DFT Simulations as Valuable Tool to Support NMR Characterization of Halide Perovskites: the Case of Pure and Mixed Halide Perovskites,Helvetica Chimica Acta

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DFT Simulations as Valuable Tool to Support NMR Characterization of Halide Perovskites: the Case of Pure and Mixed Halide Perovskites
Helvetica Chimica Acta ( IF 1.5 ) Pub Date : 2021-03-22 , DOI: 10.1002/hlca.202000231
Claudio Quarti ₁ , Eric Furet ₂ , Claudine Katan ₃

Affiliation

Solid state NMR spectroscopy is swiftly emerging as useful tool to characterize the structure, composition and dynamic properties of lead halide perovskites. On the other hand, interpretation of solid state NMR signatures is often challenging, because of the potential presence of many overlapping signals in small range of chemical shifts, hence complicating the extraction of detailed structural features. Here, we demonstrate the reliability of periodic Density Functional Theory in providing theoretical support for the NMR characterization of halide perovskite compounds, considering nuclei with spin I=1/2. For light ¹H and ¹³C nuclei, we predict NMR chemical shifts in good agreement with experiment, further highlighting the effects of motional narrowing. Accurate prediction of the NMR response of ²⁰⁷Pb nuclei is comparably more challenging, but we successfully reproduce the downshift in frequency when changing the halide composition from pure iodine to pure bromine. Furthermore, we confirm NMR as ideal tool to study mixed halide perovskite compounds, currently at the limelight for tandem solar cells and color‐tunable light emission.

中文翻译：

DFT模拟作为支持卤化物钙钛矿NMR表征的重要工具：纯卤化物和混合卤化物钙钛矿的案例

固态NMR光谱法正在迅速发展为表征卤化钙钛矿铅的结构，组成和动力学性质的有用工具。另一方面，由于在小范围的化学位移中可能存在许多重叠信号，因此固态NMR特征的解释通常具有挑战性，因此使详细结构特征的提取变得复杂。在这里，我们考虑到自旋I = 1/2的核，证明了周期性密度泛函理论在为卤化钙钛矿化合物的NMR表征提供理论支持方面的可靠性。对于光¹ H和¹³C核，我们预测NMR化学位移与实验良好吻合，进一步突出了运动变窄的影响。与之相比，准确预测²⁰⁷ Pb核的NMR反应更具挑战性，但是当将卤化物的组成从纯碘变为纯溴时，我们成功地再现了频率的下移。此外，我们确认NMR是研究混合卤化物钙钛矿化合物的理想工具，目前是串联太阳能电池和颜色可调光发射的亮点。

更新日期：2021-05-18

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