Disentangling the evolution of electrons and holes in photoexcited ZnO nanoparticles

Milne, Christopher J.; Nagornova, Natalia; Pope, Thomas; Chen, Hui-Yuan; Rossi, Thomas; Szlachetko, Jakub; Gawelda, Wojciech; Britz, Alexander; van Driel, Tim B.; Sala, Leonardo; Ebner, Simon; Katayama, Tetsuo; Southworth, Stephen H.; Doumy, Gilles; March, Anne Marie; Lehmann, C. Stefan; Mucke, Melanie; Iablonskyi, Denys; Kumagai, Yoshiaki; Knopp, Gregor; Motomura, Koji; Togashi, Tadashi; Owada, Shigeki; Yabashi, Makina; Nielsen, Martin M.; Pajek, Marek; Ueda, Kiyoshi; Abela, Rafael; Penfold, Thomas J.; Chergui, Majed

doi:10.1063/4.0000204

Title: Disentangling the evolution of electrons and holes in photoexcited ZnO nanoparticles

Journal Article · Fri Nov 03 00:00:00 EDT 2023 · Structural Dynamics

DOI:https://doi.org/10.1063/4.0000204· OSTI ID:2205591

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European XFEL, Hamburg (Germany); Paul Scherrer Inst. (PSI), Villigen (Switzerland)
Ecole Polytechnique Federale Lausanne (EPFL) (Switzerland). Lausanne Centre for Ultrafast Science (LACUS)
Newcastle University, Newcastle upon Tyne (United Kingdom)
Paul Scherrer Inst. (PSI), Villigen (Switzerland); Adam Mickiewicz Univ., Poznan (Poland)
European XFEL, Hamburg (Germany); Adam Mickiewicz Univ., Poznan (Poland); Univ. of Cantoblanco, Madrid (Spain). IMDEA Nanoscience Institute
European XFEL, Hamburg (Germany); Hamburg Centre for Ultrafast Imaging, Hamburg (Germany)
Technical Univ. of Denmark, Lyngby (Denmark)
Paul Scherrer Inst. (PSI), Villigen (Switzerland)
European XFEL, Hamburg (Germany); Japan Synchrotron Radiation Research Institute (JASRI), Hyogo (Japan)
Argonne National Laboratory (ANL), Argonne, IL (United States)
European XFEL, Hamburg (Germany)
Uppsala Univ. (Sweden)
Tohoku Univ., Sendai (Japan)
RIKEN SPring-8 Center, Sayo (Japan)
Adam Mickiewicz Univ., Poznan (Poland)

The evolution of charge carriers in photoexcited room temperature ZnO nanoparticles in solution is investigated using ultrafast ultraviolet photoluminescence spectroscopy, ultrafast Zn K-edge absorption spectroscopy, and ab initio molecular dynamics (MD) simulations. The photoluminescence is excited at 4.66 eV, well above the band edge, and shows that electron cooling in the conduction band and exciton formation occur in <500 fs, in excellent agreement with theoretical predictions. The x-ray absorption measurements, obtained upon excitation close to the band edge at 3.49 eV, are sensitive to the migration and trapping of holes. They reveal that the 2 ps transient largely reproduces the previously reported transient obtained at 100 ps time delay in synchrotron studies. In addition, the x-ray absorption signal is found to rise in ~1.4 ps, which we attribute to the diffusion of holes through the lattice prior to their trapping at singly charged oxygen vacancies. Indeed, the MD simulations show that impulsive trapping of holes induces an ultrafast expansion of the cage of Zn atoms in <200 fs, followed by an oscillatory response at a frequency of ~100 cm^-1, which corresponds to a phonon mode of the system involving the Zn sub-lattice.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB); European Research Council (ERC); Swiss National Science Foundation (SNSF); Engineering and Physical Sciences Research Council (EPSRC)

Grant/Contract Number:: AC02-06CH11357; EP/W008009/1; EP/X035514/1

OSTI ID:: 2205591

Journal Information:: Structural Dynamics, Vol. 10, Issue 6; ISSN 2329-7778

Publisher:: American Crystallographic Association/AIPCopyright Statement

Country of Publication:: United States

Language:: English

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72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS
disentangling
evolution of electrons
photoexcited ZnO nanoparticles
molecular dynamics
excitons
ultrafast X-rays
ultrafast fluorescence spectroscopy
nanoparticle
photoexcitations
X-ray absorption spectroscopy

Title: Disentangling the evolution of electrons and holes in photoexcited ZnO nanoparticles

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References (62)

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