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  4. Sequential Carrier Transfer Can Accelerate Triplet Energy Transfer from Functionalized CdSe Nanocrystals
 
research article

Sequential Carrier Transfer Can Accelerate Triplet Energy Transfer from Functionalized CdSe Nanocrystals

Wilson, Mark W. B.
•
Hasham, Minhal
•
Narayanan, Pournima
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February 13, 2023
The Journal of Physical Chemistry Letters

Nanocrystal (NC)-sensitized triplet-fusion upconversion is a rising strategy to convert long-wavelength, incoherent light into higher-energy output photons. Here, we chart the photophysics of tailor-functionalized CdSe NCs to understand energy transfer to surface anchored transmitter ligands, which can proceed via correlated exciton transfer or sequential carrier hops. Varying NC size, we observe a pronounced acceleration of energy transfer (from kquench = 0.0096 ns-1 ligand-1 to 0.064 ns-1 ligand-1) when the barrier to hole-first sequential transfer is lowered from 100 +/- 25 meV to 50 +/- 25 meV. This acceleration is 5.1x the expected effect of increased carrier wave function leakage, so we conclude that sequential transfer becomes kinetically dominant under the latter conditions. Last, transient photoluminescence shows that NC band-edge and trap states are comparably quenched by functionalization (up to similar to 98% for sequential transfer) and exhibit matched dynamics for t > 300 ns, consistent with a dynamic quasi-equilibrium where photoexcitations can ultimately be extracted even when a carrier is initially trapped.

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Type
research article
DOI
10.1021/acs.jpclett.2c03443
Web of Science ID

WOS:000933297400001

Author(s)
Wilson, Mark W. B.
Hasham, Minhal
Narayanan, Pournima
Villanueva, Francisco Yarur
Green, Philippe B.  
Imperiale, Christian J.
Date Issued

2023-02-13

Published in
The Journal of Physical Chemistry Letters
Start page

1899

End page

1909

Subjects

Chemistry, Physical

•

Nanoscience & Nanotechnology

•

Materials Science, Multidisciplinary

•

Physics, Atomic, Molecular & Chemical

•

Chemistry

•

Science & Technology - Other Topics

•

Materials Science

•

Physics

•

photon up-conversion

•

quantum dots

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semiconductor nanocrystals

•

surface

•

dependence

•

emission

•

traps

•

size

•

photoluminescence

•

migration

Editorial or Peer reviewed

REVIEWED

Written at

EPFL

Available on Infoscience
March 13, 2023
Use this identifier to reference this record
https://infoscience.epfl.ch/handle/20.500.14299/195827
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