The Doping Mechanism of Halide Perovskite Unveiled by Alkaline Earth Metals

Phung, Nga; Félix, Roberto; Meggiolaro, Daniele; Al-Ashouri, Amran; Sousa e Silva, Gabrielle; Hartmann, Claudia; Hidalgo, Juanita; Köbler, Hans; Mosconi, Edoardo; Lai, Barry; Gunder, Rene; Li, Meng; Wang, Kai-Li; Wang, Zhao-Kui; Nie, Kaiqi; Handick, Evelyn; Wilks, Regan G.; Marquez, Jose A.; Rech, Bernd; Unold, Thomas; Correa-Baena, Juan-Pablo; Albrecht, Steve; De Angelis, Filippo; Bär, Marcus; Abate, Antonio

doi:10.1021/jacs.9b11637

Title: The Doping Mechanism of Halide Perovskite Unveiled by Alkaline Earth Metals

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Abstract

Halide perovskites are a potential candidate for the next generation of photovoltaics. Chemical doping of halide perovskites is an established strategy to prepare the highest efficiency and most stable perovskite-based solar cells. Here, we unveil the doping mechanism of halide perovskites using a series of alkaline earth metals. We find that low doping levels enable the incorporation of the dopant within the perovskite lattice, whereas high doping concentrations induce surface segregation. The threshold from low to high doping regime correlates to the size of the doping element. We show that the low doping regime results in a more n-type material, while the high doping regime induces a less n-type doping character. Our work offers a comprehensive picture of the unique doping mechanism of halide perovskites, which differs from classical semiconductors. We proved the effectiveness of the low doping regime for the first time, demonstrating highly efficient methylammonium lead iodide based solar cells in both n-i-p and p-i-n architectures.

Authors:

^[1];

^[2];

^[1]; Sousa e Silva, Gabrielle ^[1];

^[1]; Hidalgo, Juanita ^[3]; Köbler, Hans ^[1]; Mosconi, Edoardo ^[2]; Lai, Barry ^[4]; Gunder, Rene ^[1]; Li, Meng ^[5]; Wang, Kai-Li ^[6];

^[7]; Nie, Kaiqi ^[8];

^[1]; Wilks, Regan G. ^[1];

^[1]; Rech, Bernd ^[9];

^[1] more »

Helmholtz-Zentrum Berlin (HZB), (Germany). German Research Centre for Materials and Energy
National Research Council-Inst. of Molecular Science and Technologies (CNR-ISTM), Perugia (Italy). Computational Lab. for Hybrid/Organic Photovoltaics (CLHYO); Istituto Italiano di Tecnologia (IIT), Genova (Italy)
Georgia Inst. of Technology, Atlanta, GA (United States)
Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
Helmholtz-Zentrum Berlin (HZB), (Germany). German Research Centre for Materials and Energy; Soochow Univ., Suzhou (China). Jiangsu Key Lab. for Carbon-Based Functional Materials & Devices and Lab. of Advanced Optoelectronic Materials
Soochow Univ., Suzhou (China). Jiangsu Key Lab. for Carbon-Based Functional Materials & Devices
Institute of Functional Nano & Soft Materials (FUNSOM), Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices, Joint International Research Laboratory of Carbon-Based Functional Materials and Devices, Soochow University, Suzhou 215123, PR China
Helmholtz-Zentrum Berlin (HZB), (Germany). German Research Centre for Materials and Energy; Soochow Univ., Suzhou (China). Jiangsu Key Lab. for Carbon-Based Functional Materials & Devices
Helmholtz-Zentrum Berlin (HZB), (Germany). German Research Centre for Materials and Energy; Technical Univ. of Berlin (Germany)
National Research Council-Inst. of Molecular Science and Technologies (CNR-ISTM), Perugia (Italy). Computational Lab. for Hybrid/Organic Photovoltaics (CLHYO); Istituto Italiano di Tecnologia (IIT), Genova (Italy); Univ. of Perugia (Italy)
Helmholtz-Zentrum Berlin (HZB), (Germany). German Research Centre for Materials and Energy; Univ. of Erlangen-Nuremberg (Germany); Helmholtz Institute Erlangen-Nürnberg for Renewable Energy (HI ERN), Berlin (Germany)
Helmholtz-Zentrum Berlin (HZB), (Germany). German Research Centre for Materials and Energy; Univ. of Naples Federico II (Italy)

Publication Date:: Thu Jan 09 00:00:00 EST 2020

Research Org.:: Argonne National Lab. (ANL), Argonne, IL (United States)

Sponsoring Org.:: European Union - Horizon 2020 Research and Innovation Programme; USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI Identifier:: 1617374

Grant/Contract Number:: AC02-06CH11357

Resource Type:: Accepted Manuscript

Journal Name:: Journal of the American Chemical Society

Additional Journal Information:: Journal Volume: 142; Journal Issue: 5; Journal ID: ISSN 0002-7863

Publisher:: American Chemical Society (ACS)

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats


                    Phung, Nga, Félix, Roberto, Meggiolaro, Daniele, Al-Ashouri, Amran, Sousa e Silva, Gabrielle, Hartmann, Claudia, Hidalgo, Juanita, Köbler, Hans, Mosconi, Edoardo, Lai, Barry, Gunder, Rene, Li, Meng, Wang, Kai-Li, Wang, Zhao-Kui, Nie, Kaiqi, Handick, Evelyn, Wilks, Regan G., Marquez, Jose A., Rech, Bernd, Unold, Thomas, Correa-Baena, Juan-Pablo, Albrecht, Steve, De Angelis, Filippo, Bär, Marcus, and Abate, Antonio. The Doping Mechanism of Halide Perovskite Unveiled by Alkaline Earth Metals.  United States: N. p., 2020. 
Web.  doi:10.1021/jacs.9b11637.

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                    Phung, Nga, Félix, Roberto, Meggiolaro, Daniele, Al-Ashouri, Amran, Sousa e Silva, Gabrielle, Hartmann, Claudia, Hidalgo, Juanita, Köbler, Hans, Mosconi, Edoardo, Lai, Barry, Gunder, Rene, Li, Meng, Wang, Kai-Li, Wang, Zhao-Kui, Nie, Kaiqi, Handick, Evelyn, Wilks, Regan G., Marquez, Jose A., Rech, Bernd, Unold, Thomas, Correa-Baena, Juan-Pablo, Albrecht, Steve, De Angelis, Filippo, Bär, Marcus, & Abate, Antonio. The Doping Mechanism of Halide Perovskite Unveiled by Alkaline Earth Metals.  United States.  https://doi.org/10.1021/jacs.9b11637

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                    Phung, Nga, Félix, Roberto, Meggiolaro, Daniele, Al-Ashouri, Amran, Sousa e Silva, Gabrielle, Hartmann, Claudia, Hidalgo, Juanita, Köbler, Hans, Mosconi, Edoardo, Lai, Barry, Gunder, Rene, Li, Meng, Wang, Kai-Li, Wang, Zhao-Kui, Nie, Kaiqi, Handick, Evelyn, Wilks, Regan G., Marquez, Jose A., Rech, Bernd, Unold, Thomas, Correa-Baena, Juan-Pablo, Albrecht, Steve, De Angelis, Filippo, Bär, Marcus, and Abate, Antonio. Thu .  
"The Doping Mechanism of Halide Perovskite Unveiled by Alkaline Earth Metals".  United States.  https://doi.org/10.1021/jacs.9b11637.  https://www.osti.gov/servlets/purl/1617374.

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@article{osti_1617374,

  title        = {The Doping Mechanism of Halide Perovskite Unveiled by Alkaline Earth Metals},

  author       = {Phung, Nga and Félix, Roberto and Meggiolaro, Daniele and Al-Ashouri, Amran and Sousa e Silva, Gabrielle and Hartmann, Claudia and Hidalgo, Juanita and Köbler, Hans and Mosconi, Edoardo and Lai, Barry and Gunder, Rene and Li, Meng and Wang, Kai-Li and Wang, Zhao-Kui and Nie, Kaiqi and Handick, Evelyn and Wilks, Regan G. and Marquez, Jose A. and Rech, Bernd and Unold, Thomas and Correa-Baena, Juan-Pablo and Albrecht, Steve and De Angelis, Filippo and Bär, Marcus and Abate, Antonio},

  abstractNote = {Halide perovskites are a potential candidate for the next generation of photovoltaics. Chemical doping of halide perovskites is an established strategy to prepare the highest efficiency and most stable perovskite-based solar cells. Here, we unveil the doping mechanism of halide perovskites using a series of alkaline earth metals. We find that low doping levels enable the incorporation of the dopant within the perovskite lattice, whereas high doping concentrations induce surface segregation. The threshold from low to high doping regime correlates to the size of the doping element. We show that the low doping regime results in a more n-type material, while the high doping regime induces a less n-type doping character. Our work offers a comprehensive picture of the unique doping mechanism of halide perovskites, which differs from classical semiconductors. We proved the effectiveness of the low doping regime for the first time, demonstrating highly efficient methylammonium lead iodide based solar cells in both n-i-p and p-i-n architectures.},

  doi          = {10.1021/jacs.9b11637},

  journal      = {Journal of the American Chemical Society},

  number       = 5,

  volume       = 142,

  place        = {United States},

  year         = {Thu Jan 09 00:00:00 EST 2020},

  month        = {Thu Jan 09 00:00:00 EST 2020}

}

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