Temperature behaviour of mixed-cation mixed-halide perovskite solar cells. Analysis of recombination mechanisms and ion migration
Résumé
In our study, we show that compositional engineering of the “A” site cation of ABX3 perovskite structure formed by a mix of organic and inorganic cations is an effective route to improve the thermal stability of perovskite solar cells (PSCs). In this work, mixed-cation mixed-halide PSCs have been fabricated and characterized with temperature, from 253 up to 333 K. The active layer based on CsRbFAMAPb(IBr)3 results in a more stable device compared to standard MAPbI3 devices. Electrical characterization reveals a decrease of the solar cell parameters with temperature. Using Impedance Spectroscopy (IS) characterization, we have estimated an activation energy for the halide ion migration of 0.63 ± 0.08 eV, an ion diffusion coefficient of 10− 14 cm2 s − 1 , and a defect density of 7.27⋅1015 cm− 3 . To our knowledge, this is the first time that these parameters have been calculated in CsRbFAMAPb(IBr)3 based devices, resulting in improved values compared to MAPbI3 devices. The worsening of device performance for temperatures above 300 K is attributed to a decrease of the spiro-OMeTAD conductivity and the degradation of the perovskite/spiro-OMeTAD interface. It is shown that for low temperatures (from 253 to 323 K), Shockley-Red-Hall (SRH) recombination in the bulk governs, while for temperatures above 323 K the increase in surface recombination becomes dominant due to the presence of non-selective contacts. Numerical simulations using SILVACO ATLAS corroborate the role of SRH in the perovskite active layer for low and medium temperatures, and the crucial influence of spiro-OMeTAD transport properties in the device performance parameters.
Description
This research was funded by Community of Madrid under the SINFOTON2-CM Research Program (S2018/NMT-4326-SINFOTON2-CM), and in the framework of the Multiannual Agreement with the Rey Juan Carlos University in line of action 1, “Encouragement of Young Phd students investigation” (Ref. M2180, “SolGenALEE”), and by Universidad Rey Juan Carlos with Research Projects M2607, M2180 and M2363. M.G.P. acknowledges the MCIN/AEI for the financial support provide for the project ALPHOMENA_PID2021-123190OB-I00 (LAser assembled Integrable PHOtonic MEtasurfaces & NAnostructures). M.C.L.-G. particularly expresses her gratitude to Lidia Contreras Bernal from ICMS (CSIC-Universidad de Sevilla) for their valuable help in perovskite solar cells fabrication.
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