Suppression of phase transitions and glass phase signatures in mixed cation halide perovskites

Mantas Simenas (), Sergejus Balciunas, Jacob N. Wilson, Sarunas Svirskas, Martynas Kinka, Andrius Garbaras, Vidmantas Kalendra, Anna Gagor, Daria Szewczyk, Adam Sieradzki, Miroslaw Maczka, Vytautas Samulionis, Aron Walsh, Robertas Grigalaitis and Juras Banys
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Mantas Simenas: Vilnius University
Sergejus Balciunas: Vilnius University
Jacob N. Wilson: Imperial College London
Sarunas Svirskas: Vilnius University
Martynas Kinka: Vilnius University
Andrius Garbaras: Center for Physical Sciences and Technology
Vidmantas Kalendra: Vilnius University
Anna Gagor: Polish Academy of Sciences
Daria Szewczyk: Polish Academy of Sciences
Adam Sieradzki: Wroclaw University of Science and Technology
Miroslaw Maczka: Polish Academy of Sciences
Vytautas Samulionis: Vilnius University
Aron Walsh: Imperial College London
Robertas Grigalaitis: Vilnius University
Juras Banys: Vilnius University

Nature Communications, 2020, vol. 11, issue 1, 1-9

Abstract: Abstract Cation engineering provides a route to control the structure and properties of hybrid halide perovskites, which has resulted in the highest performance solar cells based on mixtures of Cs, methylammonium, and formamidinium. Here, we present a multi-technique experimental and theoretical study of structural phase transitions, structural phases and dipolar dynamics in the mixed methylammonium/dimethylammonium MA1-xDMAxPbBr3 hybrid perovskites (0 ≤ x ≤ 1). Our results demonstrate a significant suppression of the structural phase transitions, enhanced disorder and stabilization of the cubic phase even for a small amount of dimethylammonium cations. As the dimethylammonium concentration approaches the solubility limit in MAPbBr3, we observe the disappearance of the structural phase transitions and indications of a glassy dipolar phase. We also reveal a significant tunability of the dielectric permittivity upon mixing of the molecular cations that arises from frustrated electric dipoles.

Date: 2020
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DOI: 10.1038/s41467-020-18938-z

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