Remarkably low trap-state density and long carrier diffusion in organolead trihalide perovskite single crystals

Alexander Rothenberger^a, Omar F. Mohammed^a, Yin Chen^a, Erkki Alarousu^a, Dong Shi^a, Osman M. Bakr^a, Valerio Adinolfi^b, Riccardo Comin^b, Mingjian Yuan^b, Andrei Buin^b, Edward H. Sargent^b

^aSolar and Photovoltaic Engineering Research Center (SPERC), King Abdullah University of Science and Technology (KAUST), Thuwal, 23955

^bDepartment of Electrical and Computer Engineering, University of Toronto, 10 King’s College Road, Toronto, Ontario, M5S 3G4

International Conference on Hybrid and Organic Photovoltaics
Proceedings of International Conference on Hybrid and Organic Photovoltaics 2015 (HOPV15)

Roma, Italy, 2015 May 11th - 13th

Organizer: Filippo De Angelis

Oral, Osman M. Bakr, presentation 301
Publication date: 5th February 2015

Along with the rapid progress in power conversion efficiency of perovskite solar cells, the key materials-based aspects behind the photovoltaic superiority of organolead trihalide perovskites are being vigorously pursued. However, the fundamental properties, and ultimate performance limits, of organolead trihalide MAPbX₃ (MA = CH₃NH₃⁺; X = Br^–, or I^–) perovskites remain obscured by extensive disorder in polycrystalline MAPbX₃ films. We report an antisolvent vapor-assisted crystallization (AVC) approach that enables us to create sizable crack-free MAPbX₃ single crystals with volumes exceeding 100 cubic millimeters. These large single crystals enabled a detailed characterization of their optical and charge transport characteristics. We observed exceptionally low trap-state densities of order 10⁹ to 10¹⁰ per cubic centimeter MAPbX₃ single crystals (comparable to the best photovoltaic-quality silicon), which is ~ 7-order-of-magnetitude lower than nanocrystalline perovskite thin films. The low trap-state density leads to both superior photophysical and transport charachteristics of the MAPbX₃ single crystals over nanocrystalline thin films. Exceptionally long photoluminescence (PL) lifetime, up to a microsecond time scale, and high charge-carrier mobility, up to a hundred cm²/Vs. was obtained in MAPbX₃ single crystals. Charge-carrier diffusion lengths exceeding 10 μm in MAPbX₃ single crystals were calculated based on the measured PL lifetime and charge-carrier mobility. By revealing the intrinsic properties of hybrid halide perovskites – here shown to be comparable to the best optoelectronic grade semiconductors – and conditions for their high-quality growth, this study demonstrates that perovskite photovoltaics stand to see further breakthroughs through substantial improvement in material purity. The emergence of these intrinsically high-quality materials suggests new avenues to deploy hybrid perovskites in an even wider range of semiconductor and optoelectronic devices.

Shi, D.; Adinolfi, V.; Comin, R.; Yuan, M.; Alarousu, E.; Buin, A.; Chen, Y.; Hoogland, S.; Rothenberger, A.; Katsiev, K.; Losovyj, Y.; Zhang, X.; Dowben, P.A.; Mohamed, O.F.; Sargent, E.H.; Bakr, O.M. Low Trap-State Density and Long Carrier Diffusion in Organolead Trihalide Perovskite Single Crystals. Science 2015, 347, 519-522.

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