Sb-Doped Metal Halide Nanocrystals: A 0D versus 3D Comparison

Dongxu Zhu^a, Matteo Zaffalon^b, Juliette Zito^a^,^c, Francesca Cova^b, Francesco Meinardi^b, Luca De Trizio^a, Ivan Infante^a, Sergio Brovelli^b, Liberato Manna^a

^aNanochemistry Department, Istituto Italiano di Tecnologia, 16163 Genova, Italy

^bDipartimento di Scienza dei Materiali, Università degli Studi di Milano Bicocca, 20125 Milano, Italy

^cDipartimento di Chimica e Chimica Industriale, Università degli Studi di Genova, 16146 Genova, Italy

Materials for Sustainable Development Conference (MATSUS)
Proceedings of MATSUS23 & Sustainable Technology Forum València (STECH23) (MATSUS23)

#NCFun23 - Fundamental Processes in Nanocrystals and 2D Materials

VALÈNCIA, Spain, 2023 March 6th - 10th

Organizers: Valerio Pinchetti and Shalini Singh

Oral, Matteo Zaffalon, presentation 138
DOI: https://doi.org/10.29363/nanoge.matsus.2023.138
Publication date: 22nd December 2022

Lead halide perovskites are emerging materials that can be synthesised at low cost on a large scale and have potentially disruptive optical performances in photonic and scintillation applications [1]. On the other hand, these materials are inherently toxic, due to the presence of Pb, and generally unstable, especially when exposed to heat, air and moisture. Therefore, there is vivid research aimed to replace Pb-based perovskites with non-toxic metal halide alternatives that may exhibit similar optical properties and, ideally, greater stability. In this context, the broad family of double perovskites (DPs) is particularly promising and offers fertile ground for new discoveries. Among the various structures, Sb³⁺-doped DPs are attracting increasing interest due to their bright and exceptionally large (more than 1.2eV) Stokes-Shifted PL [2], [3]. Here, we present colloidal nanocrystals (NCs) of Rb3InCl6, composed of isolated metal halide octahedra ("0D"), and dual perovskites of Cs2NaInCl6 and Cs2KInCl6, in which all octahedra share angles and are interconnected ("3D"), with the aim of elucidating and comparing their optical characteristics once doped with Sb3+ ions [4]. Our optical and computational analyses demonstrate the photophysical mechanism underlying PL in these systems, and that it is possible to double the quantum yield through localisation of the exciton in 0D structures by preventing its migration to trap states at the surface. Scintillation properties are evaluated by means of radioluminescence experiments and waveguide performance without resorption in large-area plastic scintillators is assessed by means of Monte Carlo ray-tracing simulations.

References:

[1] Zaffalon, M. L.; Cova, F.; Liu, M.; Cemmi, A.; Di Sarcina, I.; Rossi, F.; Carulli, F.; Erroi, A.; Rodà, C.; Perego, J.; Comotti, A.; Fasoli, M.; Meinardi, F.; Li, L.; Vedda, A.; Brovelli, S. Extreme γ-Ray Radiation Hardness and High Scintillation Yield in Perovskite Nanocrystals. Nat. Photonics 2022, 16 (12), 860–868.

[2] Noculak, A.; Morad, V.; McCall, K. M.; Yakunin, S.; Shynkarenko, Y.; Wörle, M.; Kovalenko, M. V. Bright Blue and Green Luminescence of Sb(III) in Double Perovskite Cs 2 MInCl 6 (M = Na, K) Matrices. Chem. Mater. 2020, 32 (12), 5118–5124

[3] Zhang, B.; Pinchetti, V.; Zito, J.; Ray, A.; Melcherts, A. E. M.; Ghini, M.; Pianetti, A.; Infante, I.; Brovelli, S.; De Trizio, L.; Manna, L. Isolated [SbCl 6 ] 3– Octahedra Are the Only Active Emitters in Rb 7 Sb 3 Cl 16 Nanocrystals . ACS Energy Lett. 2021, 3952–3959

[4] (1) Zaffalon, M. L.; Cova, F.; Liu, M.; Cemmi, A.; Di Sarcina, I.; Rossi, F.; Carulli, F.; Erroi, A.; Rodà, C.; Perego, J.; Comotti, A.; Fasoli, M.; Meinardi, F.; Li, L.; Vedda, A.; Brovelli, S. Extreme γ-Ray Radiation Hardness and High Scintillation Yield in Perovskite Nanocrystals. Nat. Photonics 2022, 16 (12), 860–868. https://doi.org/10.1038/s41566-022-01103-x. (2) Noculak, A.; Morad, V.; McCall, K. M.; Yakunin, S.; Shynkarenko, Y.; Wörle, M.; Kovalenko, M. V. Bright Blue and Green Luminescence of Sb(III) in Double Perovskite Cs 2 MInCl 6 (M = Na, K) Matrices. Chem. Mater. 2020, 32 (12), 5118–5124. https://doi.org/10.1021/acs.chemmater.0c01004. (3) Zhang, B.; Pinchetti, V.; Zito, J.; Ray, A.; Melcherts, A. E. M.; Ghini, M.; Pianetti, A.; Infante, I.; Brovelli, S.; De Trizio, L.; Manna, L. Isolated [SbCl 6 ] 3– Octahedra Are the Only Active Emitters in Rb 7 Sb 3 Cl 16 Nanocrystals . ACS Energy Lett. 2021, 3952–3959. https://doi.org/10.1021/acsenergylett.1c01662. (4) Zhu, D.; Zaffalon, M. L.; Zito, J.; Cova, F.; Meinardi, F.; De Trizio, L.; Infante, I.; Brovelli, S.; Manna, L. Sb-Doped Metal Halide Nanocrystals: A 0D versus 3D Comparison. ACS Energy Lett. 2021, 6 (6), 2283–2292

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