TY - JOUR
T1 - Inorganic frameworks of low-dimensional perovskites dictate the performance and stability of mixed-dimensional perovskite solar cells
AU - Febriansyah, Benny
AU - Li, Yongxin
AU - Giovanni, David
AU - Salim, Teddy
AU - Hooper, Thomas J.N.
AU - Sim, Ying
AU - Ma, Daphne
AU - Laxmi, Shoba
AU - Lekina, Yulia
AU - Koh, Teck Ming
AU - Shen, Ze Xiang
AU - Pullarkat, Sumod A.
AU - Sum, Tze Chien
AU - Mhaisalkar, Subodh G.
AU - Ager, Joel W.
AU - Mathews, Nripan
N1 - Publisher Copyright:
© 2023 The Royal Society of Chemistry.
PY - 2022/11/1
Y1 - 2022/11/1
N2 - Mixed-dimensional perovskites containing mixtures of organic cations hold great promise to deliver highly stable and efficient solar cells. However, although a plethora of relatively bulky organic cations have been reported for such purposes, a fundamental understanding of the materials' structure, composition, and phase, along with their correlated effects on the corresponding optoelectronic properties and degradation mechanism remains elusive. Herein, we systematically engineer the structures of bulky organic cations to template low-dimensional perovskites with contrasting inorganic framework dimensionality, connectivity, and coordination deformation. By combining X-ray single-crystal structural analysis with depth-profiling XPS, solid-state NMR, and femtosecond transient absorption, it is revealed that not all low-dimensional species work equally well as dopants. Instead, it was found that inorganic architectures with lesser structural distortion tend to yield less disordered energetic and defect landscapes in the resulting mixed-dimensional perovskites, augmented in materials with a longer photoluminescence (PL) lifetime, higher PL quantum yield (up to 11%), improved solar cell performance and enhanced thermal stability (T80 up to 1000 h, unencapsulated). Our study highlights the importance of designing templating organic cations that yield low-dimensional materials with much less structural distortion profiles to be used as additives in stable and efficient perovskite solar cells.
AB - Mixed-dimensional perovskites containing mixtures of organic cations hold great promise to deliver highly stable and efficient solar cells. However, although a plethora of relatively bulky organic cations have been reported for such purposes, a fundamental understanding of the materials' structure, composition, and phase, along with their correlated effects on the corresponding optoelectronic properties and degradation mechanism remains elusive. Herein, we systematically engineer the structures of bulky organic cations to template low-dimensional perovskites with contrasting inorganic framework dimensionality, connectivity, and coordination deformation. By combining X-ray single-crystal structural analysis with depth-profiling XPS, solid-state NMR, and femtosecond transient absorption, it is revealed that not all low-dimensional species work equally well as dopants. Instead, it was found that inorganic architectures with lesser structural distortion tend to yield less disordered energetic and defect landscapes in the resulting mixed-dimensional perovskites, augmented in materials with a longer photoluminescence (PL) lifetime, higher PL quantum yield (up to 11%), improved solar cell performance and enhanced thermal stability (T80 up to 1000 h, unencapsulated). Our study highlights the importance of designing templating organic cations that yield low-dimensional materials with much less structural distortion profiles to be used as additives in stable and efficient perovskite solar cells.
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U2 - 10.1039/d2mh00868h
DO - 10.1039/d2mh00868h
M3 - Article
C2 - 36426759
AN - SCOPUS:85143528110
SN - 2051-6347
VL - 10
SP - 536
EP - 546
JO - Materials Horizons
JF - Materials Horizons
IS - 2
ER -