Disentangling the evolution of electrons and holes in photoexcited ZnO nanoparticles
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...
| Main Authors: | , , , , , , , , , , , , , , , , , , , , , , , , , , , , , |
|---|---|
| Format: | Article |
| Language: | English |
| Published: |
AIP Publishing LLC and ACA
2023-11-01
|
| Series: | Structural Dynamics |
| Online Access: | http://dx.doi.org/10.1063/4.0000204 |
| _version_ | 1827391471268921344 |
|---|---|
| author | Christopher J. Milne Natalia Nagornova Thomas Pope Hui-Yuan Chen Thomas Rossi Jakub Szlachetko Wojciech Gawelda Alexander Britz Tim B. van Driel Leonardo Sala Simon Ebner Tetsuo Katayama Stephen H. Southworth Gilles Doumy Anne Marie March C. Stefan Lehmann Melanie Mucke Denys Iablonskyi Yoshiaki Kumagai Gregor Knopp Koji Motomura Tadashi Togashi Shigeki Owada Makina Yabashi Martin M. Nielsen Marek Pajek Kiyoshi Ueda Rafael Abela Thomas J. Penfold Majed Chergui |
| author_facet | Christopher J. Milne Natalia Nagornova Thomas Pope Hui-Yuan Chen Thomas Rossi Jakub Szlachetko Wojciech Gawelda Alexander Britz Tim B. van Driel Leonardo Sala Simon Ebner Tetsuo Katayama Stephen H. Southworth Gilles Doumy Anne Marie March C. Stefan Lehmann Melanie Mucke Denys Iablonskyi Yoshiaki Kumagai Gregor Knopp Koji Motomura Tadashi Togashi Shigeki Owada Makina Yabashi Martin M. Nielsen Marek Pajek Kiyoshi Ueda Rafael Abela Thomas J. Penfold Majed Chergui |
| author_sort | Christopher J. Milne |
| collection | DOAJ |
| description | 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. |
| first_indexed | 2024-03-08T17:11:26Z |
| format | Article |
| id | doaj.art-05232b4aacf64feebd0d51544385296e |
| institution | Directory Open Access Journal |
| issn | 2329-7778 |
| language | English |
| last_indexed | 2024-03-08T17:11:26Z |
| publishDate | 2023-11-01 |
| publisher | AIP Publishing LLC and ACA |
| record_format | Article |
| series | Structural Dynamics |
| spelling | doaj.art-05232b4aacf64feebd0d51544385296e2024-01-03T19:59:32ZengAIP Publishing LLC and ACAStructural Dynamics2329-77782023-11-01106064501064501-910.1063/4.0000204Disentangling the evolution of electrons and holes in photoexcited ZnO nanoparticlesChristopher J. Milne0Natalia Nagornova1Thomas Pope2Hui-Yuan Chen3Thomas Rossi4Jakub Szlachetko5Wojciech Gawelda6Alexander Britz7Tim B. van Driel8Leonardo Sala9Simon Ebner10Tetsuo Katayama11Stephen H. Southworth12Gilles Doumy13Anne Marie March14C. Stefan Lehmann15Melanie Mucke16Denys Iablonskyi17Yoshiaki Kumagai18Gregor Knopp19Koji Motomura20Tadashi Togashi21Shigeki Owada22Makina Yabashi23Martin M. Nielsen24Marek Pajek25Kiyoshi Ueda26Rafael Abela27Thomas J. Penfold28Majed Chergui29 European XFEL, D-22761 Hamburg, Germany Lausanne Centre for Ultrafast Science (LACUS), ISIC, FSB, Ecole Polytechnique Fédérale de Lausanne, CH-1015 Lausanne, Switzerland Chemistry—School of Natural and Environmental Sciences, Newcastle University, Newcastle upon Tyne, NE1 7RU, United Kingdom Lausanne Centre for Ultrafast Science (LACUS), ISIC, FSB, Ecole Polytechnique Fédérale de Lausanne, CH-1015 Lausanne, Switzerland Lausanne Centre for Ultrafast Science (LACUS), ISIC, FSB, Ecole Polytechnique Fédérale de Lausanne, CH-1015 Lausanne, Switzerland SwissFEL, Paul Scherrer Institut, 5232 Villigen-PSI, Switzerland European XFEL, D-22761 Hamburg, Germany European XFEL, D-22761 Hamburg, Germany Department of Physics, Technical University of Denmark, 2800 Kongens Lyngby, Denmark SwissFEL, Paul Scherrer Institut, 5232 Villigen-PSI, Switzerland SwissFEL, Paul Scherrer Institut, 5232 Villigen-PSI, Switzerland Japan Synchrotron Radiation Research Institute (JASRI), Kouto 1-1-1, Sayo, Hyogo 679-5198, Japan Argonne National Laboratory, 9700 S. Cass Ave., Argonne, Illinois 60439, USA Argonne National Laboratory, 9700 S. Cass Ave., Argonne, Illinois 60439, USA Argonne National Laboratory, 9700 S. Cass Ave., Argonne, Illinois 60439, USA Argonne National Laboratory, 9700 S. Cass Ave., Argonne, Illinois 60439, USA Department of Physics and Astronomy, Uppsala University, 751 20 Uppsala, Sweden Institute of Multidisciplinary Research for Advanced Materials, Tohoku University, Sendai 980-8577, Japan Institute of Multidisciplinary Research for Advanced Materials, Tohoku University, Sendai 980-8577, Japan SwissFEL, Paul Scherrer Institut, 5232 Villigen-PSI, Switzerland Institute of Multidisciplinary Research for Advanced Materials, Tohoku University, Sendai 980-8577, Japan Department of Physics, Technical University of Denmark, 2800 Kongens Lyngby, Denmark RIKEN, SPring-8 Center, Kouto 1-1-1, Sayo, Hyogo 679-5148, Japan RIKEN, SPring-8 Center, Kouto 1-1-1, Sayo, Hyogo 679-5148, Japan Department of Physics, Technical University of Denmark, 2800 Kongens Lyngby, Denmark Faculty of Physics, Adam Mickiewicz University, Uniwersytetu Poznańskiego 2, Poznań, 61-614, Poland RIKEN, SPring-8 Center, Kouto 1-1-1, Sayo, Hyogo 679-5148, Japan SwissFEL, Paul Scherrer Institut, 5232 Villigen-PSI, Switzerland Chemistry—School of Natural and Environmental Sciences, Newcastle University, Newcastle upon Tyne, NE1 7RU, United Kingdom Lausanne Centre for Ultrafast Science (LACUS), ISIC, FSB, Ecole Polytechnique Fédérale de Lausanne, CH-1015 Lausanne, SwitzerlandThe 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.http://dx.doi.org/10.1063/4.0000204 |
| spellingShingle | Christopher J. Milne Natalia Nagornova Thomas Pope Hui-Yuan Chen Thomas Rossi Jakub Szlachetko Wojciech Gawelda Alexander Britz Tim B. van Driel Leonardo Sala Simon Ebner Tetsuo Katayama Stephen H. Southworth Gilles Doumy Anne Marie March C. Stefan Lehmann Melanie Mucke Denys Iablonskyi Yoshiaki Kumagai Gregor Knopp Koji Motomura Tadashi Togashi Shigeki Owada Makina Yabashi Martin M. Nielsen Marek Pajek Kiyoshi Ueda Rafael Abela Thomas J. Penfold Majed Chergui Disentangling the evolution of electrons and holes in photoexcited ZnO nanoparticles Structural Dynamics |
| title | Disentangling the evolution of electrons and holes in photoexcited ZnO nanoparticles |
| title_full | Disentangling the evolution of electrons and holes in photoexcited ZnO nanoparticles |
| title_fullStr | Disentangling the evolution of electrons and holes in photoexcited ZnO nanoparticles |
| title_full_unstemmed | Disentangling the evolution of electrons and holes in photoexcited ZnO nanoparticles |
| title_short | Disentangling the evolution of electrons and holes in photoexcited ZnO nanoparticles |
| title_sort | disentangling the evolution of electrons and holes in photoexcited zno nanoparticles |
| url | http://dx.doi.org/10.1063/4.0000204 |
| work_keys_str_mv | AT christopherjmilne disentanglingtheevolutionofelectronsandholesinphotoexcitedznonanoparticles AT natalianagornova disentanglingtheevolutionofelectronsandholesinphotoexcitedznonanoparticles AT thomaspope disentanglingtheevolutionofelectronsandholesinphotoexcitedznonanoparticles AT huiyuanchen disentanglingtheevolutionofelectronsandholesinphotoexcitedznonanoparticles AT thomasrossi disentanglingtheevolutionofelectronsandholesinphotoexcitedznonanoparticles AT jakubszlachetko disentanglingtheevolutionofelectronsandholesinphotoexcitedznonanoparticles AT wojciechgawelda disentanglingtheevolutionofelectronsandholesinphotoexcitedznonanoparticles AT alexanderbritz disentanglingtheevolutionofelectronsandholesinphotoexcitedznonanoparticles AT timbvandriel disentanglingtheevolutionofelectronsandholesinphotoexcitedznonanoparticles AT leonardosala disentanglingtheevolutionofelectronsandholesinphotoexcitedznonanoparticles AT simonebner disentanglingtheevolutionofelectronsandholesinphotoexcitedznonanoparticles AT tetsuokatayama disentanglingtheevolutionofelectronsandholesinphotoexcitedznonanoparticles AT stephenhsouthworth disentanglingtheevolutionofelectronsandholesinphotoexcitedznonanoparticles AT gillesdoumy disentanglingtheevolutionofelectronsandholesinphotoexcitedznonanoparticles AT annemariemarch disentanglingtheevolutionofelectronsandholesinphotoexcitedznonanoparticles AT cstefanlehmann disentanglingtheevolutionofelectronsandholesinphotoexcitedznonanoparticles AT melaniemucke disentanglingtheevolutionofelectronsandholesinphotoexcitedznonanoparticles AT denysiablonskyi disentanglingtheevolutionofelectronsandholesinphotoexcitedznonanoparticles AT yoshiakikumagai disentanglingtheevolutionofelectronsandholesinphotoexcitedznonanoparticles AT gregorknopp disentanglingtheevolutionofelectronsandholesinphotoexcitedznonanoparticles AT kojimotomura disentanglingtheevolutionofelectronsandholesinphotoexcitedznonanoparticles AT tadashitogashi disentanglingtheevolutionofelectronsandholesinphotoexcitedznonanoparticles AT shigekiowada disentanglingtheevolutionofelectronsandholesinphotoexcitedznonanoparticles AT makinayabashi disentanglingtheevolutionofelectronsandholesinphotoexcitedznonanoparticles AT martinmnielsen disentanglingtheevolutionofelectronsandholesinphotoexcitedznonanoparticles AT marekpajek disentanglingtheevolutionofelectronsandholesinphotoexcitedznonanoparticles AT kiyoshiueda disentanglingtheevolutionofelectronsandholesinphotoexcitedznonanoparticles AT rafaelabela disentanglingtheevolutionofelectronsandholesinphotoexcitedznonanoparticles AT thomasjpenfold disentanglingtheevolutionofelectronsandholesinphotoexcitedznonanoparticles AT majedchergui disentanglingtheevolutionofelectronsandholesinphotoexcitedznonanoparticles |