Quantum Shell in a Shell: Engineering Colloidal Nanocrystals for a High-Intensity Excitation Regime
Name
2352207.pdf
Description
Accepted version
Size
1.34 MB
Format
Adobe PDF
Checksum (MD5)
2ed9d3b40937bb382f107106fd85bab0
Author(s)
Harankahage, Dulanjan
Cassidy, James
Beavon, Jacob
Huang, Jiamin
Brown, Niamh
Berkinsky, David B
Marder, Andrew
Kayira, Barbra
Montemurri, Michael
Anzenbacher, Pavel
Date Issued
June 6, 2023
Journal
Journal of the American Chemical Society
Publisher
American Chemical Society
Citation
Quantum Shell in a Shell: Engineering Colloidal Nanocrystals for a High-Intensity Excitation Regime
Dulanjan Harankahage, James Cassidy, Jacob Beavon, Jiamin Huang, Niamh Brown, David B. Berkinsky, Andrew Marder, Barbra Kayira, Michael Montemurri, Pavel Anzenbacher, Richard D. Schaller, Liangfeng Sun, Moungi G. Bawendi, Anton V. Malko, Benjamin T. Diroll, and Mikhail Zamkov. Journal of the American Chemical Society 2023 145 (24), 13326-13334.
Version
Author's final manuscript
Abstract
Many optoelectronic processes in colloidal semiconductor nanocrystals (NCs) suffer an efficiency decline under high-intensity excitation. This issue is caused by Auger recombination of multiple excitons, which converts the NC energy into excess heat, reducing the efficiency and life span of NC-based devices, including photodetectors, X-ray scintillators, lasers, and high-brightness light-emitting diodes (LEDs). Recently, semiconductor quantum shells (QSs) have emerged as a promising NC geometry for the suppression of Auger decay; however, their optoelectronic performance has been hindered by surface-related carrier losses. Here, we address this issue by introducing quantum shells with a CdS-CdSe-CdS-ZnS core-shell-shell-shell multilayer structure. The ZnS barrier inhibits the surface carrier decay, which increases the photoluminescence (PL) quantum yield (QY) to 90% while retaining a high biexciton emission QY of 79%. The improved QS morphology allows demonstrating one of the longest Auger lifetimes reported for colloidal NCs to date. The reduction of nonradiative losses in QSs also leads to suppressed blinking in single nanoparticles and low-threshold amplified spontaneous emission. We expect that ZnS-encapsulated quantum shells will benefit many applications exploiting high-power optical or electrical excitation regimes.
MIT Department
Massachusetts Institute of Technology. Department of Chemistry
Terms of Use
Creative Commons Attribution-Noncommercial-ShareAlike
Persistent DSpace Link
DOI of Published Version
10.1021/jacs.3c03397
