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Title: Semiconductor Nanoplatelet Excimers

Abstract

Excimers, a portmanteau of "excited dimer", are transient species that are formed from the electronic interaction of a fluorophore in the excited state with a neighbor in the ground state, which have found extensive use as laser gain media. Although common in molecular fluorophores, this work presents evidence for the formation of excimers in a new class of materials: atomically precise two-dimensional semiconductor nanoplatelets. Colloidal nanoplatelets of CdSe display two-color photoluminescence resolved at low temperatures with one band attributed to band-edge fluorescence and a second, red band attributed to excimer fluorescence. Previously reasonable explanations for two-color fluorescence, such as charging, are shown to be inconsistent with additional evidence. As with excimers in other materials systems, excimer emission is increased by increasing nanoplatelet concentration and the degree of cofacial stacking. Consistent with their promise as low-threshold gain media, amplified spontaneous emission emerges from the excimer emission line.

Authors:
ORCiD logo [1]; ORCiD logo [2];  [2];  [3]; ORCiD logo [4];  [5]; ORCiD logo [6]; ORCiD logo [3];  [5]; ORCiD logo [2]; ORCiD logo [7]
  1. Argonne National Lab. (ANL), Argonne, IL (United States). Center for Nanoscale Materials
  2. Univ. of Chicago, IL (United States). Dept. of Chemistry
  3. Northwestern Univ., Evanston, IL (United States). Dept. of Chemistry; Northwestern Univ., Evanston, IL (United States). Inst. for Sustainability and Energy
  4. Northwestern Univ., Evanston, IL (United States). Dept. of Chemistry
  5. Univ. of Chicago, IL (United States). Center for Advanced Radiation Sources (CARS)
  6. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  7. Argonne National Lab. (ANL), Argonne, IL (United States). Center for Nanoscale Materials; Northwestern Univ., Evanston, IL (United States). Dept. of Chemistry; Northwestern Univ., Evanston, IL (United States). Inst. for Sustainability and Energy
Publication Date:
Research Org.:
Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
National Science Foundation (NSF); USDOE Office of Science (SC); US Air Force Office of Scientific Research (AFOSR); USDOD
OSTI Identifier:
1479966
Alternate Identifier(s):
OSTI ID: 1494796
Report Number(s):
LA-UR-18-28426
Journal ID: ISSN 1530-6984
Grant/Contract Number:  
AC52-06NA25396; AC02-06CH11357; DGE-1324585; FA9550-15-1-0099; DMR-1710104; EAR-1634415; FG02-94ER14466; EAR-1531583
Resource Type:
Accepted Manuscript
Journal Name:
Nano Letters
Additional Journal Information:
Journal Volume: 18; Journal Issue: 11; Journal ID: ISSN 1530-6984
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
74 ATOMIC AND MOLECULAR PHYSICS; High Magnetic Field Science; amplified spontaneous emission; Excimer; nanoplatelet; photoluminescence; two-dimensional

Citation Formats

Diroll, Benjamin T., Cho, Wooje, Coropceanu, Igor, Harvey, Samantha M., Brumberg, Alexandra, Holtgrewe, Nicholas, Crooker, Scott A., Wasielewski, Michael R., Prakapenka, Vitali B., Talapin, Dmitri V., and Schaller, Richard D.. Semiconductor Nanoplatelet Excimers. United States: N. p., 2018. Web. https://doi.org/10.1021/acs.nanolett.8b02865.
Diroll, Benjamin T., Cho, Wooje, Coropceanu, Igor, Harvey, Samantha M., Brumberg, Alexandra, Holtgrewe, Nicholas, Crooker, Scott A., Wasielewski, Michael R., Prakapenka, Vitali B., Talapin, Dmitri V., & Schaller, Richard D.. Semiconductor Nanoplatelet Excimers. United States. https://doi.org/10.1021/acs.nanolett.8b02865
Diroll, Benjamin T., Cho, Wooje, Coropceanu, Igor, Harvey, Samantha M., Brumberg, Alexandra, Holtgrewe, Nicholas, Crooker, Scott A., Wasielewski, Michael R., Prakapenka, Vitali B., Talapin, Dmitri V., and Schaller, Richard D.. Mon . "Semiconductor Nanoplatelet Excimers". United States. https://doi.org/10.1021/acs.nanolett.8b02865. https://www.osti.gov/servlets/purl/1479966.
@article{osti_1479966,
title = {Semiconductor Nanoplatelet Excimers},
author = {Diroll, Benjamin T. and Cho, Wooje and Coropceanu, Igor and Harvey, Samantha M. and Brumberg, Alexandra and Holtgrewe, Nicholas and Crooker, Scott A. and Wasielewski, Michael R. and Prakapenka, Vitali B. and Talapin, Dmitri V. and Schaller, Richard D.},
abstractNote = {Excimers, a portmanteau of "excited dimer", are transient species that are formed from the electronic interaction of a fluorophore in the excited state with a neighbor in the ground state, which have found extensive use as laser gain media. Although common in molecular fluorophores, this work presents evidence for the formation of excimers in a new class of materials: atomically precise two-dimensional semiconductor nanoplatelets. Colloidal nanoplatelets of CdSe display two-color photoluminescence resolved at low temperatures with one band attributed to band-edge fluorescence and a second, red band attributed to excimer fluorescence. Previously reasonable explanations for two-color fluorescence, such as charging, are shown to be inconsistent with additional evidence. As with excimers in other materials systems, excimer emission is increased by increasing nanoplatelet concentration and the degree of cofacial stacking. Consistent with their promise as low-threshold gain media, amplified spontaneous emission emerges from the excimer emission line.},
doi = {10.1021/acs.nanolett.8b02865},
journal = {Nano Letters},
number = 11,
volume = 18,
place = {United States},
year = {2018},
month = {9}
}

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Cited by: 6 works
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Figures / Tables:

Figure 1 Figure 1: (a) Room temperature absorption (dashed lines) and PL (solid lines) of 3, 4, 5, and 6 ML CdSe NPLs prepared as solid dropcast films. (b) Corresponding absorption and PL of the same samples collected at 3 K. (c) PL from frozen solutions of 3, 4, 5, and 6more » ML CdSe NPLs at 80 K. (d) Raman spectra from the same samples as in (c). Raman spectra were collected with 479 nm light above the band gap for 4, 5, and 6 ML NPLs but not 3 ML NPLs.« less

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