- Tytuł:
- Disentangling the evolution of electrons and holes in photoexcited ZnO nanoparticles
- Autorzy:
-
Gawelda, Wojciech
Katayama, Tetsuo
Ueda, Kiyoshi
March, Anne Marie
Iablonskyi, Denis
Nielsen, Martin M.
Mucke, Melanie
Milne, Christofer
Sala, Leonardo
Pajek, Marek
Yabashi, Maina
Nagornova, Natalia
Szlachetko, Jakub
van Driel, Tim B.
Pope, Thomas
Lehmann, C. Stefan
Doumy, Giles
Motomura, Koji
Ebner, Simon
Penfold, Thomas J.
Chergui, Majed
Knopp, Gregor
Chen, Hui-Yuan
Rossi, Thomas
Southworth, Stephen H.
Togashi, Tadashi
Kumagai, Yoshiaki
Owada, Shigeki
Britz, Alexander
Abela, Rafael - Opis:
- 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.
- Dostawca treści:
- Repozytorium Uniwersytetu Jagiellońskiego
Artykuł