4.8 Article

Interfacial Oxygen-Driven Charge Localization and Plasmon Excitation in Unconventional Superconductors

Journal

ADVANCED MATERIALS
Volume 32, Issue 34, Pages -

Publisher

WILEY-V C H VERLAG GMBH
DOI: 10.1002/adma.202000153

Keywords

charge localizations; interfacial excitons; orbital hybridizations; plasmons; unconventional superconductors

Funding

  1. NUS [C-380-003-003-001]
  2. Ministry of Education, Singapore AcRF Tier-2 grants [MOE2016-T2-2-110, MOE2017 T2-1-135, MOE2018-T2-2-117, MOE2019-T2-1-163]
  3. MOE-AcRF Tier-1 [R-144-000-423-114, R-144-000-398-114, R-144-000-379-114, R-144-000-368-112]
  4. Singapore National Research Foundation under its Competitive Research Funding [R-398-000-087-281]
  5. Singapore National Research Foundation under its Competitive Research Funding (CRP Award) [NRF-CRP15-2015-01]
  6. Agency for Science, Technology, and Research (A*STAR) under its Advanced Manufacturing and Engineering (AME) Individual Research Grant (IRG) [A1983c0034]

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Charge localization is critical to the control of charge dynamics in systems such as perovskite solar cells, organic-, and nanostructure-based photovoltaics. However, the precise control of charge localization via electronic transport or defect engineering is challenging due to the complexity in reaction pathways and environmental factors. Here, charge localization in optimal-doped La(1.85)Sr(0.15)CuO(4)thin-film on SrTiO(3)substrate (LSCO/STO) is investigated, and also a high-energy plasmon is observed. Charge localization manifests as a near-infrared mid-gap state in LSCO/STO. This is ascribed to the interfacial hybridization between the Ti3d-orbitals of the substrate and O2p-orbitals of the film. The interfacial effect leads to significant changes in the many-body correlations and local-field effect. The local-field effect results in an inhomogeneous charge distribution, and due to perturbation by an external field, the high polarizability of this nonuniform charge system eventually generates the high-energy plasmon. Transformation of the electronic correlations in LSCO/STO is further demonstrated via temperature-dependent spectral-weight transfer. This study of charge localization in cuprates and interfacial hybridization provides important clues to their electronic structures and superconductive properties.

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