Experimental TDPAC and Theoretical DFT Study of Structural, Electronic, and Hyperfine Properties in (111In → )111Cd-Doped SnO2 Semiconductor: Ab Initio Modeling of the Electron-Capture-Decay After-Effects Phenomenon
| Autor: | Artur W. Carbonari, G. N. Darriba, Mario Rentería, E. L. Muñoz |
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| Rok vydání: | 2018 |
| Předmět: |
Materials science
Electron capture Hyperfine Interactions Ciencias Físicas Ab initio 02 engineering and technology DFT 01 natural sciences Molecular physics Computer Science::Emerging Technologies Impurity 0103 physical sciences 111In Electron-capture Decay Physics::Atomic Physics Physical and Theoretical Chemistry Thin film Hyperfine structure 111Cd 010302 applied physics Condensed Matter - Materials Science business.industry Doping Semiconductor 021001 nanoscience & nanotechnology Surfaces Coatings and Films Electronic Optical and Magnetic Materials Tin oxide General Energy Ab Initio Electronic Structure TDPAC After-Effects Quadrupole 0210 nano-technology business SnO2 CIENCIAS NATURALES Y EXACTAS Física de los Materiales Condensados |
| Zdroj: | The Journal of Physical Chemistry C. 122:17423-17436 |
| ISSN: | 1932-7455 1932-7447 |
| DOI: | 10.1021/acs.jpcc.8b03724 |
| Popis: | In this paper we investigate the effect of Cd doping at ultra-low concentrations in SnO$_2$ both experimentally, by measuring the temperature dependence of the electric quadrupole hyperfine interactions with time-differential perturbed angular correlation (TDPAC) spectroscopy using $^{111}$Cd as probe nuclei, and theoretically, by performing first-principles calculations based on the density functional theory. TDPAC spectra were successfully analyzed with a time-dependent on-off model for the perturbation factor. These results show combined dynamic plus static interactions whose electric-field gradients were associated in this model to different stable electronic configurations close to the Cd atoms. The dynamic regime is then originated in fast fluctuations between these different electronic configurations. First-principles calculations results show that the Cd impurity introduces a double acceptor level in the top of the valence band of the doped semiconductor and produces isotropic outward relaxations of the nearest oxygen neighbors. The variation of the calculated electric-field gradient tensor as a function of the charge state of the Cd impurity level shows an interesting behavior that explains the experimental results, giving strong support from first-principles to the electron-capture after-effects proposed scenario. The electron-capture decay of the parent $^{111}$In to $^{111}$Cd as well as the double acceptor character of the $^{111}$Cd impurity and the electric nature of the host are shown to contribute to the existence of these type of time-dependent hyperfine interactions. Comment: 35 pages, 2 Tables and 9 Figures |
| Databáze: | OpenAIRE |
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