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

Abstract

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.

Authors:
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
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
OSTI Identifier:
1427537
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
ACS Nano
Additional Journal Information:
Journal Volume: 11; Journal Issue: 9; Journal ID: ISSN 1936-0851
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; CdSe/CdS nanoplatelets; biexciton; exciton coherent motion area; quasi-2D exciton; radiative lifetime; second-order photon correlation function

Citation Formats

Ma, Xuedan, Diroll, Benjamin T., Cho, Wooje, Fedin, Igor, Schaller, Richard D., Talapin, Dmitri V., Gray, Stephen K., Wiederrecht, Gary P., and Gosztola, David J.. Size-Dependent Biexciton Quantum Yields and Carrier Dynamics of Quasi-Two-Dimensional Core/Shell Nanoplatelets. United States: N. p., 2017. Web. https://doi.org/10.1021/acsnano.7b03943.
Ma, Xuedan, Diroll, Benjamin T., Cho, Wooje, Fedin, Igor, Schaller, Richard D., Talapin, Dmitri V., Gray, Stephen K., Wiederrecht, Gary P., & Gosztola, David J.. Size-Dependent Biexciton Quantum Yields and Carrier Dynamics of Quasi-Two-Dimensional Core/Shell Nanoplatelets. United States. https://doi.org/10.1021/acsnano.7b03943
Ma, Xuedan, Diroll, Benjamin T., Cho, Wooje, Fedin, Igor, Schaller, Richard D., Talapin, Dmitri V., Gray, Stephen K., Wiederrecht, Gary P., and Gosztola, David J.. Tue . "Size-Dependent Biexciton Quantum Yields and Carrier Dynamics of Quasi-Two-Dimensional Core/Shell Nanoplatelets". United States. https://doi.org/10.1021/acsnano.7b03943. https://www.osti.gov/servlets/purl/1427537.
@article{osti_1427537,
title = {Size-Dependent Biexciton Quantum Yields and Carrier Dynamics of Quasi-Two-Dimensional Core/Shell Nanoplatelets},
author = {Ma, Xuedan and Diroll, Benjamin T. and Cho, Wooje and Fedin, Igor and Schaller, Richard D. and Talapin, Dmitri V. and Gray, Stephen K. and Wiederrecht, Gary P. and Gosztola, David J.},
abstractNote = {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.},
doi = {10.1021/acsnano.7b03943},
journal = {ACS Nano},
number = 9,
volume = 11,
place = {United States},
year = {2017},
month = {8}
}

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