[en] Hybrid organic-inorganic perovskites (HOIPs) have emerged as promising materials for optoelectronic applications, yet gaining control over their structural and electronic tunability remains a key challenge. In this study, we introduce 7H-dibenzo[c,g]carbazole (DBCz) as a novel electroactive organic cation that enables the formation of two distinct low-dimensional hybrid metal halides: a conventional 2D perovskite structure, (DBCz)2PbI4, and a previously unreported layered perovskite analogue structure with edge-sharing octahedra, DBCzPbI3. The edge-sharing phase represents a new structural motif within the hybrid metal halide family. Both materials exhibit a type-II band alignment, facilitating ultrafast photoinduced hole transfer from the inorganic to the organic layer. Using transient absorption spectroscopy, we identify the formation of DBCz-based hole polarons in both phases, and uniquely observe the charge-transfer-induced formation of triplet states and room-temperature coherent phonons for the perovskite analogue phase. These findings highlight the role of molecular design in controlling excited-state dynamics and exciton-lattice interactions in hybrid metal halides.
Disciplines :
Chemistry
Author, co-author :
Devroey, Ilan ; Hasselt University, Institute for Materials Research (imo-imomec), Hybrid Materials Design (HyMaD), Martelarenlaan 42, B-3500 Hasselt, Belgium. wouter.vangompel@uhasselt.be ; Energyville, imo-imomec, Thor Park 8320, B-3600, Genk, Belgium
Boeije, Yorrick ; University of Cambridge, Department of Chemical Engineering and Biotechnology, Philippa Fawcett Drive, Cambridge, CB3 0AS, UK. sds65@cam.ac.uk ; University of Cambridge, Department of Physics, Cavendish Laboratory, JJ Thomson Ave, Cambridge, CB3 0US, UK
Banks, Peter ; Université de Mons - UMONS > Faculté des Sciences > Service de Chimie des matériaux nouveaux
Quarti, Claudio ; Université de Mons - UMONS > Faculté des Sciences > Service de Chimie des matériaux nouveaux
La Magna, Paola ; Ghent University, Department of Chemistry, XStruct, Krijgslaan 281-S3, B-9000 Ghent, Belgium
Ciesielska, Aleksandra ; Hasselt University, Institute for Materials Research (imo-imomec), Hybrid Materials Design (HyMaD), Martelarenlaan 42, B-3500 Hasselt, Belgium. wouter.vangompel@uhasselt.be ; Energyville, imo-imomec, Thor Park 8320, B-3600, Genk, Belgium
Derveaux, Elien ; imec, imo-imomec, Wetenschapspark 1, B-3590, Diepenbeek, Belgium ; Hasselt University, Institute for Materials Research (imo-imomec), Applied and Analytical Chemistry, NMR group, Martelarenlaan 42, B-3500 Hasselt, Belgium
Adriaensens, Peter ; imec, imo-imomec, Wetenschapspark 1, B-3590, Diepenbeek, Belgium ; Hasselt University, Institute for Materials Research (imo-imomec), Applied and Analytical Chemistry, NMR group, Martelarenlaan 42, B-3500 Hasselt, Belgium
Van Hecke, Kristof ; Ghent University, Department of Chemistry, XStruct, Krijgslaan 281-S3, B-9000 Ghent, Belgium
Beljonne, David ; Université de Mons - UMONS > Faculté des Sciences > Service de Chimie des matériaux nouveaux
Stranks, Samuel D ; University of Cambridge, Department of Chemical Engineering and Biotechnology, Philippa Fawcett Drive, Cambridge, CB3 0AS, UK. sds65@cam.ac.uk ; University of Cambridge, Department of Physics, Cavendish Laboratory, JJ Thomson Ave, Cambridge, CB3 0US, UK
Van Gompel, Wouter T M ; Hasselt University, Institute for Materials Research (imo-imomec), Hybrid Materials Design (HyMaD), Martelarenlaan 42, B-3500 Hasselt, Belgium. wouter.vangompel@uhasselt.be ; Energyville, imo-imomec, Thor Park 8320, B-3600, Genk, Belgium ; imec, imo-imomec, Wetenschapspark 1, B-3590, Diepenbeek, Belgium
R150 - Institut de Recherche sur les Systèmes Complexes R400 - Institut de Recherche en Science et Ingénierie des Matériaux
Funders :
Universiteit Hasselt Fonds Wetenschappelijk Onderzoek F.R.S.-FNRS - Fonds de la Recherche Scientifique Tata Sons Tata Sons Royal Society
Funding text :
I. D. and A. C. acknowledge the Research Foundation \u2013 Flanders (FWO) for the funding of their FWO strategic basic research PhD grants (1S31325N and 1SH0X24N, respectively). P. B., P. L. M., L. L., K. V. H., C. Q., D. B., and W. T. M. V. G. acknowledge the FWO for funding through the FWO research project G0A8723N. C. Q., D. B., and W. T. M. V. G. acknowledge the FWO (G0AQV25N) and the FNRS (n\u00B0 T.0009.25) for funding through the WEAVE research project INTENSITY. This work was supported by Hasselt University and the FWO via the Hercules projects AUHL/15/2-GOH3816N and I001324N. C. Q. is a FNRS Research Associate and D. B. is FNRS Research Director. Y. B. acknowledges the Winton Programme for Physics of Sustainability for funding. S. D. S. acknowledges the Royal Society and Tata Group (grant numbers UF150033, URF\\R\\221026). Huguette Penxten and dr. Sander Smeets (UHasselt) are acknowledged and thanked for their help with the CV and NMR measurements, respectively. Prof. dr. Akshay Rao (University of Cambridge, UK) and Prof. dr. Daniel B. Turner (Boise State University, US) are thanked for fruitful discussions related to the coherent phonons in DBCzPbI3.
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