Determination of the electronic structure and UV-Vis absorption properties of (Na2-xCux)Ta4O11 from first-principle calculations

Handle URI:
http://hdl.handle.net/10754/562920
Title:
Determination of the electronic structure and UV-Vis absorption properties of (Na2-xCux)Ta4O11 from first-principle calculations
Authors:
Harb, Moussab ( 0000-0001-5540-9792 ) ; Masih, Dilshad ( 0000-0001-5322-9771 ) ; Ould-Chikh, Samy ( 0000-0002-3486-0944 ) ; Sautet, Philippe; Basset, Jean-Marie ( 0000-0003-3166-8882 ) ; Takanabe, Kazuhiro ( 0000-0001-5374-9451 )
Abstract:
Density functional theory (DFT) and density functional perturbation theory (DFPT) were applied to study the structural, electronic, and optical properties of a (Na2-xCux)Ta4O11 solid solution to accurately calculate the band gap and to predict the optical transitions in these materials using the screened coulomb hybrid (HSE06) exchange-correlation formalism. The calculated density of states showed excellent agreement with UV-vis diffuse reflectance spectra predicting a significant red-shift of the band gap from 4.58 eV (calculated 4.94 eV) to 2.76 eV (calculated 2.60 eV) as copper content increased from 0 to 83.3%. The band gap narrowing in these materials, compared to Na2Ta4O11, results from the incorporation of new occupied electronic states, which are strongly localized on the Cu 3d orbitals, and is located within 2.16-2.34 eV just above the valence band of Na2Ta4O11. These new occupied states, however, possess an electronic character localized on Cu, which makes hole mobility limited in the semiconductor. © 2013 American Chemical Society.
KAUST Department:
KAUST Catalysis Center (KCC); Physical Sciences and Engineering (PSE) Division; Chemical Science Program; Catalysis for Energy Conversion (CatEC)
Publisher:
American Chemical Society (ACS)
Journal:
The Journal of Physical Chemistry C
Issue Date:
29-Aug-2013
DOI:
10.1021/jp405995w
Type:
Article
ISSN:
19327447
Appears in Collections:
Articles; Physical Sciences and Engineering (PSE) Division; Chemical Science Program; KAUST Catalysis Center (KCC)

Full metadata record

DC FieldValue Language
dc.contributor.authorHarb, Moussaben
dc.contributor.authorMasih, Dilshaden
dc.contributor.authorOuld-Chikh, Samyen
dc.contributor.authorSautet, Philippeen
dc.contributor.authorBasset, Jean-Marieen
dc.contributor.authorTakanabe, Kazuhiroen
dc.date.accessioned2015-08-03T11:15:31Zen
dc.date.available2015-08-03T11:15:31Zen
dc.date.issued2013-08-29en
dc.identifier.issn19327447en
dc.identifier.doi10.1021/jp405995wen
dc.identifier.urihttp://hdl.handle.net/10754/562920en
dc.description.abstractDensity functional theory (DFT) and density functional perturbation theory (DFPT) were applied to study the structural, electronic, and optical properties of a (Na2-xCux)Ta4O11 solid solution to accurately calculate the band gap and to predict the optical transitions in these materials using the screened coulomb hybrid (HSE06) exchange-correlation formalism. The calculated density of states showed excellent agreement with UV-vis diffuse reflectance spectra predicting a significant red-shift of the band gap from 4.58 eV (calculated 4.94 eV) to 2.76 eV (calculated 2.60 eV) as copper content increased from 0 to 83.3%. The band gap narrowing in these materials, compared to Na2Ta4O11, results from the incorporation of new occupied electronic states, which are strongly localized on the Cu 3d orbitals, and is located within 2.16-2.34 eV just above the valence band of Na2Ta4O11. These new occupied states, however, possess an electronic character localized on Cu, which makes hole mobility limited in the semiconductor. © 2013 American Chemical Society.en
dc.publisherAmerican Chemical Society (ACS)en
dc.titleDetermination of the electronic structure and UV-Vis absorption properties of (Na2-xCux)Ta4O11 from first-principle calculationsen
dc.typeArticleen
dc.contributor.departmentKAUST Catalysis Center (KCC)en
dc.contributor.departmentPhysical Sciences and Engineering (PSE) Divisionen
dc.contributor.departmentChemical Science Programen
dc.contributor.departmentCatalysis for Energy Conversion (CatEC)en
dc.identifier.journalThe Journal of Physical Chemistry Cen
dc.contributor.institutionUniv Lyon, CNRS, Ecole Normale Super Lyon, Lab Chim, F-69364 Lyon 07, Franceen
kaust.authorHarb, Moussaben
kaust.authorMasih, Dilshaden
kaust.authorOuld-Chikh, Samyen
kaust.authorBasset, Jean-Marieen
kaust.authorTakanabe, Kazuhiroen
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