Efficient Photoluminescence and Optically-pumped Lasing in Mixed-Halide Organolead Perovskite Semiconductors
Sandeep Pathak a, Michael Price a, Felix Deschler a, Richard Friend a, Ruben Higler a
a University of Cambridge - UK, The Old Schools, Trinity Ln, Cambridge CB2 1TN, UK, Cambridge, United Kingdom
International Conference on Hybrid and Organic Photovoltaics
Proceedings of 6th International Conference on Hybrid and Organic Photovoltaics (HOPV14)
Ecublens, Switzerland, 2014 May 11th - 14th
Organizers: Michael Graetzel and Mohammad Nazeeruddin
Oral, Felix Deschler, presentation 051
Publication date: 1st March 2014

Organometallic mixed halide perovskite-based solar cells have shown a breakthrough in power conversion efficiency. Solution-processed devices with power conversion efficiencies of 10-12%1-3were reported in 2012, and have more recently exceeded 15% in devices processed by evaporation4and sequential deposition5. The fundamental questions are whether the photoexcitations in the perovskite remain as bound excitons and are later ionised at the electron and/or hole accepting interface or whether charge generation occurs in the pristine perovskite material.

We report the transient photoluminescence and absorption of devices and spin-coated perovskite films in the range from 30 fs to several µs. We find that charge generation in the pristine CH3NH3PbI3-xClx perovskite results from exciton ionisation within 1ps, and that these free charge carriers undergo bimolecular recombination on timescales of 10s to 100s of nsecs, to give photoluminescence with a quantum efficiency as high as 70%.  To exemplify the high luminescence yield of the CH3NH3PbI3-xClx perovskite, we construct and demonstrate the operation of an optically-pumped vertical cavity laser comprising a layer of perovskite between a dielectric mirror and an evaporated gold top mirror. We note that these long carrier lifetimes together with exceptionally high luminescence yield are unprecedented in such simply prepared inorganic semiconductors and that these properties are ideally suited for photovoltaic diode operation6.



1 Ball, J. M., Lee, M. M., Hey, A. & Snaith, H. J. Low-temperature processed meso-superstructured to thin-film perovskite solar cells. Energy & Environmental Science, doi:10.1039/c3ee40810h (2013). 2 Kim, H.-S. et al. Lead Iodide Perovskite Sensitized All-Solid-State Submicron Thin Film Mesoscopic Solar Cell with Efficiency Exceeding 9%. Scientific Reports 2, doi:10.1038/srep00591 (2012). 3 Lee, M. M., Teuscher, J., Miyasaka, T., Murakami, T. N. & Snaith, H. J. Efficient Hybrid Solar Cells Based on Meso-Superstructured Organometal Halide Perovskites. Science 338, 643-647, doi:10.1126/science.1228604 (2012). 4 Liu, M., Johnston, M. B. & Snaith, H. J. Efficient planar heterojunction perovskite solar cells by vapour deposition. Nature 501, 395-398, doi:10.1038/nature12509 (2013). 5 Burschka, J. et al. Sequential deposition as a route to high-performance perovskite-sensitized solar cells. Nature 499, 316-319, doi:10.1038/nature12340 (2013). 6 Miller, O. D., Yablonovitch, E. & Kurtz, S. R. Strong Internal and External Luminescence as Solar Cells Approach the Shockley-Queisser Limit. Photovoltaics, IEEE Journal of 2, 303-311, doi:10.1109/JPHOTOV.2012.2198434 (2012).
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