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      The Nature of Ion Conduction in Methylammonium Lead Iodide: A Multimethod Approach

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          Abstract

          By applying a multitude of experimental techniques including 1H, 14N, 207Pb NMR and 127I NMR/NQR, tracer diffusion, reaction cell and doping experiments, as well as stoichiometric variation, conductivity, and polarization experiments, iodine ions are unambiguously shown to be the mobile species in CH 3NH 3PbI 3, with iodine vacancies shown to represent the mechanistic centers under equilibrium conditions. Pb 2+ and CH 3NH 3 + ions do not significantly contribute to the long range transport (upper limits for their contributions are given), whereby the latter exhibit substantial local motion. The decisive electronic contribution to the mixed conductivity in the experimental window stems from electron holes. As holes can be associated with iodine orbitals, local variations of the iodine stoichiometry may be fast and enable light effects on ion transport.

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          Anomalous Hysteresis in Perovskite Solar Cells.

          Henry J Snaith, Antonio Abate, James M Ball … (2014)
          Perovskite solar cells have rapidly risen to the forefront of emerging photovoltaic technologies, exhibiting rapidly rising efficiencies. This is likely to continue to rise, but in the development of these solar cells there are unusual characteristics that have arisen, specifically an anomalous hysteresis in the current-voltage curves. We identify this phenomenon and show some examples of factors that make the hysteresis more or less extreme. We also demonstrate stabilized power output under working conditions and suggest that this is a useful parameter to present, alongside the current-voltage scan derived power conversion efficiency. We hypothesize three possible origins of the effect and discuss its implications on device efficiency and future research directions. Understanding and resolving the hysteresis is essential for further progress and is likely to lead to a further step improvement in performance.
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            Photoinduced Giant Dielectric Constant in Lead Halide Perovskite Solar Cells.

            Emilio Juarez-Perez, Rafael S. Sanchez, Laura Badia … (2014)
            Organic-inorganic lead trihalide perovskites have emerged as an outstanding photovoltaic material that demonstrated a high 17.9% conversion efficiency of sunlight to electricity in a short time. We have found a giant dielectric constant (GDC) phenomenon in these materials consisting on a low frequency dielectric constant in the dark of the order of ε0 = 1000. We also found an unprecedented behavior in which ε0 further increases under illumination or by charge injection at applied bias. We observe that ε0 increases nearly linearly with the illumination intensity up to an additional factor 1000 under 1 sun. Measurement of a variety of samples of different morphologies, compositions, and different types of contacts shows that the GDC is an intrinsic property of MAPbX3 (MA = CH3NH3(+)). We hypothesize that the large dielectric response is induced by structural fluctuations. Photoinduced carriers modify the local unit cell equilibrium and change the polarizability, assisted by the freedom of rotation of MA. The study opens a way for the understanding of a key aspect of the photovoltaic operation of high efficiency perovskite solar cells.
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              First-Principles Study of Ion Diffusion in Perovskite Solar Cell Sensitizers.

              Jun Haruyama, Keitaro Sodeyama, Liyuan Han … (2015)
              Hysteresis in current-voltage curves has been an important issue for conversion efficiency evaluation and development of perovskite solar cells (PSCs). In this study, we explored the ion diffusion effects in tetragonal CH3NH3PbI3 (MAPbI3) and trigonal (NH2)2CHPbI3 (FAPbI3) by first-principles calculations. The calculated activation energies of the anionic and cationic vacancy migrations clearly show that I(-) anions in both MAPbI3 and FAPbI3 can easily diffuse with low barriers of ca. 0.45 eV, comparable to that observed in ion-conducting materials. More interestingly, typical MA(+) cations and larger FA(+) cations both have rather low barriers as well, indicating that the cation molecules can migrate in the perovskite sensitizers when a bias voltage is applied. These results can explain the ion displacement scenario recently proposed by experiments. With the dilute diffusion theory, we discuss that smaller vacancy concentrations (higher crystallinity) and replacement of MA(+) with larger cation molecules will be essential for suppressing hysteresis as well as preventing aging behavior of PSC photosensitizers.
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                Author and article information

                Contributors
                Dr. Igor Moudrakovski: i.moudrakovski@fkf.mpg.de
                Prof. Joachim Maier: s.weiglein@fkf.mpg.de
                Journal
                Journal ID (nlm-ta): Angew Chem Int Ed Engl
                Journal ID (iso-abbrev): Angew. Chem. Int. Ed. Engl
                Journal ID (doi): 10.1002/(ISSN)1521-3773
                Journal ID (publisher-id): ANIE
                Title: Angewandte Chemie (International Ed. in English)
                Publisher: John Wiley and Sons Inc. (Hoboken )
                ISSN (Print): 1433-7851
                ISSN (Electronic): 1521-3773
                Publication date (Electronic): 30 May 2017
                Publication date (Print): 26 June 2017
                Volume: 56
                Issue: 27 ( doiID: 10.1002/anie.v56.27 )
                Pages: 7755-7759
                Affiliations
                [ 1 ] Department of Physical Chemistry of Solids Max Planck Institute for Solid State Research Heisenbergstr. 1 70569 Stuttgart Germany
                [ 2 ] Department of Chemistry and Chemical Engineering Swiss Federal Institute of Technology Station 6 1015 Lausanne Switzerland
                Author information
                http://orcid.org/0000-0002-0952-0948
                Article
                Publisher ID: ANIE201701724
                DOI: 10.1002/anie.201701724
                PMC ID: 5502889
                PubMed ID: 28558144
                SO-VID: 2fa0f8d8-3bec-4240-9f46-23e80ff65ec7
                Copyright © © 2017 The Authors. Published by Wiley-VCH Verlag GmbH & Co. KGaA.
                License:

                This is an open access article under the terms of the Creative Commons Attribution‐NonCommercial‐NoDerivs License, which permits use and distribution in any medium, provided the original work is properly cited, the use is non‐commercial and no modifications or adaptations are made.

                History
                Date received : 16 February 2017
                Date revision received : 07 April 2017
                Page count
                Figures: 5, Tables: 0, References: 53, Pages: 5, Words: 0
                Funding
                Funded by: Max-Planck-Gesellschaft
                Categories
                Subject: Communication
                Subject: Communications
                Subject: Electrochemistry
                Custom metadata
                source-schema-version-number 2.0
                component-id anie201701724
                cover-date June 26, 2017
                details-of-publishers-convertor Converter:WILEY_ML3GV2_TO_NLMPMC version:5.1.2 mode:remove_FC converted:06.07.2017

                ScienceOpen disciplines: Chemistry
                Keywords: charge carriers,halide perovskite,ion migration,methylammonium lead iodide,perovskite solar cells
                Data availability:
                ScienceOpen disciplines: Chemistry
                Keywords: charge carriers, halide perovskite, ion migration, methylammonium lead iodide, perovskite solar cells

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