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Title: Rationalizing the light-induced phase separation of mixed halide organic–inorganic perovskites

Mixed halide hybrid perovskites, CH 3NH 3Pb(I 1-xBrx) 3' represent good candidates for lowcost, high efficiency photovoltaic, and light-emitting devices. Their band gaps can be tuned from 1.6 to 2.3 eV, by changing the halide anion identity. Unfortunately, mixed halide perovskites undergo phase separation under illumination. This leads to iodide- and bromide-rich domains along with corresponding changes to the material’s optical/electrical response. Here, using combined spectroscopic measurements and theoretical modeling, we quantitatively rationalize all microscopic processes that occur during phase separation. Our model suggests that the driving force behind phase separation is the bandgap reduction of iodiderich phases. It additionally explains observed non-linear intensity dependencies, as well as self-limited growth of iodide-rich domains. Most importantly, our model reveals that mixed halide perovskites can be stabilized against phase separation by deliberately engineering carrier diffusion lengths and injected carrier densities.
Authors:
 [1] ;  [1] ;  [1] ;  [1] ;  [1] ;  [1] ;  [1] ;  [1] ;  [1]
  1. Univ. of Notre Dame, IN (United States)
Publication Date:
Grant/Contract Number:
SC0014334
Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 8; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Research Org:
Univ. of Notre Dame, IN (United States)
Sponsoring Org:
USDOE
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE
OSTI Identifier:
1425742

Draguta, Sergiu, Sharia, Onise, Yoon, Seog Joon, Brennan, Michael C., Morozov, Yurii V., Manser, Joseph S., Kamat, Prashant V., Schneider, William F., and Kuno, Masaru. Rationalizing the light-induced phase separation of mixed halide organic–inorganic perovskites. United States: N. p., Web. doi:10.1038/s41467-017-00284-2.
Draguta, Sergiu, Sharia, Onise, Yoon, Seog Joon, Brennan, Michael C., Morozov, Yurii V., Manser, Joseph S., Kamat, Prashant V., Schneider, William F., & Kuno, Masaru. Rationalizing the light-induced phase separation of mixed halide organic–inorganic perovskites. United States. doi:10.1038/s41467-017-00284-2.
Draguta, Sergiu, Sharia, Onise, Yoon, Seog Joon, Brennan, Michael C., Morozov, Yurii V., Manser, Joseph S., Kamat, Prashant V., Schneider, William F., and Kuno, Masaru. 2017. "Rationalizing the light-induced phase separation of mixed halide organic–inorganic perovskites". United States. doi:10.1038/s41467-017-00284-2. https://www.osti.gov/servlets/purl/1425742.
@article{osti_1425742,
title = {Rationalizing the light-induced phase separation of mixed halide organic–inorganic perovskites},
author = {Draguta, Sergiu and Sharia, Onise and Yoon, Seog Joon and Brennan, Michael C. and Morozov, Yurii V. and Manser, Joseph S. and Kamat, Prashant V. and Schneider, William F. and Kuno, Masaru},
abstractNote = {Mixed halide hybrid perovskites, CH3NH3Pb(I1-xBrx)3' represent good candidates for lowcost, high efficiency photovoltaic, and light-emitting devices. Their band gaps can be tuned from 1.6 to 2.3 eV, by changing the halide anion identity. Unfortunately, mixed halide perovskites undergo phase separation under illumination. This leads to iodide- and bromide-rich domains along with corresponding changes to the material’s optical/electrical response. Here, using combined spectroscopic measurements and theoretical modeling, we quantitatively rationalize all microscopic processes that occur during phase separation. Our model suggests that the driving force behind phase separation is the bandgap reduction of iodiderich phases. It additionally explains observed non-linear intensity dependencies, as well as self-limited growth of iodide-rich domains. Most importantly, our model reveals that mixed halide perovskites can be stabilized against phase separation by deliberately engineering carrier diffusion lengths and injected carrier densities.},
doi = {10.1038/s41467-017-00284-2},
journal = {Nature Communications},
number = 1,
volume = 8,
place = {United States},
year = {2017},
month = {8}
}

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