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Portrait of Tönu Pullerits; Photo: Kennet Ruona

Tönu Pullerits

Professor

Portrait of Tönu Pullerits; Photo: Kennet Ruona

Ultrafast Spectroelectrochemistry Reveals Photoinduced Carrier Dynamics in Positively Charged CdSe Nanocrystals

Author

  • Alireza Honarfar
  • Pavel Chabera
  • Weihua Lin
  • Jie Meng
  • Hassan Mourad
  • Galina Pankratova
  • Lo Gorton
  • Kaibo Zheng
  • Tõnu Pullerits

Summary, in English

Extra charges in semiconductor nanocrystals are of paramount importance for their electrically driven optoelectronic and photovoltaic applications. Optical excitations of such charged nanocrystals lead to rapid recombinationviaan Auger process, which can deteriorate the performance of the corresponding devices. While numerous articles report trion Auger processes in negatively charged nanocrystals, optical studies of well-controlled positive charging of nanocrystals and detailed studies of positive trions remain rare. In this work, we used electrochemistry to achieve positive charging of CdSe nanocrystals, so-called quantum dots (QDs), in a controlled way. Femtosecond transient absorption spectroscopy was applied forin situinvestigation of the charge carrier dynamics after optical excitation of the electrochemically charged QD assembly on TiO2. We observe that without bias (i.e., neutral QDs), sub-picosecond hot carrier cooling is followed by multiple phases of the dynamics corresponding to electron injection and transfer to the TiO2. Positive charging first leads to activation of the hole traps close to the valence band maximum, which opens a rapid recombination channel of the optical excitation. A further increase in the positive bias interrupts the electron injection to TiO2, and if nanocrystals are positively charged, it leads to Auger relaxation in a few hundred picosecond timescale. This study represents a step toward the understanding of the effect of positive charging on the performance of semiconductor nanocrystals under conditions which closely mimic their potential applications.

Department/s

  • Chemical Physics
  • NanoLund: Center for Nanoscience
  • Biochemistry and Structural Biology
  • eSSENCE: The e-Science Collaboration

Publishing year

2021-07-08

Language

English

Pages

14332-14337

Publication/Series

Journal of Physical Chemistry C

Volume

125

Issue

26

Document type

Journal article

Publisher

The American Chemical Society (ACS)

Topic

  • Condensed Matter Physics
  • Physical Chemistry

Status

Published

ISBN/ISSN/Other

  • ISSN: 1932-7447