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(X = I, Cl, Br) Methylammonium Lead Perovskite Solar Cells

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(X = I, Cl, Br) Methylammonium Lead Perovskite Solar Cells Journal of Materials Chemistry C View Article Online PAPER View Journal | View Issue Optical and electronic properties of mixed halide (X = I, Cl, Br) methylammonium lead perovskite Cite this: J. Mater. Chem. C, 2017, 5,1714 solar cells† Sekai Tombe,ab Getachew Adam,b Herwig Heilbrunner,b Dogukan Hazar Apaydin,b Christoph Ulbricht,b Niyazi Serdar Sariciftci,b Christopher J. Arendse,c Emmanuel Iwuohaa and Markus C. Scharber*b We report on the fabrication and opto-electronic characterization of solution-processed planar hetero- junction perovskite solar cells based on methylammonium (MA) lead halide derivatives, MAPbI3ÀxYx (Y = Cl, Br, I). Dissolving equimolar amounts of lead iodide (PbI2) and methylammonium iodide (H3CNH3I) together with various amounts of additional methylammonium halides, perovskite precursor solutions were obtained, which were used in the fabrication of three perovskite systems, MAPbI3,MAPbI3ÀxClx and MAPbI3ÀxBrx. The effect of the halide ratio in the perovskite formulations processed via a one-step deposition technique Creative Commons Attribution 3.0 Unported Licence. on optoelectronic properties and on photovoltaic performance of the formed perovskites was investigated. The perovskite film morphology, temperature-dependent photoluminescence properties, hysteresis behaviour in current–voltage characteristics and the photovoltaic performance as a function of chemical composition were studied using microscopic, spectroscopic and photovoltaic characterization techniques. The power con- version efficiency was found to be dependent on MAPbI3ÀxYx (Y=Cl,Br,I)perovskitefilmmorphology.By controlling perovskite precursor composition and stoichiometry, highest power conversion efficiencies of 9.2, 12.5 and 5.4% were obtained for MAPbI3,MAPbI3ÀxClx and MAPbI3ÀxBrx devices, respectively. In addition, the physical parameters of the mixed halide perovskites such as the exciton binding energy, exciton–phonon This article is licensed under a Received 6th November 2016, interaction and bandgap were determined via temperature-dependent photoluminescence spectroscopy. Accepted 23rd January 2017 Exciton binding and optical phonon energies of MAPbI3ÀxYx (Y = Cl, Br, I) were found to be in the ranges of DOI: 10.1039/c6tc04830g 49–68 meV and 29–32 meV respectively. The solution-processed MA lead halide derivatives form highly crystalline materials with chemical versatility allowing the tuning of their optical and electronic properties Open Access Article. Published on 24 January 2017. Downloaded 10/5/2021 3:22:54 PM. rsc.li/materials-c depending on the nature and the ratio of the halides employed. 1. Introduction as wind, sun, water, biomass and geothermal energy but solar photovoltaic (PV) energy stands out as the only technology with With the growing concerns about the finite supply of non- sufficient theoretical capacity to meet global electricity demands. renewable energy sources based on fossil fuels (e.g. oil, coal, There are worldwide efforts focusing on the development of natural gas, etc.), the geopolitical climate surrounding fossil PV technologies based on organic–inorganic material systems fuel production coupled with the environmental consequences which offer the prospect of significantly improved performance of greenhouse gas emissions underscores the urgency of search- and/or low cost manufacturing. Photovoltaic cells based on ing for alternative renewable and sustainable energy sources. organic–inorganic hybrid materials have shown rapid improve- Several technologies are available for the production of clean, ments over the past decade comparing favourably with existing efficient and reliable energy from renewable energy sources such inorganic semiconductor technologies in a number of key criteria such as scalability and manufacturing costs. Hybrid a SensorLab, Department of Chemistry, University of the Western Cape, organic–inorganic perovskite materials are currently among the Robert Sobukwe Road, Bellville, Cape Town 7535, South Africa most competitive candidates for semiconductor materials and b Linz Institute for Organic Solar Cells (LIOS), Institute of Physical Chemistry, have experienced the fastest increase in reported efficiencies Johannes Kepler University Linz, Altenbergerstrasse 69, 4040 Linz, Austria. ever obtained for any PV technology.1–12 E-mail: [email protected] c Department of Physics, University of the Western Cape, Private Bag X17, Bellville, The development of metal halide perovskite solar cells was 1 2 7535, South Africa triggered by the reports of Kojima et al., and Im et al. on † Electronic supplementary information (ESI) available. See DOI: 10.1039/c6tc04830g liquid electrolyte-based dye-sensitized solar cells. Perovskite 1714 | J. Mater. Chem. C, 2017, 5, 1714--1723 This journal is © The Royal Society of Chemistry 2017 View Article Online Paper Journal of Materials Chemistry C solar cell (PSC) devices have shown tremendous advancement solution-processed planar heterojunction perovskite solar cells in energy conversion efficiency starting from 3.8% in 20091 to by a systematic study of mixed halide compositions in methyl- reaching 22.1% to date.6 The certificated PCE of 22.1% is ammonium lead iodide based perovskite solar cells. higher than the certificated record PCE of polycrystalline In this work, three different perovskite systems, MAPbI3, 6 silicon solar cells indicating a competitive advantage. The MAPbI3ÀxClx and MAPbI3ÀxBrx, were prepared independently reason for the rapid increase in PCE of PSCs is that these by processing precursor formulations consisting of equimolar perovskite materials possess most of the properties required to amounts of lead iodide and methylammonium iodide as well as be excellent PV absorbers: sharp absorption edge as a function various amounts of additional methylammonium halides, MAI, of composition, superior light absorption coefficient (B105 cmÀ1), MACl and MABr. We found a correlation between photovoltaic long electron and hole diffusion lengths to suppress the recom- device performance and perovskite thin film morphology. Power bination of photoexcited charges, high carrier mobility and an conversion efficiencies of PV devices based on MAPbI3ÀxYx apparent tolerance for defects.7–12 (Y = Cl, Br, I) were observed to vary over a wide range indicating Pioneering work suggested that perovskite films exhibit that small changes in perovskite precursor formulation can have composition-/structure-dependent properties, which can be a significant effect on device performance. The lowest efficiencies accessed by various processing approaches.13 Noh et al.,7 were found for mixed-halide perovskite formulations containing showed that chemical modification of MAPbI3 by substituting bromide and the highest were found for formulations with iodide by bromide can tune the bandgaps in the range between chloride yielding highly crystalline perovskites. The physical 1.5 eV and 2.3 eV by incorporating MAPbBr3. By substituting parameters of the MAPbI3ÀxYx (Y = Cl, Br, I) perovskites such as iodine with chlorine or bromine, the emission of thin films can the exciton binding energy, exciton–phonon interaction and be varied from ultra-violet to near infrared.14 Controlling bandgap were elucidated via temperature-dependent photolumines- perovskite morphology and composition has been found to cence (PL) spectroscopy. The exciton binding energy (EB), which be critical for the development of high-performance perovskite indicates the efficiency of exciton dissociation and charge transfer, 15–17 Creative Commons Attribution 3.0 Unported Licence. solar cells. Many methods have been utilized for the deposi- was determined to 68.3 Æ 4.7, 49.7 Æ 6.2 and 58.3 Æ 4.0 meV for tion of perovskite films including the solution-processing, dual- MAPbI3, MAPbI3ÀxClx and MAPbI3ÀxBrx, respectively. source vapour deposition and vapour-assisted solution process (VASP). To date, the perovskite layer in these efficient solar cells has generally been fabricated by either vapour deposition or a two- 2. Experimental step sequential deposition process. Solution processed devices 2.1 Materials have the potential to reduce production costs substantially. Several successful perovskite device architectures have been Chemicals and solvents were used as received from commercial reported. Hybrid perovskites have demonstrated high power con- suppliers, if not stated otherwise. Pre-patterned indium doped À2 This article is licensed under a version efficiencies both in thin film planar device architectures18–22 tin oxide (ITO) coated glass (15 ohm cm ), PbI2 (99.9%, Sigma and meso-structured device architectures comprising mesoscopic Aldrich), dimethylformamide (DMF, anhydrous, Sigma Aldrich), alumina,23–25 zirconia26 or titania.27–29 It is yet unclear whether poly(3,4-ethylenedioxythiophene) polystyrene sulfonate (PEDOT:PSS) Clevios PH 1000 and Clevios PVP (Al 4083), ZonylsFS-300 fluoro- Open Access Article. Published on 24 January 2017. Downloaded 10/5/2021 3:22:54 PM. perovskite-absorber devices of different architecture types per- form equally well or if certain architectures will prove beneficial surfactant (40% in H2O, Fluka), dimethyl sulfoxide (DMSO, AnalR, over others.4,28 VWR Chemicals), [6,6]-phenyl-C61-butyric acid methyl ester (PCBM; Despite the remarkable progress in record efficiency, many SolenneBV), chlorobenzene (GPR, VWR Chemicals), chloroform fundamental aspects still need to be addressed at both the (AnalR, VWR Chemicals) and isopropanol (AnalR, Fisher material and device levels. The fundamental questions
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