TY - JOUR
T1 - Intrinsic Formamidinium Tin Iodide Nanocrystals by Suppressing the Sn(IV) Impurities
AU - Dirin, Dmitry N.
AU - Vivani, Anna
AU - Zacharias, Marios
AU - Sekh, Taras V.
AU - Cherniukh, Ihor
AU - Yakunin, Sergii
AU - Bertolotti, Federica
AU - Aebli, Marcel
AU - Schaller, Richard D.
AU - Wieczorek, Alexander
AU - Siol, Sebastian
AU - Cancellieri, Claudia
AU - Jeurgens, Lars P.H.
AU - Masciocchi, Norberto
AU - Guagliardi, Antonietta
AU - Pedesseau, Laurent
AU - Even, Jacky
AU - Kovalenko, Maksym V.
AU - Bodnarchuk, Maryna I.
N1 - Funding Information:
This project was supported by the European Union’s Horizon 2020 research and innovation program under grant agreement No 862656 (project DROP-IT). This work was partially funded by the Swiss National Science Foundation (grant number 200021_192308, project Q-Light), the European Union through Horizon 2020 Research and Innovation Program (ERC CoG Grant, grant agreement number 819740, project SCALE-HALO), and MIUR (PRIN-2017L8WW48, Project HY-TEC). We acknowledge financial support from the Swiss National Science Foundation (R’Equip program, Proposal 206021_182987). A.W. acknowledges funding from the Strategic Focus Area–Advanced Manufacturing (SFA-AM) through the project Advancing manufacturability of hybrid organic–inorganic semiconductors for large area optoelectronics (AMYS). This work was performed, in part, at the Center for Nanoscale Materials, a U.S. Department of Energy Office of Science User Facility, and supported by the U.S. Department of Energy, Office of Science, under Contract No. DE-AC02-06CH11357. The authors acknowledge the support of the Electron Microscopy center at Empa, and scientific and technical staff of the MS-X04A beamline of the Swiss Light Source at Paul Scherrer Insitut (Villigen, CH). We acknowledge that the calculations of this research have been performed using the DECI resource Prometheus at CYFRONET in Poland ( https://www.cyfronet.pl/ ) with support from the PRACE aisbl. The authors thank Dr. Martin Kotyrba for the help with the distillation in an ultrahigh vacuum and Prof. Christophe Coperet for providing Mashima’s reagent.
Funding Information:
This project was supported by the European Union’s Horizon 2020 research and innovation program under grant agreement No 862656 (project DROP-IT). This work was partially funded by the Swiss National Science Foundation (grant number 200021_192308, project Q-Light), the European Union through Horizon 2020 Research and Innovation Program (ERC CoG Grant, grant agreement number 819740, project SCALE-HALO), and MIUR (PRIN-2017L8WW48, Project HY-TEC). We acknowledge financial support from the Swiss National Science Foundation (R’Equip program, Proposal 206021_182987). A.W. acknowledges funding from the Strategic Focus Area-Advanced Manufacturing (SFA-AM) through the project Advancing manufacturability of hybrid organic-inorganic semiconductors for large area optoelectronics (AMYS). This work was performed, in part, at the Center for Nanoscale Materials, a U.S. Department of Energy Office of Science User Facility, and supported by the U.S. Department of Energy, Office of Science, under Contract No. DE-AC02-06CH11357. The authors acknowledge the support of the Electron Microscopy center at Empa, and scientific and technical staff of the MS-X04A beamline of the Swiss Light Source at Paul Scherrer Insitut (Villigen, CH). We acknowledge that the calculations of this research have been performed using the DECI resource Prometheus at CYFRONET in Poland (https://www.cyfronet.pl/) with support from the PRACE aisbl. The authors thank Dr. Martin Kotyrba for the help with the distillation in an ultrahigh vacuum and Prof. Christophe Coperet for providing Mashima’s reagent.
Publisher Copyright:
© 2023 The Authors. Published by American Chemical Society.
PY - 2023/3/8
Y1 - 2023/3/8
N2 - The long search for nontoxic 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) analogues, despite their tendency toward 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 to probe their intrinsic structural and optical properties. Intrinsic FASnI3 NCs exhibit unusually low absorption coefficients of 4 × 103 cm-1 at the first excitonic transition, a 190 meV increase of the band gap 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.
AB - The long search for nontoxic 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) analogues, despite their tendency toward 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 to probe their intrinsic structural and optical properties. Intrinsic FASnI3 NCs exhibit unusually low absorption coefficients of 4 × 103 cm-1 at the first excitonic transition, a 190 meV increase of the band gap 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.
KW - halide perovskite
KW - lead-free
KW - nanocrystals
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U2 - 10.1021/acs.nanolett.2c04927
DO - 10.1021/acs.nanolett.2c04927
M3 - Article
C2 - 36852730
AN - SCOPUS:85149129885
SN - 1530-6984
VL - 23
SP - 1914
EP - 1923
JO - Nano letters
JF - Nano letters
IS - 5
ER -
