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Title: Environmental Gating and Galvanic Effects in Single Crystals of Organic–Inorganic Halide Perovskites

Abstract

Understanding the impact of environmental gaseous on the surface of organometal halide perovskites (OMHPs) couples to the electronic and ionic transport is critically important. Here, we explore the transport behavior and origins of the gas sensitivity in MAPbBr 3 single crystals (SCs) devices using impedance spectroscopy and current relaxation measurements. Strong resistive response occurs when crystals are exposed to different environments. It was shown that SC response to the environment is extremely different at the surface as compared to the bulk due to the disorder surface chemistry. The nonlinear transport properties studied using ultrafast Kelvin probe force microscopy (G-KPFM) to unravel spatio-temporal charge dynamics at SC/electrode interface. The relaxation processes observed in pulse relaxation and G-KPFM measurements along with gas sensitivity of crystals suggest the presence of a triple-phase boundary between environment, electrode, and crystal. Results indicate that the environment is a nontrivial component in the operation of OMHP devices which is reminiscent of fuel cell systems. Furthermore, the triple-phase boundary can play a significant role in the transport properties of OMHPs due to the possibility of the redox processes coupled to the concentration of bulk ionic species. Finally, although instrumental for understanding the device characteristics of perovskites, our studiesmore » suggest a new opportunity of coupling the redox chemistry of the Br 2–Br pair that defines the bulk ionic conductivity of MAPbBr 3 with the redox chemistry of gaseous (or liquid) environment via a suitable electrocatalytic system to enable new class of energy storage devices and gas sensors.« less

Authors:
 [1]; ORCiD logo [2]; ORCiD logo [2]; ORCiD logo [2];  [2]; ORCiD logo [2];  [1];  [1];  [1]; ORCiD logo [2]; ORCiD logo [2]; ORCiD logo [1]; ORCiD logo [2]
  1. Univ. of Tennessee, Knoxville, TN (United States)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1546517
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
ACS Applied Materials and Interfaces
Additional Journal Information:
Journal Volume: 11; Journal Issue: 16; Journal ID: ISSN 1944-8244
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English

Citation Formats

Ahmadi, Mahshid, Muckley, Eric S., Ivanov, Ilia N., Lorenz, Matthias, Li, Xin, Ovchinnikova, Olga, Lukosi, Eric D., Tisdale, Jeremy T., Blount, Ethan, Kravchenko, Ivan I., Kalinin, Sergei V., Hu, Bin, and Collins, Liam. Environmental Gating and Galvanic Effects in Single Crystals of Organic–Inorganic Halide Perovskites. United States: N. p., 2019. Web. doi:10.1021/acsami.8b21112.
Ahmadi, Mahshid, Muckley, Eric S., Ivanov, Ilia N., Lorenz, Matthias, Li, Xin, Ovchinnikova, Olga, Lukosi, Eric D., Tisdale, Jeremy T., Blount, Ethan, Kravchenko, Ivan I., Kalinin, Sergei V., Hu, Bin, & Collins, Liam. Environmental Gating and Galvanic Effects in Single Crystals of Organic–Inorganic Halide Perovskites. United States. doi:10.1021/acsami.8b21112.
Ahmadi, Mahshid, Muckley, Eric S., Ivanov, Ilia N., Lorenz, Matthias, Li, Xin, Ovchinnikova, Olga, Lukosi, Eric D., Tisdale, Jeremy T., Blount, Ethan, Kravchenko, Ivan I., Kalinin, Sergei V., Hu, Bin, and Collins, Liam. Tue . "Environmental Gating and Galvanic Effects in Single Crystals of Organic–Inorganic Halide Perovskites". United States. doi:10.1021/acsami.8b21112.
@article{osti_1546517,
title = {Environmental Gating and Galvanic Effects in Single Crystals of Organic–Inorganic Halide Perovskites},
author = {Ahmadi, Mahshid and Muckley, Eric S. and Ivanov, Ilia N. and Lorenz, Matthias and Li, Xin and Ovchinnikova, Olga and Lukosi, Eric D. and Tisdale, Jeremy T. and Blount, Ethan and Kravchenko, Ivan I. and Kalinin, Sergei V. and Hu, Bin and Collins, Liam},
abstractNote = {Understanding the impact of environmental gaseous on the surface of organometal halide perovskites (OMHPs) couples to the electronic and ionic transport is critically important. Here, we explore the transport behavior and origins of the gas sensitivity in MAPbBr3 single crystals (SCs) devices using impedance spectroscopy and current relaxation measurements. Strong resistive response occurs when crystals are exposed to different environments. It was shown that SC response to the environment is extremely different at the surface as compared to the bulk due to the disorder surface chemistry. The nonlinear transport properties studied using ultrafast Kelvin probe force microscopy (G-KPFM) to unravel spatio-temporal charge dynamics at SC/electrode interface. The relaxation processes observed in pulse relaxation and G-KPFM measurements along with gas sensitivity of crystals suggest the presence of a triple-phase boundary between environment, electrode, and crystal. Results indicate that the environment is a nontrivial component in the operation of OMHP devices which is reminiscent of fuel cell systems. Furthermore, the triple-phase boundary can play a significant role in the transport properties of OMHPs due to the possibility of the redox processes coupled to the concentration of bulk ionic species. Finally, although instrumental for understanding the device characteristics of perovskites, our studies suggest a new opportunity of coupling the redox chemistry of the Br2–Br– pair that defines the bulk ionic conductivity of MAPbBr3 with the redox chemistry of gaseous (or liquid) environment via a suitable electrocatalytic system to enable new class of energy storage devices and gas sensors.},
doi = {10.1021/acsami.8b21112},
journal = {ACS Applied Materials and Interfaces},
number = 16,
volume = 11,
place = {United States},
year = {2019},
month = {4}
}

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This content will become publicly available on April 2, 2020
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