Exploring the Relationship of Microstructure and Conductivity in Metal Halide Perovskites via Active Learning-Driven Automated Scanning Probe Microscopy

Liu, Yongtao; Yang, Jonghee; Vasudevan, Rama K.; Kelley, Kyle P.; Ziatdinov, Maxim; Kalinin, Sergei V.; Ahmadi, Mahshid

doi:10.1021/acs.jpclett.3c00223

Exploring the Relationship of Microstructure and Conductivity in Metal Halide Perovskites via Active Learning-Driven Automated Scanning Probe Microscopy

Journal Article · Thu Mar 30 00:00:00 EDT 2023 · Journal of Physical Chemistry Letters

DOI:https://doi.org/10.1021/acs.jpclett.3c00223· OSTI ID:1964022

^[1]; ^[2]; ^[3]; ^[3]; ^[3]; ^[2]; ^[2]

Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Penn State University
Univ. of Tennessee, Knoxville, TN (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

Electronic transport and hysteresis in metal halide perovskites (MHPs) are key to the applications in photovoltaics, light emitting devices, and light and chemical sensors. These phenomena are strongly affected by the materials microstructure including grain boundaries, ferroic domain walls, and secondary phase inclusions. Here, we demonstrate an active machine learning framework for “driving” an automated scanning probe microscope (SPM) to discover the microstructures responsible for specific aspects of transport behavior in MHPs. In our setup, the microscope can discover the microstructural elements that maximize the onset of conduction, hysteresis, or any other characteristic that can be derived from a set of current–voltage spectra. Furthermore, this approach opens new opportunities for exploring the origins of materials functionality in complex materials by SPM and can be integrated with other characterization techniques either before (prior knowledge) or after (identification of locations of interest for detail studies) functional probing.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Pennsylvania State Univ., University Park, PA (United States); Pennsylvania State University, University Park, PA (United States)

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

Grant/Contract Number:: AC05-00OR22725; SC0021118

OSTI ID:: 1964022

Alternate ID(s):: OSTI ID: 2333855
OSTI ID: 2283162

Journal Information:: Journal of Physical Chemistry Letters, Journal Name: Journal of Physical Chemistry Letters Journal Issue: 13 Vol. 14; ISSN 1948-7185

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

References (47)

Direct Observation of Photoinduced Ion Migration in Lead Halide Perovskites Liu, Yongtao; Ievlev, Anton V.; Borodinov, Nikolay Advanced Functional Materials, Vol. 31, Issue 8 https://doi.org/10.1002/adfm.202008777	journal	November 2020
Nanoscale Insights into Photovoltaic Hysteresis in Triple‐Cation Mixed‐Halide Perovskite: Resolving the Role of Polarization and Ionic Migration Xia, Guozhan; Huang, Boyuan; Zhang, Ying Advanced Materials, Vol. 31, Issue 36 https://doi.org/10.1002/adma.201902870	journal	June 2019
Disentangling Ferroelectric Wall Dynamics and Identification of Pinning Mechanisms via Deep Learning Liu, Yongtao; Proksch, Roger; Wong, Chun Yin Advanced Materials, Vol. 33, Issue 43 https://doi.org/10.1002/adma.202103680	journal	September 2021
Hysteretic Ion Migration and Remanent Field in Metal Halide Perovskites Liu, Yongtao; Borodinov, Nikolay; Lorenz, Matthias Advanced Science, Vol. 7, Issue 19 https://doi.org/10.1002/advs.202001176	journal	August 2020
Exploring Physics of Ferroelectric Domain Walls in Real Time: Deep Learning Enabled Scanning Probe Microscopy Liu, Yongtao; Kelley, Kyle P.; Funakubo, Hiroshi Advanced Science, Vol. 9, Issue 31 https://doi.org/10.1002/advs.202203957	journal	September 2022
X‐Ray Microscopy of Halide Perovskites: Techniques, Applications, and Prospects Kodur, Moses; Kumar, Rishi E.; Luo, Yanqi Advanced Energy Materials https://doi.org/10.1002/aenm.201903170	journal	January 2020
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
Automated Experiments of Local Non‐Linear Behavior in Ferroelectric Materials Liu, Yongtao; Kelley, Kyle P.; Vasudevan, Rama K. Small, Vol. 18, Issue 48 https://doi.org/10.1002/smll.202204130	journal	October 2022
Electromechanical-mnemonic effects in BiFeO3 for electric field history-dependent crystallographic phase patterning Neumayer, S. M.; Browne, N.; Naden, A. B. Journal of Materials Science, Vol. 53, Issue 14 https://doi.org/10.1007/s10853-018-2278-4	journal	April 2018
Nanoscopic impurities trigger perovskite degradation Hao, Mingwei; Zhou, Yuanyuan Joule, Vol. 6, Issue 7 https://doi.org/10.1016/j.joule.2022.06.024	journal	July 2022
Multimodal microscopy characterization of halide perovskite semiconductors: Revealing a new world (dis)order Stranks, Samuel D. Matter, Vol. 4, Issue 12 https://doi.org/10.1016/j.matt.2021.10.025	journal	December 2021
The role of grain boundaries in perovskite solar cells Lee, Jin-Wook; Bae, Sang-Hoon; De Marco, Nicholas Materials Today Energy, Vol. 7 https://doi.org/10.1016/j.mtener.2017.07.014	journal	March 2018
Unraveling the hysteretic behavior at double cations-double halides perovskite - electrode interfaces Kim, Dohyung; Liu, Yongtao; Ievlev, Anton V. Nano Energy, Vol. 89 https://doi.org/10.1016/j.nanoen.2021.106428	journal	November 2021
Cs0.15FA0.85PbI3/CsxFA1-xPbI3 Core/Shell Heterostructure for Highly Stable and Efficient Perovskite Solar Cells Peng, Zijian; Wei, Qi; Chen, Hao Cell Reports Physical Science, Vol. 1, Issue 10 https://doi.org/10.1016/j.xcrp.2020.100224	journal	October 2020
Halide Perovskite Photovoltaics: Background, Status, and Future Prospects Jena, Ajay Kumar; Kulkarni, Ashish; Miyasaka, Tsutomu Chemical Reviews, Vol. 119, Issue 5 https://doi.org/10.1021/acs.chemrev.8b00539	journal	March 2019
Ferroelastic Fingerprints in Methylammonium Lead Iodide Perovskite Hermes, Ilka M.; Bretschneider, Simon A.; Bergmann, Victor W. The Journal of Physical Chemistry C, Vol. 120, Issue 10 https://doi.org/10.1021/acs.jpcc.5b11469	journal	January 2016
Subgrain Special Boundaries in Halide Perovskite Thin Films Restrict Carrier Diffusion Li, Wenhao; Yadavalli, Srinivas K.; Lizarazo-Ferro, David ACS Energy Letters, Vol. 3, Issue 11 https://doi.org/10.1021/acsenergylett.8b01704	journal	October 2018
Correlating Crystallographic Orientation and Ferroic Properties of Twin Domains in Metal Halide Perovskites Liu, Yongtao; Trimby, Patrick; Collins, Liam ACS Nano, Vol. 15, Issue 4 https://doi.org/10.1021/acsnano.1c00310	journal	March 2021
Role of Decomposition Product Ions in Hysteretic Behavior of Metal Halide Perovskite Liu, Yongtao; Borodinov, Nikolay; Collins, Liam ACS Nano, Vol. 15, Issue 5 https://doi.org/10.1021/acsnano.1c02097	journal	May 2021
Probing Local Ionic Dynamics in Functional Oxides at the Nanoscale Strelcov, Evgheni; Kim, Yunseok; Jesse, Stephen Nano Letters, Vol. 13, Issue 8 https://doi.org/10.1021/nl400780d	journal	July 2013
Direct observation of intrinsic twin domains in tetragonal CH3NH3PbI3 Rothmann, Mathias Uller; Li, Wei; Zhu, Ye Nature Communications, Vol. 8, Issue 1 https://doi.org/10.1038/ncomms14547	journal	February 2017
In situ dynamic observations of perovskite crystallisation and microstructure evolution intermediated from [PbI6]4− cage nanoparticles Hu, Qin; Zhao, Lichen; Wu, Jiang Nature Communications, Vol. 8, Issue 1 https://doi.org/10.1038/ncomms15688	journal	June 2017
Benign ferroelastic twin boundaries in halide perovskites for charge carrier transport and recombination Xiao, Xun; Li, Wenhao; Fang, Yanjun Nature Communications, Vol. 11, Issue 1 https://doi.org/10.1038/s41467-020-16075-1	journal	May 2020
Mapping structure heterogeneities and visualizing moisture degradation of perovskite films with nano-focus WAXS Li, Nian; Pratap, Shambhavi; Körstgens, Volker Nature Communications, Vol. 13, Issue 1 https://doi.org/10.1038/s41467-022-34426-y	journal	November 2022
Learning the right channel in multimodal imaging: automated experiment in piezoresponse force microscopy Liu, Yongtao; Vasudevan, Rama K.; Kelley, Kyle P. npj Computational Materials, Vol. 9, Issue 1 https://doi.org/10.1038/s41524-023-00985-x	journal	March 2023
Advances and challenges in understanding the microscopic structure–property–performance relationship in perovskite solar cells Zhou, Yuanyuan; Herz, Laura M.; Jen, Alex K-Y. Nature Energy, Vol. 7, Issue 9 https://doi.org/10.1038/s41560-022-01096-5	journal	September 2022
Chemical nature of ferroelastic twin domains in CH3NH3PbI3 perovskite Liu, Yongtao; Collins, Liam; Proksch, Roger Nature Materials, Vol. 17, Issue 11 https://doi.org/10.1038/s41563-018-0152-z	journal	August 2018
Nanoscale chemical heterogeneity dominates the optoelectronic response of alloyed perovskite solar cells Frohna, Kyle; Anaya, Miguel; Macpherson, Stuart Nature Nanotechnology, Vol. 17, Issue 2 https://doi.org/10.1038/s41565-021-01019-7	journal	November 2021
Heterogeneity at multiple length scales in halide perovskite semiconductors Tennyson, Elizabeth M.; Doherty, Tiarnan A. S.; Stranks, Samuel D. Nature Reviews Materials, Vol. 4, Issue 9 https://doi.org/10.1038/s41578-019-0125-0	journal	July 2019
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
Experimental discovery of structure–property relationships in ferroelectric materials via active learning Liu, Yongtao; Kelley, Kyle P.; Vasudevan, Rama K. Nature Machine Intelligence, Vol. 4, Issue 4 https://doi.org/10.1038/s42256-022-00460-0	journal	April 2022
AtomAI framework for deep learning analysis of image and spectroscopy data in electron and scanning probe microscopy Ziatdinov, Maxim; Ghosh, Ayana; Wong, Chun Yin Nature Machine Intelligence, Vol. 4, Issue 12 https://doi.org/10.1038/s42256-022-00555-8	journal	December 2022
Anisotropic carrier diffusion in single MAPbI ₃ grains correlates to their twin domains Hermes, Ilka M.; Best, Andreas; Winkelmann, Leonard Energy & Environmental Science, Vol. 13, Issue 11 https://doi.org/10.1039/D0EE01016B	journal	January 2020
Two birds with one stone: dual grain-boundary and interface passivation enables >22% efficient inverted methylammonium-free perovskite solar cells Gharibzadeh, Saba; Fassl, Paul; Hossain, Ihteaz M. Energy & Environmental Science, Vol. 14, Issue 11 https://doi.org/10.1039/D1EE01508G	journal	January 2021
Identifying high-performance and durable methylammonium-free lead halide perovskites via high-throughput synthesis and characterization An, Yu; Perini, Carlo Andrea Riccardo; Hidalgo, Juanita Energy & Environmental Science, Vol. 14, Issue 12 https://doi.org/10.1039/D1EE02691G	journal	January 2021
Twin domains modulate light-matter interactions in metal halide perovskites Liu, Yongtao; Li, Mingxing; Wang, Miaosheng APL Materials, Vol. 8, Issue 1 https://doi.org/10.1063/1.5127866	journal	January 2020
Probing polarization dynamics at specific domain configurations: Computer-vision based automated experiment in piezoresponse force microscopy Kelley, Kyle P.; Kalinin, Sergei V.; Ziatdinov, Maxim Applied Physics Letters, Vol. 119, Issue 13 https://doi.org/10.1063/5.0062046	journal	September 2021
Time resolved surface photovoltage measurements using a big data capture approach to KPFM Collins, Liam; Ahmadi, Mahshid; Qin, Jiajun Nanotechnology, Vol. 29, Issue 44 https://doi.org/10.1088/1361-6528/aad873	journal	September 2018
Disentangling ferroelectric domain wall geometries and pathways in dynamic piezoresponse force microscopy via unsupervised machine learning Kalinin, Sergei V.; Steffes, James J.; Liu, Yongtao Nanotechnology, Vol. 33, Issue 5 https://doi.org/10.1088/1361-6528/ac2f5b	journal	November 2021
Decoding the shift-invariant data: applications for band-excitation scanning probe microscopy ^* Liu, Yongtao; Vasudevan, Rama K.; Kelley, Kyle K. Machine Learning: Science and Technology, Vol. 2, Issue 4 https://doi.org/10.1088/2632-2153/ac28de	journal	October 2021
Holistically-Nested Edge Detection Xie, Saining; Tu, Zhuowen 2015 IEEE International Conference on Computer Vision (ICCV) https://doi.org/10.1109/ICCV.2015.164	conference	December 2015
Nanoscale mapping of chemical composition in organic-inorganic hybrid perovskite films Szostak, R.; Silva, J. C.; Turren-Cruz, S. -H. Science Advances, Vol. 5, Issue 10 https://doi.org/10.1126/sciadv.aaw6619	journal	October 2019
Initializing film homogeneity to retard phase segregation for stable perovskite solar cells Bai, Yang; Huang, Zijian; Zhang, Xiao Science, Vol. 378, Issue 6621 https://doi.org/10.1126/science.abn3148	journal	November 2022
Angle-Resolved Cathodoluminescence Polarimetry of Hybrid Perovskites Dhami, Bibek S.; Iyer, Vasudevan; Pant, Aniket arXiv https://doi.org/10.48550/arXiv.2201.06484	preprint	January 2022
Hyperspectral nanoscale mapping of hybrid perovskite photophysics at the single grain level Taylor, Ethan J.; Iyer, Vasudevan; Dhami, Bibek S. arXiv https://doi.org/10.48550/arXiv.2201.06546	preprint	January 2022
Mapping the Pathways of Photo-induced Ion Migration in Organic-inorganic Hybrid Halide Perovskites Kim, Taeyong; Park, Soyeon; Iyer, Vasudevan arXiv https://doi.org/10.48550/arXiv.2210.04426	preprint	January 2022
Disentangling electronic transport and hysteresis at individual grain boundaries in hybrid perovskites via automated scanning probe microscopy Liu, Yongtao; Yang, Jonghee; Lawrie, Benjamin J. arXiv https://doi.org/10.48550/arXiv.2210.14138	preprint	January 2022

Similar Records

Disentangling Electronic Transport and Hysteresis at Individual Grain Boundaries in Hybrid Perovskites via Automated Scanning Probe Microscopy

Journal Article · Sun May 07 20:00:00 EDT 2023 · ACS Nano · OSTI ID:1976045

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Exploring the Relationship of Microstructure and Conductivity in Metal Halide Perovskites via Active Learning-Driven Automated Scanning Probe Microscopy

Citation Formats

References (47)

Similar Records

Related Subjects