Tunable magnetic exchange interactions in manganese-doped inverted core-shell ZnSe-CdSe nanocrystals

David A. Bussian; Scott A. Crooker; Ming Yin; Marcin Brynda; Alexander L. Efros; Victor I. Klimov

doi:10.1038/nmat2342

Tunable magnetic exchange interactions in manganese-doped inverted core-shell ZnSe-CdSe nanocrystals

David A. Bussian, Scott A. Crooker, Ming Yin, Marcin Brynda, Alexander L. Efros, Victor I. Klimov

Los Alamos National Laboratory

Research output: Contribution to journal › Article › peer-review

190 Citations (Scopus)

Abstract

Magnetic doping of semiconductor nanostructures is actively pursued for applications in magnetic memory and spin-based electronics. Central to these efforts is a drive to control the interaction strength between carriers (electrons and holes) and the embedded magnetic atoms. In this respect, colloidal nanocrystal heterostructures provide great flexibility through growth-controlled 'engineering' of electron and hole wavefunctions in individual nanocrystals. Here, we demonstrate a widely tunable magnetic sp-d exchange interaction between electron-hole excitations (excitons) and paramagnetic manganese ions using 'inverted' core-shell nanocrystals composed of Mn 2+ -doped ZnSe cores overcoated with undoped shells of narrower-gap CdSe. Magnetic circular dichroism studies reveal giant Zeeman spin splittings of the band-edge exciton that, surprisingly, are tunable in both magnitude and sign. Effective exciton g-factors are controllably tuned from '200 to +30 solely by increasing the CdSe shell thickness, demonstrating that strong quantum confinement and wavefunction engineering in heterostructured nanocrystal materials can be used to manipulate carrier-Mn 2+ wavefunction overlap and the sp-d exchange parameters themselves.

Original language	English
Pages (from-to)	35-40
Number of pages	6
Journal	Nature materials
Volume	8
Issue number	1
DOIs	https://doi.org/10.1038/nmat2342
Publication status	Published - Jan 2009

ASJC Scopus subject areas

Chemistry(all)
Materials Science(all)
Condensed Matter Physics
Mechanics of Materials
Mechanical Engineering

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title = "Tunable magnetic exchange interactions in manganese-doped inverted core-shell ZnSe-CdSe nanocrystals",

abstract = "Magnetic doping of semiconductor nanostructures is actively pursued for applications in magnetic memory and spin-based electronics. Central to these efforts is a drive to control the interaction strength between carriers (electrons and holes) and the embedded magnetic atoms. In this respect, colloidal nanocrystal heterostructures provide great flexibility through growth-controlled 'engineering' of electron and hole wavefunctions in individual nanocrystals. Here, we demonstrate a widely tunable magnetic sp-d exchange interaction between electron-hole excitations (excitons) and paramagnetic manganese ions using 'inverted' core-shell nanocrystals composed of Mn 2+ -doped ZnSe cores overcoated with undoped shells of narrower-gap CdSe. Magnetic circular dichroism studies reveal giant Zeeman spin splittings of the band-edge exciton that, surprisingly, are tunable in both magnitude and sign. Effective exciton g-factors are controllably tuned from '200 to +30 solely by increasing the CdSe shell thickness, demonstrating that strong quantum confinement and wavefunction engineering in heterostructured nanocrystal materials can be used to manipulate carrier-Mn 2+ wavefunction overlap and the sp-d exchange parameters themselves.",

author = "Bussian, {David A.} and Crooker, {Scott A.} and Ming Yin and Marcin Brynda and Efros, {Alexander L.} and Klimov, {Victor I.}",

note = "Funding Information: We thank B. Prall for technical assistance. This work was supported by Los Alamos LDRD Funds and the Chemical Sciences, Biosciences, and Geosciences Division of the Office of Basic Energy Sciences, Office of Science, US Department of Energy (DOE). D.A.B. and V.I.K. are partially supported by the DOE Center for Integrated Nanotechnologies jointly operated by Los Alamos and Sandia National Laboratories. A.L.E. acknowledges financial support from ONR.",

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AU - Bussian, David A.

AU - Crooker, Scott A.

AU - Yin, Ming

AU - Brynda, Marcin

AU - Efros, Alexander L.

AU - Klimov, Victor I.

N1 - Funding Information: We thank B. Prall for technical assistance. This work was supported by Los Alamos LDRD Funds and the Chemical Sciences, Biosciences, and Geosciences Division of the Office of Basic Energy Sciences, Office of Science, US Department of Energy (DOE). D.A.B. and V.I.K. are partially supported by the DOE Center for Integrated Nanotechnologies jointly operated by Los Alamos and Sandia National Laboratories. A.L.E. acknowledges financial support from ONR.

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N2 - Magnetic doping of semiconductor nanostructures is actively pursued for applications in magnetic memory and spin-based electronics. Central to these efforts is a drive to control the interaction strength between carriers (electrons and holes) and the embedded magnetic atoms. In this respect, colloidal nanocrystal heterostructures provide great flexibility through growth-controlled 'engineering' of electron and hole wavefunctions in individual nanocrystals. Here, we demonstrate a widely tunable magnetic sp-d exchange interaction between electron-hole excitations (excitons) and paramagnetic manganese ions using 'inverted' core-shell nanocrystals composed of Mn 2+ -doped ZnSe cores overcoated with undoped shells of narrower-gap CdSe. Magnetic circular dichroism studies reveal giant Zeeman spin splittings of the band-edge exciton that, surprisingly, are tunable in both magnitude and sign. Effective exciton g-factors are controllably tuned from '200 to +30 solely by increasing the CdSe shell thickness, demonstrating that strong quantum confinement and wavefunction engineering in heterostructured nanocrystal materials can be used to manipulate carrier-Mn 2+ wavefunction overlap and the sp-d exchange parameters themselves.

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