Proceedings of 6th International Conference on Hybrid and Organic Photovoltaics (HOPV14)
Publication date: 1st March 2014
Methylammonium lead-iodide, MAPbI3, and the mixed halide MAPbI3-xClx analogue are dominating the field of perovskite-based photovoltaics. Despite the low Cl-doping level (~1-2%) [1] in MAPbI3-xClx this material showed improved performances in TiO2-free devices compared to MAPbI3.[2, 3] Meso-superstructured and planar heterojunction solar cells were successfully implemented with MAPbI3-xClx, [2, 3] while the same devices based on the prototype MAPbI3 perovskite showed comparably lower performances.[4] This behavior can be interpreted on the basis of the improved carrier mobility of MAPbI3-xClx,[4] which showed electron-hole diffusion lengths exceeding 1 µm, against ~one order of magnitude smaller diffusion lengths independently measured for MAPbI3.[4, 5] Recent studies suggest that both materials show comparable carrier mobility but exhibit a markedly different recombination kinetics.[6]
The intimate materials properties underlying the photovoltaic performance of MAPbI3-xClx and in particular the role of Cl-doping are however not yet clear. Here we investigate the effect of Cl-doping on the MAPbI3 perovskite by state of the art DFT and GW electronic structure calculations. The calculated band structures reveal similar band-gaps and carrier effective masses for MAPbI3 and for low levels of Cl-doping. Ab initio molecular dynamics simulations performed on MAPbI3 and MAPbI3-xClx suggest different structural properties for the Cl-doped material. The implications of these findings for charge generation and recombination in solar cells are discussed.
Optimized geometries of two representative structures of the 4% chloride-doped MAPbI3-xClx. Three different geometry orientations are shown. The position of the chloride ions is highlighted by yellow circles; Pb=light blue; I = magenta.
[1] Colella, S.; Mosconi, E.; Fedeli, P.; Listorti, A.; Gazza, F.; Orlandi, F.; Ferro, P.; Besagni, T.; Rizzo, A.; Calestani, G.; Gigli, G.; De Angelis, F.; Mosca, R. Chem. Mater. 2013, 25, 4613–4618. [2] Liu, M.; Johnston, M. B.; Snaith, H. J. Nature 2013, 501, 395-398. [3] Lee, M. M.; Teuscher, J.; Miyasaka, T.; Murakami, T. N.; Snaith, H. J. Science 2012, 338, 643-647. [4] Stranks, S. D.; Eperon, G. E.; Grancini, G.; Menelaou, C.; Alcocer, M.J.P.; Leijtens, T.; Herz, L.M.; Petrozza, A.; Snaith, H.J. Science, 2013, 342, 341-344. [5] Xing, G.; Mathews, N.; Sun, S.; Lim, S.S.; Lam, Y.M.; Grätzel, M.; Mhaisalkar, S.; Sum, T.C. Science, 2013, 342, 344-347. [6] Wehrenfennig , C.; Eperon , G.E.; Johnston , M.B.; Snaith , H.J.; Herz, L.M. Adv. Mater. 2013, DOI: 10.1002/adma.201305172
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