Correlating laser energy with compositional and atomic-level information of oxides in atom probe tomography

Hunnestad, K. A.; Hatzoglou, Constantinos; Vurpillot, F.; Nylund, Inger‐Emma; Yan, Z.; Bourret, Edith; Helvoort, Antonius T. J. van; Meier, Dennis

doi:10.1016/j.matchar.2023.113085

Cited by 3 publications

(4 citation statements)

References 57 publications

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“…This gives us more confidence to associate the third phase to partially reduced wüstite. Similar trends were observed when plotting the O + /O 2 + CSR against O level in figure 5(b) [46,47]. A comprehensive investigation of the various measurement parameters with theoretical dissociation reactions is imperative to guarantee measurement precision in APT analyses of oxide materials.…”

Section: Application To the Analysis Of Direct Reduction Of Iron Oxidessupporting

confidence: 70%

Understanding atom probe’s analytical performance for iron oxides using correlation histograms and ab initio calculations

Kim,

Bhatt,

Schreiber

et al. 2024

New J. Phys.

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Field evaporation from ionic or covalently bonded materials often leads to the emission of molecular ions. The metastability of these molecular ions, particularly under the influence of the intense electrostatic field (1010 Vm-1), makes them prone to dissociation with or without an exchange of energy amongst them. These processes can affect the analytical performance of atom probe tomography (APT). For instance, neutral species formed through dissociation may not be detected at all or with a time of flight no longer related to their mass, causing their loss from the analysis. Here, we evaluated the changes in the measured composition of FeO, Fe2O3 and Fe3O4 across a wide range of analysis conditions. Possible dissociation reactions are predicted by density-functional theory (DFT) calculations considering the spin states of the molecules. The energetically favoured reactions are traced on to the multi-hit ion correlation histograms, to confirm their existence within experiments, using an automated Python-based routine. The detected reactions are carefully analysed to reflect upon the influence of these neutrals from dissociation reactions on the performance of APT for analysing iron oxides.

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Section: Application To the Analysis Of Direct Reduction Of Iron Oxidessupporting

confidence: 70%

Understanding atom probe’s analytical performance for iron oxides using correlation histograms and ab initio calculations

Kim,

Bhatt,

Schreiber

et al. 2024

New J. Phys.

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“…In contrast, the measured concentration of O is lower than expected, indicating an accumulation of oxygen vacancies, V O . A small shift in the O profile relative to Fe and Lu is observed, which we attributed to field evaporation effects 27 (see also Fig. S3 ).…”

Section: Resultsmentioning

confidence: 66%

“…The image compression factor and field reduction factor were adjusted to make the thin film flat relative to the substrate. We note that the average oxygen concentration is lower than the nominal, which is common in APT, resulting from the detection loss of neutral O 2 molecules 27 , 30 . The charge-state-ratio (CSR) measured across the superlattice is presented in Fig.…”

Section: Methodsmentioning

confidence: 84%

3D oxygen vacancy distribution and defect-property relations in an oxide heterostructure

Hunnestad,

Das,

Hatzoglou

et al. 2024

Nat Commun

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Oxide heterostructures exhibit a vast variety of unique physical properties. Examples are unconventional superconductivity in layered nickelates and topological polar order in (PbTiO3)n/(SrTiO3)n superlattices. Although it is clear that variations in oxygen content are crucial for the electronic correlation phenomena in oxides, it remains a major challenge to quantify their impact. Here, we measure the chemical composition in multiferroic (LuFeO3)9/(LuFe2O4)1 superlattices, mapping correlations between the distribution of oxygen vacancies and the electric and magnetic properties. Using atom probe tomography, we observe oxygen vacancies arranging in a layered three-dimensional structure with a local density on the order of 1014 cm−2, congruent with the formula-unit-thick ferrimagnetic LuFe2O4 layers. The vacancy order is promoted by the locally reduced formation energy and plays a key role in stabilizing the ferroelectric domains and ferrimagnetism in the LuFeO3 and LuFe2O4 layers, respectively. The results demonstrate pronounced interactions between oxygen vacancies and the multiferroic order in this system and establish an approach for quantifying the oxygen defects with atomic-scale precision in 3D, giving new opportunities for deterministic defect-enabled property control in oxide heterostructures.

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“…The parameters were optimized to ensure that the interfaces appear flat and not curved. [53] The peak at 16 Da in the mass spectrum (see Figure S4, Supporting Information) could correspond to either O + or O 2 2+ . Following the discussion in refs.…”

Section: Methodsmentioning

confidence: 99%

Quantitative Mapping of Chemical Defects at Charged Grain Boundaries in a Ferroelectric Oxide

Hunnestad

Schultheiß

et al. 2023

Advanced Materials

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Polar discontinuities, as well as compositional and structural changes at oxide interfaces can give rise to a large variety of electronic and ionic phenomena. In contrast to earlier work focused on domain walls and epitaxial systems, this work investigates the relation between polar discontinuities and the local chemistry at grain boundaries in polycrystalline ferroelectric ErMnO3. Using orientation mapping and scanning probe microscopy (SPM) techniques, the polycrystalline material is demonstrated to develop charged grain boundaries with enhanced electronic conductance. By performing atom probe tomography (APT) measurements, an enrichment of erbium and a depletion of oxygen at all grain boundaries are found. The observed compositional changes translate into a charge that exceeds possible polarization‐driven effects, demonstrating that structural phenomena rather than electrostatics determine the local chemical composition and related changes in the electronic transport behavior. The study shows that the charged grain boundaries behave distinctly different from charged domain walls, giving additional opportunities for property engineering at polar oxide interfaces.

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Correlating laser energy with compositional and atomic-level information of oxides in atom probe tomography

Cited by 3 publications

References 57 publications

Understanding atom probe’s analytical performance for iron oxides using correlation histograms and ab initio calculations

Understanding atom probe’s analytical performance for iron oxides using correlation histograms and ab initio calculations

3D oxygen vacancy distribution and defect-property relations in an oxide heterostructure

Quantitative Mapping of Chemical Defects at Charged Grain Boundaries in a Ferroelectric Oxide

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