Quantum Motion, Relaxation and Stability of Multiple Excitons and Charge Carriers in Semiconductor Nanoplatelets
Laurens Siebbeles a
a Optoelectronic Materials (OM) section, Department of Chemical Engineering, Delft University of Technology
Materials for Sustainable Development Conference (MATSUS)
Proceedings of MATSUS Spring 2024 Conference (MATSUS24)
#Sol2D - Solution-Processed 2D Materials
Barcelona, Spain, 2024 March 4th - 8th
Organizers: Celso de Mello Donega and Jannika Lauth
Invited Speaker, Laurens Siebbeles, presentation 036
DOI: https://doi.org/10.29363/nanoge.matsus.2024.036
Publication date: 18th December 2023

We studied excitons, charge carriers and many-body complexes thereof in CdSe nanoplatelets with thickness of a few atomic layers and lateral sizes of tens of nanometers. Excitons and charge carriers were generated by photoexcitation with ultrashort laser pulses and detected by time-resolved optical absorption and terahertz conductivity measurements [1].

The shape of photoluminescence and absorption spectra varies with the lateral sizes of the nanoplatelets. We attribute this to quantum-confinement effects on the center-of-mass motion of excitons in the plane of the nanoplatelets. The spectra can be reproduced by a theoretical description of excitons based on the quantum mechanical particle-in-a-box model [2].

The initial photogeneration quantum yields of free charge carriers versus excitons were found to increase with photon energy [3]. Biexcitons and trions were observed due to formation of an exciton by a probe photon near an already present exciton or charge carrier left after the pump laser pulse. Initially hot excitons and charges were found to relax to the same energy distribution in about one picosecond for different pump photon energies. We found that excitons are stable even at high densities where they start to exhibit spatial overlap. A crossover to an electron-hole plasma of uncorrelated free electrons and holes was not observed. This counter intuitive result can be understood theoretically from the fact that the Coulomb screening length, and thus the exciton binding energy, remain non-zero even at high density [4,5].

 

References

[1] R. Tomar et al., J. Phys. Chem. C 123, 9640 (2019).

[2] M. Failla et al., Phys. Rev. B., 102, 195405 (2020).

[3] M. Failla et al., J. Phys. Chem. C, 127, 1899 (2023).

[4] F. García Flórez et al., Phys. Rev. B 100, 245302 (2019).

[5] F. García Flórez et al., Phys. Rev. B 102, 115302 (2020).

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