通过结合 XPS 分析和 PL 成像对三阳离子钙钛矿薄膜进行深度化学和光电分析,ACS Applied Materials & Interfaces

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通过结合 XPS 分析和 PL 成像对三阳离子钙钛矿薄膜进行深度化学和光电分析
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2022-03-04 , DOI: 10.1021/acsami.1c22286
Stefania Cacovich ₁ , Pia Dally _{2,

3} , Guillaume Vidon ₂ , Marie Legrand _{2,

4} , Stéphanie Gbegnon ₂ , Jean Rousset _{2,

4} , Jean-Baptiste Puel _{2,

4} , Jean-François Guillemoles ₁ , Philip Schulz ₁ , Muriel Bouttemy _{2,

3} , Arnaud Etcheberry ₃

Affiliation

研究卤化物钙钛矿层和相关界面的化学和光电特性对于充分发挥钙钛矿太阳能电池的潜力至关重要。深度剖析光电子能谱是研究卤化物钙钛矿层在从表面到本体的不同尺度的化学性质的主要工具。该技术采用离子氩束减薄，可提供准确的层厚度。然而，迫切需要证实卤化物钙钛矿薄膜化学性质数据的可靠性，以更好地评估其稳定性。本研究解决了 Ar ⁺通过结合 X 射线光电子能谱 (XPS) 和光致发光 (PL) 光谱对三阳离子混合卤化物钙钛矿的表面化学成分和光电性能进行溅射减薄。首先，通过 Ar ⁺束溅射在半电池上进行 XPS 分析：玻璃/FTO/c-TiO ₂/钙钛矿。得到的剖面显示出非常均匀和可重复的元素分布，直到靠近掩埋界面；因此，该层在其整个厚度上被认为是准均匀的，并且溅射过程是稳定的。其次，我们通过 PL 成像光学测量在稳态和瞬态状态下评估了一组代表沿轮廓选定步骤的变薄的钙钛矿层，以评估从表面到体块的光学特性的可能扰动。在产生的陨石坑内获得的 PL 光谱显示没有峰值偏移或相分离。因此，瞬态 PL 测量没有揭示溅射区域中表面复合率的任何变化。这表明溅射没有累积效应，也没有剧烈的化学和光电修饰，验证了钙钛矿层深度成分的确定。将 XPS 分析与 PL 表征相结合可以成为广泛研究光伏器件的多层和混合有机/无机界面的精确工具。

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In-Depth Chemical and Optoelectronic Analysis of Triple-Cation Perovskite Thin Films by Combining XPS Profiling and PL Imaging

The investigation of chemical and optoelectronic properties of halide perovskite layers and associated interfaces is crucial to harness the full potential of perovskite solar cells. Depth-profiling photoemission spectroscopy is a primary tool to study the chemical properties of halide perovskite layers at different scales from the surface to the bulk. The technique employs ionic argon beam thinning that provides accurate layer thicknesses. However, there is an urgent need to corroborate the reliability of data on chemical properties of halide perovskite thin films to better assess their stability. The present study addresses the question of the Ar⁺ sputtering thinning on the surface chemical composition and the optoelectronic properties of the triple-cation mixed-halide perovskite by combining X-ray photoemission spectroscopy (XPS) and photoluminescence (PL) spectroscopy. First, XPS profiling is performed by Ar⁺ beam sputtering on a half-cell: glass/FTO/c-TiO₂/perovskite. The resulting profiles show a very homogeneous and reproducible element distribution until near the buried interface; therefore, the layer is considered as quasihomogeneous all over its thickness, and the sputtering process is stable. Second, we evaluated a set of thinned perovskite layers representative of selected steps along the profile by means of PL imaging optical measurements in both steady-state and transient regimes to assess possible perturbation of the optical properties from the surface to bulk. Obtained PL spectra inside the resulting craters show no peak shift nor phase segregation. Accordingly, the transient PL measurements do not reveal any changes of the surface recombination rate in the sputtered areas. This demonstrates that there is no cumulative effect of sputtering nor drastic chemical and optoelectronic modifications, validating the determination of the in-depth composition of the perovskite layer. Combining XPS profiling with PL characterization can be a precise tool to be applied for an extensive study of the multiple layers and mixed organic/inorganic interfaces of photovoltaic devices.

更新日期：2022-03-04

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