and electron microscopy under cryogenic and UHV conditions

We present sample transfer instrumentation and integrated protocols for the preparation and correlative characterization of environmentally-sensitive materials by both atom probe tomography and electron microscopy. Ultra-high vacuum cryogenic suitcases allow specimen transfer between preparation, processing and several imaging platforms without exposure to atmospheric contamination. For expedient transfers, we installed a fast-docking station equipped with a cryogenic pump upon three systems; two atom probes, a scanning electron microscope / Xe-plasma focused ion beam and a N$_2$-atmosphere glovebox. We also installed a plasma FIB with a solid-state cooling stage to reduce beam damage and contamination, through reducing chemical activity and with the cryogenic components as passive cryogenic traps. We demonstrate the efficacy of the new laboratory protocols by the successful preparation and transfer of two highly contamination- and temperature-sensitive samples - water and ice. Analysing pure magnesium atom probe data, we show that surface oxidation can be effectively suppressed using an entirely cryogenic protocol (during specimen preparation and during transfer). Starting with the cryogenically-cooled plasma FIB, we also prepared and transferred frozen ice samples while avoiding significant melting or sublimation, suggesting that we may be able to measure the nanostructure of other normally-liquid or soft materials. Isolated cryogenic protocols within the N$_2$ glove box demonstrate the absence of ice condensation suggesting that environmental control can commence from fabrication until atom probe analysis.

cond-mat.mtrl-sci↗

arXiv2018

Characterizing solute hydrogen and hydrides in pure and alloyed titanium at the atomic scale

Ti has a high affinity for hydrogen and is a typical hydride formers. Ti-hydride are brittle phases which probably cause premature failure of Ti-alloys. Here, we used atom probe tomography and electron microscopy to investigate the hydrogen distribution in a set of specimens of commercially pure Ti, model and commercial Ti-alloys. Although likely partly introduced during specimen preparation with the focused-ion beam, we show formation of Ti-hydrides along α grain boundaries and α/\b{eta} phase boundaries in commercial pure Ti and α+\b{eta} binary model alloys. No hydrides are observed in the α phase in alloys with Al addition or quenched-in Mo supersaturation.

cond-mat.mtrl-sci↗

arXiv2015

Estimation of the reconstruction parameters for Atom Probe Tomography

The application of wide field-of-view detection systems to atom probe experiments emphasizes the importance of careful parameter selection in the tomographic reconstruction of the analysed volume, as the sensitivity to errors rises steeply with increases in analysis dimensions. In this paper, a self-consistent method is presented for the systematic determination of the main reconstruction parameters. In the proposed approach, the compression factor and the field factor are determined using geometrical projections from the desorption images. A 3D Fourier transform is then applied to a series of reconstructions and, comparing to the known material crystallography, the efficiency of the detector is estimated. The final results demonstrate a significant improvement in the accuracy of the reconstructed volumes.

physics.ins-det↗

arXiv2015

Spatial resolution in atom probe tomography

This article addresses gaps in definitions and a lack of standard measurement techniques to assess the spatial resolution in atom probe tomography. This resolution is known to be anisotropic, being better in the depth than laterally. Generally the presence of atomic planes in the tomographic reconstruction is considered as being a sufficient proof of the quality of the spatial resolution of the instrument. Based on advanced spatial distribution maps, an analysis methodology that interrogates the local neighborhood of the atoms within the tomographic reconstruction, it is shown how both the in-depth and the lateral resolution can be quantified. The influences of the crystallography and the temperature are investigated, and models are proposed to explain the observed results. We demonstrate that the absolute value of resolution is specimenspecific.

physics.ins-det↗

arXiv2015

Dynamic reconstruction for atom probe tomography

Progress in the reconstruction for atom probe tomography has been limited since the first implementation of the protocol proposed by Bas et al. in 1995. This approach, and those subsequently developed, assume that the geometric parameters used to build the three-dimensional atom map are constant over the course of an analysis. Here, we test this assumption within the analyses of low-alloyed materials. By building upon methods recently proposed to measure the tomographic reconstruction parameters, we demonstrate that this assumption can introduce significant limitations in the accuracy of the analysis. Moreover, we propose a strategy to alleviate this problem through the implementation of a new reconstruction algorithm that dynamically accommodates variations in the tomographic reconstruction parameters.

cond-mat.mtrl-sci↗

arXiv2002

Quantum walks in higher dimensions

We analyze the quantum walk in higher spatial dimensions and compare classical and quantum spreading as a function of time. Tensor products of Hadamard transformations and the discrete Fourier transform arise as natural extensions of the quantum coin toss in the one-dimensional walk simulation, and other illustrative transformations are also investigated. We find that entanglement between the dimensions serves to reduce the rate of spread of the quantum walk. The classical limit is obtained by introducing a random phase variable.

quant-ph↗