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Highly Luminescent Phase-Stable CsPbI3 Perovskite Quantum Dots Achieving Near 100% Absolute Photoluminescence Quantum Yield
ACS Nano ( IF 15.8 ) Pub Date : 2017-09-19 00:00:00 , DOI: 10.1021/acsnano.7b05442 Feng Liu 1 , Yaohong Zhang 1 , Chao Ding 1 , Syuusuke Kobayashi 1 , Takuya Izuishi 1 , Naoki Nakazawa 1 , Taro Toyoda 1, 2 , Tsuyoshi Ohta 3 , Shuzi Hayase 2, 3 , Takashi Minemoto 2, 4 , Kenji Yoshino 2, 5 , Songyuan Dai 6 , Qing Shen 1, 2
ACS Nano ( IF 15.8 ) Pub Date : 2017-09-19 00:00:00 , DOI: 10.1021/acsnano.7b05442 Feng Liu 1 , Yaohong Zhang 1 , Chao Ding 1 , Syuusuke Kobayashi 1 , Takuya Izuishi 1 , Naoki Nakazawa 1 , Taro Toyoda 1, 2 , Tsuyoshi Ohta 3 , Shuzi Hayase 2, 3 , Takashi Minemoto 2, 4 , Kenji Yoshino 2, 5 , Songyuan Dai 6 , Qing Shen 1, 2
Affiliation
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Perovskite quantum dots (QDs) as a new type of colloidal nanocrystals have gained significant attention for both fundamental research and commercial applications owing to their appealing optoelectronic properties and excellent chemical processability. For their wide range of potential applications, synthesizing colloidal QDs with high crystal quality is of crucial importance. However, like most common QD systems such as CdSe and PbS, those reported perovskite QDs still suffer from a certain density of trapping defects, giving rise to detrimental nonradiative recombination centers and thus quenching luminescence. In this paper, we show that a high room-temperature photoluminescence quantum yield of up to 100% can be obtained in CsPbI3 perovskite QDs, signifying the achievement of almost complete elimination of the trapping defects. This is realized with our improved synthetic protocol that involves introducing organolead compound trioctylphosphine–PbI2 (TOP–PbI2) as the reactive precursor, which also leads to a significantly improved stability for the resulting CsPbI3 QD solutions. Ultrafast kinetic analysis with time-resolved transient absorption spectroscopy evidence the negligible electron or hole-trapping pathways in our QDs, which explains such a high quantum efficiency. We expect the successful synthesis of the “ideal” perovskite QDs will exert profound influence on their applications to both QD-based light-harvesting and -emitting devices.
中文翻译：
高度发光的相稳定CsPbI 3钙钛矿量子点，可实现接近100％的绝对光致发光量子产率
钙钛矿量子点（QDs）作为一种新型的胶体纳米晶体，由于其吸引人的光电性能和出色的化学加工性能而受到基础研究和商业应用的广泛关注。对于潜在的广泛应用，合成具有高晶体质量的胶体量子点至关重要。但是，像大多数常见的QD系统（例如CdSe和PbS）一样，那些报道的钙钛矿QD仍然存在一定密度的俘获缺陷，从而导致有害的非辐射重组中心，从而猝灭了发光。在本文中，我们表明在CsPbI 3中可以获得高达100％的高室温光致发光量子产率。钙钛矿QD，表明几乎可以完全消除陷印缺陷。这是通过我们改进的合成方案实现的，该方案包括引入有机铅化合物三辛基膦-PbI 2（TOP-PbI 2）作为反应性前体，这也大大提高了所得CsPbI 3 QD溶液的稳定性。具有时间分辨瞬态吸收光谱的超快速动力学分析证明了我们量子点中可忽略的电子或空穴捕获途径，这解释了如此高的量子效率。我们希望成功合成“理想的”钙钛矿量子点将对其在基于量子点的光收集和发射设备中的应用产生深远的影响。
更新日期：2017-09-19
中文翻译：
高度发光的相稳定CsPbI 3钙钛矿量子点，可实现接近100％的绝对光致发光量子产率
钙钛矿量子点（QDs）作为一种新型的胶体纳米晶体，由于其吸引人的光电性能和出色的化学加工性能而受到基础研究和商业应用的广泛关注。对于潜在的广泛应用，合成具有高晶体质量的胶体量子点至关重要。但是，像大多数常见的QD系统（例如CdSe和PbS）一样，那些报道的钙钛矿QD仍然存在一定密度的俘获缺陷，从而导致有害的非辐射重组中心，从而猝灭了发光。在本文中，我们表明在CsPbI 3中可以获得高达100％的高室温光致发光量子产率。钙钛矿QD，表明几乎可以完全消除陷印缺陷。这是通过我们改进的合成方案实现的，该方案包括引入有机铅化合物三辛基膦-PbI 2（TOP-PbI 2）作为反应性前体，这也大大提高了所得CsPbI 3 QD溶液的稳定性。具有时间分辨瞬态吸收光谱的超快速动力学分析证明了我们量子点中可忽略的电子或空穴捕获途径，这解释了如此高的量子效率。我们希望成功合成“理想的”钙钛矿量子点将对其在基于量子点的光收集和发射设备中的应用产生深远的影响。
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