Molecular engineering of pure 2D lead‐iodide perovskite solar absorbers displaying reduced band gaps and dielectric confinement
Pure 2D lead‐iodide perovskites typically demonstrate poor charge transport and compromised visible light absorption, relative to their 3D congeners. This hinders their potential use as solar absorbers. Herein, the systematic tuning of pyridinium‐based templating cations is reported to introduce int...
| Main Authors: | , , , , , , , , |
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| Format: | Journal Article |
| Language: | English |
| Published: |
2020
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| Online Access: | https://hdl.handle.net/10356/142103 |
| _version_ | 1826125236195557376 |
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| author | Febriansyah, Benny Lekina, Yulia Ghosh, Biplab Harikesh, Padinhare Cholakkal Koh, Teck Ming Li, Yongxin Shen, Zexiang Mathews, Nripan England, Jason |
| author2 | School of Materials Science and Engineering |
| author_facet | School of Materials Science and Engineering Febriansyah, Benny Lekina, Yulia Ghosh, Biplab Harikesh, Padinhare Cholakkal Koh, Teck Ming Li, Yongxin Shen, Zexiang Mathews, Nripan England, Jason |
| author_sort | Febriansyah, Benny |
| collection | NTU |
| description | Pure 2D lead‐iodide perovskites typically demonstrate poor charge transport and compromised visible light absorption, relative to their 3D congeners. This hinders their potential use as solar absorbers. Herein, the systematic tuning of pyridinium‐based templating cations is reported to introduce intermolecular interactions that provide access to a series of new 2D lead‐iodide perovskites with reduced inter‐octahedral distortions (largest Pb‐(μ‐I)‐Pb bond angles of 170–179°) and very short inorganic interlayer separations (shortest I⋅⋅⋅I contacts ≤4.278–4.447 Å). These features manifest in reduced band gaps (2.35–2.46 eV) and relaxed dielectric confinement (excitonic binding energies of 130–200 meV). As a consequence, they demonstrate (more than ten‐fold) improved photo‐ and electrical conductivities relative to conventional 2D lead‐iodide perovskites, such as that templated by 2‐(1‐naphthyl)ethylammonium. Through computational studies, the origin of this behavior was shown to derive from a combination of short iodoplumbate layer separations and the aromaticity of the organic dications. |
| first_indexed | 2024-10-01T06:33:25Z |
| format | Journal Article |
| id | ntu-10356/142103 |
| institution | Nanyang Technological University |
| language | English |
| last_indexed | 2024-10-01T06:33:25Z |
| publishDate | 2020 |
| record_format | dspace |
| spelling | ntu-10356/1421032021-01-08T01:28:11Z Molecular engineering of pure 2D lead‐iodide perovskite solar absorbers displaying reduced band gaps and dielectric confinement Febriansyah, Benny Lekina, Yulia Ghosh, Biplab Harikesh, Padinhare Cholakkal Koh, Teck Ming Li, Yongxin Shen, Zexiang Mathews, Nripan England, Jason School of Materials Science and Engineering School of Physical and Mathematical Sciences Interdisciplinary Graduate School (IGS) Energy Research Institute @ NTU (ERI@N) Research Techno Plaza Science::Chemistry::Inorganic chemistry Science::Physics 2D Perovskites Crystal Engineering Pure 2D lead‐iodide perovskites typically demonstrate poor charge transport and compromised visible light absorption, relative to their 3D congeners. This hinders their potential use as solar absorbers. Herein, the systematic tuning of pyridinium‐based templating cations is reported to introduce intermolecular interactions that provide access to a series of new 2D lead‐iodide perovskites with reduced inter‐octahedral distortions (largest Pb‐(μ‐I)‐Pb bond angles of 170–179°) and very short inorganic interlayer separations (shortest I⋅⋅⋅I contacts ≤4.278–4.447 Å). These features manifest in reduced band gaps (2.35–2.46 eV) and relaxed dielectric confinement (excitonic binding energies of 130–200 meV). As a consequence, they demonstrate (more than ten‐fold) improved photo‐ and electrical conductivities relative to conventional 2D lead‐iodide perovskites, such as that templated by 2‐(1‐naphthyl)ethylammonium. Through computational studies, the origin of this behavior was shown to derive from a combination of short iodoplumbate layer separations and the aromaticity of the organic dications. NRF (Natl Research Foundation, S’pore) Accepted version 2020-06-16T01:56:51Z 2020-06-16T01:56:51Z 2020 Journal Article Febriansyah, B., Lekina, Y., Ghosh, B., Harikesh, P. C., Koh, T. M., Li, Y., . . . England, J. (2020). Molecular engineering of pure 2D lead‐iodide perovskite solar absorbers displaying reduced band gaps and dielectric confinement. ChemSusChem, 13(10), 2693-2701. doi:10.1002/cssc.202000028 1864-5631 https://hdl.handle.net/10356/142103 10.1002/cssc.202000028 10 13 2693 2701 en ChemSusChem This is the accepted version of the following article: Febriansyah, B., Lekina, Y., Ghosh, B., Harikesh, P. C., Koh, T. M., Li, Y., . . . England, J. (2020). Molecular engineering of pure 2D lead‐iodide perovskite solar absorbers displaying reduced band gaps and dielectric confinement. ChemSusChem, 13(10), 2693-2701. doi:10.1002/cssc.202000028, which has been published in final form at https://doi.org/10.1002/cssc.202000028. This article may be used for non-commercial purposes in accordance with the Wiley Self-Archiving Policy [https://authorservices.wiley.com/authorresources/Journal-Authors/licensing/self-archiving.html]. application/pdf |
| spellingShingle | Science::Chemistry::Inorganic chemistry Science::Physics 2D Perovskites Crystal Engineering Febriansyah, Benny Lekina, Yulia Ghosh, Biplab Harikesh, Padinhare Cholakkal Koh, Teck Ming Li, Yongxin Shen, Zexiang Mathews, Nripan England, Jason Molecular engineering of pure 2D lead‐iodide perovskite solar absorbers displaying reduced band gaps and dielectric confinement |
| title | Molecular engineering of pure 2D lead‐iodide perovskite solar absorbers displaying reduced band gaps and dielectric confinement |
| title_full | Molecular engineering of pure 2D lead‐iodide perovskite solar absorbers displaying reduced band gaps and dielectric confinement |
| title_fullStr | Molecular engineering of pure 2D lead‐iodide perovskite solar absorbers displaying reduced band gaps and dielectric confinement |
| title_full_unstemmed | Molecular engineering of pure 2D lead‐iodide perovskite solar absorbers displaying reduced band gaps and dielectric confinement |
| title_short | Molecular engineering of pure 2D lead‐iodide perovskite solar absorbers displaying reduced band gaps and dielectric confinement |
| title_sort | molecular engineering of pure 2d lead iodide perovskite solar absorbers displaying reduced band gaps and dielectric confinement |
| topic | Science::Chemistry::Inorganic chemistry Science::Physics 2D Perovskites Crystal Engineering |
| url | https://hdl.handle.net/10356/142103 |
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