Perspective: Theory and simulation of hybrid halide perovskites

Whalley, Lucy, Frost, Jarvist M., Jung, Young-Kwang and Walsh, Aron (2017) Perspective: Theory and simulation of hybrid halide perovskites. The Journal of Chemical Physics, 146 (22). p. 220901. ISSN 0021-9606

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Organic-inorganic halide perovskites present a number of challenges for first-principles atomistic materials modeling. Such “plastic crystals” feature dynamic processes across multiple length and time scales. These include the following: (i) transport of slow ions and fast electrons; (ii) highly anharmonic lattice dynamics with short phonon lifetimes; (iii) local symmetry breaking of the average crystallographic space group; (iv) strong relativistic (spin-orbit coupling) effects on the electronic band structure; and (v) thermodynamic metastability and rapid chemical breakdown. These issues, which affect the operation of solar cells, are outlined in this perspective. We also discuss general guidelines for performing quantitative and predictive simulations of these materials, which are relevant to metal-organic frameworks and other hybrid semiconducting, dielectric and ferroelectric compounds.

Item Type: Article
Additional Information: Funding information: The primary research underpinning this discussion was performed by Jarvist M. Frost (molecular dynamic and Monte Carlo investigations), Federico Brivio (crystal and electronic structure), Jonathan M. Skelton (lattice dynamics and vibrational spectroscopy), and Lucy Whalley (bandgap deformations). We are indebted to our large team of external collaborators including the groups of Mark van Schilfgaarde, Saiful Islam, Simon Billinge, Piers Barnes, and Mark Weller. L.D.W. would like to acknowledge support and guidance from the staff and students at the Centre for Doctoral Training in New and Sustainable Photovoltaics. This work was funded by the EPSRC (Grant Nos. EP/L01551X/1 and EP/K016288/1), the Royal Society, and the ERC (Grant No. 277757).
Subjects: F100 Chemistry
Department: Faculties > Engineering and Environment > Mathematics, Physics and Electrical Engineering
Depositing User: Elena Carlaw
Date Deposited: 04 Jun 2021 13:22
Last Modified: 31 Jul 2021 11:06

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