Homogenized halides and alkali cation segregation in alloyed organic-inorganic perovskites

Correa-Baena, Juan-Pablo; Luo, Yanqi; Brenner, Thomas M.; Snaider, Jordan; Sun, Shijing; Li, Xueying; Jensen, Mallory A.; Hartono, Noor Titan Putri; Nienhaus, Lea; Wieghold, Sarah; Poindexter, Jeremy R.; Wang, Shen; Meng, Ying Shirley; Wang, Ti; Lai, Barry; Holt, Martin V.; Cai, Zhonghou; Bawendi, Moungi G.; Huang, Libai; Buonassisi, Tonio; Fenning, David P.

doi:10.1126/science.aah5065

Homogenized halides and alkali cation segregation in alloyed organic-inorganic perovskites

Journal Article · Thu Feb 07 00:00:00 EST 2019 · Science

DOI:https://doi.org/10.1126/science.aah5065· OSTI ID:1528643

; ; ; ; Sun, Shijing; Li, Xueying; ; ; ; ; ; ; ; ; ; Holt, Martin V.; Cai, Zhonghou; ; ; more »

The role of the alkali metal cations in halide perovskite solar cells is not well understood. Using synchrotron-based nano–x-ray fluorescence and complementary measurements, we found that the halide distribution becomes homogenized upon addition of cesium iodide, either alone or with rubidium iodide, for substoichiometric, stoichiometric, and overstoichiometric preparations, where the lead halide is varied with respect to organic halide precursors. Halide homogenization coincides with long-lived charge carrier decays, spatially homogeneous carrier dynamics (as visualized by ultrafast microscopy), and improved photovoltaic device performance. We found that rubidium and potassium phase-segregate in highly concentrated clusters. Alkali metals are beneficial at low concentrations, where they homogenize the halide distribution, but at higher concentrations, they form recombination-active second-phase clusters.

View Journal Article

Research Organization:: Argonne National Lab. (ANL), Argonne, IL (United States); Energy Frontier Research Centers (EFRC) (United States). Center for Excitonics (CE); Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States); Purdue Univ., West Lafayette, IN (United States); Univ. of California, San Diego, CA (United States)

Sponsoring Organization:: California Energy Commission (United States); National Science Foundation (NSF) (United States); USDOE; USDOE Office of Energy Efficiency and Renewable Energy (EERE); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC02-06CH11357; SC0001088

OSTI ID:: 1528643

Alternate ID(s):: OSTI ID: 1493911

Journal Information:: Science, Journal Name: Science Journal Issue: 6427 Vol. 363; ISSN 0036-8075

Publisher:: American Association for the Advancement of Science (AAAS)Copyright Statement

Country of Publication:: United States

Language:: English

References (32)

The Relationship between Chemical Flexibility and Nanoscale Charge Collection in Hybrid Halide Perovskites Luo, Yanqi; Aharon, Sigalit; Stuckelberger, Michael Advanced Functional Materials, Vol. 28, Issue 18 https://doi.org/10.1002/adfm.201706995	journal	March 2018
High-Efficiency Perovskite Solar Cells Based on the Black Polymorph of HC(NH ₂ ) ₂ PbI ₃ Lee, Jin-Wook; Seol, Dong-Jin; Cho, An-Na Advanced Materials, Vol. 26, Issue 29 https://doi.org/10.1002/adma.201401137	journal	June 2014
Rubidium Multication Perovskite with Optimized Bandgap for Perovskite-Silicon Tandem with over 26% Efficiency Duong, The; Wu, YiLiang; Shen, Heping Advanced Energy Materials, Vol. 7, Issue 14 https://doi.org/10.1002/aenm.201700228	journal	April 2017
Mixed-Organic-Cation Perovskite Photovoltaics for Enhanced Solar-Light Harvesting Pellet, Norman; Gao, Peng; Gregori, Giuliano Angewandte Chemie International Edition, Vol. 53, Issue 12, p. 3151-3157 https://doi.org/10.1002/anie.201309361	journal	February 2014
Structural inhomogeneities in polycrystalline silicon on glass solar cells and their effects on device characteristics Wong, J.; Huang, J. L.; Varlamov, S. Progress in Photovoltaics: Research and Applications, Vol. 19, Issue 6 https://doi.org/10.1002/pip.1089	journal	January 2011
Three-dimensional electron microscopy simulation with the CASINO Monte Carlo software Demers, Hendrix; Poirier-Demers, Nicolas; Couture, Alexandre Réal Scanning, Vol. 33, Issue 3 https://doi.org/10.1002/sca.20262	journal	May 2011
Hybrid Perovskites for Photovoltaics: Charge-Carrier Recombination, Diffusion, and Radiative Efficiencies Johnston, Michael B.; Herz, Laura M. Accounts of Chemical Research, Vol. 49, Issue 1 https://doi.org/10.1021/acs.accounts.5b00411	journal	December 2015
Stabilizing Perovskite Structures by Tuning Tolerance Factor: Formation of Formamidinium and Cesium Lead Iodide Solid-State Alloys Li, Zhen; Yang, Mengjin; Park, Ji-Sang Chemistry of Materials, Vol. 28, Issue 1 https://doi.org/10.1021/acs.chemmater.5b04107	journal	December 2015
Role of 4- tert -Butylpyridine as a Hole Transport Layer Morphological Controller in Perovskite Solar Cells Wang, Shen; Sina, Mahsa; Parikh, Pritesh Nano Letters, Vol. 16, Issue 9 https://doi.org/10.1021/acs.nanolett.6b02158	journal	August 2016
High-Efficiency Rubidium-Incorporated Perovskite Solar Cells by Gas Quenching Zhang, Meng; Yun, Jae S.; Ma, Qingshan ACS Energy Letters, Vol. 2, Issue 2 https://doi.org/10.1021/acsenergylett.6b00697	journal	January 2017
Unreacted PbI ₂ as a Double-Edged Sword for Enhancing the Performance of Perovskite Solar Cells Jacobsson, T. Jesper; Correa-Baena, Juan-Pablo; Halvani Anaraki, Elham Journal of the American Chemical Society, Vol. 138, Issue 32 https://doi.org/10.1021/jacs.6b06320	journal	August 2016
Phase Segregation in Cs-, Rb- and K-Doped Mixed-Cation (MA) _x (FA) _{1– x} PbI ₃ Hybrid Perovskites from Solid-State NMR Kubicki, Dominik J.; Prochowicz, Daniel; Hofstetter, Albert Journal of the American Chemical Society, Vol. 139, Issue 40 https://doi.org/10.1021/jacs.7b07223	journal	September 2017
Compositional engineering of perovskite materials for high-performance solar cells Jeon, Nam Joong; Noh, Jun Hong; Yang, Woon Seok Nature, Vol. 517, Issue 7535 https://doi.org/10.1038/nature14133	journal	January 2015
Maximizing and stabilizing luminescence from halide perovskites with potassium passivation Abdi-Jalebi, Mojtaba; Andaji-Garmaroudi, Zahra; Cacovich, Stefania Nature, Vol. 555, Issue 7697 https://doi.org/10.1038/nature25989	journal	March 2018
Hysteresis-free perovskite solar cells made of potassium-doped organometal halide perovskite Tang, Zeguo; Bessho, Takeru; Awai, Fumiyasu Scientific Reports, Vol. 7, Issue 1 https://doi.org/10.1038/s41598-017-12436-x	journal	September 2017
High efficiency methylammonium lead triiodide perovskite solar cells: the relevance of non-stoichiometric precursors Roldán-Carmona, C.; Gratia, P.; Zimmermann, I. Energy & Environmental Science, Vol. 8, Issue 12 https://doi.org/10.1039/C5EE02555A	journal	January 2015
Highly efficient planar perovskite solar cells through band alignment engineering Correa Baena, Juan Pablo; Steier, Ludmilla; Tress, Wolfgang Energy & Environmental Science, Vol. 8, Issue 10 https://doi.org/10.1039/C5EE02608C	journal	January 2015
Entropic stabilization of mixed A-cation ABX ₃ metal halide perovskites for high performance perovskite solar cells Yi, Chenyi; Luo, Jingshan; Meloni, Simone Energy & Environmental Science, Vol. 9, Issue 2 https://doi.org/10.1039/C5EE03255E	journal	January 2016
Cesium-containing triple cation perovskite solar cells: improved stability, reproducibility and high efficiency Saliba, Michael; Matsui, Taisuke; Seo, Ji-Youn Energy & Environmental Science, Vol. 9, Issue 6 https://doi.org/10.1039/C5EE03874J	journal	January 2016
Exploration of the compositional space for mixed lead halogen perovskites for high efficiency solar cells Jesper Jacobsson, T.; Correa-Baena, Juan-Pablo; Pazoki, Meysam Energy & Environmental Science, Vol. 9, Issue 5 https://doi.org/10.1039/C6EE00030D	journal	January 2016
A novel quadruple-cation absorber for universal hysteresis elimination for high efficiency and stable perovskite solar cells Bu, Tongle; Liu, Xueping; Zhou, Yuan Energy & Environmental Science, Vol. 10, Issue 12 https://doi.org/10.1039/C7EE02634J	journal	January 2017
Enhanced charge carrier mobility and lifetime suppress hysteresis and improve efficiency in planar perovskite solar cells Turren-Cruz, Silver-Hamill; Saliba, Michael; Mayer, Matthew T. Energy & Environmental Science, Vol. 11, Issue 1 https://doi.org/10.1039/C7EE02901B	journal	January 2018
Formamidinium lead trihalide: a broadly tunable perovskite for efficient planar heterojunction solar cells Eperon, Giles E.; Stranks, Samuel D.; Menelaou, Christopher Energy & Environmental Science, Vol. 7, Issue 3 https://doi.org/10.1039/c3ee43822h	journal	January 2014
MAPS : A set of software tools for analysis and visualization of 3D X-ray fluorescence data sets Vogt, S. Journal de Physique IV (Proceedings), Vol. 104 https://doi.org/10.1051/jp4:20030160	journal	March 2003
Synchrotron-based investigations of the nature and impact of iron contamination in multicrystalline silicon solar cells Buonassisi, Tonio; Istratov, Andrei A.; Heuer, Matthias Journal of Applied Physics, Vol. 97, Issue 7 https://doi.org/10.1063/1.1866489	journal	April 2005
Ultrafast optical snapshots of hybrid perovskites reveal the origin of multiband electronic transitions Appavoo, Kannatassen; Nie, Wanyi; Blancon, Jean-Christophe Physical Review B, Vol. 96, Issue 19 https://doi.org/10.1103/PhysRevB.96.195308	journal	November 2017
Efficient luminescent solar cells based on tailored mixed-cation perovskites Bi, Dongqin; Tress, Wolfgang; Dar, M. Ibrahim Science Advances, Vol. 2, Issue 1 https://doi.org/10.1126/sciadv.1501170	journal	January 2016
Strained hybrid perovskite thin films and their impact on the intrinsic stability of perovskite solar cells Zhao, Jingjing; Deng, Yehao; Wei, Haotong Science Advances, Vol. 3, Issue 11 https://doi.org/10.1126/sciadv.aao5616	journal	November 2017
Incorporation of rubidium cations into perovskite solar cells improves photovoltaic performance Saliba, M.; Matsui, T.; Domanski, K. Science, Vol. 354, Issue 6309 https://doi.org/10.1126/science.aah5557	journal	September 2016
Promises and challenges of perovskite solar cells Correa-Baena, Juan-Pablo; Saliba, Michael; Buonassisi, Tonio Science, Vol. 358, Issue 6364 https://doi.org/10.1126/science.aam6323	journal	November 2017
Iodide management in formamidinium-lead-halide–based perovskite layers for efficient solar cells Yang, Woon Seok; Park, Byung-Wook; Jung, Eui Hyuk Science, Vol. 356, Issue 6345 https://doi.org/10.1126/science.aan2301	journal	June 2017
Engineering solar cells based on correlative X-ray microscopy Stuckelberger, Michael; West, Bradley; Nietzold, Tara Journal of Materials Research, Vol. 32, Issue 10 https://doi.org/10.1557/jmr.2017.108	journal	May 2017

Similar Records

Role of Alkali-Metal Cations in Electronic Structure and Halide Segregation of Hybrid Perovskites

Journal Article · Tue Jun 30 20:00:00 EDT 2020 · ACS Applied Materials and Interfaces · OSTI ID:1658811

STABILITY OF ALKALI HALIDE CRYSTALS IN TERMS OF MANY-BODY INTERACTIONS

Journal Article · Tue Dec 31 23:00:00 EST 1963 · Phys. Rev. Letters · OSTI ID:4102007

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Homogenized halides and alkali cation segregation in alloyed organic-inorganic perovskites

Citation Formats

References (32)

Similar Records

Related Subjects