For the global commercialization of highly efficient and stable perovskite solar cells(PSCs),it is necessary to effectively suppress the formation of various defects acting as nonradiative recombination sources in per...For the global commercialization of highly efficient and stable perovskite solar cells(PSCs),it is necessary to effectively suppress the formation of various defects acting as nonradiative recombination sources in perovskite light-harvesting materials.Interfacial defects between the charge-selective layer and the perovskite are easily formed in the solution process used to fabricate perovskite films.In addition,owing to the difference in thermal expansion coefficients between the substrate and the perovskite film,internal residual tensile stress inevitably occurs,resulting in increased nonradiative recombination.Herein,a simple compositional engineering scheme for realizing efficient and stable PSCs,which incorporates acetamidinium bromide(AABr)as an additive into the MAPbI_(3) lattice,is proposed.As an additive,AABr has been found to provide synergistic multiple passivation for both internal and interfacial defects.AABr was found to effectively release the tensile strain of the MAPbI_(3) film by forming a structure stabilized by NH-I hydrogen bonds,as evidenced by calculations based on density functional theory(DFT).Furthermore,the incorporated AABr additives created a charge carrier recombination barrier to enhance charge collection capability by reducing interfacial defects.Accordingly,a power conversion efficiency(PCE)of 20.18%was achieved using a planar device employing AABr-incorporated MAPbI_(3).This was substantially higher than the 18.32% PCE of a pristine MAPbI_(3)-based device.Notably,unencapsulated PSCs using AABr-incorporated MAPbI_(3) absorbers exhibited excellent long-term stability,maintaining>95% of initial PCE up to 1200 hours in ambient air.展开更多
We have studied the redox potentials and electronic properties of C60 and C59N using density functional theory method. It is found that doping C60 with one nitrogen atom results in a slight increase in redox potential...We have studied the redox potentials and electronic properties of C60 and C59N using density functional theory method. It is found that doping C60 with one nitrogen atom results in a slight increase in redox potential. Next, we have also studied C59N functionalized with various redox-active oxygen containing functional groups and strongly electron withdrawing functional groups. It is found that the intrinsic electronic structure of the molecule is the major determinant of the redox potential. Our DFT calculations show that the electron affinity to redox potential of functionalized C59N is correlated with the LUMO of the systems very well. This is the first systematic study on the redox properties and electronic structures of N-doped C60 systems.展开更多
基金supported by the Basic Science Research Program through the National Research Foundation of Korea(NRF)funded by the Ministry of Science and ICT(2020R1F1A1068664)。
文摘For the global commercialization of highly efficient and stable perovskite solar cells(PSCs),it is necessary to effectively suppress the formation of various defects acting as nonradiative recombination sources in perovskite light-harvesting materials.Interfacial defects between the charge-selective layer and the perovskite are easily formed in the solution process used to fabricate perovskite films.In addition,owing to the difference in thermal expansion coefficients between the substrate and the perovskite film,internal residual tensile stress inevitably occurs,resulting in increased nonradiative recombination.Herein,a simple compositional engineering scheme for realizing efficient and stable PSCs,which incorporates acetamidinium bromide(AABr)as an additive into the MAPbI_(3) lattice,is proposed.As an additive,AABr has been found to provide synergistic multiple passivation for both internal and interfacial defects.AABr was found to effectively release the tensile strain of the MAPbI_(3) film by forming a structure stabilized by NH-I hydrogen bonds,as evidenced by calculations based on density functional theory(DFT).Furthermore,the incorporated AABr additives created a charge carrier recombination barrier to enhance charge collection capability by reducing interfacial defects.Accordingly,a power conversion efficiency(PCE)of 20.18%was achieved using a planar device employing AABr-incorporated MAPbI_(3).This was substantially higher than the 18.32% PCE of a pristine MAPbI_(3)-based device.Notably,unencapsulated PSCs using AABr-incorporated MAPbI_(3) absorbers exhibited excellent long-term stability,maintaining>95% of initial PCE up to 1200 hours in ambient air.
文摘We have studied the redox potentials and electronic properties of C60 and C59N using density functional theory method. It is found that doping C60 with one nitrogen atom results in a slight increase in redox potential. Next, we have also studied C59N functionalized with various redox-active oxygen containing functional groups and strongly electron withdrawing functional groups. It is found that the intrinsic electronic structure of the molecule is the major determinant of the redox potential. Our DFT calculations show that the electron affinity to redox potential of functionalized C59N is correlated with the LUMO of the systems very well. This is the first systematic study on the redox properties and electronic structures of N-doped C60 systems.
