Nature Materials, volume 22, issue 8, pages 1013-1021

Spin-exchange carrier multiplication in manganese-doped colloidal quantum dots

Publication typeJournal Article
Publication date2023-07-13
Journal: Nature Materials
Quartile SCImago
Q1
Quartile WOS
Q1
Impact factor41.2
ISSN14761122, 14764660
General Chemistry
Condensed Matter Physics
General Materials Science
Mechanical Engineering
Mechanics of Materials
Abstract

Carrier multiplication is a process whereby a kinetic energy of a carrier relaxes via generation of additional electron–hole pairs (excitons). This effect has been extensively studied in the context of advanced photoconversion as it could boost the yield of generated excitons. Carrier multiplication is driven by carrier–carrier interactions that lead to excitation of a valence-band electron to the conduction band. Normally, the rate of phonon-assisted relaxation exceeds that of Coulombic collisions, which limits the carrier multiplication yield. Here we show that this limitation can be overcome by exploiting not ‘direct’ but ‘spin-exchange’ Coulomb interactions in manganese-doped core/shell PbSe/CdSe quantum dots. In these structures, carrier multiplication occurs via two spin-exchange steps. First, an exciton generated in the CdSe shell is rapidly transferred to a Mn dopant. Then, the excited Mn ion undergoes spin-flip relaxation via a spin-conserving pathway, which creates two excitons in the PbSe core. Due to the extremely fast, subpicosecond timescales of spin-exchange interactions, the Mn-doped quantum dots exhibit an up-to-threefold enhancement of the multiexciton yield versus the undoped samples, which points towards the considerable potential of spin-exchange carrier multiplication in advanced photoconversion.

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GOST |
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GOST Copy
Jin H. et al. Spin-exchange carrier multiplication in manganese-doped colloidal quantum dots // Nature Materials. 2023. Vol. 22. No. 8. pp. 1013-1021.
GOST all authors (up to 50) Copy
Jin H., Livache C., Kim W. D., Diroll B. T., Schaller R. D., Klimov V. I. Spin-exchange carrier multiplication in manganese-doped colloidal quantum dots // Nature Materials. 2023. Vol. 22. No. 8. pp. 1013-1021.
RIS |
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RIS Copy
TY - JOUR
DO - 10.1038/s41563-023-01598-x
UR - https://doi.org/10.1038/s41563-023-01598-x
TI - Spin-exchange carrier multiplication in manganese-doped colloidal quantum dots
T2 - Nature Materials
AU - Jin, Ho
AU - Livache, Clément
AU - Kim, Whi Dong
AU - Diroll, Benjamin T
AU - Schaller, Richard D
AU - Klimov, Victor I.
PY - 2023
DA - 2023/07/13 00:00:00
PB - Springer Nature
SP - 1013-1021
IS - 8
VL - 22
SN - 1476-1122
SN - 1476-4660
ER -
BibTex |
Cite this
BibTex Copy
@article{2023_Jin,
author = {Ho Jin and Clément Livache and Whi Dong Kim and Benjamin T Diroll and Richard D Schaller and Victor I. Klimov},
title = {Spin-exchange carrier multiplication in manganese-doped colloidal quantum dots},
journal = {Nature Materials},
year = {2023},
volume = {22},
publisher = {Springer Nature},
month = {jul},
url = {https://doi.org/10.1038/s41563-023-01598-x},
number = {8},
pages = {1013--1021},
doi = {10.1038/s41563-023-01598-x}
}
MLA
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MLA Copy
Jin, Ho, et al. “Spin-exchange carrier multiplication in manganese-doped colloidal quantum dots.” Nature Materials, vol. 22, no. 8, Jul. 2023, pp. 1013-1021. https://doi.org/10.1038/s41563-023-01598-x.
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