In Situ Observing and Tuning the Crystal Orientation of Two-Dimensional Layered Perovskite via the Chlorine Additive.

Precise control of crystal orientation in two-dimensional (2D) layered perovskites (LPs) is vital for their optoelectronic applications due to the structure-induced anisotropy in optical and electrical properties. Herein, we directly observe and control the crystal orientation of the butylammonium-based 2D LP films. Employing the synchrotron-based in situ grazing-incidence X-ray diffraction technique, we reveal the orientation modulation mechanism of the Cl additive by following the crystallization dynamics and chemical conversion pathways during film formation. Two new Cl-related intermediates are identified which serve as templates directing the orientational growth of the 2D LP films. We fine-tune the crystal orientation of 2D LP films through the Cl additive and incorporate the films with the requisite crystal orientations in solar cells and photodetectors. The optoelectronic performances of the devices show a strong correlation with the crystal orientation of the 2D LP films.

[1]  M. Kanatzidis,et al.  The 2D Halide Perovskite Rulebook: How the Spacer Influences Everything from the Structure to Optoelectronic Device Efficiency. , 2021, Chemical reviews.

[2]  Qiaofei Xu,et al.  Highly thermostable and efficient formamidinium-based low-dimensional perovskite solar cells. , 2020, Angewandte Chemie.

[3]  William R. Dichtel,et al.  In Situ Grazing‐Incidence Wide‐Angle Scattering Reveals Mechanisms for Phase Distribution and Disorientation in 2D Halide Perovskite Films , 2020, Advanced materials.

[4]  Jinsong Huang,et al.  Templated growth of oriented layered hybrid perovskites on 3D-like perovskites , 2020, Nature Communications.

[5]  Qiaofei Xu,et al.  In Situ Observation of Vapor-Assisted 2D-3D Heterostructure Formation for Stable and Efficient Perovskite Solar Cells. , 2020, Nano letters.

[6]  Xitao Liu,et al.  Highly Oriented Thin Films of 2D Ruddlesden-Popper Hybrid Perovskite toward Superfast Response Photodetectors. , 2019, Small.

[7]  Qiaofei Xu,et al.  A New Organic Interlayer Spacer for Stable and Efficient 2D Ruddlesden-Popper Perovskite Solar Cells. , 2019, Nano letters.

[8]  Jizheng Wang,et al.  Strategies toward High‐Performance Solution‐Processed Lateral Photodetectors , 2019, Advanced materials.

[9]  H. Ade,et al.  Unveiling the operation mechanism of layered perovskite solar cells , 2019, Nature Communications.

[10]  Wei Huang,et al.  Critical role of chloride in organic ammonium spacer on the performance of Low-dimensional Ruddlesden-Popper perovskite solar cells , 2019, Nano Energy.

[11]  G. Giri,et al.  Understanding the Formation of Vertical Orientation in Two-dimensional Metal Halide Perovskite Thin Films , 2019, Chemistry of Materials.

[12]  Jang‐Sik Lee,et al.  2D Perovskite‐Based Self‐Aligned Lateral Heterostructure Photodetectors Utilizing Vapor Deposition , 2018, Advanced Optical Materials.

[13]  M. Kanatzidis,et al.  Two-Dimensional Hybrid Halide Perovskites: Principles and Promises. , 2018, Journal of the American Chemical Society.

[14]  L. Quan,et al.  Perovskite light-emitting diodes with external quantum efficiency exceeding 20 per cent , 2018, Nature.

[15]  Yongsheng Chen,et al.  Two-Dimensional Ruddlesden-Popper Perovskite with Nanorod-like Morphology for Solar Cells with Efficiency Exceeding 15. , 2018, Journal of the American Chemical Society.

[16]  A. Jen,et al.  Two-Dimensional Perovskite Solar Cells with 14.1% Power Conversion Efficiency and 0.68% External Radiative Efficiency , 2018, ACS Energy Letters.

[17]  Hongzheng Chen,et al.  Orientation Regulation of Phenylethylammonium Cation Based 2D Perovskite Solar Cell with Efficiency Higher Than 11% , 2018 .

[18]  Dong Yang,et al.  Quasi-Two-Dimensional Halide Perovskite Single Crystal Photodetector. , 2018, ACS nano.

[19]  U. Jeng,et al.  Critical Intermediate Structure That Directs the Crystalline Texture and Surface Morphology of Organo-Lead Trihalide Perovskite. , 2017, ACS applied materials & interfaces.

[20]  Sang Yoon Lee,et al.  Printable organometallic perovskite enables large-area, low-dose X-ray imaging , 2017, Nature.

[21]  Jia Huang,et al.  Photodetectors Based on Two-Dimensional Layer-Structured Hybrid Lead Iodide Perovskite Semiconductors. , 2016, ACS applied materials & interfaces.

[22]  Sergei Tretiak,et al.  High-efficiency two-dimensional Ruddlesden–Popper perovskite solar cells , 2016, Nature.

[23]  Edward H. Sargent,et al.  Perovskite photonic sources , 2016, Nature Photonics.

[24]  D. J. Clark,et al.  Ruddlesden-Popper Hybrid Lead Iodide Perovskite 2D Homologous Semiconductors , 2016 .