Ruddlesden-Popper Halide Perovskites Research Articles

Rapid Decoherence Suppresses Charge Recombination in Multi-Layer 2D Halide Perovskites: Time-Domain Ab Initio Analysis.

Two-dimensional (2D) Ruddlesden-Popper halide perovskites are appealing candidates for optoelectronics and photovoltaics. Nonradiative electron-hole recombination constitutes a major pathway for charge and energy losses in these materials. Surprisingly, experimental recombination is slower in multilayers than a monolayer, even though multilayer systems have smaller energy gaps and higher frequency phonons that should accelerate the recombination. Focusing on (BA)2(MA) n-1Pb nI3 n+1 with n = 1 and 3, BA = CH3(CH2)3NH3, and MA = CH3NH3, we show that it is the enhancement of elastic electron-phonon scattering that suppresses charge recombination for n = 3, by causing rapid loss of electronic coherence. The scattering is enhanced in the multilayer 2D perovskites because, in contrast to the monolayer, they contain MA cations embedded into the inorganic Pb-I lattice. Although MAs do not contribute directly to electron and hole wave functions, they perturb the Pb-I lattice and create strong electric fields that interact with the charges. The rapid loss of coherence explains long excited state lifetimes that extend into nanoseconds. Both electron-hole recombination and coherence times show excellent agreement with the corresponding lifetime and line width measurements. The simulations rationalize the observed dependence of excited state lifetime in 2D layered halide perovskites on layer thickness and advance our understanding of the atomistic mechanisms underlying charge-phonon dynamics in nanoscale materials.

Role of alkyl chain length in diaminoalkane linked 2D Ruddlesden–Popper halide perovskites

A new series of 2D Ruddlesden–Popper halide perovskites with diaminoalkane as a bulky spacer with a compositional formula of (NH3(CH2)xNH3)(CH3NH3)2Pb3I10.

Ruddlesden-Popper Perovskite Solar Cells

Ruddlesden-Popper halide perovskites are now viewed as a promising avenue in perovskite solar cells in terms of both stability and high power-conversion efficiencies. We provide context to the efforts of Kanatzidis and coworkers, who, in this issue of Chem, have unveiled promising developments in the higher members of the (CH3(CH2)3NH3)2(CH3NH3)n−1PbnI3n+1 series.

High Members of the 2D Ruddlesden-Popper Halide Perovskites: Synthesis, Optical Properties, and Solar Cells of (CH3(CH2)3NH3)2(CH3NH3)4Pb5I16

Here, we present the fifth member (n = 5) of the Ruddlesden-Popper (CH3(CH2)3NH3)2(CH3NH3)n−1PbnI3n+1 family, which we successfully synthesized in high yield and purity. Phase purity could be clearly determined from its X-ray powder diffraction patterns, which feature the (0k0) Bragg reflections at low 2θ angles. The obtained pure n = 5 compound was confirmed to be a direct band-gap semiconductor with Eg = 1.83 eV. The direct nature of the band gap is supported by density functional theory calculations. Intense photoluminescence was observed at room temperature at 678 nm arising from the band edge of the material. High-quality thin films can be prepared by the hot-casting method from solutions with a pure-phase compound as a precursor. The planar solar cells fabricated with n = 5 thin films demonstrate excellent power-conversion efficiency of 8.71% with an impressive open-circuit voltage of ∼1 V. Our results point to the use of layered perovskites with higher n numbers and pure chemical composition.