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ACS Publications. Most Trusted. Most Cited. Most Read
Tuning Solvated Electrons by Polar–Nonpolar Oxide Heterostructure

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Download Hi-Res ImageDownload to MS-PowerPointCite This:J. Phys. Chem. Lett. 2018, 9, 11, 3049-3056
    Letter

    Tuning Solvated Electrons by Polar–Nonpolar Oxide Heterostructure
    Click to copy article linkArticle link copied!

    • Yanan Wang
      Yanan Wang
      ICQD/Hefei National Laboratory for Physical Sciences at Microscale and Key Laboratory of Strongly-Coupled Quantum Matter Physics, Chinese Academy of Sciences and Department of Physics, University of Science and Technology of China, Hefei, Anhui 230026, China
      More by Yanan Wang
    • Hongli Guo
      Hongli Guo
      ICQD/Hefei National Laboratory for Physical Sciences at Microscale and Key Laboratory of Strongly-Coupled Quantum Matter Physics, Chinese Academy of Sciences and Department of Physics, University of Science and Technology of China, Hefei, Anhui 230026, China
      School of Physics and Technology, Center for Nanoscience and Nanotechnology, and Key Laboratory of Artificial Micro- and Nano-structures of Ministry of Education, Wuhan University, Wuhan 430072, China
      More by Hongli Guo
    • Qijing Zheng*
      Qijing Zheng
      ICQD/Hefei National Laboratory for Physical Sciences at Microscale and Key Laboratory of Strongly-Coupled Quantum Matter Physics, Chinese Academy of Sciences and Department of Physics, University of Science and Technology of China, Hefei, Anhui 230026, China
      *Q.Z.: E-mail: [email protected]
      More by Qijing Zheng
      Orcidhttp://orcid.org/0000-0003-0022-3442
    • Wissam A. Saidi
      Wissam A. Saidi
      Department of Mechanical Engineering and Materials Science, University of Pittsburgh, Pittsburgh, Pennsylvania 15261, United States
      More by Wissam A. Saidi
      Orcidhttp://orcid.org/0000-0001-6714-4832
    • Jin Zhao*
      Jin Zhao
      ICQD/Hefei National Laboratory for Physical Sciences at Microscale and Key Laboratory of Strongly-Coupled Quantum Matter Physics, Chinese Academy of Sciences and Department of Physics, University of Science and Technology of China, Hefei, Anhui 230026, China
      Department of Physics and Astronomy, University of Pittsburgh, Pittsburgh, Pennsylvania 15260, United States
      Synergetic Innovation Center of Quantum Information & Quantum Physics, University of Science and Technology of China, Hefei, Anhui 230026, China
      *J.Z.: E-mail: [email protected]
      More by Jin Zhao
      Orcidhttp://orcid.org/0000-0003-1346-5280
    Other Access OptionsSupporting Information (1)

    The Journal of Physical Chemistry Letters

    Cite this: J. Phys. Chem. Lett. 2018, 9, 11, 3049–3056
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.jpclett.8b00938
    Published May 16, 2018
    Copyright © 2018 American Chemical Society
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    Abstract

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    Solvated electron states at the oxide/aqueous interface represent the lowest energy charge-transfer pathways, thereby playing an important role in photocatalysis and electronic device applications. However, their energies are usually higher than the conduction band minimum (CBM), which makes the solvated electrons difficult to utilize in charge-transfer processes. Thus it is essential to stabilize the energy of the solvated electron states. Taking LaAlO3/SrTiO3 (LAO/STO) oxide heterostructure with H2O-adsorbed monolayer as a prototypical system, we show using DFT and ab initio time-dependent nonadiabatic molecular dynamics simulation that the energy and dynamics of solvated electrons can be tuned by the electric field in the polar–nonpolar oxide heterostructure. In particular, for LAO/STO with p-type interface, the CBM is contributed by the solvated electron state when LAO is thicker than four unit cells. Furthermore, the solvated electron band minimum can be partially occupied when LAO is thicker than eight unit cells. We propose that the tunability of solvated electron states can be achieved on polar–nonpolar oxide heterostructure surfaces as well as on ferroelectric oxides, which is important for charge and proton transfer at oxide/aqueous interfaces.

    Copyright © 2018 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.jpclett.8b00938.

    • Computational details of ab initio NAMD and the adsorption energy (PDF)

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    Cited By

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    This article is cited by 13 publications.

    1. Zhutian Ding, Zachary K. Goldsmith, Annabella Selloni. Pathways for Electron Transfer at MgO–Water Interfaces from Ab Initio Molecular Dynamics. Journal of the American Chemical Society 2022, 144 (4) , 2002-2009. https://doi.org/10.1021/jacs.1c13250
    2. Xueke Yu, Yan Su, Wen-wu Xu, Jijun Zhao. Efficient Photoexcited Charge Separation at the Interface of a Novel 0D/2D Heterojunction: A Time-Dependent Ultrafast Dynamic Study. The Journal of Physical Chemistry Letters 2021, 12 (9) , 2312-2319. https://doi.org/10.1021/acs.jpclett.1c00023
    3. Lili Zhang, Weibin Chu, Qijing Zheng, Alexander V. Benderskii, Oleg V. Prezhdo, Jin Zhao. Suppression of Electron–Hole Recombination by Intrinsic Defects in 2D Monoelemental Material. The Journal of Physical Chemistry Letters 2019, 10 (20) , 6151-6158. https://doi.org/10.1021/acs.jpclett.9b02620
    4. Zi-ang Jia, Qing-rui Zeng, Yuan-bo Sun, Wei Feng. Controllable construction of a three-dimensional spherical LaFeO3/Bi2O3 heterojunction with enhanced photocatalytic ability for tetracycline degradation. Journal of Nanostructure in Chemistry 2023, 13 (5) , 481-495. https://doi.org/10.1007/s40097-022-00477-2
    5. Xianke Yue, Hong-Yao Liu, Yujun Zheng, Huan Yang. Photogenerated carrier dynamics at the B 4 C 3 /g-C 3 N 4 interface. Physical Chemistry Chemical Physics 2022, 24 (40) , 24860-24865. https://doi.org/10.1039/D2CP02175G
    6. Zhenfa Zheng, Qijing Zheng, Jin Zhao. Spin-orbit coupling induced demagnetization in Ni: Ab initio nonadiabatic molecular dynamics perspective. Physical Review B 2022, 105 (8) https://doi.org/10.1103/PhysRevB.105.085142
    7. Zhen-Fa Zheng, Xiang Jiang, Wei-Bin Chu, Li-Li Zhang, Hong-Li Guo, Chuan-Yu Zhao, Ya-Nan Wang, Ao-Lei Wang, Qi-Jing Zheng, Jin Zhao, , . Investigation of <i>ab initio</i> nonadiabatic molecular dynamics of excited carriers in condensed matter systems. Acta Physica Sinica 2021, 70 (17) , 177101. https://doi.org/10.7498/aps.70.20210626
    8. Qidong Zhao, Xiuming Zhao, Jingjing Cao. Advanced Nanomaterials for Degrading Persistent Organic Pollutants. 2020, 249-305. https://doi.org/10.1016/B978-0-12-814796-2.00007-1
    9. Qijing Zheng, Weibin Chu, Chuanyu Zhao, Lili Zhang, Hongli Guo, Yanan Wang, Xiang Jiang, Jin Zhao. Ab initio nonadiabatic molecular dynamics investigations on the excited carriers in condensed matter systems. WIREs Computational Molecular Science 2019, 9 (6) https://doi.org/10.1002/wcms.1411
    10. Zhenfa Zheng, Qijing Zheng, Jin Zhao. Ultrafast electron transfer dynamics in lateral transition-metal dichalcogenide heterostructures. Electronic Structure 2019, 1 (3) , 034001. https://doi.org/10.1088/2516-1075/ab3b28
    11. Yanan Wang, Yongliang Shi, Chuanyu Zhao, Qijing Zheng, Jin Zhao. Photogenerated carrier dynamics at the anatase/rutile Ti O 2 interface. Physical Review B 2019, 99 (16) https://doi.org/10.1103/PhysRevB.99.165309
    12. Huijuan Sun, Qijing Zheng, Wencai Lu, Jin Zhao. Ultrafast dynamics of solvated electrons at anatase TiO 2 /H 2 O interface. Journal of Physics: Condensed Matter 2019, 31 (11) , 114004. https://doi.org/10.1088/1361-648X/aafcf6
    13. Silviya Ninova, Ulrich Aschauer. Anion-order driven polar interfaces at LaTiO 2 N surfaces. Journal of Materials Chemistry A 2019, 7 (5) , 2129-2134. https://doi.org/10.1039/C8TA10230A
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    The Journal of Physical Chemistry Letters

    Cite this: J. Phys. Chem. Lett. 2018, 9, 11, 3049–3056
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.jpclett.8b00938
    Published May 16, 2018
    Copyright © 2018 American Chemical Society
    Request reuse permissions

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