Gabrielle Koknat1,Haipeng Lu2,3,Yi Yao1,Ji Hao2,Xixi Qin1,Chuanxiao Xiao2,Ruyi Song1,Florian Merz4,Markus Rampp5,Sebastian Kokott6,Christian Carbogno6,Tianyang Li1,Glenn Teeter2,Matthias Scheffler6,Joseph Berry2,David Mitzi1,Jeffrey Blackburn2,Volker Blum1,Matthew Beard2
Duke University1,National Renewable Energy Laboratory2,The Hong Kong University of Science and Technology3,Lenovo HPC Innovation Center4,Max Planck Computing and Data Facility5,The NOMAD laboratory at the Fritz Haber Institute of the Max Planck Society6
Gabrielle Koknat1,Haipeng Lu2,3,Yi Yao1,Ji Hao2,Xixi Qin1,Chuanxiao Xiao2,Ruyi Song1,Florian Merz4,Markus Rampp5,Sebastian Kokott6,Christian Carbogno6,Tianyang Li1,Glenn Teeter2,Matthias Scheffler6,Joseph Berry2,David Mitzi1,Jeffrey Blackburn2,Volker Blum1,Matthew Beard2
Duke University1,National Renewable Energy Laboratory2,The Hong Kong University of Science and Technology3,Lenovo HPC Innovation Center4,Max Planck Computing and Data Facility5,The NOMAD laboratory at the Fritz Haber Institute of the Max Planck Society6
2D hybrid organic-inorganic perovskites (HOIPs) are exciting materials for optoelectronic device applications due to their high degree of chemical and structural tunability. The ability to electronically dope these materials via incorporation of extrinsic dopants is essential for control over carrier concentrations. Conversely, the presence of intrinsic defects can negatively impact electronic doping efficiencies. Here, we present a systematic study of intrinsic point defects and extrinsic dopants (eg. Bi, Sn [<i>PRX Energy</i>, <b>2, 023010 </b>(2023)]), both in isolation and as combined defects, in phenylethylammonium lead iodide (PEA<sub>2</sub>PbI<sub>4</sub>). Using spin-orbit coupled hybrid density functional theory (DFT) and supercell models up to 3,383 atoms in size, we pinpoint the expected positions of dopant-derived electronic levels in the bandgap. Complementary experimental findings reinforce hypotheses of compensation mechanisms and limiting factors derived from DFT.