Defects in Halide Perovskites: Does It Help to Switch from 3D to 2D?

Haibo Xue; Zehua Chen; Shuxia Tao; Geert Brocks

doi:10.1021/acsenergylett.4c00702

Defects in Halide Perovskites: Does It Help to Switch from 3D to 2D?

ACS Energy Lett. 2024 Apr 23;9(5):2343-2350. doi: 10.1021/acsenergylett.4c00702. eCollection 2024 May 10.

Authors

Haibo Xue^{1

2}, Zehua Chen^{1

2}, Shuxia Tao^{1

2}, Geert Brocks^{1

2

3}

Affiliations

¹ Materials Simulation & Modelling, Department of Applied Physics, Eindhoven University of Technology, P.O. Box 513, 5600MB Eindhoven, The Netherlands.
² Center for Computational Energy Research, Department of Applied Physics, Eindhoven University of Technology, P.O. Box 513, 5600MB Eindhoven, The Netherlands.
³ Computational Chemical Physics, Faculty of Science and Technology and MESA+ Institute for Nanotechnology, University of Twente, P.O. Box 217, 7500AE Enschede, The Netherlands.

Abstract

Two-dimensional (2D) organic-inorganic hybrid iodide perovskites have been put forward in recent years as stable alternatives to their three-dimensional (3D) counterparts. Using first-principles calculations, we demonstrate that equilibrium concentrations of point defects in the 2D perovskites PEA₂PbI₄, BA₂PbI₄, and PEA₂SnI₄ (PEA, phenethylammonium; BA, butylammonium) are much lower than in comparable 3D perovskites. Bonding disruptions by defects are more destructive in 2D than in 3D networks, making defect formation energetically more costly. The stability of 2D Sn iodide perovskites can be further enhanced by alloying with Pb. Should, however, point defects emerge in sizable concentrations as a result of nonequilibrium growth conditions, for instance, then those defects likely hamper the optoelectronic performance of the 2D perovskites, as they introduce deep traps. We suggest that trap levels are responsible for the broad sub-bandgap emission in 2D perovskites observed in experiments.