@article{e74178c8e7094eaab071b5b1519604f6,
title = "Influence of π -conjugated cations and halogen substitution on the optoelectronic and excitonic properties of layered hybrid perovskites",
abstract = "Low-cost chemical engineering of two-dimensional layered hybrid halide perovskite structures allows for the design of hybrid semiconductor quantum wells with tailored room-temperature excitonic optical absorption, emission, and charge carrier transport properties. Here density functional theory and the Bethe-Salpeter equation are used to predict the electronic structure and optical response of layered perovskites with two representative single-ring conjugated organic spacers, ammonium-propyl-imidazole (API) and 2-phenethylammonium (PEA). The inorganic perovskite quantum well properties are further tuned by analyzing the effect of halogen (X = I, Br, Cl) substitution. We found that visible light absorption occurs primarily within the perovskite layer and that UV light absorption induces partial electron-hole separation between layers. In addition, a strong exciton binding energy and influence on absorption spectrum is found by solving the Bethe-Salpeter equation. Our results suggest that further engineering is necessary beyond the single-ring limit, by introducing more conjugated rings and/or heavier nuclei into the organic spacer. This is a promising future direction to achieve photoinduced charge separation and more generally hybrid heterostructures with attractive optoelectronic properties.",
author = "Joshua Leveillee and Claudine Katan and Liujiang Zhou and Mohite, \{Aditya D.\} and Jacky Even and Sergei Tretiak and Andr{\'e} Schleife and Neukirch, \{Amanda J.\}",
note = "The work at Los Alamos National Laboratory (LANL) was supported by the LANL LDRD program (A.J.N., A.D.M, J.L., and S.T.). The work at UIUC work was supported by the National Science Foundation under Grant No. CBET-1437230. A.D.M. acknowledges the DOE-EERE 0001647-1544 grant for this work. This work was done in part at Center for Nonlinear Studies (CNLS) and the Center for Integrated Nanotechnologies CINT), a US Department of Energy and Office of Basic Energy Sciences user facility, at LANL. This research used resources provided by the LANL Institutional Computing Program. Calculations were additionally supported by the Campus Cluster program at UIUC and this research is part of the Blue Waters sustained-petascale computing project, which is supported by the National Science Foundation (awards OCI-0725070 and ACI-1238993) and the state of Illinois. Blue Waters is a joint effort of the University of Illinois at Urbana-Champaign and its National Center for Supercomputing Applications. LANL is operated by Los Alamos National Security, LLC, for the National Nuclear Security Administration of the US Department of Energy under Contract No. DE-AC52-06NA25396. J.E. acknowledges financial support from the Institut Universitaire de France. The work at Los Alamos National Laboratory (LANL) was supported by the LANL LDRD program (A.J.N., A.D.M, J.L., and S.T.). The work at UIUC work was supported by the National Science Foundation under Grant No. CBET-1437230. A.D.M. acknowledges the DOE-EERE 0001647-1544 grant for this work. This work was done in part at Center for Nonlinear Studies (CNLS) and the Center for Integrated Nanotechnologies CINT), a US Department of Energy and Office of Basic Energy Sciences user facility, at LANL. This research used resources provided by the LANL Institutional Computing Program. Calculations were additionally supported by the Campus Cluster program at UIUC and this research is part of the Blue Waters sustained-petascale computing project, which is supported by the National Science Foundation (awards OCI-0725070 and ACI-1238993) and the state of Illinois. Blue Waters is a joint effort of the University of Illinois at Urbana-Champaign and its National Center for Supercomputing Applications. LANL is operated by Los Alamos National Security, LLC, for the National Nuclear Security Administration of the US Department of Energy under Contract No. DE-AC52-06NA25396. J.E. acknowledges financial support from the Institut Universitaire de France.",
year = "2018",
month = oct,
day = "29",
doi = "10.1103/PhysRevMaterials.2.105406",
language = "English (US)",
volume = "2",
journal = "Physical Review Materials",
issn = "2475-9953",
publisher = "American Physical Society",
number = "10",
}