TYC Soiree: Many-Body Theory Calculations on Materials – Marina Filip & Linn Leppert
Venue: LG26, Bentham House,
18 January @ 4:00 pm – 6:00 pm
Marina Filip – University of Oxford
Linn Leppert – University of Twente
A first-principles perovskites potpourri: Electronic and excited-state structure of double, layered, extended and non-perovskites
Perovskite solar cells in which methylammonium lead iodide is used as a solar absorber material, have reached maturity in the last years owing to a concerted effort to optimize material synthesis, stability, and device performance. However, the halide perovskite family features thousands of other stable members with highly tunable optoelectronic properties. In this presentation, I will provide an overview of our current understanding of the electronic and excited-state structure of several classes of perovskites – double, layered, extended – as well as some perovskite-like structures (thrown in for good measure). We use Green’s function-based many-body perturbation theory in the GW and Bethe-Salpeter Equation approach to calculate accurate bandstructures [1, 2], optical absorption spectra and excitonic properties from first principles. Our calculations allow us to map the complex landscape of electronic properties and excitons, understand the impact of chemical heterogeneity [3 – 6], dimensionality [5 -7] and temperature effects , and provide chemically intuitive rules for when to trust canonical models for excitons in these materials.
 L. Leppert, T. Rangel, J. Neaton, Phys. Rev. Materials 2019, 3, 103803.
 T. Lebeda, T. Aschebrock, J.Sun, L. Leppert, S. Kümmel, Phys. Rev. Materials 2023, 7, 093803.
 A. Slavney, B. Connor, L. Leppert, H. Karunadasa, Chem. Sci. 2019, 10, 11041.
 R.-I. Biega, M. Filip, L. Leppert, J. B. Neaton, J. Phys. Chem. Lett. 2021, 12, 2057.
 R.-I. Biega, Y. Chen, M. R. Filip, L. Leppert, Nano Lett. 2023, 23, 8155.
 H. J. Jöbsis, K. Fykouras, J. Reinders, J. van Katwijk, J. Dorresteijn, T. Arens, I. Vollmer, L. Muscarella, L. Leppert, E. M. Hutter, Advanced Functional Materials 2023, 2306106.
 B. A. Connor, L. Leppert, M. D. Smith, J. B. Neaton, H. I. Karunadasa, J. Am. Chem. Soc. 2018, 140, 5235.
 S. Krach, N. Forera-Correa, R.-I. Biega, S. E. Reyes-Lillo, L. Leppert, J. Phys. Condens. Matter 2023, 35, 174001.
 B. A. Connor, A. C. Su, A. H. Slavney, L. Leppert, H. Karunadasa, Chem. Sci. 2023, accepted manuscript.
 R.-I. Biega, M. Bokdam, K. Herrmann, J. Mohanraj, D. Skyrbek, M. Thelakkat, M. Retsch, L. Leppert, J. Phys. Chem. C 2023, 127, 9183.