Energy transfer from colloidal quantum dots to near-infrared-absorbing tetraazaporphyrins for enhanced light harvesting

Zhihua Xu, Feng Gao, Elena A. Makarova, Ahmed A Heikal, Victor N. Nemykin

Research output: Contribution to journalArticle

15 Citations (Scopus)

Abstract

We investigate the mechanisms of energy transfer from CdSe quantum dots (QDs) to porphyrin derivatives as a potential antenna system with enhanced light-harvesting efficiency. Two ferrocenyl-containing tetraazaporphyrin derivatives, namely, magnesium 2(3),7(8),12(13),17(18)-tetraferrocenyl-5,10,15,20-tetraazaporphyrin (TAPFcMg) and magnesium 2(3),7(8),12(13),17(18)-tetracyano-3(2),8(7),13(12),18(17)-tetraferrocenyl-5,10,15,20-tetraazaporphyrin (TAPFcCNMg), are used as energy acceptors in this proposed antenna system along with size-dependent QDs as donors. Our approach includes Förster resonance energy transfer (FRET) calculations as well as photoluminescence (PL) intensity and lifetime quenching measurements. Our FRET calculations indicate that higher energy transfer efficiency can be achieved with smaller quantum dot size. However, PL intensity and lifetime measurements suggest that energy transfer efficiency in QD/tetraazaporphyrin complexes is regulated by a competing trap-assisted ultrafast quenching mechanism, which is more dominant with smaller QD size. Furthermore, it is found that the trap-assisted quenching process is more active in QD/TAPFcMg than QD/TAPFcCNMg complexes. As a result, high efficiency energy transfer can be achieved in the complexes combining large QDs and TAPFcCNMg, where trap-assisted quenching mechanism is suppressed. Our study suggests that CdSe quantum dots can be promising energy transfer donors for NIR-absorbing tetraazaporphyrins to form antenna systems with enhanced light-harvesting efficiency.

Original languageEnglish (US)
Pages (from-to)9754-9761
Number of pages8
JournalJournal of Physical Chemistry C
Volume119
Issue number18
DOIs
StatePublished - May 7 2015

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Energy transfer
Semiconductor quantum dots
energy transfer
quantum dots
Infrared radiation
Quenching
quenching
antennas
traps
Antennas
Magnesium
magnesium
Photoluminescence
Derivatives
photoluminescence
life (durability)
Porphyrins
porphyrins

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Energy transfer from colloidal quantum dots to near-infrared-absorbing tetraazaporphyrins for enhanced light harvesting. / Xu, Zhihua; Gao, Feng; Makarova, Elena A.; Heikal, Ahmed A; Nemykin, Victor N.

In: Journal of Physical Chemistry C, Vol. 119, No. 18, 07.05.2015, p. 9754-9761.

Research output: Contribution to journalArticle

Xu, Zhihua ; Gao, Feng ; Makarova, Elena A. ; Heikal, Ahmed A ; Nemykin, Victor N. / Energy transfer from colloidal quantum dots to near-infrared-absorbing tetraazaporphyrins for enhanced light harvesting. In: Journal of Physical Chemistry C. 2015 ; Vol. 119, No. 18. pp. 9754-9761.
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abstract = "We investigate the mechanisms of energy transfer from CdSe quantum dots (QDs) to porphyrin derivatives as a potential antenna system with enhanced light-harvesting efficiency. Two ferrocenyl-containing tetraazaporphyrin derivatives, namely, magnesium 2(3),7(8),12(13),17(18)-tetraferrocenyl-5,10,15,20-tetraazaporphyrin (TAPFcMg) and magnesium 2(3),7(8),12(13),17(18)-tetracyano-3(2),8(7),13(12),18(17)-tetraferrocenyl-5,10,15,20-tetraazaporphyrin (TAPFcCNMg), are used as energy acceptors in this proposed antenna system along with size-dependent QDs as donors. Our approach includes F{\"o}rster resonance energy transfer (FRET) calculations as well as photoluminescence (PL) intensity and lifetime quenching measurements. Our FRET calculations indicate that higher energy transfer efficiency can be achieved with smaller quantum dot size. However, PL intensity and lifetime measurements suggest that energy transfer efficiency in QD/tetraazaporphyrin complexes is regulated by a competing trap-assisted ultrafast quenching mechanism, which is more dominant with smaller QD size. Furthermore, it is found that the trap-assisted quenching process is more active in QD/TAPFcMg than QD/TAPFcCNMg complexes. As a result, high efficiency energy transfer can be achieved in the complexes combining large QDs and TAPFcCNMg, where trap-assisted quenching mechanism is suppressed. Our study suggests that CdSe quantum dots can be promising energy transfer donors for NIR-absorbing tetraazaporphyrins to form antenna systems with enhanced light-harvesting efficiency.",
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AU - Gao, Feng

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AU - Heikal, Ahmed A

AU - Nemykin, Victor N.

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AB - We investigate the mechanisms of energy transfer from CdSe quantum dots (QDs) to porphyrin derivatives as a potential antenna system with enhanced light-harvesting efficiency. Two ferrocenyl-containing tetraazaporphyrin derivatives, namely, magnesium 2(3),7(8),12(13),17(18)-tetraferrocenyl-5,10,15,20-tetraazaporphyrin (TAPFcMg) and magnesium 2(3),7(8),12(13),17(18)-tetracyano-3(2),8(7),13(12),18(17)-tetraferrocenyl-5,10,15,20-tetraazaporphyrin (TAPFcCNMg), are used as energy acceptors in this proposed antenna system along with size-dependent QDs as donors. Our approach includes Förster resonance energy transfer (FRET) calculations as well as photoluminescence (PL) intensity and lifetime quenching measurements. Our FRET calculations indicate that higher energy transfer efficiency can be achieved with smaller quantum dot size. However, PL intensity and lifetime measurements suggest that energy transfer efficiency in QD/tetraazaporphyrin complexes is regulated by a competing trap-assisted ultrafast quenching mechanism, which is more dominant with smaller QD size. Furthermore, it is found that the trap-assisted quenching process is more active in QD/TAPFcMg than QD/TAPFcCNMg complexes. As a result, high efficiency energy transfer can be achieved in the complexes combining large QDs and TAPFcCNMg, where trap-assisted quenching mechanism is suppressed. Our study suggests that CdSe quantum dots can be promising energy transfer donors for NIR-absorbing tetraazaporphyrins to form antenna systems with enhanced light-harvesting efficiency.

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