Fundamental Structure-Property Relationships Governing the Electrochemical Activity of Epitaxial Heterostructures
EMSL Project ID
51038
Abstract
Complex oxides have the widest range of properties of any class of materials explored to date. However, with many degrees of freedom come many possible outcomes. Consequently, controlled synthesis of oxide materials, and ultimately achieving atomic precision, constitute grand challenges in materials science. Thin-film heterointerface formation is an ideal way to synthesize artificially structured materials that cannot be made by bulk methods, enabling fundamental understanding and new functionalities. Accordingly, we will uncover the relationships that exist between synthetic pathways and subsequent electron-hole pair creation, propagation and lifetime, relevant to solar energy conversion, using an integrated experimental and theoretical approach. A long-term goal is to understand the role of defects and disorder: how and why defects form along specific reaction pathways, how defects influence system properties, and how defects can be harnessed to enable new, robust functionalities and states of matter. Materials of interest will be synthesized using oxygen assisted molecular beam epitaxy, and characterized using in situ and ex situ techniques. By complementing experiments with state-of-the-art computational modeling, we will elucidate the intricate relationships between composition, structure, defect creation, kinetics of formation, and ground and excited state functional properties. Electronic, optical, photochemical and electrochemical properties will be measured and interpreted in light of materials models based on atomistic understanding. Revealing these relationships paves the way for effective and scientifically informed synthesis of complex oxides and underpins their use in solar energy harvesting and conversion
Project Details
Start Date
2019-10-01
End Date
2020-09-30
Status
Closed
Released Data Link
Team
Principal Investigator
Team Members
Related Publications
10. Lei Pan, Alexander Grutter, Xiaoyu Che, Tomohiro Nozaki, Alex Stern, Mike Street, Bing Zhang, Brian Casas, Qing Lin He, Eun Sang Choi, Steven M. Disseler, Dustin A. Gilbert, Gen Yin, Qiming Shao, Peng Zhang, Peng Deng, Yingying Wu, Xiaoyang Liu, Xufeng Kou, Sahashi Masashi, Xiaodong Han, Christian Binek, Scott Chambers, Jing Xia, Kang L. Wang, ?Exchange Interaction at a Quantum Anomalous Hall Insulator/Antiferromagnet Heterostructure?, Adv. Mater. 32, 3001460 (2020). DOI: 10.1002/adma.202001460.
1. Z. Yang, P.-V Ong, Y. He, L. Wang, M. E. Bowden, W. Xu, T. C. Droubay, C. Wang, P. V. Sushko, Y. Du, ?Direct visualization of Li dendrites effect on LiCoO2 cathodes by in situ TEM?, Small, 1803108 (2018). DOI: 10.1002/smll.201803108
2. Kelsey A. Stoerzinger, Yingge Du, Kelvin H.L. Zhang, Jun Cai, J. Trey Diulus, Ryan T. Frederick, Gregory S. Herman, Ethan J. Crumlin, Scott A. Chambers, ?Impact of Sr-Incorporation on Cr Oxidation and Water Dissociation in La(1-x)SrxCrO3?, Adv. Mater. Int. 1701363 (2018). DOI 10.1002/admi.201701363.
3. Kelsey A. Stoerzinger, Yingge Du, Steven R. Spurgeon, Demie Kepaptsoglou, Quentin M. Ramasse, Ethan J. Crumlin, Scott A. Chambers, ?Chemical and Electronic Structure Analysis of a SrTiO3 (001) / p-Ge (001) Hydrogen Evolution Photocathode?, MRS Comm. 8, 46 (2018). DOI:10.1557/mrc.2018.38.
3. Shih-Chieh Lin, Cheng-Tai Kuo, Ryan Comes, Julien E. Rault, Jean-Pascal Rueff, Slavo Nem?ák, Amina Taleb, Jeffrey B. Kortright, Julia Meyer-Ilse, Eric Gullikson, Peter Sushko, Steven R. Spurgeon, Matthias Gehlman, Lukasz Plucinski, Scott A. Chambers, and Charles S Fadley, ?Interface composition and potential profile of LaCrO3/SrTiO3 determined by standing-wave excited photoemission spectroscopy?, Phys. Rev. B 98, 165124 (2018). DOI: 10.1103/PhysRevB.98.165124
4. L. Wang, Y. Du, L. Chang, K. A. Stoerzinger, M. E. Bowden, J. Wang, S. A. Chambers, ?Interface Electronic Structure and Band Alignment at the p-n La0.88Sr0.12FeO3 / SrTiO3(001) Heterojunction?, Appl. Phys. Lett. 112, 261601 (2018). DOI: 10.1063/1.5030897.
5. S.A. Chambers, Y. Du, Z. Zhu, J. Wang, M.J. Wahila, L.F.J. Piper, A. Prakash, J. Yue, B. Jalan, S.R. Spurgeon, D.M. Kepaptsoglou, Q. M. Ramasse, P.V. Sushko, ?Interconversion of intrinsic defects in SrTiO3(001) ?, Phys. Rev. B 97, 245204 (2018). DOI: 10.1103/PhysRevB.97.245204.
6. Le Wang, Kelsey A. Stoerzinger, Lei Chang, Jiali Zhao, Yangyang Li, Chi Sin Tang, Xinmao Yin, Mark E. Bowden, Zhenzhong Yang, Haizhong Guo, Lu You, Rui Guo, Jiaou Wang, Kurash Ibrahim, Jingsheng Chen, Andrivo Rusydi, Junling Wang, Scott A. Chambers, Yingge Du, ?Tuning Bifunctional Oxygen Electrocatalysts by Changing A-site Rare-Earth Element in Perovskite Nickelates?, Adv. Funct. Mater. 1803712 (2018). DOI: 10.1002/adfm.201803712.
Dustin Gilbert, Peyton Murray, Alexandr Lonin, Steven R. Spurgeon, R. Chopdekar, Brian J. Kirby, Brian Maranville, Julie A. Borchers, A.T. N?Diaye, Kai Liu, Elke Arenholz, Yayoi Takamura, Alex J. Grutter. ?Ionic tuning of cobaltites at the nanoscale.? Phys. Rev. Mater. 2, 104402 (2018). DOI:10.1103/PhysRevMaterials.2.104402
J.C. Woicik, J.M. Ablett, N.F. Quackenbush, A.K. Rumaiz, C. Weiland, T.C. Droubay, S.A. Chambers, ?Charge-transfer excitations in the photo-ionization of NiO?, Phys. Rev. B. 97, 245142 (2018). DOI: 10.1103/PhysRevB.97.245142/.
Jishan Liu, Endong Jia, Le Wang, Kelsey A. Stoerzinger, Hua Zhou, Chi Sin Tang, Xinmao Yin, Xu He, Eric Bousquet, Mark E. Bowden, Andrew Wee, Scott A. Chambers, and Yingge Du, ?Tuning the Electronic Structure of LaNiO3 through Alloying with Strontium to Enhance Oxygen Evolution Activity?, Adv. Sci. 6, 1901073 (2019). DOI: 10.1002/advs.201901073.
Kelsey A. Stoerzinger, Le Wang, Yifan Ye, Mark Bowden, Ethan J. Crumlin, Yingge Du, Scott A. Chambers, ?Linking surface chemistry to photovoltage in Sr-substituted LaFeO3 for water oxidation?, J. Mater. Chem. A 6, 22170 (2018). DOI: 10.1039/c8ta05741a.
Lei Chang, Le Wang, Lu You, Zhenzhong Yang, Amr Abdelsamie, Qinghua Zhang, Yang Zhou, Lin Gu, Scott A. Chambers, and Junling Wang, ?Tuning Photovoltaic Performance of Perovskite Nickelates Heterostructures by Changing the A‐Site Rare‐Earth Element?, ACS Appl. Mater. Interfaces 11, 16191 (2019). DOI: 10.1021/acsami.9b01851.
Le Wang, Kelsey A. Stoerzinger, Lei Chang, Xinmao Yin, Yangyang Li, Chi Sin Tang, Endong Jia, Mark E. Bowden, Zhenzhong Yang, Amr Abdelsamie, Lu You, Rui Guo, Jingsheng Chen, Andrivo Rusydi, Junling Wang, Scott A. Chambers, Yingge Du, ?Strain Effect on Oxygen Evolution Reaction Activity of Epitaxial NdNiO3 Thin Films?, ACS Adv. Mater. Interfaces 11, 12941 (2019). DOI: 10.1021/acsami.8b21301.
Le Wang, Yingge Du, Peter V. Sushko, Mark E. Bowden, Kelsey A. Stoerzinger, Steven M. Heald, Mark. D. Scafetta, Tiffany C. Kaspar, Scott. A Chambers, ?Hole-Induced Electronic and Optical Transitions in La1-xSrxFeO3 Epitaxial Thin Films?, Phys. Rev. Mater. 3, 025401 (2019). DOI: 10.1103/PhysRevMaterials.3.025401.
Le Wang, Zhenzhong Yang, Mark E. Bowden, John W. Freeland, Peter V. Sushko, Steven R. Spurgeon, Bethany Matthews, Widitha S. Samarakoon, Hua Zhou, Zhenxing Feng, Mark H. Engelhard, Yingge Du, and Scott A. Chambers, ?Hole-Trapping-Induced Stabilization of Ni4+ in SrNiO3/LaFeO3 Superlattices?, Adv. Mater. 2005003 (2020). DOI: 10.1002/adma.202005003.
Mark D. Scafetta, Tiffany C. Kaspar, Mark E. Bowden, Steven R. Spurgeon, Bethany Matthews, Scott A. Chambers, ?Reversible Oxidation Quantified by Optical Properties in Epitaxial Fe2CrO4+δ Films on (001) MgAl2O4?, ACS Omega, 5, 3240 (2020). https://dx.doi.org/10.1021/acsomega.9b03299
Mark D. Scafetta¬, Zhenzhong Yang, Steven R. Spurgeon, Tiffany C. Kaspar, Scott A. Chambers, ?Epitaxial growth and atomic arrangement in Fe2CrO4 on crystal symmetry matched (001) MgAl2O4?, J. Vac. Sci. Technol. A 37, 031511 (2019). DOI: 10.1116/1.5093537.
M. Wu, S. Q. Chen, C. W. Huang, X. Ye, H. P. Zhou, X. C. Huang, Kelvin H. L. Zhang, W. S. Yan, L. H. Zhang, K. Kim, Y. Du, S.A. Chambers, J.-C. Zheng, and H.-Q. Wang, ?Modulation of the electronic states of perovskite SrCrO3 thin films through low-energy hydrogen plasma implantation approaches?, Front. Phys. 15, 13601 (2020). https://doi.org/10.1007/s11467-019-0923-2.
Paul S. Bagus, Connie J. Nelin, C. R. Brundle, Scott A. Chambers, ?A New Mechanism For XPS Line Broadening: The 2p-XPS of Ti(IV)?, J. Phys. Chem. C 123, 7705 (2019). DOI: 10.1021/acs.jpcc.8b05576.
Peter V. Sushko and Scott A. Chambers, ?Extracting Band Edge Profiles at Semiconductor Heterostructures from Hard X-ray Core-Level Photoelectron Spectra?, Sci. Rep., published online 3 August 2020. https://doi.org/10.1038/s41598-020-69658-9.
P.-V. Ong, Z. Yang, P. V. Sushko, Y. Du, ?Formation, structural variety, and impact of anti-phase boundaries on Li diffusion in LiCoO2 thin film cathodes?, Journal of Physical Chemistry Letters 9, 5515-5520 (2018). DOI: 10.1021/acs.jpclett.8b02185
Scott A. Chambers and Donald R. Baer, ?Introductory Guide to the Application of XPS to Epitaxial Films and Heterostructures?, J. Vac. Sci. Technol. A 38, 061201 (2020). DOI: 10.1116/6.0000465.
Scott A. Chambers and Peter V. Sushko, ?Perspective: Reconstruction of Band-edge Profiles in Heterostructures from Hard X-ray Photoelectron Line Shapes?, APL Mater. 7, 110904 (2019). https://doi.org/10.1063/1.5129155
Scott A. Chambers and Peter V. Sushko, ?Perspective: Reconstruction of Band-edge Profiles in Heterostructures from Hard X-ray Photoelectron Line Shapes?, Appl. Phys. Lett. Mater. 7, 110904 (2019). https://doi.org/10.1063/1.5129155
Scott A. Chambers and Peter V. Sushko, ?The influence of crystalline order and defects on the absolute work functions and electron affinities of TiO2- and SrO-terminated n-SrTiO3(001)?, Phys. Rev. Mater. 3, 125803 (2019). DOI: 10.1103/PhysRevMaterials.3.125803
Scott A. Chambers and Yingge Du, ?Experimental Determination of Electron Attenuation Lengths in Complex Materials by Means of Epitaxial Film Growth: Advantages and Challenges?, J. Vac. Sci. Technol. A 38, 043409 (2020). DOI: 10.1116/6.0000291.
Steven R. Spurgeon, Peter V. Sushko, Arun Devaraj, Yingge Du, Timothy C. Droubay, Scott A. Chambers, ?Onset of Phase Separation in the Double Perovskite Oxide La2MnNiO6?, Phys. Rev. B 97, 134110 (2018). DOI: 10.1103/PhysRevB.97.134110.
Tiffany C. Kaspar, Peter V. Sushko, Steven R. Spurgeon, Mark E. Bowden, David J. Keavney, Ryan B. Comes, Sahar Saremi, Lane Martin, Scott A. Chambers, ?Electronic structure and band alignment of LaMnO3 / SrTiO3 polar / non-polar heterojunctions?, Adv. Mater. Interfaces 1801428 (2018). DOI: 10.1002/admi.201801428
Y. Du, P.V. Sushko, S.R. Spurgeon, M.E. Bowden, J.M. Ablett, T.-L. Lee, N.F. Quackenbush, J.C. Woicik, S.A. Chambers, ?Layer-resolved band bending at the n-SrTiO3(001)/p-Ge(001) interface?, Phys. Rev. Mater. 2, 094602 (2018). DOI: 10.1103/PhysRevMaterials.2.094602.
Zheng Hui Lim, Nicholas F. Quackenbush, Aubrey Penn, Matthew Chrysler, Mark Bowden, Zihua Zhu, James M. Ablett, Tien-lin Lee, James M. LeBeau, Joseph C. Woicik, Peter V. Sushko, Scott A. Chambers, Joseph H. Ngai, ?Charge Transfer and Built-in Electric Fields Between a Crystalline Oxide and Silicon?, Phys. Rev. Lett. 123, 026805 (2019). DOI: 10.1103/PhysRevLett.123.026805.