Exploiting the Lability of Metal Halide Perovskites for Doping Semiconductor Nanocomposites

Mariano Calcabrini^a, Aziz Genç^b^,^c, Yu Liu^a, Tobias Kleinhanns^a, Seungho Lee^a, Dmitry N. Dirin^d^,^e, Quinten A. Akkerman^d^,^e, Maksym V. Kovalenko^d^,^e, Jordi Arbiol^b, Maria Ibáñez^a

^aInstitute of Science and Technology, Am Campus 1, Klosterneuburg

^bCatalan Institute of Nanoscience and Nanotechnology (ICN2), CSIC and BIST, Campus UAB, Edifici ICN2, Av. de Serragalliners, s/n, Bellaterra, Spain

^cMaterials Science and Engineering Department, Izmir Institute of Technology, İzmir, Turkey, Gülbahçe, İzmir Yüksek Teknoloji Enstitüsü, Izmir, Turkey

^dDepartment of Chemistry and Applied Biosciences, Vladimir-Prelog Weg 1-5/10, Zurich, Switzerland

^eEmpa-Swiss Federal Laboratories for Materials Science and Technology, Ueberlandstrasse, 129, Dübendorf, Switzerland

Online School
Proceedings of Online school on Fundamentals of Semiconductive Quantum Dots (QDsSCHOOL)

Online, Spain, 2021 May 11th - 13th

Organizers: Quinten Akkerman, Sergio Brovelli and Liberato Manna

Poster, Mariano Calcabrini, 014
DOI: https://doi.org/10.29363/nanoge.qdsschool.2021.014
Publication date: 30th April 2021

ePoster:

Cesium lead halides exhibit diverse bonding nature with covalent PbX₆^4- anions and Cs⁺ cations. These ions' low charge density renders the crystals unstable, enabling the conversion between related perovskites and non-perovskites phases.^[1] Such instability can be problematic for some applications like photovoltaics and detectors where the perovskites are exposed to high energy densities, but is this always a disadvantage?

Our most recent work shows how CsPbBr₃ converts to Cs₄PbBr₆ upon heating up with PbS producing PbS-Cs₄PbBr₆ nanocomposites.^[2] The byproduct of the transformation, PbBr₂, dissolves in the PbS matrix, increasing the carrier concentration and inducing grain growth. In this presentation, we provide evidence of the chemical transformation using temperature-dependent in-situ X-ray diffraction and high resolution transmission electron microscopy. Additionally, by controlling the amount of CsPbBr₃, we tune the charge carrier density between 10¹⁹ and 10²⁰ cm^-3. Such heavily doped nanocomposites have potential applications in thermoelectrics and optoelectronic devices. Furthermore, this doping strategy is not limited to cesium lead halides and could be applied to other unstable crystal phases.

[1] Kovalenko, M. V; Protesescu, L.; Bodnarchuk, M. I. Properties and Potential Optoelectronic Applications of Lead Halide Perovskite Nanocrystals. Science 2017, 358 (6364), 745–750. https://doi.org/10.1126/science.aam7093.

[2] Calcabrini, M.; Genç, A.; Liu, Y.; Kleinhanns, T.; Lee, S.; Dirin, D. N.; Akkerman, Q. A.; Kovalenko, M. V.; Arbiol, J.; Ibáñez, M. Exploiting the Lability of Metal Halide Perovskites for Doping Semiconductor Nanocomposites. ACS Energy Lett. 2021, 6, 581–587. https://doi.org/10.1021/acsenergylett.0c02448.

References:

[1] Kovalenko, M. V; Protesescu, L.; Bodnarchuk, M. I. Properties and Potential Optoelectronic Applications of Lead Halide Perovskite Nanocrystals. Science 2017, 358 (6364), 745–750

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