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题名: Superposition Principle in Auger Recombination of Charged and Neutral Multicarrier States in Semiconductor Quantum Dots
作者: Wu, Kaifeng1, 2;  Lim, Jaehoon1;  Klimov, Victor I.1
关键词: colloidal quantum dots ;  positively and negatively charged quantum dots ;  Auger recombination ;  multiexcitons ;  positive and negative trions
刊名: ACS NANO
发表日期: 2017-08-01
DOI: 10.1021/acsnano.7b04079
卷: 11, 期:8, 页:8437-8447
收录类别: SCI
文章类型: Article
WOS标题词: Science & Technology ;  Physical Sciences ;  Technology
类目[WOS]: Chemistry, Multidisciplinary ;  Chemistry, Physical ;  Nanoscience & Nanotechnology ;  Materials Science, Multidisciplinary
研究领域[WOS]: Chemistry ;  Science & Technology - Other Topics ;  Materials Science
英文摘要: Application of colloidal semiconductor quantum dots (QDs) in optical and optoelectronic devices is often complicated by unintentional generation of extra charges, which opens fast nonradiative Auger recombination pathways whereby the recombination energy of an exciton is quickly transferred to the extra carrier(s) and ultimately dissipated as heat. Previous studies of Auger recombination have primarily focused on neutral and, more recently, negatively charged multicarrier states. Auger dynamics of positively charged species remains more poorly explored due to difficulties in creating, stabilizing, and detecting excess holes in the QDs. Here we apply photochemical doping to prepare both negatively and positively charged CdSe/CdS QDs with two distinct core/shell interfacial profiles ("sharp" versus "smooth"). Using neutral and charged QD samples we evaluate Auger lifetimes of biexcitons, "negative and positive trions (an exciton with an extra electron or a hole, respectively), and multiply negatively charged excitons. Using these measurements, we demonstrate that Auger decay of both neutral and charged multicarrier states can be presented as" a superposition of independent elementary three=partide Auger events. As one of the manifestations of the superposition principle, we observe that the biexciton Auger decay rate can be presented as a sum of the Auger rates for independent negative and positive trion pathways. By comparing the measurements on the QDs with the "sharp" versus "smooth" interfaces, we also find that while affecting the absolute values of Auger lifetimes, manipulation of the shape of the confinement potential does not lead to violation of the superposition principle, which still allows us to accurately predict the biexciton Auger lifetimes based on the measured negative and positive trion dynamics. These findings indicate considerable robustness of the superposition principle as applied to Auger decay of charged and" neutral multicarrier states, suggesting its generality to quantum-confined nanocrystals of arbitrary compositions and complexities.
关键词[WOS]: LIGHT-EMITTING-DIODES ;  CORE-SHELL INTERFACE ;  HOT-CARRIER TRANSFER ;  CDSE NANOCRYSTALS ;  BLINKING ;  MULTIPLICATION ;  BIEXCITONS ;  SUPPRESSION ;  PERFORMANCE ;  EXCITATION
语种: 英语
WOS记录号: WOS:000408520900098
Citation statistics: 
内容类型: 期刊论文
URI标识: http://cas-ir.dicp.ac.cn/handle/321008/149890
Appears in Collections:中国科学院大连化学物理研究所_期刊论文

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作者单位: 1.Los Alamos Natl Lab, Chem Div, Los Alamos, NM 87545 USA
2.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Mol React Dynam & Collaborat Innova, 457 Zhongshan Rd, Dalian 116023, Peoples R China

Recommended Citation:
Wu, Kaifeng,Lim, Jaehoon,Klimov, Victor I.. Superposition Principle in Auger Recombination of Charged and Neutral Multicarrier States in Semiconductor Quantum Dots[J]. ACS NANO,2017,11(8):8437-8447.
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