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Title: Size-Dependent Biexciton Quantum Yields and Carrier Dynamics of Quasi-Two-Dimensional Core/Shell Nanoplatelets

Journal Article · · ACS Nano
ORCiD logo [1]; ORCiD logo [1];  [2];  [2]; ORCiD logo [3]; ORCiD logo [4];  [1];  [1];  [1]
  1. Argonne National Lab. (ANL), Argonne, IL (United States). Center for Nanoscale Materials
  2. Univ. of Chicago, IL (United States). James Franck Inst., Dept. of Chemistry
  3. Argonne National Lab. (ANL), Argonne, IL (United States). Center for Nanoscale Materials; Northwestern Univ., Evanston, IL (United States). Dept. of Chemistry
  4. Argonne National Lab. (ANL), Argonne, IL (United States). Center for Nanoscale Materials; Univ. of Chicago, IL (United States). James Franck Inst., Dept. of Chemistry

Quasi-two-dimensional nanoplatelets (NPLs) possess fundamentally different excitonic properties from zero-dimensional quantum dots. We study lateral size-dependent photon emission statistics and carrier dynamics of individual NPLs using second-order photon correlation (g(2)(τ)) spectroscopy and photoluminescence (PL) intensity-dependent lifetime analysis. Room-temperature radiative lifetimes of NPLs can be derived from maximum PL intensity periods in PL time traces. It first decreases with NPL lateral size and then stays constant, deviating from the electric dipole approximation. Analysis of the PL time traces further reveals that the single exciton quantum yield in NPLs decreases with NPL lateral size and increases with protecting shell thickness, indicating the importance of surface passivation on NPL emission quality. Second-order photon correlation (g(2)(τ)) studies of single NPLs show that the biexciton quantum yield is strongly dependent on the lateral size and single exciton quantum yield of the NPLs. In large NPLs with unity single exciton quantum yield, the corresponding biexciton quantum yield can reach unity. In conclusion, these findings reveal that by careful growth control and core–shell material engineering, NPLs can be of great potential for light amplification and integrated quantum photonic applications.

Research Organization:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
Grant/Contract Number:
AC02-06CH11357
OSTI ID:
1427537
Journal Information:
ACS Nano, Vol. 11, Issue 9; ISSN 1936-0851
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 59 works
Citation information provided by
Web of Science

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Low‐Threshold Amplified Spontaneous Emission and Lasing from Thick‐Shell CdSe/CdS Core/Shell Nanoplatelets Enabled by High‐Temperature Growth journal December 2019
Influence of morphology on the blinking mechanisms and the excitonic fine structure of single colloidal nanoplatelets journal January 2018
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