通过表面终止配体工程调制混合维数3D / 2D钙钛矿中的能带对准,Chemistry of Materials

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通过表面终止配体工程调制混合维数3D / 2D钙钛矿中的能带对准
Chemistry of Materials ( IF 7.2 ) Pub Date : 2019-12-24 , DOI: 10.1021/acs.chemmater.9b02560
Arup Mahata _{1,

2} , Edoardo Mosconi ₂ , Daniele Meggiolaro ₂ , Filippo De Angelis _{2,

3}

Affiliation

三维（3D）/二维（2D）混合尺寸钙钛矿潜在地克服了常规3D钙钛矿的稳定性问题，而不会显着损害太阳能电池的性能。3D / 2D钙钛矿异质结构依赖于3D / 2D界面上能级的对齐，这决定了载流子的限制以及可能的电荷分离。使用最新的第一性原理计算，我们显示了间隔阳离子的局限偶极子和钙钛矿表面终止在决定界面能取向方面具有至关重要的作用。考虑到实验使用的BA ₂ PbI ₄（BA =正丁基铵）和AVA ₂ PbI ₄（AVA =质子化氨基戊酸）2D钙钛矿与原型MAPbI ₃ 3D钙钛矿的界面，我们系统地研究了3D和2D量子阱界面处的能带排列，其中考虑了不同类型的表面终止。我们的研究表明，BA ₂碘化铅₄具有MAPbI频带边缘的良好对准₃不论MAPbI的表面终止的₃然而，具有取决于表面终止2D和3D部分之间的频带边缘位置的改变。在另一方面，AVA的取向₂碘化铅₄与MAPbI ₃对表面终止非常敏感，凭借-COOH基团的受限界面偶极子具有良好的取向。这项研究为3D / 2D钙钛矿中的界面工程提供了全局图片，为进一步探索空穴/电子传输材料在薄膜优先面上的锚固提供了必要的背景，以改善载流子的提取。

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Modulating Band Alignment in Mixed Dimensionality 3D/2D Perovskites by Surface Termination Ligand Engineering

Three-dimensional (3D)/two-dimensional (2D) mixed dimensional perovskites have potentially overcome the stability issues of conventional 3D perovskites without significantly compromising the solar cell performance. 3D/2D perovskite heterostructures rely on the alignment of energy levels across the 3D/2D interface, which determines carrier confinement and possibly charge separation. Using state-of-the-art first-principles calculations, we show that the confined dipoles of spacer cations and the perovskite surface termination have a crucial role in determining interfacial energy alignment. Considering the experimentally employed BA₂PbI₄ (BA = n-butylammonium) and AVA₂PbI₄ (AVA = protonated aminovaleric acid) 2D perovskite interfaces with the prototypical MAPbI₃ 3D perovskite, we systematically investigate the band alignment at the interfaces of 3D and 2D quantum wells considering different types of surface terminations. Our study shows that BA₂PbI₄ has favorable alignment of band edges with MAPbI₃ irrespective of the surface termination of MAPbI₃, however, with the alteration of the band edge positions between 2D and 3D parts depending on surface termination. On the other hand, the alignment of AVA₂PbI₄ with MAPbI₃ is very much sensitive to surface termination, having favorable alignment by virtue of confined interface dipoles of the −COOH groups. This study provides a global picture of the interface engineering in 3D/2D perovskites, setting the required background to further explore the anchoring of hole/electron transport materials at the preferential side of the film for improved carrier extraction.

更新日期：2019-12-25

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