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.
julkaisussa: Chemistry - A European Journal, Vuosikerta 24, Nro 64, 16.11.2018, s. 17062-17071.Tutkimustuotos › › vertaisarvioitu
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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 -