Details
Original language | English |
---|---|
Article number | 2201126 |
Journal | Advanced functional materials |
Volume | 32 |
Issue number | 24 |
Early online date | 8 Mar 2022 |
Publication status | Published - 8 Jun 2022 |
Abstract
Once the optical, electronic, or photocatalytic properties of a semiconductor are set by adjusting composition, crystal phase, and morphology, one cannot change them anymore, respectively, on demand. Materials enabling postsynthetic and reversible switching of features such as absorption coefficient, bandgap, or charge carrier dynamics are highly desired. Hybrid perovskites facilitate exceptional possibilities for progress in the field of smart semiconductors because active organic molecules become an integral constituent of the crystalline structure. This paper reports the integration of ferrocene ligands into semiconducting 2D phases based on lead bromide. The complex crystal structures of the resulting, novel ferrovskite (≃ ferrocene perovskite) phases are determined by 3D electron diffraction. The ferrocene ligands exhibit strong structure-directing effects on the 2D hybrid phases, which is why the formation of exotic types of face- and edge-sharing lead bromide octahedra is observed. The bandgap of the materials ranges from 3.06 up to 3.51 eV, depending on the connectivity of the octahedra. By deploying the redox features of ferrocene, one can create defect states or even a defect band leading to control over the direction of exciton migration and energy transport in the semiconductor, enabling fluorescence via indirect to direct gap transition.
Keywords
- ferrocene materials, hybrid perovskites, MicroED, molecular switches, semiconductors
ASJC Scopus subject areas
- Chemistry(all)
- General Chemistry
- Materials Science(all)
- General Materials Science
- Physics and Astronomy(all)
- Condensed Matter Physics
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In: Advanced functional materials, Vol. 32, No. 24, 2201126, 08.06.2022.
Research output: Contribution to journal › Article › Research › peer review
}
TY - JOUR
T1 - Design of Active Defects in Semiconductors: 3D Electron Diffraction Revealed Novel Organometallic Lead Bromide Phases Containing Ferrocene as Redox Switches
AU - Fillafer, Nicole
AU - Kuper, Henning
AU - Schaate, Andreas
AU - Locmelis, Sonja
AU - Becker, Joerg August
AU - Krysiak, Yaşar
AU - Polarz, Sebastian
N1 - Funding Information: The authors thank the German Research Foundation for funding (project PO 780/22-1). The authors thank Ute Kolb for access to the transmission electron microscope FEI Tecnai F30 S-TWIN at the EM Center in Mainz (EZMZ) of the university Mainz. The authors are grateful to Lukáš Palatinus for access to the TEM FEI Tecnai 20 at the Institute of Physics of the Czech Academy of Sciences. The authors thank Stefan Schupp for organizing the PESA measurements and Stephen Klimke for the Mößbauer analysis. The authors thank the LNQE Research Center for the use of the XPS. Open access funding enabled and organized by Projekt DEAL. Funding Information: The authors thank the German Research Foundation for funding (project PO 780/22‐1). The authors thank Ute Kolb for access to the transmission electron microscope FEI Tecnai F30 S‐TWIN at the EM Center in Mainz (EZMZ) of the university Mainz. The authors are grateful to Lukáš Palatinus for access to the TEM FEI Tecnai 20 at the Institute of Physics of the Czech Academy of Sciences. The authors thank Stefan Schupp for organizing the PESA measurements and Stephen Klimke for the Mößbauer analysis. The authors thank the LNQE Research Center for the use of the XPS.
PY - 2022/6/8
Y1 - 2022/6/8
N2 - Once the optical, electronic, or photocatalytic properties of a semiconductor are set by adjusting composition, crystal phase, and morphology, one cannot change them anymore, respectively, on demand. Materials enabling postsynthetic and reversible switching of features such as absorption coefficient, bandgap, or charge carrier dynamics are highly desired. Hybrid perovskites facilitate exceptional possibilities for progress in the field of smart semiconductors because active organic molecules become an integral constituent of the crystalline structure. This paper reports the integration of ferrocene ligands into semiconducting 2D phases based on lead bromide. The complex crystal structures of the resulting, novel ferrovskite (≃ ferrocene perovskite) phases are determined by 3D electron diffraction. The ferrocene ligands exhibit strong structure-directing effects on the 2D hybrid phases, which is why the formation of exotic types of face- and edge-sharing lead bromide octahedra is observed. The bandgap of the materials ranges from 3.06 up to 3.51 eV, depending on the connectivity of the octahedra. By deploying the redox features of ferrocene, one can create defect states or even a defect band leading to control over the direction of exciton migration and energy transport in the semiconductor, enabling fluorescence via indirect to direct gap transition.
AB - Once the optical, electronic, or photocatalytic properties of a semiconductor are set by adjusting composition, crystal phase, and morphology, one cannot change them anymore, respectively, on demand. Materials enabling postsynthetic and reversible switching of features such as absorption coefficient, bandgap, or charge carrier dynamics are highly desired. Hybrid perovskites facilitate exceptional possibilities for progress in the field of smart semiconductors because active organic molecules become an integral constituent of the crystalline structure. This paper reports the integration of ferrocene ligands into semiconducting 2D phases based on lead bromide. The complex crystal structures of the resulting, novel ferrovskite (≃ ferrocene perovskite) phases are determined by 3D electron diffraction. The ferrocene ligands exhibit strong structure-directing effects on the 2D hybrid phases, which is why the formation of exotic types of face- and edge-sharing lead bromide octahedra is observed. The bandgap of the materials ranges from 3.06 up to 3.51 eV, depending on the connectivity of the octahedra. By deploying the redox features of ferrocene, one can create defect states or even a defect band leading to control over the direction of exciton migration and energy transport in the semiconductor, enabling fluorescence via indirect to direct gap transition.
KW - ferrocene materials
KW - hybrid perovskites
KW - MicroED
KW - molecular switches
KW - semiconductors
UR - http://www.scopus.com/inward/record.url?scp=85125960261&partnerID=8YFLogxK
U2 - 10.1002/adfm.202201126
DO - 10.1002/adfm.202201126
M3 - Article
AN - SCOPUS:85125960261
VL - 32
JO - Advanced functional materials
JF - Advanced functional materials
SN - 1616-301X
IS - 24
M1 - 2201126
ER -