Metal halide semiconductors: materials discovery beyond ABX3 perovskites
Lead Research Organisation:
University of Oxford
Department Name: Oxford Physics
Abstract
Climate change and energy security are some of the greatest challenges to be faced by mankind over the coming century. Renewable sources of energy and increases in energy efficiency are key solutions that will allow the world to maintain and enhance its current level of prosperity. Photovoltaic cells, in particular, allow large-scale, sustainable generation of electricity: the solar energy incident on the surface of the earth in one hour is enough to provide the whole world's current annual energy requirements. In addition, light-emitting diodes for solid-state lighting can significantly reduce the power demand for lighting, but still require further improvements in cost per given quality of light. Further advances in these fields rely crucially on the discovery and development of new semiconducting materials that can efficiently turn light into electricity, and vice versa.
The relatively recent use of hybrid metal halide perovskite semiconductors in photovoltaic and light-emitting devices has been particularly exciting here. These materials now deliver solar cells with power conversion efficiencies exceeding 25% for single-junction thin-film cells (close to the thermodynamic limit of 30%), and efficient light-emitting diodes. However, some issues remain with this current class of ABX3 metal halide perovskites, including toxicity of lead which is incorporated in the highest performing materials, as well as long-term material stability, and stable band-gap tunability, required for higher efficiency tandem solar cells and colour-tunable light emission. Therefore, the discovery of a new catalogue of semiconductors which overcome such issues would be extremely exciting at this point.
This research programme will enable the discovery of new semiconductors within the broader class of metal-halide compositions (beyond the now well-established group of ABX3 perovskites) which is still unexplored to a surprising extent. New materials discovery will be enabled by a closely-knit feedback loop based on the complementary and world-leading expertise portfolios of the four co-investigators, encompassing computational modelling and prediction, materials synthesis, thin-film fabrication and passivation and combinatorial spectroscopic characterization. These activities will evolve in three well-defined strands, focusing on computational design, materials synthesis and processing, and experimental assessment of critical material properties. These strands will be carried out in parallel, will be exceptionally well interlinked, and evolve as part of a feedback loop in which any new finding in one strand will feed highly useful information into the other two strands. This co-ordinated effort will allow us to turn discovery of new semiconductors from the current slow, trial-and-error, needle-in-a-haystack search into a rapid, targeted and systematic exploration of a vast group of potential candidate materials. Such directed discovery will unearth a new library of high-performance materials, given that the currently available materials are likely to be just the tip of the iceberg of actually available, but as yet undiscovered semiconductors.
The relatively recent use of hybrid metal halide perovskite semiconductors in photovoltaic and light-emitting devices has been particularly exciting here. These materials now deliver solar cells with power conversion efficiencies exceeding 25% for single-junction thin-film cells (close to the thermodynamic limit of 30%), and efficient light-emitting diodes. However, some issues remain with this current class of ABX3 metal halide perovskites, including toxicity of lead which is incorporated in the highest performing materials, as well as long-term material stability, and stable band-gap tunability, required for higher efficiency tandem solar cells and colour-tunable light emission. Therefore, the discovery of a new catalogue of semiconductors which overcome such issues would be extremely exciting at this point.
This research programme will enable the discovery of new semiconductors within the broader class of metal-halide compositions (beyond the now well-established group of ABX3 perovskites) which is still unexplored to a surprising extent. New materials discovery will be enabled by a closely-knit feedback loop based on the complementary and world-leading expertise portfolios of the four co-investigators, encompassing computational modelling and prediction, materials synthesis, thin-film fabrication and passivation and combinatorial spectroscopic characterization. These activities will evolve in three well-defined strands, focusing on computational design, materials synthesis and processing, and experimental assessment of critical material properties. These strands will be carried out in parallel, will be exceptionally well interlinked, and evolve as part of a feedback loop in which any new finding in one strand will feed highly useful information into the other two strands. This co-ordinated effort will allow us to turn discovery of new semiconductors from the current slow, trial-and-error, needle-in-a-haystack search into a rapid, targeted and systematic exploration of a vast group of potential candidate materials. Such directed discovery will unearth a new library of high-performance materials, given that the currently available materials are likely to be just the tip of the iceberg of actually available, but as yet undiscovered semiconductors.
Organisations
Publications
Alvertis A
(2023)
Importance of nonuniform Brillouin zone sampling for ab initio Bethe-Salpeter equation calculations of exciton binding energies in crystalline solids
in Physical Review B
Biega R
(2023)
Chemical Mapping of Excitons in Halide Double Perovskites
Biega RI
(2023)
Chemical Mapping of Excitons in Halide Double Perovskites.
in Nano letters
Buizza L
(2021)
Interplay of Structure, Charge-Carrier Localization and Dynamics in Copper-Silver-Bismuth-Halide Semiconductors
in Advanced Functional Materials
Buizza LRV
(2021)
Charge-Carrier Mobility and Localization in Semiconducting Cu2AgBiI6 for Photovoltaic Applications.
in ACS energy letters
Chen Y
(2022)
Optoelectronic Properties of Mixed Iodide-Bromide Perovskites from First-Principles Computational Modeling and Experiment.
in The journal of physical chemistry letters
Chen Y
(2023)
Tunable Interlayer Delocalization of Excitons in Layered Organic-Inorganic Halide Perovskites
in The Journal of Physical Chemistry Letters
Duijnstee EA
(2023)
Understanding the Degradation of Methylenediammonium and Its Role in Phase-Stabilizing Formamidinium Lead Triiodide.
in Journal of the American Chemical Society
Elmestekawy KA
(2022)
Controlling Intrinsic Quantum Confinement in Formamidinium Lead Triiodide Perovskite through Cs Substitution.
in ACS nano
Filip M
(2022)
Screening of Excitons by Organic Cations in Quasi-Two-Dimensional Organic-Inorganic Lead-Halide Perovskites
in Nano Letters
Filip MR
(2021)
Phonon Screening of Excitons in Semiconductors: Halide Perovskites and Beyond.
in Physical review letters
Gant S
(2022)
Optimally tuned starting point for single-shot G W calculations of solids
in Physical Review Materials
Hooijer R
(2022)
Silver-Bismuth Based 2D Double Perovskites (4FPEA) 4 AgBiX 8 ( X = Cl, Br, I): Highly Oriented Thin Films with Large Domain Sizes and Ultrafast Charge-Carrier Localization
in Advanced Optical Materials
Hu S
(2024)
Narrow Bandgap Metal Halide Perovskites for All-Perovskite Tandem Photovoltaics
in Chemical Reviews
Huang YT
(2022)
Strong absorption and ultrafast localisation in NaBiS2 nanocrystals with slow charge-carrier recombination.
in Nature communications
Jia Z
(2023)
Charge-Carrier Dynamics of Solution-Processed Antimony- and Bismuth-Based Chalcogenide Thin Films
in ACS Energy Letters
Jin H
(2023)
Alumina Nanoparticle Interfacial Buffer Layer for Low-Bandgap Lead-Tin Perovskite Solar Cells
in Advanced Functional Materials
Kober-Czerny M
(2022)
Excellent Long-Range Charge-Carrier Mobility in 2D Perovskites
in Advanced Functional Materials
Lal S
(2023)
Bandlike Transport and Charge-Carrier Dynamics in BiOI Films.
in The journal of physical chemistry letters
Li J
(2023)
Correction to "Zwitterions in 3D Perovskites: Organosulfide-Halide Perovskites"
in Journal of the American Chemical Society
Li J
(2022)
Zwitterions in 3D Perovskites: Organosulfide-Halide Perovskites.
in Journal of the American Chemical Society
Lim V
(2022)
Impact of Hole-Transport Layer and Interface Passivation on Halide Segregation in Mixed-Halide Perovskites
in Advanced Functional Materials
Lim V
(2022)
Air-Degradation Mechanisms in Mixed Lead-Tin Halide Perovskites for Solar Cells
in Advanced Energy Materials
Lohmann KB
(2022)
Solvent-Free Method for Defect Reduction and Improved Performance of p-i-n Vapor-Deposited Perovskite Solar Cells.
in ACS energy letters
McArthur J
(2023)
Minimal Molecular Building Blocks for Screening in Quasi-Two-Dimensional Organic-Inorganic Lead Halide Perovskites.
in Nano letters
Ohad G
(2022)
Band gaps of halide perovskites from a Wannier-localized optimally tuned screened range-separated hybrid functional
in Physical Review Materials
Ohad G
(2023)
Optical absorption spectra of metal oxides from time-dependent density functional theory and many-body perturbation theory based on optimally-tuned hybrid functionals
in Physical Review Materials
Putland B
(2024)
Compositional Transformation and Impurity-Mediated Optical Transitions in Co-Evaporated Cu 2 AgBiI 6 Thin Films for Photovoltaic Applications
in Advanced Energy Materials
Righetto M
(2023)
Cation-Disorder Engineering Promotes Efficient Charge-Carrier Transport in AgBiS 2 Nanocrystal Films
in Advanced Materials
Righetto M
(2023)
Alloying Effects on Charge-Carrier Transport in Silver-Bismuth Double Perovskites
in The Journal of Physical Chemistry Letters
Rothmann M
(2023)
Atomistic Understanding of the Coherent Interface Between Lead Iodide Perovskite and Lead Iodide
in Advanced Materials Interfaces
Sansom HC
(2021)
Highly Absorbing Lead-Free Semiconductor Cu2AgBiI6 for Photovoltaic Applications from the Quaternary CuI-AgI-BiI3 Phase Space.
in Journal of the American Chemical Society
Sansom HC
(2021)
Chemical Control of the Dimensionality of the Octahedral Network of Solar Absorbers from the CuI-AgI-BiI3 Phase Space by Synthesis of 3D CuAgBiI5.
in Inorganic chemistry
Schmidt-Mende L
(2021)
Roadmap on organic-inorganic hybrid perovskite semiconductors and devices
in APL Materials
Sebastiá-Luna P
(2023)
Chalcohalide Antiperovskite Thin Films with Visible Light Absorption and High Charge-Carrier Mobility Processed by Solvent-Free and Low-Temperature Methods
in Chemistry of Materials
Wright AD
(2021)
Ultrafast Excited-State Localization in Cs2AgBiBr6 Double Perovskite.
in The journal of physical chemistry letters
Xia CQ
(2021)
Limits to Electrical Mobility in Lead-Halide Perovskite Semiconductors.
in The journal of physical chemistry letters
Yan S
(2023)
A Templating Approach to Controlling the Growth of Coevaporated Halide Perovskites.
in ACS energy letters
Yan S
(2023)
Correction to "A Templating Approach to Controlling the Growth of Coevaporated Halide Perovskites".
in ACS energy letters
Yuan Q
(2023)
Thermally Stable Perovskite Solar Cells by All-Vacuum Deposition.
in ACS applied materials & interfaces