Wang Yue, Yu Dejian, Wang Zeng, Li Xiaoming, Chen Xiaoxuan, Nalla Venkatram, Zeng Haibo, Sun Handong
Division of Physics and Applied Physics, School of Physical and Mathematical Sciences, Nanyang Technological University, Singapore, 637371, Singapore.
Centre for Disruptive Photonic Technologies (CDPT), School of Physical and Mathematical Sciences, Nanyang Technological University, Singapore, 637371, Singapore.
Small. 2017 Sep;13(34). doi: 10.1002/smll.201701587. Epub 2017 Jul 11.
With regards to developing miniaturized coherent light sources, the temperature-insensitivity in gain spectrum and threshold is highly desirable. Quantum dots (QDs) are predicted to possess a temperature-insensitive threshold by virtue of the separated electronic states; however, it is never observed in colloidal QDs due to the poor thermal stability. Besides, for the classical II-VI QDs, the gain profile generally redshifts with increasing temperature, plaguing the device chromaticity. Herein, this paper addresses the above two issues simultaneously by embedding ligands-free CsPbBr nanocrystals in a wider band gap Cs PbBr matrix by solution-phase synthesis. The unique electronic structures of CsPbBr nanocrystals enable temperature-insensitive gain spectrum while the lack of ligands and protection from Cs PbBr matrix ensure the thermal stability and high temperature operation. Specifically, a color drift-free stimulated emission irrespective of temperature change (20-150 °C) upon two-photon pumping is presented and the characteristic temperature is determined to be as high as ≈260 K. The superior gain properties of the CsPbBr /Cs PbBr perovskite nanocomposites are directly validated by a vertical cavity surface emitting laser operating at temperature as high as 100 °C. The results shed light on manipulating optical gain from the advantageous CsPbBr nanocrystals and represent a significant step toward the temperature-insensitive frequency-upconverted lasers.
关于开发小型化相干光源,增益谱和阈值中的温度不敏感性是非常可取的。量子点(QDs)由于其分离的电子态而被预测具有温度不敏感阈值;然而,由于热稳定性差,在胶体量子点中从未观察到这种情况。此外,对于经典的II-VI族量子点,增益谱通常会随着温度升高而红移,这困扰着器件的色度。在此,本文通过溶液相合成法将无配体的CsPbBr纳米晶体嵌入宽带隙CsPbBr基质中,同时解决了上述两个问题。CsPbBr纳米晶体独特的电子结构实现了温度不敏感的增益谱,而缺乏配体以及CsPbBr基质的保护确保了热稳定性和高温运行。具体而言,展示了在双光子泵浦下,无论温度如何变化(20-150°C)都无颜色漂移的受激发射,并且特征温度被确定高达≈260K。CsPbBr/CsPbBr钙钛矿纳米复合材料的优异增益特性通过在高达100°C的温度下工作的垂直腔面发射激光器得到直接验证。这些结果为利用CsPbBr纳米晶体的有利光学增益提供了启示,并朝着温度不敏感的频率上转换激光器迈出了重要一步。