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• W2315128529 abstract "We have gained insight into the internal degree of atomic disorder in isolated size-selected Fe nanoparticles (NPs) (ensuremath{sim}2--6 nm in size) supported on SiO${}_{2}$/Si(111) and Al${}_{2}$O${}_{3}$(0001) from precise measurements of the low-energy (low-$E$) part of the phonon density of states [PDOS, $g$($E$)] via ${}^{57}$Fe nuclear resonant inelastic x-ray scattering (NRIXS) combined with transmission electron microscopy (TEM) measurements. An intriguing size-dependent trend was observed, namely, an increase of the low-$E$ excess density of phonon states (as compared to the PDOS of bulk bcc Fe) with increasing NP size. This is unexpected, since usually the enhancement of the density of low-$E$ phonon modes is attributed to low-coordinated atoms at the NP surface, whose relative content increases with decreasing NP size due to the increase in the surface-to-volume ratio. Our NPs are covered by a Ti-coating layer, which essentially restores the local neighborhood of surface Fe atoms towards bulk-like coordination, reducing the surface effect. Our data can be qualitatively explained by the existence of low-coordinated Fe atoms located at grain boundaries or other defects with structural disorder in the interior of the large NPs (ensuremath{sim}3--6 nm), while our small NPs (ensuremath{sim}2 nm) are single grain and, therefore, characterized by a higher degree of structural order. This conclusion is corroborated by the observation of Debye behavior at low energy [$g$($E$) ensuremath{sim} ${E}^{n}$ with $n$ ensuremath{sim} 2] for the small NPs, but non-Debye behavior (with $n$ ensuremath{sim} 1.4) for the large NPs. The PDOS was used to determine thermodynamic properties of the Fe NPs. Finally, our results demonstrate that, in combination with TEM, NRIXS is a suitable technique to investigate atomic disorder/defects in NPs. We anticipate that our findings are universal for similar NPs with bcc structure." @default.
• W2315128529 created "2016-06-24" @default.
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• W2315128529 date "2012-10-02" @default.
• W2315128529 modified "2023-09-23" @default.
• W2315128529 title "Size-dependent evolution of the atomic vibrational density of states and thermodynamic properties of isolated Fe nanoparticles" @default.
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• W2315128529 doi "https://doi.org/10.1103/physrevb.86.165406" @default.
• W2315128529 hasPublicationYear "2012" @default.
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