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:

Kwon, Hyejin  ^[1];

• Search DOE PAGES for author "Kwon, Hyejin"
• Search DOE PAGES for ORCID "0000-0003-0548-6970"

Kim, Mijin  ^[1];

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• Search DOE PAGES for ORCID "0000-0002-7781-9466"

Nutz, Manuel ^[2]; Hartmann, Nicolai F.  ^[3];

• Search DOE PAGES for author "Hartmann, Nicolai F."
• Search DOE PAGES for ORCID "0000-0002-4174-532X"

Perrin, Vivien ^[4]; Meany, Brendan ^[1]; Hofmann, Matthias S. ^[2]; Clark, Charles W. ^[5]; Htoon, Han  ^[3];

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• Search DOE PAGES for ORCID "0000-0003-3696-2896"

Doorn, Stephen K.  ^[3];

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• Search DOE PAGES for ORCID "0000-0002-9535-2062"

Högele, Alexander  ^[2];

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• Search DOE PAGES for ORCID "0000-0002-0178-9117"

Wang, YuHuang  ^[6]

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• Search DOE PAGES for ORCID "0000-0002-5664-1849"

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+ Show Author Affiliations

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:

Wed Oct 16 00:00:00 EDT 2019

Research Org.:

Los Alamos National Laboratory (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