Decreasing the electronic confinement in layered perovskites through intercalation
Abstract
We show that post-synthetic small-molecule intercalation can significantly reduce the electronic confinement of 2D hybrid perovskites. Using a combined experimental and theoretical approach, we explain structural, optical, and electronic effects of intercalating highly polarizable molecules in layered perovskites designed to stabilize the intercalants. Polarizable molecules in the organic layers substantially alter the optical and electronic properties of the inorganic layers. By calculating the spatially resolved dielectric profiles of the organic and inorganic layers within the hybrid structure, we show that the intercalants afford organic layers that are more polarizable than the inorganic layers. This strategy reduces the confinement of excitons generated in the inorganic layers and affords the lowest exciton binding energy for an n = 1 perovskite of which we are aware. We also demonstrate a method for computationally evaluating the exciton's binding energy by solving the Bethe–Salpeter equation for the exciton, which includes an ab initio determination of the material's dielectric profile across organic and inorganic layers. This new semi-empirical method goes beyond the imprecise phenomenological approximation of abrupt dielectric-constant changes at the organic–inorganic interfaces. This work shows that incorporation of polarizable molecules in the organic layers, through intercalation or covalent attachment, is a viable strategy for tuningmore »
- Authors:
-
- Stanford Univ., CA (United States)
- Centre National de la Recherche Scientifique (CNRS), Rennes (France)
- Univ. of Rennes (France)
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF); Global Climate and Energy Project (GCEP); Alfred P. Sloan Fellowship; CINES; Grand Equipement National de Calcul Intensif (GENCI); University of Rennes 1; Fondation d'entreprises banque Populaire de l'Ouest
- OSTI Identifier:
- 1624941
- Grant/Contract Number:
- AC02-05CH11231; DMR-1351538; DGE-114747; x2016096724; x2015096724; PEROPHOT 2015
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Chemical Science
- Additional Journal Information:
- Journal Volume: 8; Journal Issue: 3; Journal ID: ISSN 2041-6520
- Publisher:
- Royal Society of Chemistry
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Chemistry
Citation Formats
Smith, Matthew D., Pedesseau, Laurent, Kepenekian, Mikaël, Smith, Ian C., Katan, Claudine, Even, Jacky, and Karunadasa, Hemamala I. Decreasing the electronic confinement in layered perovskites through intercalation. United States: N. p., 2017.
Web. doi:10.1039/c6sc02848a.
Smith, Matthew D., Pedesseau, Laurent, Kepenekian, Mikaël, Smith, Ian C., Katan, Claudine, Even, Jacky, & Karunadasa, Hemamala I. Decreasing the electronic confinement in layered perovskites through intercalation. United States. https://doi.org/10.1039/c6sc02848a
Smith, Matthew D., Pedesseau, Laurent, Kepenekian, Mikaël, Smith, Ian C., Katan, Claudine, Even, Jacky, and Karunadasa, Hemamala I. Sun .
"Decreasing the electronic confinement in layered perovskites through intercalation". United States. https://doi.org/10.1039/c6sc02848a. https://www.osti.gov/servlets/purl/1624941.
@article{osti_1624941,
title = {Decreasing the electronic confinement in layered perovskites through intercalation},
author = {Smith, Matthew D. and Pedesseau, Laurent and Kepenekian, Mikaël and Smith, Ian C. and Katan, Claudine and Even, Jacky and Karunadasa, Hemamala I.},
abstractNote = {We show that post-synthetic small-molecule intercalation can significantly reduce the electronic confinement of 2D hybrid perovskites. Using a combined experimental and theoretical approach, we explain structural, optical, and electronic effects of intercalating highly polarizable molecules in layered perovskites designed to stabilize the intercalants. Polarizable molecules in the organic layers substantially alter the optical and electronic properties of the inorganic layers. By calculating the spatially resolved dielectric profiles of the organic and inorganic layers within the hybrid structure, we show that the intercalants afford organic layers that are more polarizable than the inorganic layers. This strategy reduces the confinement of excitons generated in the inorganic layers and affords the lowest exciton binding energy for an n = 1 perovskite of which we are aware. We also demonstrate a method for computationally evaluating the exciton's binding energy by solving the Bethe–Salpeter equation for the exciton, which includes an ab initio determination of the material's dielectric profile across organic and inorganic layers. This new semi-empirical method goes beyond the imprecise phenomenological approximation of abrupt dielectric-constant changes at the organic–inorganic interfaces. This work shows that incorporation of polarizable molecules in the organic layers, through intercalation or covalent attachment, is a viable strategy for tuning 2D perovskites towards mimicking the reduced electronic confinement and isotropic light absorption of 3D perovskites while maintaining the greater synthetic tunability of the layered architecture.},
doi = {10.1039/c6sc02848a},
journal = {Chemical Science},
number = 3,
volume = 8,
place = {United States},
year = {Sun Jan 01 00:00:00 EST 2017},
month = {Sun Jan 01 00:00:00 EST 2017}
}
Web of Science
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