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Slow hole localization and fast electron cooling in Cu-doped InP/ZnSe quantum dots

P. Tim Prins, Dirk A. W. Spruijt, Mark J. J. Mangnus, Freddy T. Rabouw, Daniel Vanmaekelbergh, Celso de Mello Donega and Pieter Geiregat (UGent)
(2022) JOURNAL OF PHYSICAL CHEMISTRY LETTERS. 13. p.9950-9956
Author
Organization
Abstract
Impurity doping of low-dimensional semiconductors is an interesting route towards achieving control over carrier dynamics and energetics, e.g., to improve hot carrier extraction, or to obtain strongly Stokes shifted luminescence. Such studies remain, however, underexplored for the emerging family of III-V colloidal quantum dots (QDs). Here, we show through a detailed global analysis of multiresonant pump-probe spectroscopy that electron cooling in copper-doped InP quantum dot (QDs) proceeds on subpicosecond time scales. Conversely, hole localization on Cu dopants is remarkably slow (1.8 ps), yet still leads to very efficient subgap emission. Due to this slow hole localization, common Auger assisted pathways in electron cooling cannot be blocked by Cu doping III-V systems, in contrast with the case of II-VI QDs. Finally, we argue that the structural relaxation around the Cu dopants, estimated to impart a reorganization energy of 220 meV, most likely proceeds simultaneously with the localization itself leading to efficient luminescence.
Keywords
General Materials Science, Physical and Theoretical Chemistry, ULTRAFAST CARRIER DYNAMICS, HIGHLY EFFICIENT, AUGER PROCESSES, RELAXATION, NANOCRYSTALS, INTRABAND, ABSORPTION, EMISSION, PHOTOLUMINESCENCE, SUPPRESSION

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MLA
Prins, P. Tim, et al. “Slow Hole Localization and Fast Electron Cooling in Cu-Doped InP/ZnSe Quantum Dots.” JOURNAL OF PHYSICAL CHEMISTRY LETTERS, vol. 13, 2022, pp. 9950–56, doi:10.1021/acs.jpclett.2c02764.
APA
Prins, P. T., Spruijt, D. A. W., Mangnus, M. J. J., Rabouw, F. T., Vanmaekelbergh, D., de Mello Donega, C., & Geiregat, P. (2022). Slow hole localization and fast electron cooling in Cu-doped InP/ZnSe quantum dots. JOURNAL OF PHYSICAL CHEMISTRY LETTERS, 13, 9950–9956. https://doi.org/10.1021/acs.jpclett.2c02764
Chicago author-date
Prins, P. Tim, Dirk A. W. Spruijt, Mark J. J. Mangnus, Freddy T. Rabouw, Daniel Vanmaekelbergh, Celso de Mello Donega, and Pieter Geiregat. 2022. “Slow Hole Localization and Fast Electron Cooling in Cu-Doped InP/ZnSe Quantum Dots.” JOURNAL OF PHYSICAL CHEMISTRY LETTERS 13: 9950–56. https://doi.org/10.1021/acs.jpclett.2c02764.
Chicago author-date (all authors)
Prins, P. Tim, Dirk A. W. Spruijt, Mark J. J. Mangnus, Freddy T. Rabouw, Daniel Vanmaekelbergh, Celso de Mello Donega, and Pieter Geiregat. 2022. “Slow Hole Localization and Fast Electron Cooling in Cu-Doped InP/ZnSe Quantum Dots.” JOURNAL OF PHYSICAL CHEMISTRY LETTERS 13: 9950–9956. doi:10.1021/acs.jpclett.2c02764.
Vancouver
1.
Prins PT, Spruijt DAW, Mangnus MJJ, Rabouw FT, Vanmaekelbergh D, de Mello Donega C, et al. Slow hole localization and fast electron cooling in Cu-doped InP/ZnSe quantum dots. JOURNAL OF PHYSICAL CHEMISTRY LETTERS. 2022;13:9950–6.
IEEE
[1]
P. T. Prins et al., “Slow hole localization and fast electron cooling in Cu-doped InP/ZnSe quantum dots,” JOURNAL OF PHYSICAL CHEMISTRY LETTERS, vol. 13, pp. 9950–9956, 2022.
@article{8770434,
  abstract     = {{Impurity doping of low-dimensional semiconductors is an interesting route towards achieving control over carrier dynamics and energetics, e.g., to improve hot carrier extraction, or to obtain strongly Stokes shifted luminescence. Such studies remain, however, underexplored for the emerging family of III-V colloidal quantum dots (QDs). Here, we show through a detailed global analysis of multiresonant pump-probe spectroscopy that electron cooling in copper-doped InP quantum dot (QDs) proceeds on subpicosecond time scales. Conversely, hole localization on Cu dopants is remarkably slow (1.8 ps), yet still leads to very efficient subgap emission. Due to this slow hole localization, common Auger assisted pathways in electron cooling cannot be blocked by Cu doping III-V systems, in contrast with the case of II-VI QDs. Finally, we argue that the structural relaxation around the Cu dopants, estimated to impart a reorganization energy of 220 meV, most likely proceeds simultaneously with the localization itself leading to efficient luminescence.}},
  author       = {{Prins, P. Tim and Spruijt, Dirk A. W. and Mangnus, Mark J. J. and Rabouw, Freddy T. and Vanmaekelbergh, Daniel and de Mello Donega, Celso and Geiregat, Pieter}},
  issn         = {{1948-7185}},
  journal      = {{JOURNAL OF PHYSICAL CHEMISTRY LETTERS}},
  keywords     = {{General Materials Science,Physical and Theoretical Chemistry,ULTRAFAST CARRIER DYNAMICS,HIGHLY EFFICIENT,AUGER PROCESSES,RELAXATION,NANOCRYSTALS,INTRABAND,ABSORPTION,EMISSION,PHOTOLUMINESCENCE,SUPPRESSION}},
  language     = {{eng}},
  pages        = {{9950--9956}},
  title        = {{Slow hole localization and fast electron cooling in Cu-doped InP/ZnSe quantum dots}},
  url          = {{http://doi.org/10.1021/acs.jpclett.2c02764}},
  volume       = {{13}},
  year         = {{2022}},
}
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