Reduction of fluorescence resonance energy transfer by space control between quantum dots via direct bonding of reactive ligands to the polymer matrix for color conversion films

Changmin Lee; Bokyoung Kim; Hoseok Jin; Hyungsuk Moon; Jungwoo Kim; Heeyeop Chae

doi:10.1364/JOSAB.36.001479

Journal of the Optical Society of America B
Vol. 36,
Issue 6,
pp. 1479-1484
(2019)
•https://doi.org/10.1364/JOSAB.36.001479

Reduction of fluorescence resonance energy transfer by space control between quantum dots via direct bonding of reactive ligands to the polymer matrix for color conversion films

Changmin Lee, Bokyoung Kim, Hoseok Jin, Hyungsuk Moon, Jungwoo Kim, and Heeyeop Chae

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Changmin Lee, Bokyoung Kim, Hoseok Jin, Hyungsuk Moon, Jungwoo Kim, and Heeyeop Chae, "Reduction of fluorescence resonance energy transfer by space control between quantum dots via direct bonding of reactive ligands to the polymer matrix for color conversion films," J. Opt. Soc. Am. B 36, 1479-1484 (2019)

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Table of Contents Category
- Quantum Optics
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About this Article
History
- Original Manuscript: March 11, 2019
- Revised Manuscript: April 14, 2019
- Manuscript Accepted: April 21, 2019
- Published: May 14, 2019

Abstract

Fluorescence resonance energy transfer (FRET) between quantum dots (QDs) is one of main mechanisms that cause efficiency to drop in photoluminescence (PL) applications. In this work, we reduced FRET by controlling the distance between the QDs via chemical reactions between the QD ligands and long-chain linkers. The oleic acid ligands of the QDs were replaced with ligands containing reactive alcohol groups without any degradation in the quantum yield by a one-pot reaction. The alcohol groups of the QD ligands were reacted with polycaprolactone diol, which acted as a spacer, and tris(isocyanatohexyl)cyanurate to form cross-linked urethane bonds. The interconnected QD film showed 26% higher quantum efficiency and 19% longer PL decay time than that of a conventional film in which the QDs were randomly embedded in PMMA. The interconnection of the designed QD and the long spacer with the cross-linker is believed to prevent FRET between QDs and enhance the quantum yield of the QD films.

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	6-Mercaptohexanol	1-Octanethiol	Ratio
Analyzed value (by ${}^{1}H$ -NMR integration)	1(Integration value of the peak at 3.6 ppm)	2.33(Integration value of the peak at 0.95 ppm)	2.33
Amount supplied	29.2 mmol	46.1 mmol	1.58
Number of protons at hydroxyl containing carbon or terminal carbon.	2 (protons at hydroxyl containing carbon)	3 (protons at the terminal carbon)	–
Experimentally supplied value	$29.2 mmol \times 2 = 58.4$ (A)	$46.1 mmol \times 3 = 138.3$ (B)	2.37 (B/A)

Component	Mass (g)	MW	mmol	No. of Functional Groups	Total Functional Group ( $mmol \times no. of Groups$ )
Alcohol-group-substituted QDs	0.33	–	0.26	1	0.26
Poly- $ε$ -caprolactone diol	1.80	1000	1.80	2	3.60
Tris(isocyanatohexyl)cyanurate	0.65	504.58	1.29	3	3.86

Sample ID	Absolute PL QY (%)	Emission $λ_{\max}$ (nm)	Thickness (μm)
Oleic-acid-capped QDs in solution	91.0	529.3	–
QDs with alcohol ligands in solution	92.0	529.5	–
QD with alcohol ligands in a balanced urethane film	40.8	533.5	2.01
QD with alcohol ligands in an unbalanced urethane film	35.1	534.9	1.92
QD with alcohol ligands blended in PMMA	31.6	536.3	2.21

Sample	$A_{1}$ (%)	$τ_{1}$ (ns)	$A_{2}$ (%)	$τ_{2}$ (ns)	$τ_{ave}$ (ns)
QDs with alcohol ligands in solution	90.5	10.1	9.5	34.6	12.4
QD with alcohol ligands in a balanced urethane film	91.4	6.58	8.6	22.4	7.93
QD with alcohol ligands in an unbalanced urethane film	91.9	6.12	8.1	22.2	7.42
QD with alcohol ligands blended in PMMA	94.3	5.85	5.7	20.3	6.67

	6-Mercaptohexanol	1-Octanethiol	Ratio
Analyzed value (by ${}^{1}H$ -NMR integration)	1(Integration value of the peak at 3.6 ppm)	2.33(Integration value of the peak at 0.95 ppm)	2.33
Amount supplied	29.2 mmol	46.1 mmol	1.58
Number of protons at hydroxyl containing carbon or terminal carbon.	2 (protons at hydroxyl containing carbon)	3 (protons at the terminal carbon)	–
Experimentally supplied value	$29.2 mmol \times 2 = 58.4$ (A)	$46.1 mmol \times 3 = 138.3$ (B)	2.37 (B/A)

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Journal of the Optical Society of America B