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Abstract
The stellar optoelectronic properties of metal halide perovskites provide enormous promise for next-generation optical devices with excellent conversion efficiencies and lower manufacturing costs. However, there is a long-standing ambiguity as to whether the perovskite surface/interface (e.g. structure, charge transfer or source of off-target recombination) or bulk properties are the more determining factor in device performance. Here we fabricate an array of CsPbI3 crystal and hybrid glass composites by sintering and globally visualise the property-performance landscape. Our findings reveal that the interface is the primary determinant of the crystal phases, optoelectronic quality, and stability of CsPbI3. In particular, the presence of a diffusion “alloying” layer is discovered to be critical for passivating surface traps, and beneficially altering the energy landscape of crystal phases. However, high-temperature sintering results in the promotion of a non-stoichiometric perovskite and excess traps at the interface, despite the short-range structure of halide is retained within the alloying layer. By shedding light on functional hetero-interfaces, our research offers the key factors for engineering high-performance perovskite devices.
MOF glass nanocomposites allow researchers to study lead halide perovskites’ bulk and interfacial regions in relation to their optoelectronic properties. Here authors provide insights for the advancement of stable and efficient perovskite optoelectronic devices design.
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1 The University of Queensland, School of Chemical Engineering, St Lucia, Australia (GRID:grid.1003.2) (ISNI:0000 0000 9320 7537)
2 National Institute of Chemistry, Department of Inorganic Chemistry and Technology, Ljubljana, Slovenia (GRID:grid.454324.0) (ISNI:0000 0001 0661 0844)
3 The University of New South Wales, School of Chemical Engineering, Kensington, Australia (GRID:grid.1005.4) (ISNI:0000 0004 4902 0432)
4 The University of Queensland, School of Mathematics and Physics, St Lucia, Australia (GRID:grid.1003.2) (ISNI:0000 0000 9320 7537)
5 RMIT University, School of Science, Melbourne, Australia (GRID:grid.1017.7) (ISNI:0000 0001 2163 3550)
6 European Synchrotron Radiation Facility, Grenoble, France (GRID:grid.5398.7) (ISNI:0000 0004 0641 6373)
7 Nagasaki University, Graduate School of Engineering, Nagasaki, Japan (GRID:grid.174567.6) (ISNI:0000 0000 8902 2273)
8 Australian Synchrotron, Clayton, Australia (GRID:grid.248753.f) (ISNI:0000 0004 0562 0567)
9 The University of Queensland, Australian Institute for Bioengineering and Nanotechnology, St Lucia, Australia (GRID:grid.1003.2) (ISNI:0000 0000 9320 7537)
10 The University of Queensland, School of Mathematics and Physics, St Lucia, Australia (GRID:grid.1003.2) (ISNI:0000 0000 9320 7537); The University of Queensland, Australian Institute for Bioengineering and Nanotechnology, St Lucia, Australia (GRID:grid.1003.2) (ISNI:0000 0000 9320 7537)
11 Sichuan University, State Key Laboratory of Oral Diseases, National Clinical Research Center for Oral Diseases, West China Hospital of Stomatology, Chengdu, China (GRID:grid.13291.38) (ISNI:0000 0001 0807 1581); Sichuan Provincial Engineering Research Center of Oral Biomaterials, Chengdu, China (GRID:grid.13291.38)
12 The University of Queensland, School of Chemical Engineering, St Lucia, Australia (GRID:grid.1003.2) (ISNI:0000 0000 9320 7537); University of Technology Sydney, Ultimo, Australia (GRID:grid.117476.2) (ISNI:0000 0004 1936 7611)
13 University of California, Materials Research Laboratory, Santa Barbara, USA (GRID:grid.468726.9) (ISNI:0000 0004 0486 2046)
14 Université Paris-Saclay, CNRS, Laboratoire de Physique des Solides, Orsay, France (GRID:grid.462447.7) (ISNI:0000 0000 9404 6552)
15 University of Leeds, School of Chemical and Process Engineering and School of Chemistry, Leeds, UK (GRID:grid.9909.9) (ISNI:0000 0004 1936 8403)
16 The University of Queensland, School of Chemical Engineering, St Lucia, Australia (GRID:grid.1003.2) (ISNI:0000 0000 9320 7537); The University of Queensland, Australian Institute for Bioengineering and Nanotechnology, St Lucia, Australia (GRID:grid.1003.2) (ISNI:0000 0000 9320 7537)