Tuning the electronic and optical properties of complex oxide epitaxial films and superlattices for efficient visible light harvesting
EMSL Project ID
48341
Abstract
We propose an aggressive program of epitaxial film synthesis, detailed and definitive materials characterization, optical and electronic properties measurements, and carefully coordinated ab initio simulations aimed at developing new concepts and oxide materials for efficient visible solar light harvesting. Our end goal is to prepare complex oxide multilayers that would be useful for advanced solar photochemical and photovoltaic appications. We propose to test the hypothesis that the photophysical and photochemical properties of complex oxides can be tailored for efficient visible light harvesting by controlling the crystallographic positions of the cations. We will prepare three families of oxides as compositionally and structurally well-defined single-crystal epitaxial films: (i) perovskites of the form ABO3, where A is a mix of Sr and La and B is a mix of Cr and Fe, (ii) corundums of the form M2O3, where M is a mix of Fe and Cr, and, (iii) the inverse spinel CrFe2O4. We seek to answer three fundamental questions: (i) How are carrier lifetimes altered by local bonding arrangements imposed by either different crystal structures, superlattice formation or vacancy ordering? (ii) How is photoactivity affected by manipulating deposition conditions so that a reducible cation (such as Fe) is present in multiple charge states within the same lattice? (iii) Does the strain resulting from imperfect lattice matching with the substrate allow the optical properties of the film to be tuned? By strategically combining theory and experiment on structurally and compositionally well-defined materials, we will be able to address these fundamental questions at a deep level.
Project Details
Project type
Large-Scale EMSL Research
Start Date
2014-10-01
End Date
2016-09-30
Status
Closed
Released Data Link
Team
Principal Investigator
Co-Investigator(s)
Team Members
Related Publications
Electrically coupling complex oxides to semiconductors: A route to novel material functionalities
Ngai J, K Ahmadi-Majlan, MJ Moghadam, M Chrysler, D Kumah, F Walker, C Ahn, TC Droubay, Y Du, SA Chambers, ME Bowden, X Shen, and D Su. 2017. "Electrically coupling complex oxides to semiconductors: a route to novel material functionalities." Journal of Materials Research 32(2):249-259. doi:10.1557/jmr.2016.496
Interface Structure, Band Alignment, and Built-In Potentials at LaFeO3/n−SrTiO3 Heterojunctions
Comes RB, and SA Chambers. 2016. "Interface Structure, Band Alignment, and Built-In Potentials at LaFeO3/n-SrTiO3 Heterojunctions." Physical Review Letters 117(22):Article No. 226802. doi:10.1103/PhysRevLett.117.226802
Electronic and Optical Properties of a Semiconducting Spinel (Fe 2 CrO 4 )
Chambers SA, TC Droubay, TC Kaspar, IH Nayyar, ME McBriarty, SM Heald, DJ Keavney, ME Bowden, and P Sushko. 2017. "Electronic and Optical Properties of a Semiconducting Spinel (Fe2CrO4)." Advanced Functional Materials 27(9):Article No. 1605040. doi:10.1002/adfm.201605040
Defect compensation by Cr vacancies and oxygen interstitials inTi4+-dopedCr2O3epitaxial thin films
Kaspar TC, P Sushko, ME Bowden, SM Heald, A Papadogianni, CM Tschammer, O Bierwagen, and SA Chambers. 2016. "Defect compensation by Cr vacancies and oxygen interstitials in Ti4+-doped Cr2O3 epitaxial thin films." Physical Review. B, Condensed Matter and Materials Physics 94(15):Article No. 155409. doi:10.1103/PhysRevB.94.155409
Effect of doping and chemical ordering on the optoelectronic properties of complex oxides: Fe2O3–V2O3 solid solutions and hetero-structures
Nayyar IH, SE Chamberlin, TC Kaspar, N Govind, SA Chambers, and P Sushko. 2017. "Effect of doping and chemical ordering on the optoelectronic properties of complex oxides: Fe2O3–V2O3 solid solutions and hetero-structures." Physical Chemistry Chemical Physics. PCCP 19(2):1097-1107. doi:10.1039/C6CP06087K
Interface-Induced Polarization in SrTiO3-LaCrO3Superlattices
Comes RB, SR Spurgeon, SM Heald, DM Kepaptsoglou, L Jones, PV Ong, ME Bowden, QM Ramasse, P Sushko, and SA Chambers. 2016. "Interface-Induced Polarization in SrTiO3-LaCrO3 Superlattices ." Advanced Materials Interfaces 3(6):Art. No. 1500779. doi:10. 1002/admi. 201500779
Built-In Potential in Fe2O3-Cr2O3Superlattices for Improved Photoexcited Carrier Separation
Kaspar TC, DK Schreiber, SR Spurgeon, ME McBriarty, GM Carroll, DR Gamelin, and SA Chambers. 2016. "Built-in Potential in Fe2O3-Cr2O3 Superlattices for Improved Photoexcited Carrier Separation." Advanced Materials 28(8):1616-1622. doi:10. 1002/adma. 201504545
Quasi 2D Ultrahigh Carrier Density in a Complex Oxide Broken-Gap Heterojunction
Xu P, TC Droubay, JS Jeong, KA Mkhoyan, P Sushko, SA Chambers, and B Jalan. 2016. "Quasi 2D Ultrahigh Carrier Density in a Complex Oxide Broken Gap Heterojunction." Advanced Materials Interfaces 3(2):Article No. 1500432. doi:10. 1002/admi. 201500432
Infrared optical absorption in low-spin Fe2+-doped SrTiO3
Comes RB, TC Kaspar, SM Heald, ME Bowden, and SA Chambers. 2016. "Infrared Optical Absorption in Low-spin Fe2+-doped SrTiO3." Journal of Physics: Condensed Matter 28(3):Article No. 035901. doi:10.1088/0953-8984/28/3/035901
Band alignment of epitaxial SrTiO3 thin films with (LaAlO3)0.3-(Sr2AlTaO6)0.7 (001)
Comes RB, A Xu, B Jalan, and SA Chambers. 2015. "Band alignment of epitaxial SrTiO3 thin films with (LaAlO3)0.3-(Sr2AlTaO6)0.7 (001)." Applied Physics Letters 107:131601.1 - 131601.4. doi:10.1063/1.4932063
Crystallographic dependence of photocatalytic activity of WO3thin films prepared by molecular beam epitaxy
Li G, T Varga, P Yan, Z Wang, CM Wang, SA Chambers, and Y Du. 2015. "Crystallographic Dependence of Photocatalytic Activity of WO3 Thin Films Prepared by Molecular Beam Epitaxy." Physical Chemistry Chemical Physics. PCCP 17(23):15119-15123. doi:10.1039/c5cp01344e
Etalon-induced baseline drift and correction in atom flux sensors based on atomic absorption spectroscopy
Du Y, and SA Chambers. 2014. "Etalon-induced Baseline Drift And Correction In Atom Flux Sensors Based On Atomic Absorption Spectroscopy." Applied Physics Letters 105(16):163113(1)-163113(5). doi:10.1063/1.4898638
Self-corrected sensors based on atomic absorption spectroscopy for atom flux measurements in molecular beam epitaxy
Du Y, TC Droubay, AV Liyu, G Li, and SA Chambers. 2014. "Self-corrected Sensors Based On Atomic Absorption Spectroscopy For Atom Flux Measurements In Molecular Beam Epitaxy." Applied Physics Letters 104(16):Article No. 163110. doi:10.1063/1.4873544
Electronic structure and optical properties of α-(Fe1-xVx)2O3 solid-solution thin films
Chamberlin SE, IH Nayyar, TC Kaspar, P Sushko, and SA Chambers. 2015. "Electronic structure and optical properties of α-(Fe1-xVx)2O3 solid-solution thin films." Applied Physics Letters 106(4):041905. doi:10.1063/1.4906597
Stability at the surface
Chambers SA. 2014. "Stability at the surface." Science 346(6214):1186-1187. doi:10.1126/science.aaa1543
Dominance of Interface Chemistry over the Bulk Properties in Determining the Electronic Structure of Epitaxial Metal/Perovskite Oxide Heterojunctions
Chambers SA, Y Du, M Gu, TC Droubay, S Hepplestone, and P Sushko. 2015. "Dominance of interface chemistry over the bulk properties in determining the electronic structure of epitaxial metal/perovskite oxide heterojunctions." Chemistry of Materials 27(11):4093-4098. doi:10.1021/acs.chemmater.5b01118
Photochemical Outcomes of Adsorbed Oxygen: Desorption, Dissociation, and Passivation by Coadsorbed Water
Henderson MA. 2015. "Photochemical Outcomes of Adsorbed Oxygen: Desorption, Dissociation and Passivation by Coadsorbed Water." The Journal of Physical Chemistry C. doi:10.1021/acs.jpcc.5b05972
Perovskite Sr-Doped LaCrO3as a New p-Type Transparent Conducting Oxide
Zhang H, Y Du, A Papadogianni, O Bierwagen, S Sallis, LFJ Piper, ME Bowden, V Shutthanandan, P Sushko, and SA Chambers. 2015. "Perovskite Sr-doped LaCrO3 as a new p-type transparent conducting oxide." Advanced Materials DOI: 10.1002/adma.201501959
Electronic and magnetic properties of epitaxial perovskite SrCrO3(0 0 1)
Zhang H, Y Du, P Sushko, ME Bowden, V Shutthanandan, L Qiao, G Cao, Z Gai, S Sallis, LFJ Piper, and SA Chambers. 2015. "Electronic and magnetic properties of epitaxial perovskite SrCrO3(001)." Journal of Physics: Condensed Matter 27(24):245605. doi:10.1088/0953-8984/27/24/245605
Hole-induced insulator-to-metal transition inLa1−xSrxCrO3epitaxial films
Zhang H, Y Du, P Sushko, ME Bowden, V Shutthanandan, S Sallis, LFJ Piper, and SA Chambers. 2015. "Hole-induced metal-insulator transition in La1-xSrxCrO3 epitaxial films." Physical Review. B, Condensed Matter and Materials Physics 91(15):155129. doi:10.1103/PhysRevB.91.155129
Band-Gap Reduction and Dopant Interaction in Epitaxial La,Cr Co-doped SrTiO3 Thin Films
Comes RB, P Sushko, SM Heald, RJ Colby, ME Bowden, and SA Chambers. 2014. "Band-Gap Reduction and Dopant Interaction in Epitaxial La,Cr Co-doped SrTiO3 Thin Films." Chemistry of Materials 26(24):7073-7082. doi:10.1021/cm503541u
Real-time cumulant approach for charge-transfer satellites in x-ray photoemission spectra
Kas JJ, FD Vila, JJ Rehr, and SA Chambers. 2015. "Real time cumulant approach for charge transfer satellites in x-ray photoemission spectra." Physical Review. B, Condensed Matter 91(12):121112-5. doi:10.1103/PhysRevB.91.121112
Visible light carrier generation in co-doped epitaxial titanate films
Comes RB, SY Smolin, TC Kaspar, R Gao, BA Apgar, LW Martin, ME Bowden, J Baxter, and SA Chambers. 2015. "Visible light carrier generation in co-doped epitaxial titanate films." Applied Physics Letters 109:, doi:10.1063/1.4913930
Epitaxial niobium dioxide thin films by reactive-biased target ion beam deposition
Wang Y, RB Comes, S Kittiwatanakul, SA Wolf, and J Lu. 2015. "Epitaxial niobium dioxide thin films by reactive-biased target ion beam deposition." Journal of Vacuum Science and Technology A--Vacuum, Surfaces and Films 33(2):021516. doi:10.1116/1.4906143