Journal
SCIENTIFIC REPORTS
Volume 7, Issue -, Pages -Publisher
NATURE PUBLISHING GROUP
DOI: 10.1038/s41598-017-08275-5
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Funding
- ISOLDE collaboration
- European Union Seventh Framework through ENSAR [262010]
- European Union Seventh Framework Programme [310339]
- Fund for Scientific Research-Flanders
- KU Leuven BOF [SF/14/013, CREA/14/13, STRT/14/002]
- South African National Research Foundation
- Department of Science and Technology
- Icelandic Research Fund [110017021-23]
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The underlying mechanism driving the structural amorphous-to-crystalline transition in Group VI chalcogenides is still a matter of debate even in the simplest GeTe system. We exploit the extreme sensitivity of Fe-57 emission Mssbauer spectroscopy, following dilute implantation of Mn-57 (T1/2 = 1.5 min) at ISOLDE/CERN, to study the electronic charge distribution in the immediate vicinity of the Fe-57 probe substituting Ge (Fe-Ge), and to interrogate the local environment of Fe-Ge over the amorphous-crystalline phase transition in GeTe thin films. Our results show that the local structure of as-sputtered amorphous GeTe is a combination of tetrahedral and defect-octahedral sites. The main effect of the crystallization is the conversion from tetrahedral to defect-free octahedral sites. We discover that only the tetrahedral fraction in amorphous GeTe participates to the change of the Fe-Ge-Te chemical bonds, with a net electronic charge density transfer of similar to 1.6 e/a(0) between Fe-Ge and neighboring Te atoms. This charge transfer accounts for a lowering of the covalent character during crystallization. The results are corroborated by theoretical calculations within the framework of density functional theory. The observed atomic-scale chemical-structural changes are directly connected to the macroscopic phase transition and resistivity switch of GeTe thin films.
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