3D Lead-Organoselenide-Halide Perovskites and their Mixed-Chalcogenide and Mixed-Halide Alloys
Jiayi Li
Department of Chemistry, Stanford University, Stanford, California, 94305 United States
Search for more papers by this authorDr. Yang Wang
Department of Chemical and Biomolecular Engineering, College of Chemistry, UC Berkeley, Berkeley, California, 94720 United States
Search for more papers by this authorDr. Santanu Saha
Department of Physics, University of Oxford, Clarendon Laboratory, Parks Road, Oxford, OX1 3PU United Kingdom
Institut de Recherche sur les Ceramiques (IRCER), UMR CNRS 7315, Université de Limoges, 12 Rue Atlantis, Limoges, 87068 France
Search for more papers by this authorDr. Zhihengyu Chen
Department of Chemistry, Stony Brook University, Stony Brook, New York, 11794 United States
Search for more papers by this authorJan Hofmann
Department of Chemistry, Stony Brook University, Stony Brook, New York, 11794 United States
Search for more papers by this authorJason Misleh
Department of Chemistry, Stanford University, Stanford, California, 94305 United States
Search for more papers by this authorProf. Karena W. Chapman
Department of Chemistry, Stony Brook University, Stony Brook, New York, 11794 United States
Search for more papers by this authorProf. Jeffrey A. Reimer
Department of Chemical and Biomolecular Engineering, College of Chemistry, UC Berkeley, Berkeley, California, 94720 United States
Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California, 94720 United States
Search for more papers by this authorCorresponding Author
Prof. Marina R. Filip
Department of Physics, University of Oxford, Clarendon Laboratory, Parks Road, Oxford, OX1 3PU United Kingdom
Search for more papers by this authorCorresponding Author
Prof. Hemamala I. Karunadasa
Department of Chemistry, Stanford University, Stanford, California, 94305 United States
Stanford Institute for Materials and Energy Sciences (SIMES), SLAC National Accelerator Laboratory, Menlo Park, California, 94025 United States
Search for more papers by this authorJiayi Li
Department of Chemistry, Stanford University, Stanford, California, 94305 United States
Search for more papers by this authorDr. Yang Wang
Department of Chemical and Biomolecular Engineering, College of Chemistry, UC Berkeley, Berkeley, California, 94720 United States
Search for more papers by this authorDr. Santanu Saha
Department of Physics, University of Oxford, Clarendon Laboratory, Parks Road, Oxford, OX1 3PU United Kingdom
Institut de Recherche sur les Ceramiques (IRCER), UMR CNRS 7315, Université de Limoges, 12 Rue Atlantis, Limoges, 87068 France
Search for more papers by this authorDr. Zhihengyu Chen
Department of Chemistry, Stony Brook University, Stony Brook, New York, 11794 United States
Search for more papers by this authorJan Hofmann
Department of Chemistry, Stony Brook University, Stony Brook, New York, 11794 United States
Search for more papers by this authorJason Misleh
Department of Chemistry, Stanford University, Stanford, California, 94305 United States
Search for more papers by this authorProf. Karena W. Chapman
Department of Chemistry, Stony Brook University, Stony Brook, New York, 11794 United States
Search for more papers by this authorProf. Jeffrey A. Reimer
Department of Chemical and Biomolecular Engineering, College of Chemistry, UC Berkeley, Berkeley, California, 94720 United States
Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California, 94720 United States
Search for more papers by this authorCorresponding Author
Prof. Marina R. Filip
Department of Physics, University of Oxford, Clarendon Laboratory, Parks Road, Oxford, OX1 3PU United Kingdom
Search for more papers by this authorCorresponding Author
Prof. Hemamala I. Karunadasa
Department of Chemistry, Stanford University, Stanford, California, 94305 United States
Stanford Institute for Materials and Energy Sciences (SIMES), SLAC National Accelerator Laboratory, Menlo Park, California, 94025 United States
Search for more papers by this authorAbstract
We incorporate Se into the 3D halide perovskite framework using the zwitterionic ligand: SeCYS (+NH3(CH2)2Se−), which occupies both the X− and A+ sites in the prototypical ABX3 perovskite. The new organoselenide-halide perovskites: (SeCYS)PbX2 (X=Cl, Br) expand upon the recently discovered organosulfide-halide perovskites. Single-crystal X-ray diffraction and pair distribution function analysis reveal the average structures of the organoselenide-halide perovskites, whereas the local lead coordination environments and their distributions were probed through solid-state 77Se and 207Pb NMR, complemented by theoretical simulations. Density functional theory calculations illustrate that the band structures of (SeCYS)PbX2 largely resemble those of their S analogs, with similar band dispersion patterns, yet with a considerable band gap decrease. Optical absorbance measurements indeed show band gaps of 2.07 and 1.86 eV for (SeCYS)PbX2 with X=Cl and Br, respectively. We further demonstrate routes to alloying the halides (Cl, Br) and chalcogenides (S, Se) continuously tuning the band gap from 1.86 to 2.31 eV–straddling the ideal range for tandem solar cells or visible-light photocatalysis. The comprehensive description of the average and local structures, and how they can fine-tune the band gap and potential trap states, respectively, establishes the foundation for understanding this new perovskite family, which combines solid-state and organo-main-group chemistry.
Conflict of Interests
The authors declare no conflict of interest.
Open Research
Data Availability Statement
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