Formamidinium‐Based Dion‐Jacobson Layered Hybrid Perovskites: Structural Complexity and Optoelectronic Properties. (19th July 2020)

• Record Type: Journal Article
• Authors: Gélvez‐Rueda, 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
• Is Part Of: Advanced functional materials. Volume 30:Number 38(2020)
• Page Start: n/a
• Page End: n/a
• Publication Date: 2020-07-19
• Subjects: 2D perovskites -- Dion‐Jacobson structures -- layered hybrid perovskites -- perovskite solar cells -- photoconductivity; Materials -- Periodicals; Chemical vapor deposition -- Periodicals; 620.11
• DOI: 10.1002/adfm.202003428
• Languages: English
• ISSNs: 1616-301X

Abstract

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 I3 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. Abstract : Layered hybrid perovskites based on (PDMA)FA n –1 Pb n I3 n +1 ( n = 1–3; PDMA = 1, 4‐phenylenedimethanammonium) compositions are investigated by using combination of techniques, including X‐ray scattering measurements, molecular dynamics simulations, and density functional theory calculations, along with time‐resolved microwave conductivity measurements, to unravel unique structural and photophysical properties relevant to optoelectronic applications.