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Ligand dynamics and temperature effects upon formation of nanocomposites based on semiconductor CdSе/ZnS quantum dots and porphyrins: ensemble and single object measurements

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DOI
10.6060/mhc2012.120571z
Authors
Zenkevich, E. I.
Blaudeck, T.
Kowerko, D.
Stupak, A. P.
Cichos, F.
Borczyskowski, C. von
Date
2012
Bibliographic entry
Ligand dynamics and temperature effects upon formation of nanocomposites based on semiconductor CdSе/ZnS quantum dots and porphyrins: ensemble and single object measurements / E. I. Zenkevich [et al.] // Macroheterocycles. – 2012. – Vol. 5, № 2. – P. 98-114.
Abstract
Dye molecules with pyridyl side substituents (porphyrins and heterocyclic perylene diimides) coordinatively attached to semiconductor CdSe/ZnS quantum dots (QDs) surface form quasi-stable “QD-Dye” nanocomposites of various geometry in the competition with capping molecules (tri-n-octyl phosphine oxide or long chain amines) exchange. This results in photoluminescence (PL) quenching of the QDs both due to Foerster resonance energy transfer and formation of non-radiative surface states. QD surface is inhomogeneous with respect to the involved attachment and detachment processes. The formation of “QD-Porphyrin” nanocomposites is realized at least two time scales (60 and 600 s), which is attributed to a reorganisation of tri-n-octylphosphine oxide capping shell. In a low temperature range of 220÷240 K related changes in QD absorption and emission reveal a phase transition of the capping shell (tri-n-octyl phosphine oxide and amine). In “QD-Dye” nanocomposites, this phase transition is enhanced considerably by only a few attached dye molecules and has impact on the QD core structure followed by changes of PL quenching and exciton-phonon coupling. A combination of ensemble and single molecule spectroscopy of “QD-Dye” nanocomposites reveals that few or even only one attached dye molecule change the surface distribution and energy of dye related surface trap states considerably.
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https://rep.bntu.by/handle/data/30190
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