Quadruple cation mixed halide perovskite, GA_0.015Cs_0.046MA_0.152FA_0.787Pb(I_0.815Br_0.185)₃, single crystals were grown for the first time using an inverse temperature crystallization process. Solar cell devices in n-i-p stack configuration using thin films of the same materials showed power conversion efficiency above 20%. Complementary time-resolved spectroscopy confirmed that polycrystalline thin films and single crystals identically composed exhibit similar carrier dynamics in the picosecond range. Cooling of excited carriers and bandgap renormalization occur on the same time scale of 200–300 fs. The radiative recombination coefficient (1.2 × 10^–9 cm³/s) is comparable to values reported for a GaAs semiconductor. At low excitation density, a long carrier lifetime of 3.2 μs was recorded possibly due to the passivation of recombination centers. This study clarifies discrepancies about the lifetime of hot carriers, the impact of radiative recombination, and the role of recombination centers on solar cell performance. The quadruple cation perovskites displayed short time dynamics with slow recombination of charge carriers.

中文翻译：

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四重阳离子钙钛矿中激发电子的飞秒至微秒动力学

四重阳离子混合卤化物钙钛矿，GA _0.015 Cs _0.046 MA _0.152 FA _0.787 Pb（I _0.815 Br _0.185）₃，使用逆温度结晶工艺首次生长了单晶。使用相同材料的薄膜制成的压区堆叠结构的太阳能电池器件的功率转换效率超过20％。互补的时间分辨光谱证实，相同组成的多晶薄膜和单晶在皮秒范围内表现出相似的载流子动力学。激发载流子的冷却和带隙重归一化发生在200-300 fs的同一时间范围内。辐射复合系数（1.2×10^–9 cm ³ / s）与GaAs半导体的报告值相当。在低激发密度下，可能由于重组中心的钝化而记录到3.2μs的较长载流子寿命。这项研究澄清了关于热载流子寿命，辐射重组的影响以及重组中心对太阳能电池性能的作用的差异。四重阳离子钙钛矿显示出短时间的动力学，且载流子的重组很慢。