Electronic structure and optical properties of halide double perovskites from a Wannier-localized optimally-tuned screened range-separated hybrid functional

Francisca Sagredo, Stephen E. Gant, Guy Ohad, Jonah B. Haber, Marina R. Filip, Leeor Kronik, Jeffrey B. Neaton

Research output: Contribution to journalArticlepeer-review

Abstract

Halide double perovskites are a chemically diverse and growing class of compound semiconductors that are promising for optoelectronic applications. However, the prediction of their fundamental gaps and optical properties with density functional theory (DFT) and ab initio many-body perturbation theory has been a significant challenge. Recently, a nonempirical Wannier-localized optimally tuned screened range-separated hybrid (WOT-SRSH) functional has been shown to accurately produce the fundamental band gaps of a wide set of semiconductors and insulators, including lead halide perovskites. Here, we apply the WOT-SRSH functional to five halide double perovskites and compare the results with those obtained from other known functionals and previous GW calculations. We also use the approach as a starting point for GW calculations and we compute the band structures and optical absorption spectrum for Cs2AgBiBr6, using both time-dependent DFT and the GW-Bethe-Salpeter equation approach. We show that the WOT-SRSH functional leads to accurate fundamental and optical band gaps, as well as optical absorption spectra, consistent with spectroscopic measurements, thereby establishing WOT-SRSH as a viable method for the accurate prediction of optoelectronic properties of halide double perovskites.

Original languageEnglish
Article number105401
JournalPhysical Review Materials
Volume8
Issue number10
DOIs
Publication statusPublished - Oct 2024

Funding

F.S. thanks L. Leppert for insightful discussions. The authors acknowledge Giulia Longo (Northumbria University) and Laura Herz (Oxford University) for sharing the data published in Ref. . L.K. acknowledges support from the Arieh and Mintzy Katzman Professoral Chair and the Helen and Martin Kimmel Award for Innovative investigation. M.R.F. acknowledges support from the UK Engineering and Physical Sciences Research Council (EPSRC), Grant No. EP/V010840/1. This work is funded through NSF\u2013Binational Science Foundation Grant No. DMR-2015991 and by the Israel Science Foundation. This work was also partially supported by the Center for Computational Study of Excited-State Phenomena in Energy Materials as part of the Computational Materials Sciences Program, which provided advanced codes, at the Lawrence Berkeley National Laboratory, funded by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division, under Contract No. DE-AC02-05CH11231. Computational resources were provided by the NSF funded XSEDE (now ACCESS) program, through supercomputer Stampede2 at the Texas Advanced Computing Center (TACC) through the allocation TG-DMR190070.

All Science Journal Classification (ASJC) codes

  • General Materials Science
  • Physics and Astronomy (miscellaneous)

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