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Title: Biexciton and trion energy transfer from CdSe/CdS giant nanocrystals to Si substrates

Abstract

Observation of energy transfer (ET) from multiexcitonic (MX) complexes in nanocrystal quantum dots (NQDs) has been severely restricted due to efficient nonradiative Auger recombination leading to very low MX emission quantum yields. Here we employed “giant” CdSe/CdS NQDs with suppressed Auger recombination to study ET of biexcitons (BX) and charged excitons (trions) into Si substrate. Photoluminescence (PL) measurements of (sub)monolayers of gNQDs controllably assembled on various interacting surfaces and augmented by single gNQD's imaging reveal appearance of BX spectral signatures and progressive acceleration of PL lifetimes of all excitonic species on Si substrates. From statistical analysis of a large number of PL lifetime traces, representative exciton, trion and BX ET efficiencies are measured as ~75%, 55% and 45% respectively. Detailed analysis of the MX's radiative rates demonstrate the crucial role of the radiative (waveguide) ET in maintaining high overall transfer efficiency despite the prevalent Auger recombination. Furthermore, our observations point towards practical utilization of MX-bearing nanocrystals in future optoelectronics architectures.

Authors:
 [1];  [1];  [1]; ORCiD logo [2];  [2]; ORCiD logo [2]; ORCiD logo [1];  [1]; ORCiD logo [1]
  1. The Univ. of Texas at Dallas, Richardson, TX (United States)
  2. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Publication Date:
Research Org.:
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1570617
Report Number(s):
LA-UR-18-28800
Journal ID: ISSN 2040-3364; NANOHL
Grant/Contract Number:  
89233218CNA000001
Resource Type:
Accepted Manuscript
Journal Name:
Nanoscale
Additional Journal Information:
Journal Volume: 9; Journal Issue: 48; Journal ID: ISSN 2040-3364
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; Material Science

Citation Formats

Guo, Tianle, Sampat, Siddharth, Rupich, Sara M., Hollingsworth, Jennifer A., Buck, Matthew, Htoon, Han, Chabal, Yves J., Gartstein, Yuri N., and Malko, Anton V. Biexciton and trion energy transfer from CdSe/CdS giant nanocrystals to Si substrates. United States: N. p., 2017. Web. doi:10.1039/C7NR06272A.
Guo, Tianle, Sampat, Siddharth, Rupich, Sara M., Hollingsworth, Jennifer A., Buck, Matthew, Htoon, Han, Chabal, Yves J., Gartstein, Yuri N., & Malko, Anton V. Biexciton and trion energy transfer from CdSe/CdS giant nanocrystals to Si substrates. United States. doi:10.1039/C7NR06272A.
Guo, Tianle, Sampat, Siddharth, Rupich, Sara M., Hollingsworth, Jennifer A., Buck, Matthew, Htoon, Han, Chabal, Yves J., Gartstein, Yuri N., and Malko, Anton V. Wed . "Biexciton and trion energy transfer from CdSe/CdS giant nanocrystals to Si substrates". United States. doi:10.1039/C7NR06272A. https://www.osti.gov/servlets/purl/1570617.
@article{osti_1570617,
title = {Biexciton and trion energy transfer from CdSe/CdS giant nanocrystals to Si substrates},
author = {Guo, Tianle and Sampat, Siddharth and Rupich, Sara M. and Hollingsworth, Jennifer A. and Buck, Matthew and Htoon, Han and Chabal, Yves J. and Gartstein, Yuri N. and Malko, Anton V.},
abstractNote = {Observation of energy transfer (ET) from multiexcitonic (MX) complexes in nanocrystal quantum dots (NQDs) has been severely restricted due to efficient nonradiative Auger recombination leading to very low MX emission quantum yields. Here we employed “giant” CdSe/CdS NQDs with suppressed Auger recombination to study ET of biexcitons (BX) and charged excitons (trions) into Si substrate. Photoluminescence (PL) measurements of (sub)monolayers of gNQDs controllably assembled on various interacting surfaces and augmented by single gNQD's imaging reveal appearance of BX spectral signatures and progressive acceleration of PL lifetimes of all excitonic species on Si substrates. From statistical analysis of a large number of PL lifetime traces, representative exciton, trion and BX ET efficiencies are measured as ~75%, 55% and 45% respectively. Detailed analysis of the MX's radiative rates demonstrate the crucial role of the radiative (waveguide) ET in maintaining high overall transfer efficiency despite the prevalent Auger recombination. Furthermore, our observations point towards practical utilization of MX-bearing nanocrystals in future optoelectronics architectures.},
doi = {10.1039/C7NR06272A},
journal = {Nanoscale},
number = 48,
volume = 9,
place = {United States},
year = {2017},
month = {11}
}

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