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Nanoscale Confinement of Photo-Injected Electrons at Hybrid Interfaces

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Download Hi-Res ImageDownload to MS-PowerPointCite This:J. Phys. Chem. Lett. 2021, 12, 49, 11951-11959
    Physical Insights into Light Interacting with Matter

    Nanoscale Confinement of Photo-Injected Electrons at Hybrid Interfaces
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    • Stefan Neppl
      Stefan Neppl
      Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States
      More by Stefan Neppl
      Orcidhttps://orcid.org/0000-0003-0536-1932
    • Johannes Mahl
      Johannes Mahl
      Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States
      Physics Department, Universität Hamburg and Center for Free-Electron Laser Science, 22761 Hamburg, Germany
      More by Johannes Mahl
    • Friedrich Roth
      Friedrich Roth
      Institute of Experimental Physics, TU Bergakademie Freiberg, 09599 Freiberg, Germany
      More by Friedrich Roth
    • Giuseppe Mercurio
      Giuseppe Mercurio
      Physics Department, Universität Hamburg and Center for Free-Electron Laser Science, 22761 Hamburg, Germany
      More by Giuseppe Mercurio
    • Guosong Zeng
      Guosong Zeng
      Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States
      Liquid Sunlight Alliance, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States
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    • Francesca M. Toma
      Francesca M. Toma
      Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States
      Liquid Sunlight Alliance, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States
      More by Francesca M. Toma
      Orcidhttps://orcid.org/0000-0003-2332-0798
    • Nils Huse
      Nils Huse
      Physics Department, Universität Hamburg and Center for Free-Electron Laser Science, 22761 Hamburg, Germany
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      Orcidhttps://orcid.org/0000-0002-3281-7600
    • Peter Feulner
      Peter Feulner
      Physics Department, Technische Universität München, 85748 Garching, Germany
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    • Oliver Gessner*
      Oliver Gessner
      Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States
      *[email protected]
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      Orcidhttps://orcid.org/0000-0003-4709-2822
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    The Journal of Physical Chemistry Letters

    Cite this: J. Phys. Chem. Lett. 2021, 12, 49, 11951–11959
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    https://doi.org/10.1021/acs.jpclett.1c02648
    Published December 9, 2021
    Copyright © 2021 American Chemical Society
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    Abstract

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    A prerequisite for advancing hybrid solar light harvesting systems is a comprehensive understanding of the spatiotemporal dynamics of photoinduced interfacial charge separation. Here, we demonstrate access to this transient charge redistribution for a model hybrid system of nanoporous zinc oxide (ZnO) and ruthenium bipyridyl chromophores. The site-selective probing of the molecular electron donor and semiconductor acceptor by time-resolved X-ray photoemission provides direct insight into the depth distribution of the photoinjected electrons and their interaction with the local band structure on a nanometer length scale. Our results show that these electrons remain localized within less than 6 nm from the interface, due to enhanced downward band bending by the photoinjected charge carriers. This spatial confinement suggests that light-induced charge generation and transport in nanoscale ZnO photocatalytic devices proceeds predominantly within the defect-rich surface region, which may lead to enhanced surface recombination and explain their lower performance compared to titanium dioxide (TiO2)-based systems.

    Copyright © 2021 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.jpclett.1c02648.

    • (A) Experimental details, sample preparation and characterization; (B) peak fitting analysis of the trXPS spectra; (C) ground state electronic structure of the N3/ZnO interface; (D) control trXPS experiments on bare ZnO electrodes; (E) laser fluence dependence of trXPS effects; (F) retrieving potential gradients by numerical XPS peak simulations; (G) parallel plate capacitor model for interfacial potential drop; (H) rate equation model for 2-step charge injection and recombination; (I) time-resolved XPS of N3 adsorbed to a gold substrate (PDF)

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    Cited By

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    This article is cited by 5 publications.

    1. Lin X. Chen, Junko Yano. Deciphering Photoinduced Catalytic Reaction Mechanisms in Natural and Artificial Photosynthetic Systems on Multiple Temporal and Spatial Scales Using X-ray Probes. Chemical Reviews 2024, 124 (9) , 5421-5469. https://doi.org/10.1021/acs.chemrev.3c00560
    2. Abinash Das, Dongyu Liu, Riu Riu Wary, Andrey S. Vasenko, Oleg V. Prezhdo, Ranjith G. Nair. Enhancement of Photocatalytic and Photoelectrochemical Performance of ZnO by Mg Doping: Experimental and Density Functional Theory Insights. The Journal of Physical Chemistry Letters 2023, 14 (18) , 4134-4141. https://doi.org/10.1021/acs.jpclett.3c00736
    3. Johannes Mahl, Oliver Gessner, Johannes V. Barth, Peter Feulner, Stefan Neppl. Strong Potential Gradients and Electron Confinement in ZnO Nanoparticle Films: Implications for Charge-Carrier Transport and Photocatalysis. ACS Applied Nano Materials 2021, 4 (11) , 12213-12221. https://doi.org/10.1021/acsanm.1c02730
    4. Lukas Wenthaus, Nikolay M. Kabachnik, Mario Borgwardt, Steffen Palutke, Dmytro Kutnyakhov, Federico Pressacco, Markus Scholz, Dmitrii Potorochin, Nils Wind, Stefan Düsterer, Günter Brenner, Oliver Gessner, Serguei Molodtsov, Wolfgang Eberhardt, Friedrich Roth. Insights into the laser-assisted photoelectric effect from solid-state surfaces. Physical Review B 2024, 110 (23) https://doi.org/10.1103/PhysRevB.110.235406
    5. Lukas Gierster, Olga Turkina, Jan‐Christoph Deinert, Sesha Vempati, Elsie Baeta, Yves Garmshausen, Stefan Hecht, Claudia Draxl, Julia Stähler. Right On Time: Ultrafast Charge Separation Before Hybrid Exciton Formation. Advanced Science 2024, 11 (31) https://doi.org/10.1002/advs.202403765
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    The Journal of Physical Chemistry Letters

    Cite this: J. Phys. Chem. Lett. 2021, 12, 49, 11951–11959
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.jpclett.1c02648
    Published December 9, 2021
    Copyright © 2021 American Chemical Society
    Request reuse permissions

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