%0 Journal Article %A Li, Xiangyang %A Li, Xingxing %A Yang, Jinlong %D 2020 %T Two-Dimensional Multifunctional Metal–Organic Frameworks with Simultaneous Ferro-/Ferrimagnetism and Vertical Ferroelectricity %U https://acs.figshare.com/articles/journal_contribution/Two-Dimensional_Multifunctional_Metal_Organic_Frameworks_with_Simultaneous_Ferro-_Ferrimagnetism_and_Vertical_Ferroelectricity/12283985 %R 10.1021/acs.jpclett.0c01033.s001 %2 https://ndownloader.figshare.com/files/22638605 %K PcFeO %K 2 D organometallic frameworks %K organometallic frameworks K 3 Fe 2 %K ferro %K PcMO 8 %K 2 D K 3 M 2 %K Vertical Ferroelectricity Exploring 2 D multifunctional materials %K ferroelectricity %K polarization %K 2 D K 3 Cr 2 %K K 3 M 2 %K Curie %K K 3 Fe 2 %X Exploring 2D multifunctional materials with intrinsic ferro-/ferrimagnetism and vertical ferroelectricity is a highly desirable but challenging task. Here, motivated by the recently synthesized organometallic frameworks K3Fe2[PcFeO8], we propose to realize such materials in a series of 2D K3M2[PcMO8] (M = Cr–Co) nanosheets. First-principles calculations suggest 2D K3Cr2[PcCrO8] as a ferromagnetic half metal with a Curie temperature of 140 K, whereas others (M = Mn, Fe, and Co) are all ferrimagnetic semiconductors with the Curie temperatures between 66 and 150 K. Moreover, the structural distortion due to the out-of-plane K+ counterions leads to a significant vertical electric polarization. The estimated intensity of polarization for K3Fe2[PcFeO8] is 143 pC/m, with the ferroelectric phase-transition barrier being 0.38 eV per formula. This work highlights the potential of 2D organometallic frameworks such as K3M2[PcMO8] as a versatile platform for designing multifunctional materials with simultaneous ferro-/ferrimagnetism and vertical ferroelectricity. %I ACS Publications