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Brodu, A.; Ballottin, M.V.; Buhot, J.; van Harten, E.J.; Dupont, D.; La Porta, A.; Prins, P.T.; Tessier, M.D.; Versteegh, M.A.M.; Zwiller, V.; Bals, S.; Hens, Z.; Rabouw, F.T.; Christianen, P.C.M.; de Donega, C.M.; Vanmaekelbergh, D. |
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Title |
Exciton Fine Structure and Lattice Dynamics in InP/ZnSe Core/Shell Quantum Dots |
Type |
A1 Journal article |
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Year |
2018 |
Publication |
ACS Photonics |
Abbreviated Journal |
Acs Photonics |
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Volume |
5 |
Issue |
5 |
Pages |
3353-3362 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
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. |
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Wos |
000442185900049 |
Publication Date |
2018-07-18 |
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Edition |
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ISSN |
2330-4022 |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
6.756 |
Times cited |
40 |
Open Access |
OpenAccess |
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Notes |
; We acknowledge the support of the HFML-RU/FOM, member of the European Magnetic Field Laboratory (EMFL). D.V. and Z.H. acknowledge support by the European Commission via the Marie-Sklodowska Curie action Phonsi (H2020-MSCA-ITN-642656) and the Marie Sklodowska-Curie Action Compass (H2020 MSCA-RISE-691185). Z.H. acknowledges the Research Foundation Flanders (project 17006602) and Ghent University (GOA no. 01G01513). Z.H. and S.B. acknowledge SIM vzw (SBO-QDOCCO). F.T.R. acknowledges financial support from The Netherlands Organisation for Scientific Research NWO (Gravitation program Multiscale Catalytic Energy Conversion and VENI grant number 722.017.002). This work was also supported by the Dutch NWO-Physics Program DDC13, ERC Advanced Grant 692691 “First step”, and ERC Starting Grant 335078 “COLOURATOM”. ; ecas_sara |
Approved |
Most recent IF: 6.756 |
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Call Number |
UA @ lucian @ c:irua:153753UA @ admin @ c:irua:153753 |
Serial |
5100 |
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