Atom Probe Tomography Investigation of Clustering in Model P2O5-Doped Borosilicate Glasses for Nuclear Waste Vitrification.

Atom probe tomography (APT) has been utilized to investigate the microstructure of two model borosilicate glasses designed to understand the solubility limits of phosphorous pentoxide (P2O5). This component is found in certain high-level radioactive defence wastes destined for vitrification, where phase separation can potentially lead to a number of issues relating to the processing of the glass and its long-term chemical and structural stability. The development of suitable focused ion beam (FIB)-preparation routes and APT analysis conditions were initially determined for the model glasses, before examining their detailed microstructures. In a 3.0 mol% P2O5-doped glass, both visual inspection and sensitive statistical analysis of the APT data show homogeneous microstructures, while raising the content to 4.0 mol% initiates the formation of phosphorus-enriched nanoscale precipitates. This study confirms the expected inhomogeneities and phase separation of these glasses and offers routes to characterizing these at near-atomic scale resolution using APT.

Multivariate analysis of FcR-mediated NK cell functions identifies unique clustering among humans and rhesus macaques.

Rhesus macaques (RMs) are a common pre-clinical model used to test HIV vaccine efficacy and passive immunization strategies. Yet, it remains unclear to what extent the Fc-Fc receptor (FcR) interactions impacting antiviral activities of antibodies in RMs recapitulate those in humans. Here, we evaluated the FcR-related functionality of natural killer cells (NKs) from peripheral blood of uninfected humans and RMs to identify intra- and inter-species variation. NKs were screened for FcγRIIIa (human) and FcγRIII (RM) genotypes (FcγRIII(a)), receptor signaling, and antibody-dependent cellular cytotoxicity (ADCC), the latter mediated by a cocktail of monoclonal IgG1 antibodies with human or RM Fc. FcγRIII(a) genetic polymorphisms alone did not explain differences in NK effector functionality in either species cohort. Using the same parameters, hierarchical clustering separated each species into two clusters. Importantly, in principal components analyses, ADCC magnitude, NK contribution to ADCC, FcγRIII(a) cell-surface expression, and frequency of phosphorylated CD3ζ NK cells all contributed similarly to the first principal component within each species, demonstrating the importance of measuring multiple facets of NK cell function. Although ADCC potency was similar between species, we detected significant differences in frequencies of NK cells and pCD3ζ+ cells, level of cell-surface FcγRIII(a) expression, and NK-mediated ADCC (P<0.001), indicating that a combination of Fc-FcR parameters contribute to overall inter-species functional differences. These data strongly support the importance of multi-parameter analyses of Fc-FcR NK-mediated functions when evaluating efficacy of passive and active immunizations in pre- and clinical trials and identifying correlates of protection. The results also suggest that pre-screening animals for multiple FcR-mediated NK function would ensure even distribution of animals among treatment groups in future preclinical trials.

van der Waals Epitaxy, Superlubricity, and Polarization of the 2D Ferroelectric SnS.

Tin monosulfide (SnS) is a two-dimensional layered semiconductor that exhibits in-plane ferroelectric order at very small thicknesses and is of interest in highly scaled devices. Here we report the epitaxial growth of SnS on hexagonal boron nitride (hBN) using a pulsed metal-organic chemical vapor deposition process. Lattice matching is observed between the SnS(100) and hBN{11̅0} planes, with no evidence of strain. Atomic force microscopy reveals superlubricity along the commensurate direction of the SnS/hBN interface, and first-principles calculations suggest that friction is controlled by the edges of the SnS islands, rather than interface interactions. Differential phase contrast imaging detects remnant polarization in SnS islands with domains that are not dictated by step-edges in the SnS. The growth of ferroelectric SnS on high quality hBN substrates is a promising step toward electrically switchable ferroelectric semiconducting devices.

Large-Scale Atom Probe Tomography Data Mining: Methods and Application to Inform Hydrogen Behavior.

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 sample materials. The behavior of contaminant hydrogen is analyzed and correlated with voltage, electric field, and sample 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.

Understanding photochemical pathways of laser-induced metal ion reduction through byproduct analysis.

Laser-induced reduction of metal ions is attracting increasing attention as a sustainable route to ligand-free metal nanoparticles. In this work, we investigate the photochemical reactions involved in reduction of Ag+ and [AuCl4]- upon interaction with lasers with nanosecond and femtosecond pulse duration, using strong-field ionization mass spectrometry and spectroscopic assays to identify stable molecular byproducts. Whereas Ag+ in aqueous isopropyl alcohol (IPA) is reduced through plasma-mediated mechanisms upon femtosecond laser excitation, low-fluence nanosecond laser excitation induces electron transfer from IPA to Ag+. Both nanosecond and femtosecond laser excitation of aqueous [AuCl4]- produce reactive chlorine species by Au-Cl bond homolysis. Formation of numerous volatile products by IPA decomposition during both femtosecond and nanosecond laser excitation of [AuCl4]- is attributed to enhanced optical breakdown by the Au nanoparticle products of [AuCl4]- reduction. These mechanistic insights can inform the design of laser synthesis procedures to improve control over metal nanoparticle properties and enhance byproduct yields.

Chromosome-level genome and high nitrogen stress response of the widespread and ecologically important wetland plant Typha angustifolia.

Typha angustifolia L., known as narrowleaf cattail, is widely distributed in Eurasia but has been introduced to North America. Typha angustifolia is a semi-aquatic, wetland obligate plant that is widely distributed in Eurasia and North America. It is ecologically important for nutrient cycling in wetlands where it occurs and is used in phytoremediation and traditional medicine. In order to construct a high-quality genome for Typha angustifolia and investigate genes in response to high nitrogen stress, we carried out complete genome sequencing and high-nitrogen-stress experiments. We generated a chromosomal-level genome of T. angustifolia, which had 15 pseudochromosomes, a size of 207 Mb, and a contig N50 length of 13.57 Mb. Genome duplication analyses detected no recent whole-genome duplication (WGD) event for T. angustifolia. An analysis of gene family expansion and contraction showed that T. angustifolia gained 1,310 genes and lost 1,426 genes. High-nitrogen-stress experiments showed that a high nitrogen level had a significant inhibitory effect on root growth and differential gene expression analyses using 24 samples found 128 differentially expressed genes (DEGs) between the nitrogen-treated and control groups. DEGs in the roots and leaves were enriched in alanines, aspartate, and glutamate metabolism, nitrogen metabolism, photosynthesis, phenylpropanoid biosynthesis, plant-pathogen interaction, and mitogen-activated protein kinase pathways, among others. This study provides genomic data for a medicinal and ecologically important herb and lays a theoretical foundation for plant-assisted water pollution remediation.

Edge and Interface Resistances Create Distinct Trade-Offs When Optimizing the Microstructure of Printed van der Waals Thin-Film Transistors.

Inks based on two-dimensional (2D) materials could be used to tune the properties of printed electronics while maintaining compatibility with scalable manufacturing processes. However, a very wide range of performances have been reported in printed thin-film transistors in which the 2D channel material exhibits considerable variation in microstructure. The lack of quantitative physics-based relationships between film microstructure and transistor performance limits the codesign of exfoliation, sorting, and printing processes to inefficient empirical approaches. To rationally guide the development of 2D inks and related processing, we report a gate-dependent resistor network model that establishes distinct microstructure-performance relationships created by near-edge and intersheet resistances in printed van der Waals thin-film transistors. The model is calibrated by analyzing electrical output characteristics of model transistors consisting of overlapping 2D nanosheets with varied thicknesses that are mechanically exfoliated and transferred. Kelvin probe force microscopy analysis on the model transistors leads to the discovery that the nanosheet edges, not the intersheet resistance, limit transport due to their impact on charge carrier depletion and scattering. Our model suggests that when transport in a 2D material network is limited by the near-edge resistance, the optimum nanosheet thickness is dictated by a trade-off between charged impurity screening and gate screening, and the film mobilities are more sensitive to variations in printed nanosheet density. Removal of edge states can enable the realization of higher mobilities with thinner nanosheets due to reduced junction resistances and reduced gate screening. Our analysis of the influence of nanosheet edges on the effective film mobility not only examines the prospects of extant exfoliation methods to achieve the optimum microstructure but also provides important perspectives on processes that are essential to maximizing printed film performance.

Defining genetic diversity of rhesus macaque Fcγ receptors with long-read RNA sequencing.

Fcγ receptors (FcγRs) are membrane-bound glycoproteins that bind to the fragment crystallizable (Fc) constant regions of IgG antibodies. Interactions between IgG immune complexes and FcγRs can initiate signal transduction that mediates important components of the immune response including activation of immune cells for clearance of opsonized pathogens or infected host cells. In humans, many studies have identified associations between FcγR gene polymorphisms and risk of infection, or progression of disease, suggesting a gene-level impact on FcγR-dependent immune responses. Rhesus macaques are an important translational model for most human health interventions, yet little is known about the breadth of rhesus macaque FcγR genetic diversity. This lack of knowledge prevents evaluation of the impact of FcγR polymorphisms on outcomes of preclinical studies performed in rhesus macaques. In this study we used long-read RNA sequencing to define the genetic diversity of FcγRs in 206 Indian-origin Rhesus macaques, Macaca mulatta. We describe the frequency of single nucleotide polymorphisms, insertions, deletions, frame-shift mutations, and isoforms. We also index the identified diversity using predicted and known rhesus macaque FcγR and Fc-FcγR structures. Future studies that define the functional significance of this genetic diversity will facilitate a better understanding of the correlation between human and macaque FcγR biology that is needed for effective translation of studies with antibody-mediated outcomes performed in rhesus macaques.

A Correlative Study of Interfacial Segregation in a Cu-Doped TiNiSn Thermoelectric half-Heusler Alloy.

The performance of thermoelectric materials depends on both their atomic-scale chemistry and the nature of microstructural details such as grain boundaries and inclusions. Here, the elemental distribution throughout a TiNiCu0.1Sn thermoelectric material has been examined in a correlative study deploying atom-probe tomography (APT) and electron microscopies and spectroscopies. Elemental mapping and electron diffraction reveal two distinct types of grain boundary that are either topologically rough and meandering in profile or more regular and geometric. Transmission electron microscopy studies indicate that the Cu dopant segregates at both grain boundary types, attributed to extrusion from the bulk during hot-pressing. The geometric boundaries are found to have a degree of crystallographic coherence between neighboring grains; the rough boundaries are decorated with oxide impurity precipitates. APT was used to study the three-dimensional character of rough grain boundaries and reveals that Cu is present as discrete, elongated nanoprecipitates cosegregating alongside larger substoichiometric titanium oxide precipitates. Away from the grain boundary, the alloy microstructure is relatively homogeneous, and the atom-probe results suggest a statistical and uniform distribution of Cu with no evidence for segregation within grains. The extrusion suggests a solubility limit for Cu in the bulk material, with the potential to influence carrier and phonon transport properties across grain boundaries. These results underline the importance of fully understanding localized variations in chemistry that influence the functionality of materials, particularly at grain boundaries.

Phylogenomic Analyses of Alismatales Shed Light into Adaptations to Aquatic Environments.

Land plants first evolved from freshwater algae, and flowering plants returned to water as early as the Cretaceous and multiple times subsequently. Alismatales is the largest clade of aquatic angiosperms including all marine angiosperms, as well as terrestrial plants. We used Alismatales to explore plant adaptations to aquatic environments by analyzing a data set that included 95 samples (89 Alismatales species) covering four genomes and 91 transcriptomes (59 generated in this study). To provide a basis for investigating adaptations, we assessed phylogenetic conflict and whole-genome duplication (WGD) events in Alismatales. We recovered a relationship for the three main clades in Alismatales as (Tofieldiaceae, Araceae) + core Alismatids. We also found phylogenetic conflict among the three main clades that was best explained by incomplete lineage sorting and introgression. Overall, we identified 18 putative WGD events across Alismatales. One of them occurred at the most recent common ancestor of core Alismatids, and three occurred at seagrass lineages. We also found that lineage and life-form were both important for different evolutionary patterns for the genes related to freshwater and marine adaptation. For example, several light- or ethylene-related genes were lost in the seagrass Zosteraceae, but are present in other seagrasses and freshwater species. Stomata-related genes were lost in both submersed freshwater species and seagrasses. Nicotianamine synthase genes, which are important in iron intake, expanded in both submersed freshwater species and seagrasses. Our results advance the understanding of the adaptation to aquatic environments and WGDs using phylogenomics.

Landscape Genomics Provides Evidence of Ecotypic Adaptation and a Barrier to Gene Flow at Treeline for the Arctic Foundation Species Eriophorum vaginatum.

Global climate change has resulted in geographic range shifts of flora and fauna at a global scale. Extreme environments, like the Arctic, are seeing some of the most pronounced changes. This region covers 14% of the Earth's land area, and while many arctic species are widespread, understanding ecotypic variation at the genomic level will be important for elucidating how range shifts will affect ecological processes. Tussock cottongrass (Eriophorum vaginatum L.) is a foundation species of the moist acidic tundra, whose potential decline due to competition from shrubs may affect ecosystem stability in the Arctic. We used double-digest Restriction Site-Associated DNA sequencing to identify genomic variation in 273 individuals of E. vaginatum from 17 sites along a latitudinal gradient in north central Alaska. These sites have been part of 30 + years of ecological research and are inclusive of a region that was part of the Beringian refugium. The data analyses included genomic population structure, demographic models, and genotype by environment association. Genome-wide SNP investigation revealed environmentally associated variation and population structure across the sampled range of E. vaginatum, including a genetic break between populations north and south of treeline. This structure is likely the result of subrefugial isolation, contemporary isolation by resistance, and adaptation. Forty-five candidate loci were identified with genotype-environment association (GEA) analyses, with most identified genes related to abiotic stress. Our results support a hypothesis of limited gene flow based on spatial and environmental factors for E. vaginatum, which in combination with life history traits could limit range expansion of southern ecotypes northward as the tundra warms. This has implications for lower competitive attributes of northern plants of this foundation species likely resulting in changes in ecosystem productivity.

Responses of root phenology in ecotypes of Eriophorum vaginatum to transplantation and warming in the Arctic.

The effect of climate change on phenology and growth is less understood for belowground plant tissues than for aboveground plant tissues, particularly in high-latitude regions. Ecotypes within a species adapted to a locality may display different responses to climate change. We established two common garden plots in the Arctic tundra north of the Brooks Range in northern Alaska. Three ecotypes of Eriophorum vaginatum along a latitudinal gradient were transplanted into common gardens, and half of the transplants were warmed using open-top chambers (OTCs). Minirhizotrons were used to track the root phenology during the growing seasons of 2016 and 2017. Warming with OTCs (approximately +1 °C in air) did not affect the root biomass, root production or root phenology. The southern ecotype (from 67°16'N) of Eriophorum vaginatum transplanted northward experienced delayed startup and root production compared to two northern ecotypes (from 68°38'N and 69°25'N), although significant differences were not observed in the three ecotypes in terms of root production, root biomass and growth duration at the two sites. Our results suggest that as the climate warms, ecotypes of Eriophorum vaginatum may be able to adjust their duration of root growth and root productivity by phenotypic plasticity, although the degree of plasticity controlling the root startup time may vary between southern and northern ecotypes.

Origin of the enhanced Nb3Sn performance by combined Hf and Ta doping.

In recent years there has been an increasing effort in improving the performance of Nb3Sn for high-field applications, in particular for the fabrication of conductors suitable for the realization of the Future Circular Collider (FCC) at CERN. This challenging task has led to the investigation of new routes to advance the high-field pinning properties, the irreversibility and the upper critical fields (HIrr and Hc2, respectively). The effect of hafnium addition to the standard Nb-4Ta alloy has been recently demonstrated to be particularly promising and, in this paper, we investigate the origins of the observed improvements of the superconducting properties. Electron microscopy, Extended X-ray Absorption Fine Structure Spectroscopy (EXAFS) and Atom Probe Tomography (APT) characterization clearly show that, in presence of oxygen, both fine Nb3Sn grains and HfO2 nanoparticles form. Although EXAFS is unable to detect significant amounts of Hf in the A15 structure, APT does indeed reveal some residual intragrain metallic Hf. To investigate the layer properties in more detail, we created a microbridge from a thin lamella extracted by Focused Ion Beam (FIB) and measured the transport properties of Ta-Hf-doped Nb3Sn. Hc2(0) is enhanced to 30.8 T by the introduction of Hf, ~ 1 T higher than those of only Ta-doped Nb3Sn, and, even more importantly the position of the pinning force maximum exceeds 6 T, against the typical ~ 4.5-4.7 T of the only Ta-doped material. These results show that the improvements generated by Hf addition can significantly enhance the high-field performance, bringing Nb3Sn closer to the requirements necessary for FCC realization.

Atom Probe Tomography of a Cu-Doped TiNiSn Thermoelectric Material: Nanoscale Structure and Optimization of Analysis Conditions.

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.

Structural and compositional analysis of (InGa)(AsSb)/GaAs/GaP Stranski-Krastanov quantum dots.

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 sample with a very high density of ∼4 × 1011 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 ∼InxGa1 - xAs1 - ySby, 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.

Nothing in Evolution Makes Sense Except in the Light of Biology.

A key question in biology is the predictability of the evolutionary process. If we can correctly predict the outcome of evolution, we may be better equipped to anticipate and manage species' adaptation to climate change, habitat loss, invasive species, or emerging infectious diseases, as well as improve our basic understanding of the history of life on Earth. In the present article, we ask the questions when, why, and if the outcome of future evolution is predictable. We first define predictable and then discuss two conflicting views: that evolution is inherently unpredictable and that evolution is predictable given the ability to collect the right data. We identify factors that generate unpredictability, the data that might be required to make predictions at some level of precision or at a specific timescale, and the intellectual and translational value of understanding when prediction is or is not possible.

Atom probe tomography.

Atom probe tomography (APT) provides three-dimensional compositional mapping with sub-nanometre resolution. The sensitivity of APT is in the range of parts per million for all elements, including light elements such as hydrogen, carbon or lithium, enabling unique insights into the composition of performance-enhancing or lifetime-limiting microstructural features and making APT ideally suited to complement electron-based or X-ray-based microscopies and spectroscopies. Here, we provide an introductory overview of APT ranging from its inception as an evolution of field ion microscopy to the most recent developments in specimen preparation, including for nanomaterials. We touch on data reconstruction, analysis and various applications, including in the geosciences and the burgeoning biological sciences. We review the underpinnings of APT performance and discuss both strengths and limitations of APT, including how the community can improve on current shortcomings. Finally, we look forwards to true atomic-scale tomography with the ability to measure the isotopic identity and spatial coordinates of every atom in an ever wider range of materials through new specimen preparation routes, novel laser pulsing and detector technologies, and full interoperability with complementary microscopy techniques.

Ligand-Protected Ultrasmall Pd Nanoclusters Supported on Metal Oxide Surfaces for CO Oxidation: Does the Ligand Activate or Passivate the Pd Nanocatalyst?

Herein, we report on the synthesis of ultrasmall Pd nanoclusters (∼2 nm) protected by L-cysteine [HOCOCH(NH2 )CH2 SH] ligands (Pdn (L-Cys)m ) and supported on the surfaces of CeO2 , TiO2 , Fe3 O4 , and ZnO nanoparticles for CO catalytic oxidation. The Pdn (L-Cys)m nanoclusters supported on the reducible metal oxides CeO2 , TiO2 and Fe3 O4 exhibit a remarkable catalytic activity towards CO oxidation, significantly higher than the reported Pd nanoparticle catalysts. The high catalytic activity of the ligand-protected clusters Pdn (L-Cys)m is observed on the three reducible oxides where 100 % CO conversion occurs at 93-110 °C. The high activity is attributed to the ligand-protected Pd nanoclusters where the L-cysteine ligands aid in achieving monodispersity of the Pd clusters by limiting the cluster size to the active sub-2-nm region and decreasing the tendency of the clusters for agglomeration. In the case of the ceria support, a complete removal of the L-cysteine ligands results in connected agglomerated Pd clusters which are less reactive than the ligand-protected clusters. However, for the TiO2 and Fe3 O4 supports, complete removal of the ligands from the Pdn (L-Cys)m clusters leads to a slight decrease in activity where the T100% CO conversion occurs at 99 °C and 107 °C, respectively. The high porosity of the TiO2 and Fe3 O4 supports appears to aid in efficient encapsulation of the bare Pdn nanoclusters within the mesoporous pores of the support.

In situ transport measurements reveal source of mobility enhancement of MoS2 and MoTe2 during dielectric deposition.

Layered transition metal dichalcogenides (TMDs) and other two-dimensional (2D) materials are promising candidates for enhancing the capabilities of complementary metal-oxide-semiconductor (CMOS) technology. Field-effect transistors (FETs) made with 2D materials often exhibit mobilities below their theoretical limit, and strategies such as encapsulation with dielectrics grown by atomic layer deposition (ALD) have been explored to tune carrier concentration and improve mobility. While molecular adsorbates are known to dope 2D materials and influence charge scattering mechanisms, it is not well understood how ALD reactants affect 2D transistors during growth, motivating in situ or operando studies. Here, we report electrical characterization of MoS2 and MoTe2 FETs during ALD of MoOx. The field effect mobility improves significantly within the first five cycles of ALD growth using Mo(NMe2)4 as the metal-organic precursor and H2O as the oxidant. Analyses of the in situ transconductance at the growth temperature and ex situ variable temperature transconductance measurements indicate that the majority of the mobility enhancement observed at the beginning of dielectric growth is due to screening of charged impurity scattering by the adlayer. Control experiments show that exposure to only H2O or O2 induces more modest and reversible electronic changes in MoTe2 FETs, indicating that negligible oxidation of the TMD takes place during the ALD process. Due to the strong influence of the first <2 nm of deposition, when the dielectric adlayer may be discontinuous and still evolving in stoichiometry, this work highlights the need for further assessment of nucleation layers and initial deposition chemistry, which may be more important than the bulk composition of the oxide itself in optimizing performance and reproducibility.

Processing APT Spectral Backgrounds for Improved Quantification.

We describe a method to estimate background noise in atom probe tomography (APT) mass spectra and to use this information to enhance both background correction and quantification. Our approach is mathematically general in form for any detector exhibiting Poisson noise with a fixed data acquisition time window, at voltages varying through the experiment. We show that this accurately estimates the background observed in real experiments. The method requires, as a minimum, the z-coordinate and mass-to-charge-state data as input and can be applied retrospectively. Further improvements are obtained with additional information such as acquisition voltage. Using this method allows for improved estimation of variance in the background, and more robust quantification, with quantified count limits at parts-per-million concentrations. To demonstrate applications, we show a simple peak detection implementation, which quantitatively suppresses false positives arising from random noise sources. We additionally quantify the detectability of 121-Sb in a standardized-doped Si microtip as (1.5 × 10−5, 3.8 × 10−5) atomic fraction, α = 0.95. This technique is applicable to all modes of APT data acquisition and is highly general in nature, ultimately allowing for improvements in analyzing low ionic count species in datasets.