Understanding atom probe’s analytical performance for iron oxides using correlation histograms and ab initio calculations
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 (10 ^10 Vm ^−1 ), makes them prone to dissociation with or without an exchange of...
| Main Authors: | , , , , , , |
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| Format: | Article |
| Language: | English |
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IOP Publishing
2024-01-01
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| Series: | New Journal of Physics |
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| Online Access: | https://doi.org/10.1088/1367-2630/ad309e |
| _version_ | 1797261514431791104 |
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| author | Se-Ho Kim Shalini Bhatt Daniel K Schreiber Jörg Neugebauer Christoph Freysoldt Baptiste Gault Shyam Katnagallu |
| author_facet | Se-Ho Kim Shalini Bhatt Daniel K Schreiber Jörg Neugebauer Christoph Freysoldt Baptiste Gault Shyam Katnagallu |
| author_sort | Se-Ho Kim |
| collection | DOAJ |
| description | 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 (10 ^10 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 molecules 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, Fe _2 O _3 and Fe _3 O _4 across a wide range of analysis conditions. Possible dissociation reactions are predicted by density-functional theory 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 analyzed to reflect upon the influence of these neutrals from dissociation reactions on the performance of APT for analysing iron oxides. |
| first_indexed | 2024-04-24T23:42:26Z |
| format | Article |
| id | doaj.art-8b5bb22074f34a0a80823e64b71edfb8 |
| institution | Directory Open Access Journal |
| issn | 1367-2630 |
| language | English |
| last_indexed | 2024-04-24T23:42:26Z |
| publishDate | 2024-01-01 |
| publisher | IOP Publishing |
| record_format | Article |
| series | New Journal of Physics |
| spelling | doaj.art-8b5bb22074f34a0a80823e64b71edfb82024-03-15T10:35:18ZengIOP PublishingNew Journal of Physics1367-26302024-01-0126303302110.1088/1367-2630/ad309eUnderstanding atom probe’s analytical performance for iron oxides using correlation histograms and ab initio calculationsSe-Ho Kim0https://orcid.org/0000-0003-1227-8897Shalini Bhatt1https://orcid.org/0000-0002-7156-7376Daniel K Schreiber2Jörg Neugebauer3https://orcid.org/0000-0002-7903-2472Christoph Freysoldt4https://orcid.org/0000-0002-7896-3478Baptiste Gault5https://orcid.org/0000-0002-4934-0458Shyam Katnagallu6https://orcid.org/0000-0002-6812-2309Max-Planck-Institut für Eisenforschung , Max-Planck-Straße 1, 40237 Düsseldorf, Germany; Materials Science and Engineering, Korea University , Seoul 02841, Republic of KoreaMax-Planck-Institut für Eisenforschung , Max-Planck-Straße 1, 40237 Düsseldorf, GermanyEnergy and Environment Directorate, Pacific Northwest National Laboratory , Richland, WA 99352, United States of AmericaMax-Planck-Institut für Eisenforschung , Max-Planck-Straße 1, 40237 Düsseldorf, GermanyMax-Planck-Institut für Eisenforschung , Max-Planck-Straße 1, 40237 Düsseldorf, GermanyMax-Planck-Institut für Eisenforschung , Max-Planck-Straße 1, 40237 Düsseldorf, Germany; Department of Materials, Imperial College London, Royal School of Mines , Exhibition Road, London SW7 2AZ, United KingdomMax-Planck-Institut für Eisenforschung , Max-Planck-Straße 1, 40237 Düsseldorf, GermanyField 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 (10 ^10 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 molecules 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, Fe _2 O _3 and Fe _3 O _4 across a wide range of analysis conditions. Possible dissociation reactions are predicted by density-functional theory 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 analyzed to reflect upon the influence of these neutrals from dissociation reactions on the performance of APT for analysing iron oxides.https://doi.org/10.1088/1367-2630/ad309eoxidesatom probecorrelation histogrammolecular dissociationdensity functional theory |
| spellingShingle | Se-Ho Kim Shalini Bhatt Daniel K Schreiber Jörg Neugebauer Christoph Freysoldt Baptiste Gault Shyam Katnagallu Understanding atom probe’s analytical performance for iron oxides using correlation histograms and ab initio calculations New Journal of Physics oxides atom probe correlation histogram molecular dissociation density functional theory |
| title | Understanding atom probe’s analytical performance for iron oxides using correlation histograms and ab initio calculations |
| title_full | Understanding atom probe’s analytical performance for iron oxides using correlation histograms and ab initio calculations |
| title_fullStr | Understanding atom probe’s analytical performance for iron oxides using correlation histograms and ab initio calculations |
| title_full_unstemmed | Understanding atom probe’s analytical performance for iron oxides using correlation histograms and ab initio calculations |
| title_short | Understanding atom probe’s analytical performance for iron oxides using correlation histograms and ab initio calculations |
| title_sort | understanding atom probe s analytical performance for iron oxides using correlation histograms and ab initio calculations |
| topic | oxides atom probe correlation histogram molecular dissociation density functional theory |
| url | https://doi.org/10.1088/1367-2630/ad309e |
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