Direct Measurements of Magnetic Polarons in Cd1–xMnx Se Nanocrystals from Resonant Photoluminescence
Abstract
In semiconductors, quantum confinement can greatly enhance the interaction between band carriers (electrons and holes) and dopant atoms. One manifestation of this enhancement is the increased stability of exciton magnetic polarons in magnetically doped nanostructures. In the limit of very strong 0D confinement that is realized in colloidal semiconductor nanocrystals, a single exciton can exert an effective exchange field Bex on the embedded magnetic dopants that exceeds several tesla. Here we use the very sensitive method of resonant photoluminescence (PL) to directly measure the presence and properties of exciton magnetic polarons in colloidal Cd1–xMnxSe nanocrystals. Despite small Mn2+ concentrations (x = 0.4–1.6%), large polaron binding energies up to ~26 meV are observed at low temperatures via the substantial Stokes shift between the pump laser and the resonant PL maximum, indicating nearly complete alignment of all Mn2+ spins by Bexex ≈ 10 T in these nanocrystals, in good agreement with theoretical estimates. Further, the emission line widths provide direct insight into the statistical fluctuations of the Mn2+ spins. In conclusion, these resonant PL studies provide detailed insight into collective magnetic phenomena, especially in lightly doped nanocrystals where conventional techniques such as nonresonant PL or time-resolved PL provide ambiguous results.
- Authors:
-
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Univ. of Wyoming, Laramie, WY (United States). Dept. of Physics and Astronomy
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
- Univ. degli Studi di Milano (Italy). Dipartimento di Scienza dei Materiali
- Technische Univ., Dortmund (Germany); Russian Academy of Sciences (RAS), St. Petersburg (Russian Federation). Ioffe Physical Technical Inst.
- Publication Date:
- Research Org.:
- Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1364552
- Report Number(s):
- LA-UR-17-20406
Journal ID: ISSN 1530-6984
- Grant/Contract Number:
- AC52-06NA25396
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nano Letters
- Additional Journal Information:
- Journal Volume: 17; Journal Issue: 5; Journal ID: ISSN 1530-6984
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; 77 NANOSCIENCE AND NANOTECHNOLOGY; High Magnetic Field Science; nanocrystals, polaron
Citation Formats
Rice, W. D., Liu, W., Pinchetti, V., Yakovlev, D. R., Klimov, V. I., and Crooker, S. A. Direct Measurements of Magnetic Polarons in Cd1–xMnx Se Nanocrystals from Resonant Photoluminescence. United States: N. p., 2017.
Web. doi:10.1021/acs.nanolett.7b00421.
Rice, W. D., Liu, W., Pinchetti, V., Yakovlev, D. R., Klimov, V. I., & Crooker, S. A. Direct Measurements of Magnetic Polarons in Cd1–xMnx Se Nanocrystals from Resonant Photoluminescence. United States. https://doi.org/10.1021/acs.nanolett.7b00421
Rice, W. D., Liu, W., Pinchetti, V., Yakovlev, D. R., Klimov, V. I., and Crooker, S. A. Fri .
"Direct Measurements of Magnetic Polarons in Cd1–xMnx Se Nanocrystals from Resonant Photoluminescence". United States. https://doi.org/10.1021/acs.nanolett.7b00421. https://www.osti.gov/servlets/purl/1364552.
@article{osti_1364552,
title = {Direct Measurements of Magnetic Polarons in Cd1–xMnx Se Nanocrystals from Resonant Photoluminescence},
author = {Rice, W. D. and Liu, W. and Pinchetti, V. and Yakovlev, D. R. and Klimov, V. I. and Crooker, S. A.},
abstractNote = {In semiconductors, quantum confinement can greatly enhance the interaction between band carriers (electrons and holes) and dopant atoms. One manifestation of this enhancement is the increased stability of exciton magnetic polarons in magnetically doped nanostructures. In the limit of very strong 0D confinement that is realized in colloidal semiconductor nanocrystals, a single exciton can exert an effective exchange field Bex on the embedded magnetic dopants that exceeds several tesla. Here we use the very sensitive method of resonant photoluminescence (PL) to directly measure the presence and properties of exciton magnetic polarons in colloidal Cd1–xMnxSe nanocrystals. Despite small Mn2+ concentrations (x = 0.4–1.6%), large polaron binding energies up to ~26 meV are observed at low temperatures via the substantial Stokes shift between the pump laser and the resonant PL maximum, indicating nearly complete alignment of all Mn2+ spins by Bexex ≈ 10 T in these nanocrystals, in good agreement with theoretical estimates. Further, the emission line widths provide direct insight into the statistical fluctuations of the Mn2+ spins. In conclusion, these resonant PL studies provide detailed insight into collective magnetic phenomena, especially in lightly doped nanocrystals where conventional techniques such as nonresonant PL or time-resolved PL provide ambiguous results.},
doi = {10.1021/acs.nanolett.7b00421},
journal = {Nano Letters},
number = 5,
volume = 17,
place = {United States},
year = {Fri Apr 07 00:00:00 EDT 2017},
month = {Fri Apr 07 00:00:00 EDT 2017}
}
Web of Science
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