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Title: Direct Measurements of Magnetic Polarons in Cd1–xMnx Se Nanocrystals from Resonant Photoluminescence

Journal Article · · Nano Letters
 [1];  [2]; ORCiD logo [3];  [4]; ORCiD logo [2]; ORCiD logo [2]
  1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Univ. of Wyoming, Laramie, WY (United States). Dept. of Physics and Astronomy
  2. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  3. Univ. degli Studi di Milano (Italy). Dipartimento di Scienza dei Materiali
  4. Technische Univ., Dortmund (Germany); Russian Academy of Sciences (RAS), St. Petersburg (Russian Federation). Ioffe Physical Technical Inst.

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.

Research Organization:
Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC52-06NA25396
OSTI ID:
1364552
Report Number(s):
LA-UR-17-20406
Journal Information:
Nano Letters, Vol. 17, Issue 5; ISSN 1530-6984
Publisher:
American Chemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 29 works
Citation information provided by
Web of Science

References (45)

High-Quality Manganese-Doped ZnSe Nanocrystals journal January 2001
Organometallic Synthesis and Spectroscopic Characterization of Manganese-Doped CdSe Nanocrystals journal March 2000
Giant internal magnetic fields in Mn doped nanocrystal quantum dots journal May 2000
Doping semiconductor nanocrystals journal July 2005
Mn 2 + as a Radial Pressure Gauge in Colloidal Core/Shell Nanocrystals journal December 2007
Optical properties of manganese-doped nanocrystals of ZnS journal January 1994
Mn 2+ -Doped CdSe Quantum Dots: New Inorganic Materials for Spin-Electronics and Spin-Photonics journal December 2008
Tunable magnetic exchange interactions in manganese-doped inverted core–shell ZnSe–CdSe nanocrystals journal December 2008
Diluted magnetic semiconductors journal August 1988
Giant Zeeman splitting in nucleation-controlled doped CdSe:Mn2+ quantum nanoribbons journal November 2009
Quantum Confinement-Controlled Exchange Coupling in Manganese(II)-Doped CdSe Two-Dimensional Quantum Well Nanoribbons journal September 2012
Time-resolved photoluminescence study of CdSe/CdMnS/CdS core/multi-shell nanoplatelets journal June 2016
Magnetic polarons in a single diluted magnetic semiconductor quantum dot journal September 2000
Dynamical Spin Response in Semimagnetic Quantum Dots journal December 2001
Monitoring Statistical Magnetic Fluctuations on the Nanometer Scale journal August 2002
Longitudinal and transverse fluctuations of magnetization of the excitonic magnetic polaron in a semimagnetic single quantum dot journal November 2003
Optically-induced magnetization of CdMnTe self-assembled quantum dots journal April 2004
Probing the Spin State of a Single Magnetic Ion in an Individual Quantum Dot journal November 2004
Microluminescence from Cd 1 − x Mn x Te magnetic quantum dots containing only a few Mn ions journal April 2007
Tailoring Magnetism in Quantum Dots journal May 2007
Robust magnetic polarons in type-II (Zn,Mn)Te/ZnSe magnetic quantum dots journal November 2010
Quantum Interference in Exciton-Mn Spin Interactions in a CdTe Semiconductor Quantum Dot journal November 2011
Magnetic polaron formation and exciton spin relaxation in single Cd 1 x Mn x Te quantum dots journal February 2011
Designing quantum dots for solotronics journal January 2014
Exciton magnetic polaron in semimagnetic semiconductor nanocrystals journal April 1997
Light-Induced Spontaneous Magnetization in Doped Colloidal Quantum Dots journal August 2009
Picosecond Dynamics of Excitonic Magnetic Polarons in Colloidal Diffusion-Doped Cd 1– x Mn x Se Quantum Dots journal October 2015
Revealing giant internal magnetic fields due to spin fluctuations in magnetically doped colloidal nanocrystals journal November 2015
Dynamics of Spin Organization in Diluted Magnetic Semiconductors journal January 1995
Exciton localization in semimagnetic semiconductors probed by magnetic polarons journal December 1999
Picosecond time-resolved photoluminescence studies of exciton-magnetic polaron complexes in Cd1−xMnxSe journal September 1985
Magnetic polaron formation of localized excitons in semimagnetic semiconductor alloys of Cd0.8Mn0.2Te journal December 1987
Two dimensional exciton magnetic polaron in CdTe/Cd1−xMnxTe quantum well structures journal April 1992
Localized exciton magnetic polarons in Cd 1 x Mn x Te journal April 1994
Exciton magnetic polarons in the semimagnetic alloys Cd 1 x y Mn x Mg y Te journal November 1994
Exciton localization by magnetic polarons and alloy fluctuations in the diluted magnetic semiconductor Cd 1 x Mn x Te journal February 1995
Dynamics of excitonic magnetic polarons in nanostructure diluted magnetic semiconductors journal November 1999
Exciton magnetic polarons in (100)- and (120)-oriented semimagnetic digital alloys (Cd,Mn)Te journal August 1998
Bound magnetic polarons in the very dilute regime journal February 2008
Spectrally Resolved Dynamics of Energy Transfer in Quantum-Dot Assemblies: Towards Engineered Energy Flows in Artificial Materials journal October 2002
Förster energy transfer of dark excitons enhanced by a magnetic field in an ensemble of CdTe colloidal nanocrystals journal September 2015
Size dependence of exciton fine structure in CdSe quantum dots journal June 1996
Observation of the "Dark Exciton" in CdSe Quantum Dots journal November 1995
Bright-exciton fine structure and anisotropic exchange in CdSe nanocrystal quantum dots journal June 2006
Kinetic Exchange between the Conduction Band Electrons and Magnetic Ions in Quantum-Confined Structures journal August 1999

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Light Emitting Spin Active Electronic States in Ultra-Thin Mn Doped CdSe Layered Nanosheets journal February 2019
Mechanism of Mn emission: Energy transfer vs charge transfer dynamics in Mn-doped quantum dots journal February 2020
Short range proximity effect induced by exchange interaction in tunnel-coupled CdTe and (Cd,Mn)Te quantum wells journal January 2020
Spin Physics of Excitons in Colloidal Nanocrystals journal August 2018
Controlling Quantum Confinement and Magnetic Doping of Cesium Lead Halide Perovskite Nanocrystals journal November 2018