3D lead-organoselenide-halide perovskites and their mixed-chalcogenide and mixed-halide alloys
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 organos...
| Main Authors: | , , , , , , , , , |
|---|---|
| Format: | Journal article |
| Jezik: | English |
| Izdano: |
Wiley
2024
|
| _version_ | 1826314713847300096 |
|---|---|
| author | Karunadasa, H Li, J Wang, Y Saha, S Chen, Z Hofmann, J Misleh, J Chapman, KW Filip, MR Reimer, JA |
| author_facet | Karunadasa, H Li, J Wang, Y Saha, S Chen, Z Hofmann, J Misleh, J Chapman, KW Filip, MR Reimer, JA |
| author_sort | Karunadasa, H |
| collection | OXFORD |
| description | 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 bandgap decrease. Optical absorbance measurements indeed show bandgaps 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 bandgap 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 bandgap and potential trap states, respectively, establishes the foundation for understanding this new perovskite family, which combines solid-state and organo-main-group chemistry. |
| first_indexed | 2024-12-09T03:11:49Z |
| format | Journal article |
| id | oxford-uuid:7279a36d-c151-4c71-b2dd-d17e91192b7e |
| institution | University of Oxford |
| language | English |
| last_indexed | 2024-12-09T03:11:49Z |
| publishDate | 2024 |
| publisher | Wiley |
| record_format | dspace |
| spelling | oxford-uuid:7279a36d-c151-4c71-b2dd-d17e91192b7e2024-10-08T15:54:52Z3D lead-organoselenide-halide perovskites and their mixed-chalcogenide and mixed-halide alloysJournal articlehttp://purl.org/coar/resource_type/c_dcae04bcuuid:7279a36d-c151-4c71-b2dd-d17e91192b7eEnglishSymplectic ElementsWiley2024Karunadasa, HLi, JWang, YSaha, SChen, ZHofmann, JMisleh, JChapman, KWFilip, MRReimer, JAWe 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 bandgap decrease. Optical absorbance measurements indeed show bandgaps 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 bandgap 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 bandgap and potential trap states, respectively, establishes the foundation for understanding this new perovskite family, which combines solid-state and organo-main-group chemistry. |
| spellingShingle | Karunadasa, H Li, J Wang, Y Saha, S Chen, Z Hofmann, J Misleh, J Chapman, KW Filip, MR Reimer, JA 3D lead-organoselenide-halide perovskites and their mixed-chalcogenide and mixed-halide alloys |
| title | 3D lead-organoselenide-halide perovskites and their mixed-chalcogenide and mixed-halide alloys |
| title_full | 3D lead-organoselenide-halide perovskites and their mixed-chalcogenide and mixed-halide alloys |
| title_fullStr | 3D lead-organoselenide-halide perovskites and their mixed-chalcogenide and mixed-halide alloys |
| title_full_unstemmed | 3D lead-organoselenide-halide perovskites and their mixed-chalcogenide and mixed-halide alloys |
| title_short | 3D lead-organoselenide-halide perovskites and their mixed-chalcogenide and mixed-halide alloys |
| title_sort | 3d lead organoselenide halide perovskites and their mixed chalcogenide and mixed halide alloys |
| work_keys_str_mv | AT karunadasah 3dleadorganoselenidehalideperovskitesandtheirmixedchalcogenideandmixedhalidealloys AT lij 3dleadorganoselenidehalideperovskitesandtheirmixedchalcogenideandmixedhalidealloys AT wangy 3dleadorganoselenidehalideperovskitesandtheirmixedchalcogenideandmixedhalidealloys AT sahas 3dleadorganoselenidehalideperovskitesandtheirmixedchalcogenideandmixedhalidealloys AT chenz 3dleadorganoselenidehalideperovskitesandtheirmixedchalcogenideandmixedhalidealloys AT hofmannj 3dleadorganoselenidehalideperovskitesandtheirmixedchalcogenideandmixedhalidealloys AT mislehj 3dleadorganoselenidehalideperovskitesandtheirmixedchalcogenideandmixedhalidealloys AT chapmankw 3dleadorganoselenidehalideperovskitesandtheirmixedchalcogenideandmixedhalidealloys AT filipmr 3dleadorganoselenidehalideperovskitesandtheirmixedchalcogenideandmixedhalidealloys AT reimerja 3dleadorganoselenidehalideperovskitesandtheirmixedchalcogenideandmixedhalidealloys |