Coloration and oxygen vacancies in wide band gap oxide semiconductors: Absorption at metallic nanoparticles induced by vacancy clustering-A case study on indium oxide

被引:26
作者
Albrecht, M. [1 ]
Schewski, R. [1 ]
Irmscher, K. [1 ]
Galazka, Z. [1 ]
Markurt, T. [1 ]
Naumann, M. [1 ]
Schulz, T. [1 ]
Uecker, R. [1 ]
Fornari, R. [1 ]
Meuret, S. [2 ]
Kociak, M. [2 ]
机构
[1] Leibniz Inst Kristallzuchtung, D-12489 Berlin, Germany
[2] Univ Paris 11, CNRS, Phys Solides Lab, F-91405 Orsay, France
关键词
SPECTRA; RESOLUTION; GROWTH; AL2O3; CR-3;
D O I
10.1063/1.4863211
中图分类号
O59 [应用物理学];
学科分类号
摘要
In this paper, we show by optical and electron microscopy based investigations that vacancies in oxides may cluster and form metallic nanoparticles that induce coloration by extinction of visible light. Optical extinction in this case is caused by generation of localized surface plasmon resonances at metallic particles embedded in the dielectric matrix. Based on Mie's approach, we are able to fit the absorption due to indium nanoparticles in In2O3 to our absorption measurements. The experimentally found particle distribution is in excellent agreement with the one obtained from fitting by Mie theory. Indium particles are formed by precipitation of oxygen vacancies. From basic thermodynamic consideration and assuming theoretically calculated activation energies for vacancy formation and migration, we find that the majority of oxygen vacancies form just below the melting point. Since they are ionized at this temperature they are Coulomb repulsive. Upon cooling, a high supersaturation of oxygen vacancies forms in the crystal that precipitates once the Fermi level crosses the transition energy level from the charged to the neutral charge state. From our considerations we find that the ionization energy of the oxygen vacancy must be higher than 200 meV. (C) 2014 AIP Publishing LLC.
引用
收藏
页数:12
相关论文
共 37 条
[1]   Ab initio modeling of diffusion in indium oxide [J].
Agoston, Peter ;
Albe, Karsten .
PHYSICAL REVIEW B, 2010, 81 (19)
[2]   Intrinsic n-Type Behavior in Transparent Conducting Oxides: A Comparative Hybrid-Functional Study of In2O3, SnO2, and ZnO [J].
Agoston, Peter ;
Albe, Karsten ;
Nieminen, Risto M. ;
Puska, Martti J. .
PHYSICAL REVIEW LETTERS, 2009, 103 (24)
[3]   Geometry, electronic structure and thermodynamic stability of intrinsic point defects in indium oxide [J].
Agoston, Peter ;
Erhart, Paul ;
Klein, Andreas ;
Albe, Karsten .
JOURNAL OF PHYSICS-CONDENSED MATTER, 2009, 21 (45)
[4]   HIGH-TEMPERATURE BEHAVIOR OF IN2O3 [J].
DEWIT, JHW .
JOURNAL OF SOLID STATE CHEMISTRY, 1975, 13 (03) :192-200
[5]   ELECTRON-CONCENTRATION AND MOBILITY IN IN2O3 [J].
DEWIT, JHW ;
VANUNEN, G ;
LAHEY, M .
JOURNAL OF PHYSICS AND CHEMISTRY OF SOLIDS, 1977, 38 (08) :819-824
[6]  
Donecker J, 2002, CRYST RES TECHNOL, V37, P147, DOI 10.1002/1521-4079(200202)37:2/3<147::AID-CRAT147>3.0.CO
[7]  
2-9
[8]   ORIGINS OF COLOURS OF YELLOW, GREEN AND BLUE SAPPHIRES [J].
FERGUSON, J ;
FIELDING, PE .
CHEMICAL PHYSICS LETTERS, 1971, 10 (03) :262-&
[9]   Indium-oxide polymorphs from first principles: Quasiparticle electronic states [J].
Fuchs, F. ;
Bechstedt, F. .
PHYSICAL REVIEW B, 2008, 77 (15)
[10]   Melt growth, characterization and properties of bulk In2O3 single crystals [J].
Galazka, Z. ;
Uecker, R. ;
Irmscher, K. ;
Schulz, D. ;
Klimm, D. ;
Albrecht, M. ;
Pietsch, M. ;
Ganschow, S. ;
Kwasniewski, A. ;
Fornari, R. .
JOURNAL OF CRYSTAL GROWTH, 2013, 362 :349-352