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Doctoral Thesis
DOI
https://doi.org/10.11606/T.43.2004.tde-21122005-113934
Document
Author
Full name
John Carlos Mantilla Ochoa
E-mail
Institute/School/College
Knowledge Area
Date of Defense
Published
São Paulo, 2004
Supervisor
Committee
Bindilatti, Valdir (President)
Goya, Gerardo Fabian
Hamada, Margarida Mizue
Oliveira, Adilson Jesus Aparecido de
Ueta, Antonio Yukio
Title in Portuguese
ESTUDO DAS PROPRIEDADES ESTRUTURAIS E MAGNÉTICAS DO SISTEMA Zn1-xMnxIn2Se4
Keywords in Portuguese
Crescimento de cristais
Cristalografia estrutural
Propriedades magneticas
Abstract in Portuguese
Neste trabalho de tese é apresentado um estudo sistemático do crescimento e das propriedades magnéticas e estruturais dos compostos semicondutores magnéticos diluídos (SMD) Zn1-xMnxIn2Se4. Amostras monocristalinas com concentrações de Mn $0leqslant xleqslant 1.00$ foram obtidas pela técnica de transporte químico em fase vapor (CVT). Através de técnicas de difração de raios-X (padrões de pó e diagramas de Laue), estudou-se a evolução da estrutura desde a fase romboédrica do MnIn2Se4, até a fase tetraédrica do ZnIn2Se4. Observou-se a existência de uma fase pura romboédrica para $xgeqslant 0.87$, uma fase pura tetragonal para$xleqslant 0.25$ e uma mistura destas duas fases para x entre 0.67 e 0.35. Espectros de ressonância paramagnética eletrônica (EPR) foram obtidos em temperaturas T desde 4 K até 300 K, para diversas concentrações de Mn. Todos os espectros têm o pico de absorção principal centrado em g=2. A largura pico a pico da linha de ressonância, $deltaHpp$, decresce com o aumento da concentração de manganês e com o aumento da temperatura. Este comportamento está intimamente relacionado com a interação de troca entre os íons magnéticos. A partir de análises da dependência de $deltaHpp$ com a temperatura se extraíram estimativas para a temperatura de Curie-Weiss, $ heta$ e para a temperatura de congelamento Tf das fases de vidro de spin. Medidas da susceptibilidade magnética em modo DC foram realizadas para temperaturas $2Kleqslant Tleqslant 300K$. Dos dados de alta temperatura (T>100 K), resultaram estimativas para o parâmetro $ heta$, bem como para a concentração x de Mn. Os valores de $ heta$ obtidos destas medidas concordam bem com os obtidos de EPR e foram utilizados para estimar as constantes de troca antiferromagnéticas nos dois extremos de concentração da série. Nas amostras com alta concentração de Mn, $xgeqslant 0.67$, irreversibilidades características de uma transição para uma fase de vidro de spin foram observadas em temperaturas abaixo de 4K. Para melhor caracterizar estas transições, medidas da susceptibilidade AC e DC para diversas freqüências e campos magnéticos foram realizadas em temperaturas entre 2 e 20 K. A susceptibilidade DC em baixos campos mostra picos agudos em Tf ~ 2.5, 3.0 e 3.5 K, respectivamente para as amostras com x=0,67; 0,87 e 1,00. Nas três amostras, observa-se irreversibilidade entre medidas com esfriamento na ausência de campo (ZFC) e em presença de campo (FC). Evidência de um verdadeiro fenômeno de transição de fase é fornecida pelo crescimento da susceptibilidade não linear, $chiNL$, próximo de Tf.. Análises de escala estáticas de $chiNL$ e análises de escala dinâmicas desenvolvidas a partir de dados da susceptibilidade AC resultaram em expoentes críticos consistentes com os obtidos em outros vidros de spin com interação de curto alcance.
Title in English
STUDY OF THE STRUCTURAL AND MAGNETIC PROPERTIES OF Zn1-xMnxIn2Se4 SYSTEM
Keywords in English
Crystal growth
Magnetic properties
Structural Cristallographic
Abstract in English
This work reports a systematic study on the crystal growth and magnetic and structural properties of the diluted magnetic semiconductors (SMD) Zn1-xMnxIn2Se4. Crystals with Mn concentrations $0leqslant xleqslant 1.00$ were grown by chemical vapour transport (CVT). Through x-ray powder diffraction patterns and Laue diagrams of single crystal we studied the transformation from the layered rhombohedral structure of MnIn2Se4 to the tetragonal structure of ZnIn2Se4. We observe the presence of a purely rhombohedral phase for $xgeqslant 0.87$, a purely tetragonal phase for $xleqslant 0.25$ and a two-phase mixture for x between 0.67 and 0.35. Electron Paramagnetic Resonance (EPR) spectroscopy has been performed in the temperature range 4.2 K to 300 K for various concentrations of Mn. All the spectra had the main absorption peak centered at g=2. The resonance peak-to-peak line width, ÄHpp, decreases with increasing concentration of manganese and with increasing temperature. This behavior is intimately related with the exchange interaction between magnetic ions. The analysis of the temperature dependence of ÄHpp resulted in estimates for the Curie-Weiss temperature $ heta$ and for the freezing temperature Tf of the spin glass phase. The DC magnetic susceptibility has been investigated in the range between $2Kleqslant Tleqslant 300K$. The high temperature data (T>100 K) gave estimates for the parameter $ heta$, as well as for the concentration x of Mn. The values of $ heta$ obtained in this way are in good agreement with those obtained from EPR and were used to estimate the antiferromagnetic exchange constants for the two extremes of concentration of the system. For the samples with high concentration of Mn, $xgeqslant 0.67$, irreversibilities characteristic of a spin glass transition have been observed at temperatures below 4K. To better characterize this transition, AC and DC susceptibility measurements for different frequencies and magnetic fields were made in the temperature range between 2 and 20 K. The low field AC susceptibility displayed sharp peaks at Tf ~2.5, 3.0 and 3.5 K for samples with x= 0.67, 0.87 and 1.00, respectively. Irreversibility between zero field cooled (ZFC) and field cooled (FC) DC measurements was observed in the three samples. Evidence of a true phase transition phenomenon is given by the steep increase of the nonlinear susceptibility $chiNL$ when approaching Tf from above. Static scaling analysis of $chiNL$ and dynamic scaling analysis of the AC susceptibility data have been carried out, which yielded critical exponents consistent with those obtained in other spin-glasses with short-range interactions.
 
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Johndoc2004.pdf (2.91 Mbytes)
Publishing Date
2006-02-20
 
WARNING: The material described below relates to works resulting from this thesis or dissertation. The contents of these works are the author's responsibility.
  • MANTILLA, J C, et al. Magnetic resonance in the Zn_{1-x}Mn_xIn_2Se_4 dilute magnetic semiconductor system [doi:10.1088/0953-8984/17/17/025]. Journal of Physics. Condensed Matter [online], 2005, vol. 17, p. 2755-2762.
  • MANTILLA, J C, et al. Dynamic susceptibility measurements at the spin-glass transition in the Zn1-xMnxIn2Se4 semiconductor [doi:10.1088/0953-8984/19/38/386225]. Journal of Physics. Condensed Matter [online], 2007, vol. 19, p. 386225.
  • MANTILLA, J C, et al. Spin glass behavior in MnIn2Se4 and Zn(1-x)MnxIn2Se4 magnetic semiconductors [doi:10.1016/j.jmmm.2003.12.1080]. Journal of Magnetism and Magnetic Materials [online], 2004, vol. 272, p. 1308-1309.
  • Mantilla, J, et al. Experimental evidence of the spin-glass transition in the diluted magnetic semiconductor Zn 1− x Mn x In 2 Se 4 [doi:10.1088/0953-8984/20/45/455211]. Journal of Physics. Condensed Matter [online], 2008, vol. 20, p. 455211.
  • MANTILLA, J. C., et al. Structure of Zn(1-x)MnxIn2Se4 crystals grown by chemical vapour transport [doi:10.1088/0953-8984/16/21/005]. Journal of Physics. Condensed Matter [online], 2004, vol. 16, p. 3255-3562.
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