Modeling of Semiconductors and Correlated Oxides with Point Defects by First Principles Methods

Handle URI:
http://hdl.handle.net/10754/322206
Title:
Modeling of Semiconductors and Correlated Oxides with Point Defects by First Principles Methods
Authors:
Wang, Hao
Abstract:
Point defects in silicon, vanadium dioxide, and doped ceria are investigated by density functional theory. Defects involving vacancies and interstitial oxygen and carbon in silicon are after formed in outer space and significantly affect device performances. The screened hybrid functional by Heyd-Scuseria-Ernzerhof is used to calculate formation energies, binding energies, and electronic structures of the defective systems because standard density functional theory underestimates the bang gap of silicon. The results indicate for the A-center a −2 charge state. Tin is proposed to be an effective dopant to suppress the formation of A-centers. For the total energy difference between the A- and B-type carbon related G-centers we find close agreement with the experiment. The results indicate that the C-type G-center is more stable than both the A- and B-types. The electronic structures of the monoclinic and rutile phases of vanadium dioxide are also studied using the Heyd-Scuseria-Ernzerhof functional. The ground states of the pure phases obtained by calculations including spin polarization disagree with the experimental observations that the monoclinic phase should not be magnetic, the rutile phase should be metallic, and the monoclinic phase should have a lower total energy than the rutile phase. By tuning the Hartree-Fock fraction α to 10% the agreement with experiments is improved in terms of band gaps and relative energies of the phases. A calculation scheme is proposed to simulate the relationship between the transition temperature of the metal-insulator transition and the dopant concentration in tungsten doped vanadium dioxide. We achieve good agreement with the experimental situation. 18.75% and 25% yttrium, lanthanum, praseodymium, samarium, and gadolinium doped ceria supercells generated by the special quasirandom structure approach are employed to investigate the impact of doping on the O diffusion. The experimental behavior of the conductivity for the different dopants is understood in terms of the calculated lattice constants and the O migration barriers obtained from nudged elastic band calculations.
Advisors:
Schwingenschlögl, Udo ( 0000-0003-4179-7231 )
Committee Member:
Alshareef, Husam N.; Eppinger, Jörg ( 0000-0001-7886-7059 ) ; Grau-Crespo, Ricardo ( 0000-0001-8845-1719 ) ; Manchon, Aurelien ( 0000-0002-4768-293X )
KAUST Department:
Physical Sciences and Engineering (PSE) Division
Program:
Materials Science and Engineering
Issue Date:
15-Jun-2014
Type:
Dissertation
Appears in Collections:
Dissertations; Physical Sciences and Engineering (PSE) Division; Materials Science and Engineering Program

Full metadata record

DC FieldValue Language
dc.contributor.advisorSchwingenschlögl, Udoen
dc.contributor.authorWang, Haoen
dc.date.accessioned2014-06-24T05:31:28Z-
dc.date.available2014-06-24T05:31:28Z-
dc.date.issued2014-06-15en
dc.identifier.urihttp://hdl.handle.net/10754/322206en
dc.description.abstractPoint defects in silicon, vanadium dioxide, and doped ceria are investigated by density functional theory. Defects involving vacancies and interstitial oxygen and carbon in silicon are after formed in outer space and significantly affect device performances. The screened hybrid functional by Heyd-Scuseria-Ernzerhof is used to calculate formation energies, binding energies, and electronic structures of the defective systems because standard density functional theory underestimates the bang gap of silicon. The results indicate for the A-center a −2 charge state. Tin is proposed to be an effective dopant to suppress the formation of A-centers. For the total energy difference between the A- and B-type carbon related G-centers we find close agreement with the experiment. The results indicate that the C-type G-center is more stable than both the A- and B-types. The electronic structures of the monoclinic and rutile phases of vanadium dioxide are also studied using the Heyd-Scuseria-Ernzerhof functional. The ground states of the pure phases obtained by calculations including spin polarization disagree with the experimental observations that the monoclinic phase should not be magnetic, the rutile phase should be metallic, and the monoclinic phase should have a lower total energy than the rutile phase. By tuning the Hartree-Fock fraction α to 10% the agreement with experiments is improved in terms of band gaps and relative energies of the phases. A calculation scheme is proposed to simulate the relationship between the transition temperature of the metal-insulator transition and the dopant concentration in tungsten doped vanadium dioxide. We achieve good agreement with the experimental situation. 18.75% and 25% yttrium, lanthanum, praseodymium, samarium, and gadolinium doped ceria supercells generated by the special quasirandom structure approach are employed to investigate the impact of doping on the O diffusion. The experimental behavior of the conductivity for the different dopants is understood in terms of the calculated lattice constants and the O migration barriers obtained from nudged elastic band calculations.en
dc.language.isoenen
dc.subjectFirst Principlesen
dc.subjectPoint Defectsen
dc.subjectMaterials Modelingen
dc.subjectOxidesen
dc.subjectSemiconductorsen
dc.titleModeling of Semiconductors and Correlated Oxides with Point Defects by First Principles Methodsen
dc.typeDissertationen
dc.contributor.departmentPhysical Sciences and Engineering (PSE) Divisionen
thesis.degree.grantorKing Abdullah University of Science and Technologyen_GB
dc.contributor.committeememberAlshareef, Husam N.en
dc.contributor.committeememberEppinger, Jörgen
dc.contributor.committeememberGrau-Crespo, Ricardoen
dc.contributor.committeememberManchon, Aurelienen
thesis.degree.disciplineMaterials Science and Engineeringen
thesis.degree.nameDoctor of Philosophyen
dc.person.id101877en
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