TY - JOUR
T1 - Suppression of phase transitions and glass phase signatures in mixed cation halide perovskites
AU - Simenas, Mantas
AU - Balciunas, Sergejus
AU - Wilson, Jacob N.
AU - Svirskas, Sarunas
AU - Kinka, Martynas
AU - Garbaras, Andrius
AU - Kalendra, Vidmantas
AU - Gagor, Anna
AU - Szewczyk, Daria
AU - Sieradzki, Adam
AU - Maczka, Miroslaw
AU - Samulionis, Vytautas
AU - Walsh, Aron
AU - Grigalaitis, Robertas
AU - Banys, Juras
N1 - Funding Information:
This project has been funded by the Research Council of Lithuania (LMTLT) (agreement No. S-MIP-19-4) and by EPSRC (Grant No. EP/K016288/1). AW is supported by a Royal Society University Research Fellowship and J.N.W. acknowledges useful discussions with Jarvist Frost on the Starrynight code. We are grateful to the UK Materials and Molecular Modelling Hub for computational resources, which is partially funded by EPSRC (EP/ P020194/1).
Publisher Copyright:
© 2020, The Author(s).
PY - 2020/12/1
Y1 - 2020/12/1
N2 - 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.
AB - 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.
UR - http://www.scopus.com/inward/record.url?scp=85092269584&partnerID=8YFLogxK
U2 - 10.1038/s41467-020-18938-z
DO - 10.1038/s41467-020-18938-z
M3 - Article
C2 - 33037192
AN - SCOPUS:85092269584
SN - 2041-1723
VL - 11
JO - Nature Communications
JF - Nature Communications
IS - 1
M1 - 5103
ER -