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Title: Interconversion between Free Charges and Bound Excitons in 2D Hybrid Lead Halide Perovskites

The optoelectronic properties of hybrid perovskites can be easily tailored by varying their components. Specifically, mixing the common short organic cation (methylammonium (MA)) with a larger one (e.g., butyl ammonium (BA)) results in 2-dimensional perovskites with varying thicknesses of inorganic layers separated by the large organic cation. In both of these applications, a detailed understanding of the dissociation and recombination of electron–hole pairs is of prime importance. Here in this work, we give a clear experimental demonstration of the interconversion between bound excitons and free charges as a function of temperature by combining microwave conductivity techniques with photoluminescence measurements. We demonstrate that the exciton binding energy varies strongly (between 80 and 370 meV) with the thickness of the inorganic layers. Additionally, we show that the mobility of charges increases with the layer thickness, in agreement with calculated effective masses from electronic structure calculations.
Authors:
 [1] ; ORCiD logo [1] ;  [2] ;  [1] ; ORCiD logo [2] ; ORCiD logo [2] ; ORCiD logo [1] ; ORCiD logo [2] ; ORCiD logo [1]
  1. Delft Univ. of Technology (Netherlands). Section Optoelectronic Materials, Dept. of Chemical Engineering
  2. Northwestern Univ., Evanston, IL (United States). Argonne-Northwestern Solar Energy Research Center (ANSER), Dept. of Chemistry
Publication Date:
Grant/Contract Number:
SC0001059; 712.014.007
Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. C
Additional Journal Information:
Journal Volume: 121; Journal Issue: 47; Journal ID: ISSN 1932-7447
Publisher:
American Chemical Society
Research Org:
Northwestern Univ., Evanston, IL (United States). Argonne-Northwestern Solar Energy Research (ANSER)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE
OSTI Identifier:
1413217

Gélvez-Rueda, María C., Hutter, Eline M., Cao, Duyen H., Renaud, Nicolas, Stoumpos, Constantinos C., Hupp, Joseph T., Savenije, Tom J., Kanatzidis, Mercouri G., and Grozema, Ferdinand C.. Interconversion between Free Charges and Bound Excitons in 2D Hybrid Lead Halide Perovskites. United States: N. p., Web. doi:10.1021/acs.jpcc.7b10705.
Gélvez-Rueda, María C., Hutter, Eline M., Cao, Duyen H., Renaud, Nicolas, Stoumpos, Constantinos C., Hupp, Joseph T., Savenije, Tom J., Kanatzidis, Mercouri G., & Grozema, Ferdinand C.. Interconversion between Free Charges and Bound Excitons in 2D Hybrid Lead Halide Perovskites. United States. doi:10.1021/acs.jpcc.7b10705.
Gélvez-Rueda, María C., Hutter, Eline M., Cao, Duyen H., Renaud, Nicolas, Stoumpos, Constantinos C., Hupp, Joseph T., Savenije, Tom J., Kanatzidis, Mercouri G., and Grozema, Ferdinand C.. 2017. "Interconversion between Free Charges and Bound Excitons in 2D Hybrid Lead Halide Perovskites". United States. doi:10.1021/acs.jpcc.7b10705. https://www.osti.gov/servlets/purl/1413217.
@article{osti_1413217,
title = {Interconversion between Free Charges and Bound Excitons in 2D Hybrid Lead Halide Perovskites},
author = {Gélvez-Rueda, María C. and Hutter, Eline M. and Cao, Duyen H. and Renaud, Nicolas and Stoumpos, Constantinos C. and Hupp, Joseph T. and Savenije, Tom J. and Kanatzidis, Mercouri G. and Grozema, Ferdinand C.},
abstractNote = {The optoelectronic properties of hybrid perovskites can be easily tailored by varying their components. Specifically, mixing the common short organic cation (methylammonium (MA)) with a larger one (e.g., butyl ammonium (BA)) results in 2-dimensional perovskites with varying thicknesses of inorganic layers separated by the large organic cation. In both of these applications, a detailed understanding of the dissociation and recombination of electron–hole pairs is of prime importance. Here in this work, we give a clear experimental demonstration of the interconversion between bound excitons and free charges as a function of temperature by combining microwave conductivity techniques with photoluminescence measurements. We demonstrate that the exciton binding energy varies strongly (between 80 and 370 meV) with the thickness of the inorganic layers. Additionally, we show that the mobility of charges increases with the layer thickness, in agreement with calculated effective masses from electronic structure calculations.},
doi = {10.1021/acs.jpcc.7b10705},
journal = {Journal of Physical Chemistry. C},
number = 47,
volume = 121,
place = {United States},
year = {2017},
month = {11}
}