Solution-Grown CsPbBr3/Cs4PbBr6 Perovskite Nanocomposites: Toward Temperature-Insensitive Optical Gain

4 years ago

Solution-Grown CsPbBr3/Cs4PbBr6 Perovskite Nanocomposites: Toward Temperature-Insensitive Optical Gain

Xiaoxuan Chen, Venkatram Nalla, Zeng Wang, Yue Wang, Haibo Zeng, Xiaoming Li, Handong Sun, Dejian Yu

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 CsPbBr3 nanocrystals in a wider band gap Cs4PbBr6 matrix by solution-phase synthesis. The unique electronic structures of CsPbBr3 nanocrystals enable temperature-insensitive gain spectrum while the lack of ligands and protection from Cs4PbBr6 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 CsPbBr3/Cs4PbBr6 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 CsPbBr3 nanocrystals and represent a significant step toward the temperature-insensitive frequency-upconverted lasers. Temperature-insensitive optical gain is achieved by exploiting a novel lasing material composed of ligands-free CsPbBr3 nanocrystals embedded in a wider band gap Cs4PbBr6 matrix based on low-temperature solution-phase synthesis. The unique electronic structures of CsPbBr3 nanocrystals enable temperature-insensitive gain profile while the lack of ligands and protection from Cs4PbBr6 matrix ensure the thermal stability and high temperature operation.

Publisher URL: http://onlinelibrary.wiley.com/resolve/doi

DOI: 10.1002/smll.201701587