Photophysical Properties of SrTaO2N Thin Films and Influence of Anion Ordering: A Joint Theoretical and Experimental Investigation

Handle URI:
http://hdl.handle.net/10754/623889
Title:
Photophysical Properties of SrTaO2N Thin Films and Influence of Anion Ordering: A Joint Theoretical and Experimental Investigation
Authors:
Ziani, Ahmed ( 0000-0001-7059-0999 ) ; Le Paven, Claire; Le Gendre, Laurent; Marlec, Florent; Benzerga, Ratiba; Tessier, Franck; Cheviré, François; Hedhili, Mohamed N. ( 0000-0002-3624-036X ) ; Garcia-Esparza, Angel T.; Melissen, Sigismund; Sautet, Philippe; Le Bahers, Tangui; Takanabe, Kazuhiro ( 0000-0001-5374-9451 )
Abstract:
Converting photon energy into chemical energy using inorganic materials requires the successful capture of photons, exciton dissociation, and the charge carrier diffusion. This study reports a thorough analysis of the optoelectronic properties of visible-light-responsive SrTaON perovskites to quantify their absorption coefficient and the generated charge carriers' effective masses, dielectric constants, and electronic structures. The measurements on such intrinsic properties were attempted using both epitaxial and polycrystalline SrTaON films deposited by radiofrequency magnetron sputtering under N reactive plasma. Density functional theory calculations using the HSE06 functional provided reliable values of these optoelectronic properties. Such quantities obtained by both measurements and calculations gave excellent correspondence and provide possible variations that account for the small discrepancies observed. One of the significant factors determining the optical properties was found to be the anion ordering in the perovskite structure imposed by the cations. As a result, the different anion ordering has a noticeable influence on the optical properties and high sensitivity of the hole effective mass. Determination of relative band positions with respect to the water redox properties was also attempted by Mott-Schottky analysis. All these results offer the opportunity to understand why SrTaON possesses intrinsically all the ingredients needed for an efficient water splitting device.
KAUST Department:
KAUST Catalysis Center (KCC); Physical Sciences and Engineering (PSE) Division; Imaging and Characterization Core Lab
Citation:
Ziani A, Le Paven C, Le Gendre L, Marlec F, Benzerga R, et al. (2017) Photophysical Properties of SrTaO2N Thin Films and Influence of Anion Ordering: A Joint Theoretical and Experimental Investigation. Chemistry of Materials 29: 3989–3998. Available: http://dx.doi.org/10.1021/acs.chemmater.7b00414.
Publisher:
American Chemical Society (ACS)
Journal:
Chemistry of Materials
Issue Date:
10-Apr-2017
DOI:
10.1021/acs.chemmater.7b00414
Type:
Article
ISSN:
0897-4756; 1520-5002
Sponsors:
The research reported in this work was supported by the King Abdullah University of Science and Technology.
Additional Links:
http://pubs.acs.org/doi/abs/10.1021/acs.chemmater.7b00414
Appears in Collections:
Articles; Advanced Nanofabrication, Imaging and Characterization Core Lab; Physical Sciences and Engineering (PSE) Division; KAUST Catalysis Center (KCC)

Full metadata record

DC FieldValue Language
dc.contributor.authorZiani, Ahmeden
dc.contributor.authorLe Paven, Claireen
dc.contributor.authorLe Gendre, Laurenten
dc.contributor.authorMarlec, Florenten
dc.contributor.authorBenzerga, Ratibaen
dc.contributor.authorTessier, Francken
dc.contributor.authorCheviré, Françoisen
dc.contributor.authorHedhili, Mohamed N.en
dc.contributor.authorGarcia-Esparza, Angel T.en
dc.contributor.authorMelissen, Sigismunden
dc.contributor.authorSautet, Philippeen
dc.contributor.authorLe Bahers, Tanguien
dc.contributor.authorTakanabe, Kazuhiroen
dc.date.accessioned2017-05-31T11:23:12Z-
dc.date.available2017-05-31T11:23:12Z-
dc.date.issued2017-04-10en
dc.identifier.citationZiani A, Le Paven C, Le Gendre L, Marlec F, Benzerga R, et al. (2017) Photophysical Properties of SrTaO2N Thin Films and Influence of Anion Ordering: A Joint Theoretical and Experimental Investigation. Chemistry of Materials 29: 3989–3998. Available: http://dx.doi.org/10.1021/acs.chemmater.7b00414.en
dc.identifier.issn0897-4756en
dc.identifier.issn1520-5002en
dc.identifier.doi10.1021/acs.chemmater.7b00414en
dc.identifier.urihttp://hdl.handle.net/10754/623889-
dc.description.abstractConverting photon energy into chemical energy using inorganic materials requires the successful capture of photons, exciton dissociation, and the charge carrier diffusion. This study reports a thorough analysis of the optoelectronic properties of visible-light-responsive SrTaON perovskites to quantify their absorption coefficient and the generated charge carriers' effective masses, dielectric constants, and electronic structures. The measurements on such intrinsic properties were attempted using both epitaxial and polycrystalline SrTaON films deposited by radiofrequency magnetron sputtering under N reactive plasma. Density functional theory calculations using the HSE06 functional provided reliable values of these optoelectronic properties. Such quantities obtained by both measurements and calculations gave excellent correspondence and provide possible variations that account for the small discrepancies observed. One of the significant factors determining the optical properties was found to be the anion ordering in the perovskite structure imposed by the cations. As a result, the different anion ordering has a noticeable influence on the optical properties and high sensitivity of the hole effective mass. Determination of relative band positions with respect to the water redox properties was also attempted by Mott-Schottky analysis. All these results offer the opportunity to understand why SrTaON possesses intrinsically all the ingredients needed for an efficient water splitting device.en
dc.description.sponsorshipThe research reported in this work was supported by the King Abdullah University of Science and Technology.en
dc.publisherAmerican Chemical Society (ACS)en
dc.relation.urlhttp://pubs.acs.org/doi/abs/10.1021/acs.chemmater.7b00414en
dc.titlePhotophysical Properties of SrTaO2N Thin Films and Influence of Anion Ordering: A Joint Theoretical and Experimental Investigationen
dc.typeArticleen
dc.contributor.departmentKAUST Catalysis Center (KCC)en
dc.contributor.departmentPhysical Sciences and Engineering (PSE) Divisionen
dc.contributor.departmentImaging and Characterization Core Laben
dc.identifier.journalChemistry of Materialsen
dc.contributor.institutionInstitut d'Electronique et de Télécommunications de Rennes (IETR), Equipe FunMAT, IUT Saint-Brieuc, Université de Rennes 1, Saint Brieuc, 22000, , , Franceen
dc.contributor.institutionInstitut des Sciences Chimiques de Rennes (ISCR), Equipe Verres et Céramiques, Université de Rennes 1, Rennes Cedex, 35042, , , Franceen
dc.contributor.institutionUniv Lyon, ENS de Lyon, CNRS, Université Claude Bernard Lyon 1, Laboratoire de Chimie UMR 5182, Lyon, F-69342, , , , , , Franceen
dc.contributor.institutionDepartment of Chemical and Biomolecular Engineering, University of California Los Angeles (UCLA), Los Angeles, CA, 90095, , United Statesen
kaust.authorZiani, Ahmeden
kaust.authorHedhili, Mohamed N.en
kaust.authorTakanabe, Kazuhiroen
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