Allegro Isabel, Li Yang, Richards Bryce S, Paetzold Ulrich W, Lemmer Uli, Howard Ian A
Light Technology Institute, Karlsruhe Institute of Technology, Engesserstrasse 13, 76131 Karlsruhe, Germany.
Institute of Microstructure Technology, Karlsruhe Institute of Technology, Hermann-von-Helmholtz-Platz 1, 76344 Eggenstein-Leopoldshafen, Germany.
J Phys Chem Lett. 2021 Mar 11;12(9):2293-2298. doi: 10.1021/acs.jpclett.1c00099. Epub 2021 Mar 2.
Recently, continuous-wave (CW) lasing was demonstrated at room temperature in quasi-2D perovskites. For 3D films, CW lasing at room temperature remains challenging. Issues hampering 3D materials include the temperature dependence of the (a) distribution of carrier energies, (b) buildup of photoinduced nonradiative channels, and (c) rates of bimolecular versus Auger recombination. We study the latter in a phase-stable 3D perovskite using high-index substrates to completely suppress amplified spontaneous emission (ASE). The bimolecular recombination coefficient decreases from 80 to 290 K (from (6.4 to 1.1) × 10 cm s), whereas the Auger coefficient stays constant at 3 × 10 cm s. Above 250 K, the Auger rate exceeds the bimolecular rate at carrier densities corresponding to the ASE threshold. At lower temperatures, the decrease in the bimolecular rate coefficient with increasing temperature and the fraction of photoluminescence in the ASE band determine the temperature dependence of the ASE threshold.
最近,在准二维钙钛矿中实现了室温连续波(CW)激光发射。对于三维薄膜,室温下的连续波激光发射仍然具有挑战性。阻碍三维材料实现室温连续波激光发射的问题包括:(a)载流子能量分布的温度依赖性;(b)光致非辐射通道的积累;(c)双分子复合与俄歇复合的速率。我们使用高折射率衬底在相稳定的三维钙钛矿中研究了后者,以完全抑制放大自发辐射(ASE)。双分子复合系数在80至290 K范围内从(6.4至1.1)×10⁻¹⁰ cm³ s⁻¹减小,而俄歇系数保持在3×10⁻³¹ cm⁻⁶ s⁻¹不变。在250 K以上,在对应于ASE阈值的载流子密度下,俄歇复合速率超过双分子复合速率。在较低温度下,双分子速率系数随温度升高的降低以及ASE波段中光致发光的比例决定了ASE阈值的温度依赖性。