Processing of Lead Halide Perovskite Thin Films Studied with In-Situ Real-Time X-ray Scattering.

Lead halide perovskites have been of paramount interest for solution-processable solar cells, reaching power conversion efficiencies larger than 25%. In this spotlight, we will provide a systematic overview of the influence of different solution-based processing routes of lead halide perovskites on their phase transformation and conversion as revealed through in-situ X-ray-scattering experiments. These experiments were performed in conditions closely mimicking thin film processing methods and conditions used for thin film solar cell device fabrication and therefore provide critical information about the mechanism of the phase transformation, its onset, the kinetics, as well as the emergence and disappearance of various (meso)phases along the way. The measurements capture the overall solidification and conversion process of lead halide perovskite inks into solid films via so-called one-step and two-step spin-coating processes as well as blade coating and hot casting. Processing routes are applied to films based on basic components as well as mixtures of different anions and cations, solvents, and antisolvents, all of which deeply affect the thin film microstructure and morphology of the light-absorbing semiconductor and associated solar cell devices.

[1]  L. Schelhas,et al.  Structural Evolution During Perovskite Crystal Formation and Degradation: In Situ and Operando X‐Ray Diffraction Studies , 2019, Advanced Energy Materials.

[2]  W. Su,et al.  Formation Mechanism and Control of Perovskite Films from Solution to Crystalline Phase Studied by in Situ Synchrotron Scattering. , 2016, ACS applied materials & interfaces.

[3]  Ruipeng Li,et al.  Perovskite Photovoltaics: Hybrid Perovskite Thin‐Film Photovoltaics: In Situ Diagnostics and Importance of the Precursor Solvate Phases (Adv. Mater. 2/2017) , 2017 .

[4]  Mercouri G Kanatzidis,et al.  Semiconducting tin and lead iodide perovskites with organic cations: phase transitions, high mobilities, and near-infrared photoluminescent properties. , 2013, Inorganic chemistry.

[5]  J. Howse,et al.  Perovskite Crystallization Dynamics during Spin-Casting: An In Situ Wide-Angle X-ray Scattering Study , 2020, ACS applied energy materials.

[6]  P. Müller‐Buschbaum,et al.  Time‐Resolved Orientation and Phase Analysis of Lead Halide Perovskite Film Annealing Probed by In Situ GIWAXS , 2022, Advanced Optical Materials.

[7]  Peng Gao,et al.  Mixed-organic-cation perovskite photovoltaics for enhanced solar-light harvesting. , 2014, Angewandte Chemie.

[8]  M. Grätzel,et al.  Kinetics of Ion-Exchange Reactions in Hybrid Organic-Inorganic Perovskite Thin Films Studied by In Situ Real-Time X-ray Scattering. , 2018, The journal of physical chemistry letters.

[9]  N. Tamura,et al.  Out-of-equilibrium processes in crystallization of organic-inorganic perovskites during spin coating , 2021, Nature Communications.

[10]  Zhibin Yang,et al.  High‐Performance Fully Printable Perovskite Solar Cells via Blade‐Coating Technique under the Ambient Condition , 2015 .

[11]  Kai Zhu,et al.  Towards stable and commercially available perovskite solar cells , 2016, Nature Energy.

[12]  A. Amassian,et al.  Room‐Temperature Partial Conversion of α‐FAPbI3 Perovskite Phase via PbI2 Solvation Enables High‐Performance Solar Cells , 2020, Advanced Functional Materials.

[13]  Michael Saliba,et al.  Thermally Induced Structural Evolution and Performance of Mesoporous Block Copolymer-Directed Alumina Perovskite Solar Cells , 2014, ACS nano.

[14]  R. Kaner,et al.  Crystalline Liquid-like Behavior: Surface-Induced Secondary Grain Growth of Photovoltaic Perovskite Thin Film. , 2019, Journal of the American Chemical Society.

[15]  M. Green,et al.  Nucleation and Growth Control of HC(NH2)2PbI3 for Planar Perovskite Solar Cell , 2016 .

[16]  Christopher J. Tassone,et al.  Roll-to-Roll Printing of Perovskite Solar Cells , 2018, ACS Energy Letters.

[17]  A. Amassian,et al.  Scalable Ambient Fabrication of High-Performance CsPbI2Br Solar Cells , 2019, Joule.

[18]  Detlef-Matthias Smilgies,et al.  Origin of vertical orientation in two-dimensional metal halide perovskites and its effect on photovoltaic performance , 2018, Nature Communications.

[19]  Wen-Hau Zhang,et al.  Toward Greener Solution Processing of Perovskite Solar Cells , 2020 .

[20]  Mukundan Thelakkat,et al.  Capturing the Sun: A Review of the Challenges and Perspectives of Perovskite Solar Cells , 2017 .

[21]  Young Chan Kim,et al.  Compositional engineering of perovskite materials for high-performance solar cells , 2015, Nature.

[22]  Y. Galagan Perovskite Solar Cells: Toward Industrial-Scale Methods. , 2018, The journal of physical chemistry letters.

[23]  T. Kelly,et al.  Elucidating the Failure Mechanisms of Perovskite Solar Cells in Humid Environments Using In Situ Grazing-Incidence Wide-Angle X-ray Scattering , 2018, ACS Energy Letters.

[24]  Wei Zhang,et al.  In situ dynamic observations of perovskite crystallisation and microstructure evolution intermediated from [PbI6]4− cage nanoparticles , 2017, Nature Communications.

[25]  Wei Huang,et al.  Growth and Degradation Kinetics of Organic–Inorganic Hybrid Perovskite Films Determined by In Situ Grazing‐Incidence X‐Ray Scattering Techniques , 2021, Small methods.

[26]  Ruipeng Li,et al.  Efficient Hybrid Mixed‐Ion Perovskite Photovoltaics: In Situ Diagnostics of the Roles of Cesium and Potassium Alkali Cation Addition , 2020 .

[27]  R. Munir,et al.  Blade-Coated Hybrid Perovskite Solar Cells with Efficiency > 17%: An In Situ Investigation , 2018 .

[28]  Seh-Won Ahn,et al.  Investigation of Thermally Induced Degradation in CH3NH3PbI3 Perovskite Solar Cells using In-situ Synchrotron Radiation Analysis , 2017, Scientific Reports.

[29]  Y. Qi,et al.  Advances and challenges to the commercialization of organic–inorganic halide perovskite solar cell technology , 2017 .

[30]  R. Munir,et al.  Phase Transition Control for High-Performance Blade-Coated Perovskite Solar Cells , 2018, Joule.

[31]  R. Friend,et al.  Degradation mechanisms of perovskite solar cells under vacuum and one atmosphere of nitrogen , 2021, Nature Energy.

[32]  Liang Ma,et al.  Toward Eco-friendly and Stable Perovskite Materials for Photovoltaics , 2018, Joule.

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

[34]  Guangda Niu,et al.  Inorganic CsPbI3 Perovskite‐Based Solar Cells: A Choice for a Tandem Device , 2017 .

[35]  Zhuoying Chen,et al.  Revealing Crystallization Dynamics and the Compositional Control Mechanism of 2D Perovskite Film Growth by In Situ Synchrotron-Based GIXRD , 2019, ACS Energy Letters.

[36]  Longlong Wu,et al.  In Situ Real‐Time Study of the Dynamic Formation and Conversion Processes of Metal Halide Perovskite Films , 2018, Advanced materials.

[37]  Adriano S. Marques,et al.  Revealing the Perovskite Film Formation Using the Gas Quenching Method by In Situ GIWAXS: Morphology, Properties, and Device Performance , 2020, Advanced Functional Materials.

[38]  Xinhui Lu,et al.  A Systematic Review of Metal Halide Perovskite Crystallization and Film Formation Mechanism Unveiled by In Situ GIWAXS , 2021, Advanced materials.

[39]  Aram Amassian,et al.  Impact of the Solvation State of Lead Iodide on Its Two‐Step Conversion to MAPbI3: An In Situ Investigation , 2019, Advanced Functional Materials.

[40]  Ulrich Wiesner,et al.  Crystallization kinetics of organic-inorganic trihalide perovskites and the role of the lead anion in crystal growth. , 2015, Journal of the American Chemical Society.

[41]  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.

[42]  Ruipeng Li,et al.  The Role of Alkali Metal Cations on Electronic Structure and Halide Segregation of Hybrid Perovskites. , 2020, ACS applied materials & interfaces.

[43]  M. Grätzel,et al.  Sequential deposition as a route to high-performance perovskite-sensitized solar cells , 2013, Nature.

[44]  Peng Gao,et al.  Efficient luminescent solar cells based on tailored mixed-cation perovskites , 2016, Science Advances.

[45]  Sang Il Seok,et al.  High-performance photovoltaic perovskite layers fabricated through intramolecular exchange , 2015, Science.

[46]  Christopher J. Tassone,et al.  Impact of Processing on Structural and Compositional Evolution in Mixed Metal Halide Perovskites during Film Formation , 2020, Advanced Functional Materials.

[47]  Aram Amassian,et al.  Look fast: Crystallization of conjugated molecules during solution shearing probed in‐situ and in real time by X‐ray scattering , 2013 .

[48]  Ruipeng Li,et al.  Perovskite Solar Cells toward Eco-Friendly Printing , 2021, Research.

[49]  D. Smilgies GISAXS : A versatile tool to assess structure and self‐assembly kinetics in block copolymer thin films , 2021, Journal of Polymer Science.

[50]  Sang Il Seok,et al.  Solvent engineering for high-performance inorganic-organic hybrid perovskite solar cells. , 2014, Nature materials.

[51]  P. Müller‐Buschbaum,et al.  Structure of Organometal Halide Perovskite Films as Determined with Grazing‐Incidence X‐Ray Scattering Methods , 2017 .

[52]  Christopher J. Tassone,et al.  Scalable Fabrication of Perovskite Solar Cells to Meet Climate Targets , 2018, Joule.

[53]  Dong Uk Lee,et al.  Iodide management in formamidinium-lead-halide–based perovskite layers for efficient solar cells , 2017, Science.

[54]  J. Teuscher,et al.  Efficient Hybrid Solar Cells Based on Meso-Superstructured Organometal Halide Perovskites , 2012, Science.

[55]  Aram Amassian,et al.  Kinetic Stabilization of the Sol–Gel State in Perovskites Enables Facile Processing of High‐Efficiency Solar Cells , 2019, Advanced materials.

[56]  Aram Amassian,et al.  Multi-cation Synergy Suppresses Phase Segregation in Mixed-Halide Perovskites , 2019, Joule.

[57]  Ruipeng Li,et al.  Sequential Formation of Tunable‐Bandgap Mixed‐Halide Lead‐Based Perovskites: In Situ Investigation and Photovoltaic Devices , 2020 .

[58]  Jae Bum Jeon,et al.  Antisolvent with an Ultrawide Processing Window for the One‐Step Fabrication of Efficient and Large‐Area Perovskite Solar Cells , 2018, Advanced materials.

[59]  Yong Chen,et al.  From convective assembly to Landau-Levich deposition of multilayered phospholipid films of controlled thickness. , 2009, Langmuir : the ACS journal of surfaces and colloids.

[60]  M. Green,et al.  The emergence of perovskite solar cells , 2014, Nature Photonics.

[61]  A. Priyadarshi,et al.  Evolution of Perovskite Crystallization in Printed Mesoscopic Perovskite Solar Cells , 2019, Energy Technology.