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Impact of Tin Fluoride Additive on the Properties of Mixed Tin-Lead Iodide Perovskite Semiconductors

机译:氟化锡添加剂对混合锡铅碘化碘化钙钙矿半导体性能的影响

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Mixed tin-lead halide perovskites are promising low-bandgap absorbers for all-perovskite tandem solar cells that offer higher efficiencies than single-junction devices. A significant barrier to higher performance and stability is the ready oxidation of tin, commonly mitigated by various additives whose impact is still poorly understood for mixed tin-lead perovskites. Here, the effects of the commonly used SnF(2)additive are revealed for FA(0)(.)(83)Cs(0)(.)(17)Sn(x)Pb(1-)(x)I(3)perovskites across the full compositional lead-tin range and SnF(2)percentages of 0.1-20% of precursor tin content. SnF(2)addition causes a significant reduction in the background hole density associated with tin vacancies, yielding longer photoluminescence lifetimes, decreased energetic disorder, reduced Burstein-Moss shifts, and higher charge-carrier mobilities. Such effects are optimized for SnF(2)addition of 1%, while for 5% SnF(2)and above, additional nonradiative recombination pathways begin to appear. It is further found that the addition of SnF(2)reduces a tetragonal distortion in the perovskite structure deriving from the presence of tin vacancies that cause strain, particularly for high tin content. The optical phonon response associated with inorganic lattice vibrations is further explored, exhibiting a shift to higher frequency and significant broadening with increasing tin fraction, in accordance with lower effective atomic metal masses and shorter phonon lifetimes.
机译:混合锡铅卤化卤化卤化物佩罗夫斯基酯是有前途的用于全钙钛矿串联太阳能电池的低带隙吸收器,其提供比单结装置更高的效率。更高的性能和稳定性的显着障碍是锡的准备氧化,通常被各种添加剂减轻,其影响仍然是混合锡引导钙钛矿的影响。这里,常用的SNF(2)添加剂的效果被揭示FA(0)(。)(83)Cs(0)(0)(17)sn(x)pb(1 - )(x)i( 3)钙锌矿横跨完整的成分铅锡和SNF(2)百分比的前体锡含量的0.1-20%。 SNF(2)加法导致与锡空位相关的背景孔密度显着降低,产生更长的光致发光寿命,减少了能量紊乱,减少了伯士岛 - 莫斯班次,以及更高的电荷 - 载体迁移。这种效果针对SNF(2)加入1%而优化,而对于5%SNF(2)及以上,额外的非相互作用途径开始出现。进一步发现,添加SNF(2)的添加降低了从导致菌株的锡空位的存在的钙钛矿结构中的四字变形,特别是对于高锡含量。进一步探索与无机晶格振动相关的光学声子响应,根据较低的有效原子金属质量和较短的声子寿命,随着锡馏分的增加而表现出较高频率和显着展赖的转变。

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