Element-specific contributions to improved magnetic heating of theranostic CoFe2O4 nanoparticles decorated with Pd
Decoration with Pd clusters increases the magnetic heating ability of cobalt ferrite (CFO) nanoparticles by a factor of two. The origin of this previous finding is unraveled by element-specific X-ray absorption spectroscopy (XAS) and magnetic circular dichroism (XMCD) combined with atomic multiplet...
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Published in | Scientific reports Vol. 11; no. 1; p. 15843 |
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Abstract | Decoration with Pd clusters increases the magnetic heating ability of cobalt ferrite (CFO) nanoparticles by a factor of two. The origin of this previous finding is unraveled by element-specific X-ray absorption spectroscopy (XAS) and magnetic circular dichroism (XMCD) combined with atomic multiplet simulations and density functional theory (DFT) calculations. While the comparison of XAS spectra with atomic multiplet simulations show that the inversion degree is not affected by Pd decoration and, thus, can be excluded as a reason for the improved heating performance, XMCD reveals two interrelated responsible sources: significantly larger Fe and Co magnetic moments verify an increased total magnetization which enhances the magnetic heating ability. This is accompanied by a remarkable change in the field-dependent magnetization particularly for Co ions which exhibit an increased low-field susceptibility and a reduced spin canting behavior in higher magnetic fields. Using DFT calculations, these findings are explained by reduced superexchange between ions on octahedral lattice sites via oxygen in close vicinity of Pd, which reinforces the dominating antiparallel superexchange interaction between ions on octahedral and tetrahedral lattice sites and thus reduces spin canting. The influence of the delocalized nature of Pd 4d electrons on the neighboring ions is discussed and the conclusions are illustrated with spin density isosurfaces of the involved ions. The presented results pave the way to design nanohybrids with tailored electronic structure and magnetic properties. |
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AbstractList | Decoration with Pd clusters increases the magnetic heating ability of cobalt ferrite (CFO) nanoparticles by a factor of two. The origin of this previous finding is unraveled by element-specific X-ray absorption spectroscopy (XAS) and magnetic circular dichroism (XMCD) combined with atomic multiplet simulations and density functional theory (DFT) calculations. While the comparison of XAS spectra with atomic multiplet simulations show that the inversion degree is not affected by Pd decoration and, thus, can be excluded as a reason for the improved heating performance, XMCD reveals two interrelated responsible sources: significantly larger Fe and Co magnetic moments verify an increased total magnetization which enhances the magnetic heating ability. This is accompanied by a remarkable change in the field-dependent magnetization particularly for Co ions which exhibit an increased low-field susceptibility and a reduced spin canting behavior in higher magnetic fields. Using DFT calculations, these findings are explained by reduced superexchange between ions on octahedral lattice sites via oxygen in close vicinity of Pd, which reinforces the dominating antiparallel superexchange interaction between ions on octahedral and tetrahedral lattice sites and thus reduces spin canting. The influence of the delocalized nature of Pd 4d electrons on the neighboring ions is discussed and the conclusions are illustrated with spin density isosurfaces of the involved ions. The presented results pave the way to design nanohybrids with tailored electronic structure and magnetic properties. Abstract Decoration with Pd clusters increases the magnetic heating ability of cobalt ferrite (CFO) nanoparticles by a factor of two. The origin of this previous finding is unraveled by element-specific X-ray absorption spectroscopy (XAS) and magnetic circular dichroism (XMCD) combined with atomic multiplet simulations and density functional theory (DFT) calculations. While the comparison of XAS spectra with atomic multiplet simulations show that the inversion degree is not affected by Pd decoration and, thus, can be excluded as a reason for the improved heating performance, XMCD reveals two interrelated responsible sources: significantly larger Fe and Co magnetic moments verify an increased total magnetization which enhances the magnetic heating ability. This is accompanied by a remarkable change in the field-dependent magnetization particularly for Co ions which exhibit an increased low-field susceptibility and a reduced spin canting behavior in higher magnetic fields. Using DFT calculations, these findings are explained by reduced superexchange between ions on octahedral lattice sites via oxygen in close vicinity of Pd, which reinforces the dominating antiparallel superexchange interaction between ions on octahedral and tetrahedral lattice sites and thus reduces spin canting. The influence of the delocalized nature of Pd 4d electrons on the neighboring ions is discussed and the conclusions are illustrated with spin density isosurfaces of the involved ions. The presented results pave the way to design nanohybrids with tailored electronic structure and magnetic properties. Abstract Decoration with Pd clusters increases the magnetic heating ability of cobalt ferrite (CFO) nanoparticles by a factor of two. The origin of this previous finding is unraveled by element-specific X-ray absorption spectroscopy (XAS) and magnetic circular dichroism (XMCD) combined with atomic multiplet simulations and density functional theory (DFT) calculations. While the comparison of XAS spectra with atomic multiplet simulations show that the inversion degree is not affected by Pd decoration and, thus, can be excluded as a reason for the improved heating performance, XMCD reveals two interrelated responsible sources: significantly larger Fe and Co magnetic moments verify an increased total magnetization which enhances the magnetic heating ability. This is accompanied by a remarkable change in the field-dependent magnetization particularly for Co ions which exhibit an increased low-field susceptibility and a reduced spin canting behavior in higher magnetic fields. Using DFT calculations, these findings are explained by reduced superexchange between ions on octahedral lattice sites via oxygen in close vicinity of Pd, which reinforces the dominating antiparallel superexchange interaction between ions on octahedral and tetrahedral lattice sites and thus reduces spin canting. The influence of the delocalized nature of Pd 4d electrons on the neighboring ions is discussed and the conclusions are illustrated with spin density isosurfaces of the involved ions. The presented results pave the way to design nanohybrids with tailored electronic structure and magnetic properties. |
ArticleNumber | 15843 |
Author | Smekhova, Alevtina Giesen, Margret Schmitz-Antoniak, Carolin Ghazanfari, Mohammad Reza Chen, Kai Radu, Florin Shams, S. Fatemeh Schmitz, Detlef Weschke, Eugen Luo, Chen |
Author_xml | – sequence: 1 givenname: S. Fatemeh surname: Shams fullname: Shams, S. Fatemeh email: f.shams@fz-juelich.de organization: Peter-Grünberg-Institut (PGI-6), Forschungszentrum Jülich – sequence: 2 givenname: Detlef surname: Schmitz fullname: Schmitz, Detlef organization: Helmholtz-Zentrum Berlin für Materialien und Energie – sequence: 3 givenname: Alevtina surname: Smekhova fullname: Smekhova, Alevtina organization: Peter-Grünberg-Institut (PGI-6), Forschungszentrum Jülich, Helmholtz-Zentrum Berlin für Materialien und Energie – sequence: 4 givenname: Mohammad Reza surname: Ghazanfari fullname: Ghazanfari, Mohammad Reza organization: Institute of Chemistry and Biochemistry, Freie Universität Berlin – sequence: 5 givenname: Margret surname: Giesen fullname: Giesen, Margret organization: Peter-Grünberg-Institut (PGI-6), Forschungszentrum Jülich – sequence: 6 givenname: Eugen surname: Weschke fullname: Weschke, Eugen organization: Helmholtz-Zentrum Berlin für Materialien und Energie – sequence: 7 givenname: Kai surname: Chen fullname: Chen, Kai organization: Helmholtz-Zentrum Berlin für Materialien und Energie – sequence: 8 givenname: Chen surname: Luo fullname: Luo, Chen organization: Helmholtz-Zentrum Berlin für Materialien und Energie – sequence: 9 givenname: Florin surname: Radu fullname: Radu, Florin organization: Helmholtz-Zentrum Berlin für Materialien und Energie – sequence: 10 givenname: Carolin surname: Schmitz-Antoniak fullname: Schmitz-Antoniak, Carolin organization: Peter-Grünberg-Institut (PGI-6), Forschungszentrum Jülich, Technische Hochschule Wildau |
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CitedBy_id | crossref_primary_10_1016_j_jallcom_2023_171433 crossref_primary_10_1038_s41598_023_50635_x crossref_primary_10_1007_s10948_023_06577_6 crossref_primary_10_1063_5_0163166 crossref_primary_10_1007_s10854_022_08456_7 |
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Snippet | Decoration with Pd clusters increases the magnetic heating ability of cobalt ferrite (CFO) nanoparticles by a factor of two. The origin of this previous... Abstract Decoration with Pd clusters increases the magnetic heating ability of cobalt ferrite (CFO) nanoparticles by a factor of two. The origin of this... Abstract Decoration with Pd clusters increases the magnetic heating ability of cobalt ferrite (CFO) nanoparticles by a factor of two. The origin of this... |
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SubjectTerms | 639/766 639/766/119 639/766/119/997 Absorption spectroscopy Circular dichroism Cobalt Humanities and Social Sciences Ions Magnetic fields Magnetic properties multidisciplinary Nanoparticles Science Science (multidisciplinary) Spectrum analysis X-ray absorption spectroscopy |
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Title | Element-specific contributions to improved magnetic heating of theranostic CoFe2O4 nanoparticles decorated with Pd |
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