Intrinsic Formamidinium Tin Iodide Nanocrystals by Suppressing the Sn(IV) Impurities

Dirin, Dmitry N.; Vivani, Anna; Zacharias, Marios; Sekh, Taras V.; Cherniukh, Ihor; Yakunin, Sergii; Bertolotti, Federica; Aebli, Marcel; Schaller, Richard D.; Wieczorek, Alexander; Siol, Sebastian; Cancellieri, Claudia; Jeurgens, Lars P. H.; Masciocchi, Norberto; Guagliardi, Antonietta; Pedesseau, Laurent; Even, Jacky; Kovalenko, Maksym V.; Bodnarchuk, Maryna I.

doi:10.1021/acs.nanolett.2c04927

Title: Intrinsic Formamidinium Tin Iodide Nanocrystals by Suppressing the Sn(IV) Impurities

Abstract

The long search for non-toxic alternatives to lead halide perovskites (LHPs) has shown that some compelling properties of LHPs, such as low effective masses of carriers, can only be attained in their closest Sn(II) and Ge(II) analogs, despite their tendency to oxidation. Judicious choice of chemistry allowed formamidinium tin iodide (FASnI₃) to reach a power conversion efficiency of 14.81% in photovoltaic devices. This progress motivated us to develop a synthesis of colloidal FASnI₃ NCs with a concentration of Sn(IV) reduced to an insignificant level and probe their intrinsic structural and optical properties. Intrinsic FASnI₃ NCs exhibit unusually low absorption coefficients of 4 x 10³ cm^-1 at the first excitonic transition, a 190 meV increase of the bandgap as compared to the bulk material, and a lack of excitonic resonances. These features are attributed to a highly disordered lattice, distinct from the bulk FASnI₃ as supported by structural characterizations and first-principles calculations.

Authors:

^[1]; Vivani, Anna ^[2]; Zacharias, Marios ^[3]; Sekh, Taras V. ^[1]; Cherniukh, Ihor ^[1];

^[1];

^[2]; Aebli, Marcel ^[1];

^[4];

^[5];

^[2];

^[6];

^[3];

^[1];

^[1]

Eidgenoessische Technische Hochschule (ETH), Zurich (Switzerland); Swiss Federal Laboratories for Materials Science and Technology (Empa), Dübendorf (Switzerland)
Università dell’Insubria, Como (Italy)
Univ. of Rennes (France); Centre National de la Recherche Scientifique (CNRS) (France). Institut FOTON
Argonne National Laboratory (ANL), Argonne, IL (United States). Center for Nanoscale Materials; Northwestern Univ., Evanston, IL (United States)
Swiss Federal Laboratories for Materials Science and Technology (Empa), Dübendorf (Switzerland)
National Research Council (CNR), Como (Italy). Istituto di Cristallografia and Total Scattering Laboratory (To.Sca.Lab)

Publication Date:: Tue Feb 28 00:00:00 EST 2023

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

Sponsoring Org.:: USDOE Office of Science (SC); European Union (EU); Swiss National Science Foundation (SNSF)

OSTI Identifier:: 1999518

Grant/Contract Number:: AC02-06CH11357; 862656; 200021_192308; 819740

Resource Type:: Accepted Manuscript

Journal Name:: Nano Letters

Additional Journal Information:: Journal Volume: 23; Journal Issue: 5; Journal ID: ISSN 1530-6984

Publisher:: American Chemical Society

Country of Publication:: United States

Language:: English

Subject:: 77 NANOSCIENCE AND NANOTECHNOLOGY; halide perovskite; lead-free; nanocrystals

Citation Formats


                    Dirin, Dmitry N., Vivani, Anna, Zacharias, Marios, Sekh, Taras V., Cherniukh, Ihor, Yakunin, Sergii, Bertolotti, Federica, Aebli, Marcel, Schaller, Richard D., Wieczorek, Alexander, Siol, Sebastian, Cancellieri, Claudia, Jeurgens, Lars P. H., Masciocchi, Norberto, Guagliardi, Antonietta, Pedesseau, Laurent, Even, Jacky, Kovalenko, Maksym V., and Bodnarchuk, Maryna I. Intrinsic Formamidinium Tin Iodide Nanocrystals by Suppressing the Sn(IV) Impurities.  United States: N. p., 2023. 
Web.  doi:10.1021/acs.nanolett.2c04927.

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                    Dirin, Dmitry N., Vivani, Anna, Zacharias, Marios, Sekh, Taras V., Cherniukh, Ihor, Yakunin, Sergii, Bertolotti, Federica, Aebli, Marcel, Schaller, Richard D., Wieczorek, Alexander, Siol, Sebastian, Cancellieri, Claudia, Jeurgens, Lars P. H., Masciocchi, Norberto, Guagliardi, Antonietta, Pedesseau, Laurent, Even, Jacky, Kovalenko, Maksym V., & Bodnarchuk, Maryna I. Intrinsic Formamidinium Tin Iodide Nanocrystals by Suppressing the Sn(IV) Impurities.  United States.  https://doi.org/10.1021/acs.nanolett.2c04927

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                    Dirin, Dmitry N., Vivani, Anna, Zacharias, Marios, Sekh, Taras V., Cherniukh, Ihor, Yakunin, Sergii, Bertolotti, Federica, Aebli, Marcel, Schaller, Richard D., Wieczorek, Alexander, Siol, Sebastian, Cancellieri, Claudia, Jeurgens, Lars P. H., Masciocchi, Norberto, Guagliardi, Antonietta, Pedesseau, Laurent, Even, Jacky, Kovalenko, Maksym V., and Bodnarchuk, Maryna I. Tue .  
"Intrinsic Formamidinium Tin Iodide Nanocrystals by Suppressing the Sn(IV) Impurities".  United States.  https://doi.org/10.1021/acs.nanolett.2c04927.  https://www.osti.gov/servlets/purl/1999518.

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@article{osti_1999518,

  title        = {Intrinsic Formamidinium Tin Iodide Nanocrystals by Suppressing the Sn(IV) Impurities},

  author       = {Dirin, Dmitry N. and Vivani, Anna and Zacharias, Marios and Sekh, Taras V. and Cherniukh, Ihor and Yakunin, Sergii and Bertolotti, Federica and Aebli, Marcel and Schaller, Richard D. and Wieczorek, Alexander and Siol, Sebastian and Cancellieri, Claudia and Jeurgens, Lars P. H. and Masciocchi, Norberto and Guagliardi, Antonietta and Pedesseau, Laurent and Even, Jacky and Kovalenko, Maksym V. and Bodnarchuk, Maryna I.},

  abstractNote = {The long search for non-toxic alternatives to lead halide perovskites (LHPs) has shown that some compelling properties of LHPs, such as low effective masses of carriers, can only be attained in their closest Sn(II) and Ge(II) analogs, despite their tendency to oxidation. Judicious choice of chemistry allowed formamidinium tin iodide (FASnI3) to reach a power conversion efficiency of 14.81% in photovoltaic devices. This progress motivated us to develop a synthesis of colloidal FASnI3 NCs with a concentration of Sn(IV) reduced to an insignificant level and probe their intrinsic structural and optical properties. Intrinsic FASnI3 NCs exhibit unusually low absorption coefficients of 4 x 103 cm-1 at the first excitonic transition, a 190 meV increase of the bandgap as compared to the bulk material, and a lack of excitonic resonances. These features are attributed to a highly disordered lattice, distinct from the bulk FASnI3 as supported by structural characterizations and first-principles calculations.},

  doi          = {10.1021/acs.nanolett.2c04927},

  journal      = {Nano Letters},

  number       = 5,

  volume       = 23,

  place        = {United States},

  year         = {Tue Feb 28 00:00:00 EST 2023},

  month        = {Tue Feb 28 00:00:00 EST 2023}

}

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Abstract

Citation Formats

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Perovskite light-emitting diodes with external quantum efficiency exceeding 20 per cent
journal, October 2018

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journal, June 2021

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Ligand-engineered bandgap stability in mixed-halide perovskite LEDs
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journal, August 2018

Chemical tuning of dynamic cation off-centering in the cubic phases of hybrid tin and lead halide perovskites
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journal, August 2018

Electron-hole diffusion lengths > 175 μm in solution-grown CH ₃ NH ₃ PbI ₃ single crystals
journal, January 2015

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journal, February 2016

Identifying defect-tolerant semiconductors with high minority-carrier lifetimes: beyond hybrid lead halide perovskites
journal, May 2015

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journal, August 2018

Concepts for chemical state analysis at constant probing depth by lab‐based XPS/HAXPES combining soft and hard X‐ray sources
journal, April 2020

Perovskite CH ₃ NH ₃ PbI ₃ (Cl) Single Crystals: Rapid Solution Growth, Unparalleled Crystalline Quality, and Low Trap Density toward 10 ⁸ cm ^–3
journal, July 2016

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journal, August 2020

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journal, August 2018

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journal, April 2018

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journal, September 2019

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journal, January 2018

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journal, June 2020

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journal, November 2018

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journal, October 2019

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journal, April 2018

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journal, August 2017

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journal, June 2022

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journal, November 2017

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journal, July 2013

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journal, January 2018

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journal, December 2020

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journal, June 2020

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journal, April 2021

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Stable, High‐Sensitivity and Fast‐Response Photodetectors Based on Lead‐Free Cs ₂ AgBiBr ₆ Double Perovskite Films
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