113Cd Solid-State NMR at 21.1 T Reveals the Local Structure and Passivation Mechanism of Cadmium in Hybrid and All-Inorganic Halide Perovskites,ACS Energy Letters

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113Cd Solid-State NMR at 21.1 T Reveals the Local Structure and Passivation Mechanism of Cadmium in Hybrid and All-Inorganic Halide Perovskites
ACS Energy Letters ( IF 19.3 ) Pub Date : 2020-08-21 , DOI: 10.1021/acsenergylett.0c01420
Dominik J. Kubicki ₁ , Daniel Prochowicz ₂ , Albert Hofstetter ₁ , Brennan J. Walder ₁ , Lyndon Emsley ₁

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Cadmium doping has recently emerged as an efficacious strategy for defect suppression and band gap tuning in hybrid as well as all-inorganic halide perovskites. However, the cadmium speciation in these materials is unknown. Here, we use high-field cadmium-113 NMR spectroscopy in conjunction with chemical shift calculations by fully relativistic density functional theory to establish the phase composition of cadmium-doped lead halide perovskites. We find that cadmium does not incorporate into the 3D perovskite lattice of MA- and FA-based lead halide perovskites (MAPbI₃ and the gold-standard triple cation mixed-halide composition). Instead, it forms separate, cadmium-rich nonperovskite phases for as little as 1 mol % Cd²⁺ doping. Conversely, we find that cadmium can incorporate into the 3D perovskite lattice of CsPbBr₃ via homovalent Pb²⁺ substitution up to around 10 mol %. Our results thus reveal the atomic-level mechanism of this recently developed defect passivation strategy.

中文翻译：

在21.1 T处的¹¹³ Cd固态NMR显示了杂化和全无机卤化物钙钛矿中镉的局部结构和钝化机理。

镉掺杂最近已成为一种有效的策略，可用于杂化及全无机卤化物钙钛矿中的缺陷抑制和带隙调整。但是，这些材料中的镉形态未知。在这里，我们使用高场镉-113 NMR光谱结合化学位移计算，通过完全相对论密度泛函理论来建立掺镉卤化铅钙钛矿的相组成。我们发现，镉不会掺入MA和FA基卤化铅钙钛矿（MAPbI ₃和金标准三阳离子混合卤化物组成）的3D钙钛矿晶格中。相反，它会形成低至1 mol％Cd ^2+的单独的富镉非钙钛矿相。掺杂。相反地，我们发现镉可以通过高达10 mol％的同价Pb ²⁺取代而掺入CsPbBr ₃的3D钙钛矿晶格中。因此，我们的结果揭示了这种最近开发的缺陷钝化策略的原子级机制。

更新日期：2020-09-11

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