TY - JOUR
T1 - A charge transfer framework that describes supramolecular interactions governing structure and properties of 2D perovskites
AU - Zhao, Xiaoming
AU - Ball, Melissa L.
AU - Kakekhani, Arvin
AU - Liu, Tianran
AU - Rappe, Andrew M.
AU - Loo, Yueh Lin
N1 - Funding Information:
The authors thank Dr. Esther Tsai and Dr. Ruipeng Li for help with X-ray scattering measurements, which were conducted at the Center for Functional Nanomaterials (CFN) and the Complex Materials Scattering (CMS) beamline of the National Synchrotron Light Source II (NSLS-II), which both are U.S. DOE Office of Science Facilities, at Brookhaven National Laboratory under Contract No. DE-SC0012704. The authors acknowledge the use of Princeton’s Imaging and Analysis Center, which is partially supported by the Princeton Center for Complex Materials, a National Science Foundation (NSF)-MRSEC program (DMR-1420541). Y.-L.L. acknowledges support from the National Science Foundation, under grant CMMI-1824674. X.Z. was partially supported on a Princeton Catalysis Initiative grant to Y.-L.L. M.L.B. is supported by a Princeton Presidential Post-doctoral Fellowship. A.K. was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, under Award #DE-FG02-07ER46431. A.M.R. acknowledges the support of the Office of Naval Research, under grant number N00014-20-1-2701. The authors also acknowledge computational support from the High-Performance Computing Modernization Office of the Department of Defense. Computational support was provided by the National Energy Research Scientific Computing Center (NERSC), a U.S. Department of Energy, Office of Science User Facility located at Lawrence Berkeley National Laboratory, operated under Contract No. DE-AC02-05CH11231.
Publisher Copyright:
© 2022, The Author(s).
PY - 2022/12
Y1 - 2022/12
N2 - The elucidation of structure-to-function relationships for two-dimensional (2D) hybrid perovskites remains a primary challenge for engineering efficient perovskite-based devices. By combining insights from theory and experiment, we describe the introduction of bifunctional ligands that are capable of making strong hydrogen bonds within the organic bilayer. We find that stronger intermolecular interactions draw charge away from the perovskite layers, and we have formulated a simple and intuitive computational descriptor, the charge separation descriptor (CSD), that accurately describes the relationship between the Pb-I-Pb angle, band gap, and in-plane charge transport with the strength of these interactions. A higher CSD value correlates to less distortion of the Pb-I-Pb angle, a reduced band gap, and higher in-plane mobility of the perovskite. These improved material properties result in improved device characteristics of the resulting solar cells.
AB - The elucidation of structure-to-function relationships for two-dimensional (2D) hybrid perovskites remains a primary challenge for engineering efficient perovskite-based devices. By combining insights from theory and experiment, we describe the introduction of bifunctional ligands that are capable of making strong hydrogen bonds within the organic bilayer. We find that stronger intermolecular interactions draw charge away from the perovskite layers, and we have formulated a simple and intuitive computational descriptor, the charge separation descriptor (CSD), that accurately describes the relationship between the Pb-I-Pb angle, band gap, and in-plane charge transport with the strength of these interactions. A higher CSD value correlates to less distortion of the Pb-I-Pb angle, a reduced band gap, and higher in-plane mobility of the perovskite. These improved material properties result in improved device characteristics of the resulting solar cells.
UR - http://www.scopus.com/inward/record.url?scp=85133678426&partnerID=8YFLogxK
UR - http://www.scopus.com/inward/citedby.url?scp=85133678426&partnerID=8YFLogxK
U2 - 10.1038/s41467-022-31567-y
DO - 10.1038/s41467-022-31567-y
M3 - Article
C2 - 35804028
AN - SCOPUS:85133678426
SN - 2041-1723
VL - 13
JO - Nature communications
JF - Nature communications
IS - 1
M1 - 3970
ER -