High-Throughput Automated Exploration of Phase Growth Behaviors in Quasi-2D Formamidinium Metal Halide Perovskites

Yang, Jonghee; Lawrie, Benjamin J.; Kalinin, Sergei V.; Ahmadi, Mahshid

doi:10.1002/aenm.202302337

Title: High-Throughput Automated Exploration of Phase Growth Behaviors in Quasi-2D Formamidinium Metal Halide Perovskites

Journal Article · 24 September 2023 · Advanced Energy Materials

DOI: https://doi.org/10.1002/aenm.202302337 · OSTI ID:2006941

^[1];

^[2]; Kalinin, Sergei V. ^[1];

^[1]

Univ. of Tennessee, Knoxville, TN (United States)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Quasi-2D metal halide perovskites (MHPs) are an emerging material platform for sustainable functional optoelectronics, but the uncontrollable, broad phase distribution remains a critical challenge for applications. Nevertheless, the basic principles for controlling phases in quasi-2D MHPs remain poorly understood, due to the rapid crystallization kinetics during the conventional thin-film fabrication process. In this work, a high-throughput automated synthesis-characterization-analysis workflow is implemented to accelerate material exploration in formamidinium (FA)-based quasi-2D MHP compositional space, revealing the early-stage phase growth behaviors fundamentally determining the phase distributions. Upon comprehensive exploration with varying synthesis conditions including 2D:3D composition ratios, antisolvent injection rates, and temperatures in an automated synthesis-characterization platform, it is observed that the prominent n = 2 2D phase restricts the growth kinetics of 3D-like phases—α-FAPbI₃ MHPs with spacer-coordinated surface—across the MHP compositions. Thermal annealing is a critical step for proper phase growth, although it can lead to the emergence of unwanted local PbI₂ crystallites. Additionally, fundamental insights into the precursor chemistry associated with spacer-solvent interaction determining the quasi-2D MHP morphologies and microstructures are demonstrated. The high-throughput study provides comprehensive insights into the fundamental principles in quasi-2D MHP phase control, enabling new control of the functionalities in complex materials systems for sustainable device applications.

View Accepted Manuscript (DOE)

Cite

Export

Save

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF); National Science Foundation (NSF); Alfred P. Sloan Foundation

Grant/Contract Number:: AC05-00OR22725; 2043205; FG-2022-18275

OSTI ID:: 2006941

Journal Information:: Advanced Energy Materials, Vol. 13, Issue 43; ISSN 1614-6832

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

References (50)

Stabilization of Metastable Halide Perovskite Lattices in the 2D Limit Fu, Yongping Advanced Materials, Vol. 34, Issue 9 https://doi.org/10.1002/adma.202108556	journal	January 2022
Understanding the ligand-assisted reprecipitation of CsPbBr3 nanocrystals via high-throughput robotic synthesis approach Sanchez, Sheryl L.; Tang, Yipeng; Hu, Bin Matter, Vol. 6, Issue 9 https://doi.org/10.1016/j.matt.2023.05.023	journal	September 2023
Deterministic fabrication of 3D/2D perovskite bilayer stacks for durable and efficient solar cells Sidhik, Siraj; Wang, Yafei; De Siena, Michael Science, Vol. 377, Issue 6613 https://doi.org/10.1126/science.abq7652	journal	September 2022
Controlled growth of perovskite layers with volatile alkylammonium chlorides Park, Jaewang; Kim, Jongbeom; Yun, Hyun-Sung Nature, Vol. 616, Issue 7958 https://doi.org/10.1038/s41586-023-05825-y	journal	February 2023
The 2D Halide Perovskite Rulebook: How the Spacer Influences Everything from the Structure to Optoelectronic Device Efficiency Li, Xiaotong; Hoffman, Justin M.; Kanatzidis, Mercouri G. Chemical Reviews, Vol. 121, Issue 4 https://doi.org/10.1021/acs.chemrev.0c01006	journal	January 2021
A general approach to high-efficiency perovskite solar cells by any antisolvent Taylor, Alexander D.; Sun, Qing; Goetz, Katelyn P. Nature Communications, Vol. 12, Issue 1 https://doi.org/10.1038/s41467-021-22049-8	journal	March 2021
Seed‐Assisted Growth of Methylammonium‐Free Perovskite for Efficient Inverted Perovskite Solar Cells Wang, Pengjiu; Chen, Xu; Liu, Tianyu Small Methods, Vol. 6, Issue 5 https://doi.org/10.1002/smtd.202200048	journal	March 2022
Ligand-engineered bandgap stability in mixed-halide perovskite LEDs Hassan, Yasser; Park, Jong Hyun; Crawford, Michael L. Nature, Vol. 591, Issue 7848 https://doi.org/10.1038/s41586-021-03217-8	journal	March 2021
A Universal Perovskite Nanocrystal Ink for High‐Performance Optoelectronic Devices Song, Hochan; Yang, Jonghee; Jeong, Woo Hyeon Advanced Materials, Vol. 35, Issue 8 https://doi.org/10.1002/adma.202209486	journal	December 2022
Toward self-organizing low-dimensional organic–inorganic hybrid perovskites: Machine learning-driven co-navigation of chemical and compositional spaces Yang, Jonghee; Kalinin, Sergei V.; Cubuk, Ekin D. MRS Bulletin, Vol. 48, Issue 2 https://doi.org/10.1557/s43577-023-00490-y	journal	February 2023
Solvent engineering for high-performance inorganic–organic hybrid perovskite solar cells Jeon, Nam Joong; Noh, Jun Hong; Kim, Young Chan Nature Materials, Vol. 13, Issue 9, p. 897-903 https://doi.org/10.1038/nmat4014	journal	July 2014
Small grains as recombination hot spots in perovskite solar cells An, Qingzhi; Paulus, Fabian; Becker-Koch, David Matter, Vol. 4, Issue 5 https://doi.org/10.1016/j.matt.2021.02.020	journal	May 2021
Stable α/δ phase junction of formamidinium lead iodide perovskites for enhanced near-infrared emission Ma, Fusheng; Li, Jiangwei; Li, Wenzhe Chemical Science, Vol. 8, Issue 1 https://doi.org/10.1039/C6SC03542F	journal	January 2017
Influence of Solvent Coordination on Hybrid Organic–Inorganic Perovskite Formation Hamill, J. Clay; Schwartz, Jeffrey; Loo, Yueh-Lin ACS Energy Letters, Vol. 3, Issue 1 https://doi.org/10.1021/acsenergylett.7b01057	journal	November 2017
Solvent Engineering of Colloidal Quantum Dot Inks for Scalable Fabrication of Photovoltaics Yang, Jonghee; Kim, Minseon; Lee, Seungjin ACS Applied Materials & Interfaces, Vol. 13, Issue 31 https://doi.org/10.1021/acsami.1c06352	journal	July 2021
Structural and thermodynamic limits of layer thickness in 2D halide perovskites Soe, Chan Myae Myae; Nagabhushana, G. P.; Shivaramaiah, Radha Proceedings of the National Academy of Sciences, Vol. 116, Issue 1 https://doi.org/10.1073/pnas.1811006115	journal	December 2018
Local nanoscale phase impurities are degradation sites in halide perovskites Macpherson, Stuart; Doherty, Tiarnan A. S.; Winchester, Andrew J. Nature, Vol. 607, Issue 7918 https://doi.org/10.1038/s41586-022-04872-1	journal	May 2022
Understanding Film Formation Morphology and Orientation in High Member 2D Ruddlesden-Popper Perovskites for High-Efficiency Solar Cells Soe, Chan Myae Myae; Nie, Wanyi; Stoumpos, Constantinos C. Advanced Energy Materials, Vol. 8, Issue 1 https://doi.org/10.1002/aenm.201700979	journal	September 2017
Unravelling Light-Induced Degradation of Layered Perovskite Crystals and Design of Efficient Encapsulation for Improved Photostability Fang, Hong-Hua; Yang, Jie; Tao, Shuxia Advanced Functional Materials, Vol. 28, Issue 21 https://doi.org/10.1002/adfm.201800305	journal	April 2018
Stabilizing black-phase formamidinium perovskite formation at room temperature and high humidity Hui, Wei; Chao, Lingfeng; Lu, Hui Science, Vol. 371, Issue 6536 https://doi.org/10.1126/science.abf7652	journal	March 2021
2D perovskite stabilized phase-pure formamidinium perovskite solar cells Lee, Jin-Wook; Dai, Zhenghong; Han, Tae-Hee Nature Communications, Vol. 9, Issue 1 https://doi.org/10.1038/s41467-018-05454-4	journal	August 2018
Chemical Robotics Enabled Exploration of Stability in Multicomponent Lead Halide Perovskites via Machine Learning Higgins, Kate; Valleti, Sai Mani; Ziatdinov, Maxim ACS Energy Letters, Vol. 5, Issue 11 https://doi.org/10.1021/acsenergylett.0c01749	journal	October 2020
Distribution control enables efficient reduced-dimensional perovskite LEDs Ma, Dongxin; Lin, Kebin; Dong, Yitong Nature, Vol. 599, Issue 7886 https://doi.org/10.1038/s41586-021-03997-z	journal	November 2021
Understanding the Solution Chemistry of Lead Halide Perovskites Precursors Radicchi, Eros; Mosconi, Edoardo; Elisei, Fausto ACS Applied Energy Materials, Vol. 2, Issue 5 https://doi.org/10.1021/acsaem.9b00206	journal	April 2019
Thermal engineering of FAPbI3 perovskite material via radiative thermal annealing and in situ XRD Pool, Vanessa L.; Dou, Benjia; Van Campen, Douglas G. Nature Communications, Vol. 8, Issue 1 https://doi.org/10.1038/ncomms14075	journal	January 2017
Pseudo-halide anion engineering for α-FAPbI3 perovskite solar cells Jeong, Jaeki; Kim, Minjin; Seo, Jongdeuk Nature, Vol. 592, Issue 7854 https://doi.org/10.1038/s41586-021-03406-5	journal	April 2021
Metastable Dion-Jacobson 2D structure enables efficient and stable perovskite solar cells Zhang, Fei; Park, So Yeon; Yao, Canglang Science, Vol. 375, Issue 6576 https://doi.org/10.1126/science.abj2637	journal	January 2022
Crystalline Liquid-like Behavior: Surface-Induced Secondary Grain Growth of Photovoltaic Perovskite Thin Film Xue, Jingjing; Wang, Rui; Wang, Kai-Li Journal of the American Chemical Society, Vol. 141, Issue 35 https://doi.org/10.1021/jacs.9b06940	journal	August 2019
Effect of intramolecular hydrogen-bond formation on the molecular conformation of amino acids Giubertoni, Giulia; Sofronov, Oleksandr O.; Bakker, Huib J. Communications Chemistry, Vol. 3, Issue 1 https://doi.org/10.1038/s42004-020-0329-7	journal	June 2020
Energy Funneling in Quasi‐2D Ruddlesden–Popper Perovskites: Charge Transfer versus Resonant Energy Transfer Gan, Zhixing; Chen, Weijian; Liu, Cihui Advanced Photonics Research, Vol. 3, Issue 1 https://doi.org/10.1002/adpr.202100283	journal	November 2021
Layered Hybrid Formamidinium Lead Iodide Perovskites: Challenges and Opportunities Milić, Jovana V.; Zakeeruddin, Shaik M.; Grätzel, Michael Accounts of Chemical Research, Vol. 54, Issue 12 https://doi.org/10.1021/acs.accounts.0c00879	journal	June 2021
Understanding Degradation Mechanisms and Improving Stability of Perovskite Photovoltaics Boyd, Caleb C.; Cheacharoen, Rongrong; Leijtens, Tomas Chemical Reviews, Vol. 119, Issue 5 https://doi.org/10.1021/acs.chemrev.8b00336	journal	November 2018
High-performance large-area quasi-2D perovskite light-emitting diodes Sun, Changjiu; Jiang, Yuanzhi; Cui, Minghuan Nature Communications, Vol. 12, Issue 1 https://doi.org/10.1038/s41467-021-22529-x	journal	April 2021
Understanding the Role of Cesium on Chemical Complexity in Methylammonium‐Free Metal Halide Perovskites Yang, Jonghee; LaFollette, Diana K.; Lawrie, Benjamin J. Advanced Energy Materials https://doi.org/10.1002/aenm.202202880	journal	December 2022
Perovskite energy funnels for efficient light-emitting diodes Yuan, Mingjian; Quan, Li Na; Comin, Riccardo Nature Nanotechnology, Vol. 11, Issue 10 https://doi.org/10.1038/nnano.2016.110	journal	June 2016
A PKB-SPEG signaling nexus links insulin resistance with diabetic cardiomyopathy by regulating calcium homeostasis Quan, Chao; Du, Qian; Li, Min Nature Communications, Vol. 11, Issue 1 https://doi.org/10.1038/s41467-020-16116-9	journal	May 2020
Revisiting the Aqueous Solutions of Dimethyl Sulfoxide by Spectroscopy in the Mid- and Near-Infrared: Experiments and Car–Parrinello Simulations Wallace, Victoria M.; Dhumal, Nilesh R.; Zehentbauer, Florian M. The Journal of Physical Chemistry B, Vol. 119, Issue 46 https://doi.org/10.1021/acs.jpcb.5b09196	journal	November 2015
Phase Transition Control for High Performance Ruddlesden-Popper Perovskite Solar Cells Zhang, Xu; Munir, Rahim; Xu, Zhuo Advanced Materials, Vol. 30, Issue 21 https://doi.org/10.1002/adma.201707166	journal	April 2018
Perovskite solar cells with atomically coherent interlayers on SnO2 electrodes Min, Hanul; Lee, Do Yoon; Kim, Junu Nature, Vol. 598, Issue 7881 https://doi.org/10.1038/s41586-021-03964-8	journal	October 2021
Stabilization of the Metastable Lead Iodide Perovskite Phase via Surface Functionalization Fu, Yongping; Wu, Tao; Wang, Jue Nano Letters, Vol. 17, Issue 7 https://doi.org/10.1021/acs.nanolett.7b01500	journal	June 2017
Intercalating-Organic-Cation-Induced Stability Bowing in Quasi-2D Metal-Halide Perovskites Zhang, Jiyun; Langner, Stefan; Wu, Jianchang ACS Energy Letters, Vol. 7, Issue 1 https://doi.org/10.1021/acsenergylett.1c02081	journal	December 2021
Semiconductor physics of organic–inorganic 2D halide perovskites Blancon, Jean-Christophe; Even, Jacky; Stoumpos, Costas. C. Nature Nanotechnology, Vol. 15, Issue 12 https://doi.org/10.1038/s41565-020-00811-1	journal	December 2020
Tailoring the Energy Landscape in Quasi-2D Halide Perovskites Enables Efficient Green-Light Emission Quan, Li Na; Zhao, Yongbiao; García de Arquer, F. Pelayo Nano Letters, Vol. 17, Issue 6 https://doi.org/10.1021/acs.nanolett.7b00976	journal	May 2017
Discovery of a New Intermediate Enables One‐Step Deposition of High‐Quality Perovskite Films via Solvent Engineering Hu, Chen; Shivarudraiah, Sunil B.; Sung, Herman H. Y. Solar RRL, Vol. 5, Issue 4 https://doi.org/10.1002/solr.202000712	journal	February 2021
Tailoring the Functionality of Organic Spacer Cations for Efficient and Stable Quasi‐2D Perovskite Solar Cells Fu, Weifei; Liu, Hongbin; Shi, Xueliang Advanced Functional Materials, Vol. 29, Issue 25 https://doi.org/10.1002/adfm.201900221	journal	April 2019
Ultra-bright, efficient and stable perovskite light-emitting diodes Kim, Joo Sung; Heo, Jung-Min; Park, Gyeong-Su Nature, Vol. 611, Issue 7937 https://doi.org/10.1038/s41586-022-05304-w	journal	November 2022
A bilayer conducting polymer structure for planar perovskite solar cells with over 1,400 hours operational stability at elevated temperatures Zhao, Yicheng; Heumueller, Thomas; Zhang, Jiyun Nature Energy, Vol. 7, Issue 2 https://doi.org/10.1038/s41560-021-00953-z	journal	December 2021
Ab initio random structure searching of organic molecular solids: assessment and validation against experimental data Zilka, Miri; Dudenko, Dmytro V.; Hughes, Colan E. Physical Chemistry Chemical Physics, Vol. 19, Issue 38 https://doi.org/10.1039/C7CP04186A	journal	January 2017
Suppressing phase disproportionation in quasi-2D perovskite light-emitting diodes Wang, Kang; Lin, Zih-Yu; Zhang, Zihan Nature Communications, Vol. 14, Issue 1 https://doi.org/10.1038/s41467-023-36118-7	journal	January 2023
High-Throughput Study of Antisolvents on the Stability of Multicomponent Metal Halide Perovskites through Robotics-Based Synthesis and Machine Learning Approaches Higgins, Kate; Ziatdinov, Maxim; Kalinin, Sergei V. Journal of the American Chemical Society, Vol. 143, Issue 47 https://doi.org/10.1021/jacs.1c10045	journal	November 2021

Similar Records

Decoding the Broadband Emission of 2D Pb-Sn Halide Perovskites through High-Throughput Exploration

Journal Article · 2024 · Advanced Functional Materials · OSTI ID:2491457

Foadian, Elham; Yang, Jonghee; Harris, Sumner B.; +7 more

In-situ X-Ray Analysis of Rapid Thermal Processing for Thin-Film Solar Cells: Closing the Gap between Production and Laboratory Efficiency

Technical Report · 2017 · OSTI ID:1395583

Toney, Michael F.; van Hest, Maikel F. A. M.

Understanding the Role of Cesium on Chemical Complexity in Methylammonium-Free Metal Halide Perovskites

Journal Article · 2022 · Advanced Energy Materials · OSTI ID:1961963

Yang, Jonghee; LaFollette, Diana K.; Lawrie, Benjamin J.; +6 more

Related Subjects

36 MATERIALS SCIENCE
2D perovskites
accelerated materials discovery
high-throughput synthesis
phase growths

Title: High-Throughput Automated Exploration of Phase Growth Behaviors in Quasi-2D Formamidinium Metal Halide Perovskites

Citation Formats

References (50)

Similar Records

Related Subjects