基于I型核壳量子点的宽光谱响应的高效能量转移体系
收稿日期: 2015-12-17
网络出版日期: 2016-03-22
基金资助
项目受国家自然科学基金(No. 51502085)和湖北省自然科学基金(No. 2013CFB064)资助.
Panchromatic and High-efficient Energy Transfer Assembly Based on Type I Core-shell Quantum Dots
Received date: 2015-12-17
Online published: 2016-03-22
Supported by
Project supported by the National Natural Science Foundation of China (No. 51502085) and Natural Science Foundation of Hubei Province (No. 2013CFB064).
针对常规Förster共振能量转移(FRET)体系中能量转移效率低的问题, 合成了可见光吸收的I型CIS@ZnS核-壳量子点作为能量供体, 近红外方酸(SQ)染料作为能量受体, 采用超声自组装的方式首次制备了光谱匹配、间距可调的高效FRET能量转移体系. 超快/时间分辨光谱证明了CIS和SQ之间的FRET能量转移机制: CIS*+SQ→CIS+SQ*. 荧光猝灭动力学数据显示, CIS@ZnS与SQ之间的能量转移对量子点的尺寸存在依赖性, 由CIS@ZnS尺寸增加引起的荧光量子产率和供体-受体间距的增加使得体系的FRET能量转移效率(ηFRET)先增大后减小, 并且在壳层反应时间为20 min时体系的ηFRET值达到最佳值62.8%. 该研究对于开发新型、高效、全谱响应的太阳能电池将具有一定的理论及实际应用价值.
陈美华 , 潘峥 , 尹月锋 , 刘洁 , 刘梦媛 , 贾紫君 , 梁桂杰 . 基于I型核壳量子点的宽光谱响应的高效能量转移体系[J]. 化学学报, 2016 , 74(4) : 330 -334 . DOI: 10.6023/A15120785
In order to overcome the low energy transfer efficiency of the conventional FRET (Förster resonance energy transfer) system, a novel spectra-matching and distance-controllable CIS@ZnS-SQ FRET assembly has been prepared via ultrasonic self-assembly method, by using the synthesized visible CIS@ZnS type I core-shell quantum dots as energy donor and the near infrared SQ dyes as acceptor. Through controllable synthesis of quantum dots, the absorption and fluorescence performance of FRET system were adjusted by the size of CIS@ZnS, while the distance of energy donor-acceptor and the non-valid charge recombination in the FRET system were controlled by the wide-band shell of quantum dots. The excitons transfer and recombination kinetics in CIS@ZnS-SQ assembly were investigated by the pump-probe femtosecond ultrafast transient absorption measurements, with which results in the FRET-type energy transfer mechanism: CIS*+SQ→CIS+SQ* has been proven and a high energy transfer rate of about 5.0×1010 s-1 has been gained between CIS@ZnS and SQ. The excitons' lifetime and FRET energy transfer efficiency were calculated from the fluorescence decay kinetic curves tested by time-resolved fluorescence measurements. The results show that the energy transfer in CIS@ZnS-SQ depends on the size of CIS@ZnS quantum dots. As the size of CIS@ZnS (mainly refers to the ZnS shell thickness) increases from 2.1±0.4 nm to 2.9±0.4 nm, 4.1±0.3 nm, 5.4±0.5 nm and 7.2±0.5 nm, the fluorescence quantum yield of CIS@ZnS improves from 5.4% to 26%, 33%, 38% and 43.3% as well as the distance between CIS@ZnS and SQ (energy donor and acceptor) increases gradually, which makes the FRET energy transfer efficiency (ηFRET) first rise and then decline. As a result, an optimal ηFRET value of 62.8% was gained in the FRET assembly when the reaction time of ZnS shell was 20 min. This research will have a promising theoretical and practical value for the development of the panchromatic and high-efficiency solar cells.
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