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Title: Probing Trions at Chemically Tailored Trapping Defects

Abstract

Trions, charged excitons that are reminiscent of hydrogen and positronium ions, have been intensively studied for energy harvesting, light-emitting diodes, lasing, and quantum computing applications because of their inherent connection with electron spin and dark excitons. However, these quasi-particles are typically present as a minority species at room temperature making it difficult for quantitative experimental measurements. Here, we show that by chemically engineering the well depth of sp3 quantum defects through a series of alkyl functional groups covalently attached to semiconducting carbon nanotube hosts, trions can be efficiently generated and localized at the trapping chemical defects. The exciton-electron binding energy of the trapped trion approaches 119 meV, which more than doubles that of “free” trions in the same host material (54 meV) and other nanoscale systems (2–45 meV). Magnetoluminescence spectroscopy suggests the absence of dark states in the energetic vicinity of trapped trions. Unexpectedly, the trapped trions are approximately 7.3-fold brighter than the brightest previously reported and 16 times as bright as native nanotube excitons, with a photoluminescence lifetime that is more than 100 times larger than that of free trions. These intriguing observations are understood by an efficient conversion of dark excitons to bright trions at the defect sites.more » This work makes trions synthetically accessible and uncovers the rich photophysics of these tricarrier quasi-particles, which may find broad implications in bioimaging, chemical sensing, energy harvesting, and light emitting in the short-wave infrared.« less

Authors:
ORCiD logo [1]; ORCiD logo [1];  [2]; ORCiD logo [3];  [4];  [1];  [2];  [5]; ORCiD logo [3]; ORCiD logo [3]; ORCiD logo [2]; ORCiD logo [6]
  1. Univ. of Maryland, College Park, MD (United States). Dept. of Chemistry and Biochemistry
  2. Ludwig Maximilian Univ. of Munich, Munich (Germany). Faculty of Physics
  3. Los Alamos National Lab. (LANL), Los Alamos, NM (United States). Center for Integrated Nanotechnologies (CINT)
  4. Fakultat für Physik, Center for NanoScience and Munich Quantum Center, Ludwig-Maximilians-Universitat München, Geschwister-Scholl-Platz 1, D-80539 München, Germany
  5. National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States). Joint Quantum Inst.
  6. Univ. of Maryland, College Park, MD (United States). Dept. of Chemistry and Biochemistry and Maryland NanoCenter
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); USDOE Laboratory Directed Research and Development (LDRD) Program; National Science Foundation (NSF); European Research Council (ERC); German Research Foundation (DFG); National Institutes of Health (NIH)
OSTI Identifier:
1688779
Report Number(s):
LA-UR-17-30363
Journal ID: ISSN 2374-7951
Grant/Contract Number:  
89233218CNA000001; PFIY-1839165; CHE-1507974; CHE-1904488; 336749; R01GM114167
Resource Type:
Accepted Manuscript
Journal Name:
ACS Central Science (Online)
Additional Journal Information:
Journal Name: ACS Central Science (Online); Journal Volume: 5; Journal Issue: 11; Journal ID: ISSN 2374-7951
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; excitons; binding energy; quantum mechanics; defects; carbon nanotubes

Citation Formats

Kwon, Hyejin, Kim, Mijin, Nutz, Manuel, Hartmann, Nicolai F., Perrin, Vivien, Meany, Brendan, Hofmann, Matthias S., Clark, Charles W., Htoon, Han, Doorn, Stephen K., Högele, Alexander, and Wang, YuHuang. Probing Trions at Chemically Tailored Trapping Defects. United States: N. p., 2019. Web. doi:10.1021/acscentsci.9b00707.
Kwon, Hyejin, Kim, Mijin, Nutz, Manuel, Hartmann, Nicolai F., Perrin, Vivien, Meany, Brendan, Hofmann, Matthias S., Clark, Charles W., Htoon, Han, Doorn, Stephen K., Högele, Alexander, & Wang, YuHuang. Probing Trions at Chemically Tailored Trapping Defects. United States. https://doi.org/10.1021/acscentsci.9b00707
Kwon, Hyejin, Kim, Mijin, Nutz, Manuel, Hartmann, Nicolai F., Perrin, Vivien, Meany, Brendan, Hofmann, Matthias S., Clark, Charles W., Htoon, Han, Doorn, Stephen K., Högele, Alexander, and Wang, YuHuang. Wed . "Probing Trions at Chemically Tailored Trapping Defects". United States. https://doi.org/10.1021/acscentsci.9b00707. https://www.osti.gov/servlets/purl/1688779.
@article{osti_1688779,
title = {Probing Trions at Chemically Tailored Trapping Defects},
author = {Kwon, Hyejin and Kim, Mijin and Nutz, Manuel and Hartmann, Nicolai F. and Perrin, Vivien and Meany, Brendan and Hofmann, Matthias S. and Clark, Charles W. and Htoon, Han and Doorn, Stephen K. and Högele, Alexander and Wang, YuHuang},
abstractNote = {Trions, charged excitons that are reminiscent of hydrogen and positronium ions, have been intensively studied for energy harvesting, light-emitting diodes, lasing, and quantum computing applications because of their inherent connection with electron spin and dark excitons. However, these quasi-particles are typically present as a minority species at room temperature making it difficult for quantitative experimental measurements. Here, we show that by chemically engineering the well depth of sp3 quantum defects through a series of alkyl functional groups covalently attached to semiconducting carbon nanotube hosts, trions can be efficiently generated and localized at the trapping chemical defects. The exciton-electron binding energy of the trapped trion approaches 119 meV, which more than doubles that of “free” trions in the same host material (54 meV) and other nanoscale systems (2–45 meV). Magnetoluminescence spectroscopy suggests the absence of dark states in the energetic vicinity of trapped trions. Unexpectedly, the trapped trions are approximately 7.3-fold brighter than the brightest previously reported and 16 times as bright as native nanotube excitons, with a photoluminescence lifetime that is more than 100 times larger than that of free trions. These intriguing observations are understood by an efficient conversion of dark excitons to bright trions at the defect sites. This work makes trions synthetically accessible and uncovers the rich photophysics of these tricarrier quasi-particles, which may find broad implications in bioimaging, chemical sensing, energy harvesting, and light emitting in the short-wave infrared.},
doi = {10.1021/acscentsci.9b00707},
journal = {ACS Central Science (Online)},
number = 11,
volume = 5,
place = {United States},
year = {2019},
month = {10}
}

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