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Formamidinium‐Based Dion‐Jacobson Layered Hybrid Perovskites: Structural Complexity and Optoelectronic Properties
Author(s) -
GélvezRueda María C.,
Ahlawat Paramvir,
Merten Lena,
Jahanbakhshi Farzaneh,
Mladenović Marko,
Hinderhofer Alexander,
Dar M. Ibrahim,
Li Yang,
Dučinskas Algirdas,
Carlsen Brian,
Tress Wolfgang,
Ummadisingu Amita,
Zakeeruddin Shaik M.,
Schreiber Frank,
Hagfeldt Anders,
Rothlisberger Ursula,
Grozema Ferdinand C.,
Milić Jovana V.,
Graetzel Michael
Publication year - 2020
Publication title -
advanced functional materials
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 6.069
H-Index - 322
eISSN - 1616-3028
pISSN - 1616-301X
DOI - 10.1002/adfm.202003428
Subject(s) - formamidinium , perovskite (structure) , materials science , bifunctional , hybrid material , phase (matter) , density functional theory , crystallography , nanotechnology , computational chemistry , chemistry , organic chemistry , catalysis
Abstract Layered hybrid perovskites have emerged as a promising alternative to stabilizing hybrid organic–inorganic perovskite materials, which are predominantly based on Ruddlesden‐Popper structures. Formamidinium (FA)‐based Dion‐Jacobson perovskite analogs are developed that feature bifunctional organic spacers separating the hybrid perovskite slabs by introducing 1,4‐phenylenedimethanammonium (PDMA) organic moieties. While these materials demonstrate competitive performances as compared to other FA‐based low‐dimensional perovskite solar cells, the underlying mechanisms for this behavior remain elusive. Here, the structural complexity and optoelectronic properties of materials featuring (PDMA)FA n –1 Pb n I 3 n +1 ( n = 1–3) formulations are unraveled using a combination of techniques, including X‐ray scattering measurements in conjunction with molecular dynamics simulations and density functional theory calculations. While theoretical calculations suggest that layered Dion‐Jacobson perovskite structures are more prominent with the increasing number of inorganic layers ( n ), this is accompanied with an increase in formation energies that render n > 2 compositions difficult to obtain, in accordance with the experimental evidence. Moreover, the underlying intermolecular interactions and their templating effects on the Dion‐Jacobson structure are elucidated, defining the optoelectronic properties. Consequently, despite the challenge to obtain phase‐pure n > 1 compositions, time‐resolved microwave conductivity measurements reveal high photoconductivities and long charge carrier lifetimes. This comprehensive analysis thereby reveals critical features for advancing layered hybrid perovskite optoelectronics.