Experimental TDPAC and Theoretical DFT Study of Structural, Electronic, and Hyperfine Properties in (In-111 ->)Cd-111-Doped SnO2 Semiconductor: Ab Initio Modeling of the Electron-Capture-Decay After-Effects Phenomenon

Autor(es)

Darriba, German N. ^{[1, 2]} ; Munoz, Emiliano L. ^[3] ; Carbonari, Artur W. ^[4] ; Renteria, Mario ^{[1, 2]}

Afiliação do(s) autor(es)

^[1] Univ Nacl La Plata, Fac Ciencias Exactas, CONICET, Dept Fis, CC 67, RA-1900 La Plata, Buenos Aires - Argentina

^[2] Univ Nacl La Plata, Fac Ciencias Exactas, CONICET, IFLP, CC 67, RA-1900 La Plata, Buenos Aires - Argentina

^[3] Univ Nacl La Plata, Fac Ingn, RA-1900 La Plata, Buenos Aires - Argentina

^[4] Univ Sao Paulo, CNEN, IPEN, Sao Paulo, SP - Brazil

• Tipo de documento: Artigo Científico
• Fonte: Journal of Physical Chemistry C; v. 122, n. 30, p. 17423-17436, AUG 2 2018.
• Citações Web of Science: 3

Resumo

In this paper we investigate the effect of Cd doping at ultralow concentrations in SnO2 both experimentally, by measuring the temperature dependence of the electric quadrupole hyperfine interactions with time-differential gamma-gamma perturbed angular correlation (TDPAC) spectroscopy using Cd-111 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 calculation 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 In-111 to( 111)Cd as well as the double acceptor character of the Cd-111 impurity and the electric nature of the host are shown to contribute to the existence of these types of time-dependent hyperfine interactions. (AU)

• Processo FAPESP: 14/14001-1 - Projeto e construção de um espectrômetro digital: um equipamento mais eficiente e moderno para investigação de materiais utilizando técnica PAC
• Beneficiário: Rajendra Narain Saxena
• Modalidade de apoio: Auxílio à Pesquisa - Regular