Wei Peng1,2,3, Jun Yin1, Kang-Ting Ho4, Olivier Ouellette5, Michele De Bastiani1, Banavoth Murali1, Omar El Tall6, Chao Shen4, Xiaohe Miao7, Jun Pan1, Erkki Alarousu1, Jr-Hau He4, Boon S Ooi4, Omar F Mohammed1, Edward Sargent5, Osman M Bakr1,2,3. 1. Division of Physical Sciences and Engineering, King Abdullah University of Science and Technology (KAUST) , Thuwal 23955-6900, Saudi Arabia. 2. KAUST Solar Center, King Abdullah University of Science and Technology (KAUST) , Thuwal 23955-6900, Saudi Arabia. 3. KAUST Catalysis Center, King Abdullah University of Science and Technology (KAUST) , Thuwal 23955-6900, Saudi Arabia. 4. Division of Computer, Electrical and Mathematical Sciences and Engineering, King Abdullah University of Science and Technology (KAUST) , Thuwal 23955-6900, Saudi Arabia. 5. Department of Electrical and Computer Engineering, University of Toronto , 10 King's College Road, Toronto, Ontario M5S 3G4, Canada. 6. Analytical Core Lab, King Abdullah University of Science and Technology (KAUST) , Thuwal 23955-6900, Saudi Arabia. 7. Imaging and Characterization Core Lab, King Abdullah University of Science and Technology (KAUST) , Thuwal 23955-6900, Saudi Arabia.
Abstract
Unintentional self-doping in semiconductors through shallow defects is detrimental to optoelectronic device performance. It adversely affects junction properties and it introduces electronic noise. This is especially acute for solution-processed semiconductors, including hybrid perovskites, which are usually high in defects due to rapid crystallization. Here, we uncover extremely low self-doping concentrations in single crystals of the two-dimensional perovskites (C6H5C2H4NH3)2PbI4·(CH3NH3PbI3)n-1 (n = 1, 2, and 3), over three orders of magnitude lower than those of typical three-dimensional hybrid perovskites, by analyzing their conductivity behavior. We propose that crystallization of hybrid perovskites containing large organic cations suppresses defect formation and thus favors a low self-doping level. To exemplify the benefits of this effect, we demonstrate extraordinarily high light-detectivity (1013 Jones) in (C6H5C2H4NH3)2PbI4·(CH3NH3PbI3)n-1 photoconductors due to the reduced electronic noise, which makes them particularly attractive for the detection of weak light signals. Furthermore, the low self-doping concentration reduces the equilibrium charge carrier concentration in (C6H5C2H4NH3)2PbI4·(CH3NH3PbI3)n-1, advantageous in the design of p-i-n heterojunction solar cells by optimizing band alignment and promoting carrier depletion in the intrinsic perovskite layer, thereby enhancing charge extraction.
Unintentn>an class="Chemical">ional self-doping in semiconductors through shallow defects is detrimental to optoelectronic device performance. It adversely affects junction properties and it introduces electronic noise. This is especially acute for solution-processed semiconductors, including hybrid perovskites, which are usually high in defects due to rapid crystallization. Here, we uncover extremely low self-doping concentrations in single crystals of the two-dimensional perovskites (C6H5C2H4NH3)2PbI4·(CH3NH3PbI3)n-1 (n = 1, 2, and 3), over three orders of magnitude lower than those of typical three-dimensional hybrid perovskites, by analyzing their conductivity behavior. We propose that crystallization of hybrid perovskites containing large organic cations suppresses defect formation and thus favors a low self-doping level. To exemplify the benefits of this effect, we demonstrate extraordinarily high light-detectivity (1013 Jones) in (C6H5C2H4NH3)2PbI4·(CH3NH3PbI3)n-1 photoconductors due to the reduced electronic noise, which makes them particularly attractive for the detection of weak light signals. Furthermore, the low self-doping concentration reduces the equilibrium charge carrier concentration in (C6H5C2H4NH3)2PbI4·(CH3NH3PbI3)n-1, advantageous in the design of p-i-n heterojunction solar cells by optimizing band alignment and promoting carrier depletion in the intrinsic perovskite layer, thereby enhancing charge extraction.
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