TY - JOUR
T1 - Auger Recombination Lifetime Scaling for Type i and Quasi-Type II Core/Shell Quantum Dots
AU - Philbin, John P.
AU - Rabani, Eran
N1 - Publisher Copyright:
Copyright © 2020 American Chemical Society.
PY - 2020/7/2
Y1 - 2020/7/2
N2 - Having already achieved near-unity quantum yields, with promising properties for light-emitting diode, lasing, and charge separation applications, colloidal core/shell quantum dots have great technological potential. The shell thickness and band alignment of the shell and core materials are known to influence the efficiency of these devices. In many such applications, improving the efficiency requires a deep understanding of multiexcitonic states. Herein, we elucidate the shell thickness and band alignment dependencies of the biexciton Auger recombination lifetime for quasi-type II CdSe/CdS and type I CdSe/ZnS core/shell quantum dots. We find that the biexciton Auger recombination lifetime increases with the total nanocrystal volume for quasi-type II CdSe/CdS core/shell quantum dots and is independent of the shell thickness for type I CdSe/ZnS core/shell quantum dots. To perform these calculations and compute Auger recombination lifetimes, we developed a low-scaling approach based on the stochastic resolution of identity. The numerical approach provided a framework for studying the scaling of the biexciton Auger recombination lifetimes in terms of the shell thickness dependencies of the exciton radii, Coulomb couplings, and density of final states in quasi-type II CdSe/CdS and type I CdSe/ZnS core/shell quantum dots.
AB - Having already achieved near-unity quantum yields, with promising properties for light-emitting diode, lasing, and charge separation applications, colloidal core/shell quantum dots have great technological potential. The shell thickness and band alignment of the shell and core materials are known to influence the efficiency of these devices. In many such applications, improving the efficiency requires a deep understanding of multiexcitonic states. Herein, we elucidate the shell thickness and band alignment dependencies of the biexciton Auger recombination lifetime for quasi-type II CdSe/CdS and type I CdSe/ZnS core/shell quantum dots. We find that the biexciton Auger recombination lifetime increases with the total nanocrystal volume for quasi-type II CdSe/CdS core/shell quantum dots and is independent of the shell thickness for type I CdSe/ZnS core/shell quantum dots. To perform these calculations and compute Auger recombination lifetimes, we developed a low-scaling approach based on the stochastic resolution of identity. The numerical approach provided a framework for studying the scaling of the biexciton Auger recombination lifetimes in terms of the shell thickness dependencies of the exciton radii, Coulomb couplings, and density of final states in quasi-type II CdSe/CdS and type I CdSe/ZnS core/shell quantum dots.
UR - http://www.scopus.com/inward/record.url?scp=85087528735&partnerID=8YFLogxK
U2 - 10.1021/acs.jpclett.0c01460
DO - 10.1021/acs.jpclett.0c01460
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C2 - 32513003
AN - SCOPUS:85087528735
SN - 1948-7185
VL - 11
SP - 5132
EP - 5138
JO - Journal of Physical Chemistry Letters
JF - Journal of Physical Chemistry Letters
IS - 13
ER -