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Exciton Fine Structure and Lattice Dynamics in InP/ZnSe Core/Shell Quantum Dots
Univ Utrecht, Debye Inst Nanomat Sci, NL-3584 CC Utrecht, Netherlands..
Radboud Univ Nijmegen, High Field Magnet Lab, HFML EMFL, NL-6525 ED Nijmegen, Netherlands..
Radboud Univ Nijmegen, High Field Magnet Lab, HFML EMFL, NL-6525 ED Nijmegen, Netherlands..
Univ Utrecht, Debye Inst Nanomat Sci, NL-3584 CC Utrecht, Netherlands..
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2018 (English)In: ACS Photonics, E-ISSN 2330-4022, Vol. 5, no 8, p. 3353-3362Article in journal (Refereed) Published
Abstract [en]

Nanocrystalline InP quantum dots (QDs) hold promise for heavy-metal-free optoelectronic applications due to their bright and size tunable emission in the visible range. Photochemical stability and high photoluminescence (PL) quantum yield are obtained by a diversity of epitaxial shells around the InP core. To understand and optimize the emission line shapes, the exciton fine structure of InP core/shell QD systems needs be investigated. Here, we study the exciton fine structure of InP/ZnSe core/shell QDs with core diameters ranging from 2.9 to 3.6 nm (PL peak from 2.3 to 1.95 eV at 4 K). PL decay measurements as a function of temperature in the 10 mK to 300 K range show that the lowest exciton fine structure state is a dark state, from which radiative recombination is assisted by coupling to confined acoustic phonons with energies ranging from 4 to 7 meV, depending on the core diameter. Circularly polarized fluorescence line-narrowing (FLN) spectroscopy at 4 K under high magnetic fields (up to 30 T) demonstrates that radiative recombination from the dark F = +/- 2 state involves acoustic and optical phonons, from both the InP core and the ZnSe shell. Our data indicate that the highest intensity FLN peak is an acoustic phonon replica rather than a zero-phonon line, implying that the energy separation observed between the F = +/- 1 state and the highest intensity peak in the FLN spectra (6 to 16 meV, depending on the InP core size) is larger than the splitting between the dark and bright fine structure exciton states.

Place, publisher, year, edition, pages
American Chemical Society (ACS), 2018. Vol. 5, no 8, p. 3353-3362
Keywords [en]
exciton fine structure, InP/ZnSe core/shell quantum dots, acoustic and optical phonons, high magnetic field
National Category
Condensed Matter Physics
Identifiers
URN: urn:nbn:se:kth:diva-234626DOI: 10.1021/acsphotonics.8b00615ISI: 000442185900049PubMedID: 30175158Scopus ID: 2-s2.0-85050499716OAI: oai:DiVA.org:kth-234626DiVA, id: diva2:1247801
Note

QC 20180913

Available from: 2018-09-13 Created: 2018-09-13 Last updated: 2018-09-13Bibliographically approved

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Versteegh, Marijn A. M.Zwiller, Val

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