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High-Yield Generation of Triplet Excited States by an Efficient Sequential Photoinduced Process from Energy Transfer to Singlet Fission in Pentacene-Modified CdSe/ZnS Quantum Dots

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High-Yield Generation of Triplet Excited States by an Efficient Sequential Photoinduced Process from Energy Transfer to Singlet Fission in Pentacene-Modified CdSe/ZnS Quantum Dots. / Sakai, Hayato; Inaya, Ryutaro; Tkachenko, Nikolai V.; Hasobe, Taku.

In: Chemistry - A European Journal, Vol. 24, No. 64, 16.11.2018, p. 17062-17071.

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@article{d79af2841d1f4c53ae4fb098f92105dc,
title = "High-Yield Generation of Triplet Excited States by an Efficient Sequential Photoinduced Process from Energy Transfer to Singlet Fission in Pentacene-Modified CdSe/ZnS Quantum Dots",
abstract = "Singlet fission (SF) is expected to improve photoenergy conversion systems by generating two electrons from one photon. Pentacenes meet the energy-level matching condition between a singlet and two triplet states: [E(S1)≥2E(T1)]. However, the molar absorption coefficients of pentacenes in the approximately 400–500 nm region are limited, whereas quantum dots, such as CdSe/ZnS (QD), possess high fluorescence quantum yields and particle-size-dependent fluorescence wavelengths. Thus, a combination of QD (D) and pentacene (A) provides a system of both an enhanced light-harvesting efficiency throughout the solar spectrum and an efficient conversion of the harvested light into the triplet states by SF. Based on these points, m-phenylene-bridged triisopropylsilane (TIPS)-pentacene dimer-functionalized QD (denoted as m-(Pc)2-QD) was synthesized to examine the sequential photoinduced process from energy transfer to SF. In femtosecond transient absorption measurements, initial energy transfer from QD to pentacene (quantum yield: 87 {\%}) and subsequent SF were efficiently observed. The quantum yield of triplet states of pentacene units (ΦΤ) based on the excitation of QD attained is 160±6.7 {\%}.",
keywords = "energy transfer, pentacene, quantum dot, sequential photophysical process, singlet fission",
author = "Hayato Sakai and Ryutaro Inaya and Tkachenko, {Nikolai V.} and Taku Hasobe",
year = "2018",
month = "11",
day = "16",
doi = "10.1002/chem.201803257",
language = "English",
volume = "24",
pages = "17062--17071",
journal = "Chemistry: A European Journal",
issn = "0947-6539",
publisher = "WILEY-V C H VERLAG GMBH",
number = "64",

}

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TY - JOUR

T1 - High-Yield Generation of Triplet Excited States by an Efficient Sequential Photoinduced Process from Energy Transfer to Singlet Fission in Pentacene-Modified CdSe/ZnS Quantum Dots

AU - Sakai, Hayato

AU - Inaya, Ryutaro

AU - Tkachenko, Nikolai V.

AU - Hasobe, Taku

PY - 2018/11/16

Y1 - 2018/11/16

N2 - Singlet fission (SF) is expected to improve photoenergy conversion systems by generating two electrons from one photon. Pentacenes meet the energy-level matching condition between a singlet and two triplet states: [E(S1)≥2E(T1)]. However, the molar absorption coefficients of pentacenes in the approximately 400–500 nm region are limited, whereas quantum dots, such as CdSe/ZnS (QD), possess high fluorescence quantum yields and particle-size-dependent fluorescence wavelengths. Thus, a combination of QD (D) and pentacene (A) provides a system of both an enhanced light-harvesting efficiency throughout the solar spectrum and an efficient conversion of the harvested light into the triplet states by SF. Based on these points, m-phenylene-bridged triisopropylsilane (TIPS)-pentacene dimer-functionalized QD (denoted as m-(Pc)2-QD) was synthesized to examine the sequential photoinduced process from energy transfer to SF. In femtosecond transient absorption measurements, initial energy transfer from QD to pentacene (quantum yield: 87 %) and subsequent SF were efficiently observed. The quantum yield of triplet states of pentacene units (ΦΤ) based on the excitation of QD attained is 160±6.7 %.

AB - Singlet fission (SF) is expected to improve photoenergy conversion systems by generating two electrons from one photon. Pentacenes meet the energy-level matching condition between a singlet and two triplet states: [E(S1)≥2E(T1)]. However, the molar absorption coefficients of pentacenes in the approximately 400–500 nm region are limited, whereas quantum dots, such as CdSe/ZnS (QD), possess high fluorescence quantum yields and particle-size-dependent fluorescence wavelengths. Thus, a combination of QD (D) and pentacene (A) provides a system of both an enhanced light-harvesting efficiency throughout the solar spectrum and an efficient conversion of the harvested light into the triplet states by SF. Based on these points, m-phenylene-bridged triisopropylsilane (TIPS)-pentacene dimer-functionalized QD (denoted as m-(Pc)2-QD) was synthesized to examine the sequential photoinduced process from energy transfer to SF. In femtosecond transient absorption measurements, initial energy transfer from QD to pentacene (quantum yield: 87 %) and subsequent SF were efficiently observed. The quantum yield of triplet states of pentacene units (ΦΤ) based on the excitation of QD attained is 160±6.7 %.

KW - energy transfer

KW - pentacene

KW - quantum dot

KW - sequential photophysical process

KW - singlet fission

U2 - 10.1002/chem.201803257

DO - 10.1002/chem.201803257

M3 - Article

VL - 24

SP - 17062

EP - 17071

JO - Chemistry: A European Journal

JF - Chemistry: A European Journal

SN - 0947-6539

IS - 64

ER -