TY - JOUR
T1 - Formamidinium-Based Dion-Jacobson Layered Hybrid Perovskites
T2 - Structural Complexity and Optoelectronic Properties
AU - Gélvez-Rueda, María C.
AU - Ahlawat, Paramvir
AU - Merten, Lena
AU - Jahanbakhshi, Farzaneh
AU - Mladenović, Marko
AU - Hinderhofer, Alexander
AU - Dar, M. Ibrahim
AU - Li, Yang
AU - Grozema, Ferdinand C.
AU - More Authors, null
N1 - Accepted Author Manuscript
PY - 2020
Y1 - 2020
N2 - 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)FAn–1PbnI3n+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.
AB - 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)FAn–1PbnI3n+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.
KW - 2D perovskites
KW - Dion-Jacobson structures
KW - layered hybrid perovskites
KW - perovskite solar cells
KW - photoconductivity
UR - http://www.scopus.com/inward/record.url?scp=85088153930&partnerID=8YFLogxK
U2 - 10.1002/adfm.202003428
DO - 10.1002/adfm.202003428
M3 - Article
AN - SCOPUS:85088153930
SN - 1616-301X
VL - 30
JO - Advanced Functional Materials
JF - Advanced Functional Materials
IS - 38
M1 - 2003428
ER -