Mixed Halide Ordering as a Tool for the Stabilization of Ruddlesden–Popper Structures

Ovčar, Juraj; Leung, Tik Lun; Grisanti, Luca; Skoko, Željko; Vrankić, Martina; Low, Kam‐Hung; Wang, Shixun; You, Pei-Ying; Ahn, Hyeyoung; Lončarić, Ivor; Djurišić, Aleksandra B.; Popović, Jasminka

doi:10.1021/acs.chemmater.1c03815

Cited by 10 publications

(22 citation statements)

References 108 publications

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“…The optical measurements indicated that synthesis starting from a one-to-one iodide-bromide stoichiometry results in t-BA 2 PbBr 2 I 2 , a crystallized n = 1 RP phase, while syntheses starting from pure bromide or pure iodide stoichiometries do not yield Q2DP structures. 22 We confirmed the instability of the pure halide Q2DPs by calculating the formation energies of the global minima found with GO-MHALP as well as by XRD measurements.…”

Section: (4amp)pbbrsupporting

confidence: 70%

“…We confirmed that not only the specific halide distribution was correctly predicted by GO-MHALP, but also that the structural details were predicted very precisely. 22 While the accuracy of the classical potential itself can be significantly improved, within our method it is not necessary for it to be extremely precise. We have shown that the sufficient condition for a very accurate prediction is only that the global minimum of the potential is connected to the DFT global minimum by a DFT local relaxation.…”

Section: Discussionmentioning

confidence: 99%

“…E.g., classical potentials for Q2DPs containing iodine instead of bromide can be constructed in a completely analogous manner as described in Section 2.2, but using the parameters for MAPbI 3 . 26,28 As detailed in an another work, 22 we employed GO-MHALP to predict a mixed halide structure. We use the Berthelot rule to calculate the Buckingham parameters for Pb − Pb and Br − I interactions:…”

Section: Potentials For Iodine and Mixed Halide Systemsmentioning

confidence: 99%

“…We used tert-butyl ammonium (t-BA) as the organic spacer. While this is detailed in a separate work, 22 we here deepen the discussion of the application of GO-MHALP to that challenging case. The optical measurements indicated that synthesis starting from a one-to-one iodide-bromide stoichiometry results in t-BA 2 PbBr 2 I 2 , a crystallized n = 1 RP phase, while syntheses starting from pure bromide or pure iodide stoichiometries do not yield Q2DP structures.…”

Section: (4amp)pbbrmentioning

confidence: 99%

“…Aditionally, we have extended the method to predict an unknown Q2DP structure containing mixed-halide perovskite octahedra PbBr 3 I 3 . 22…”

Section: Introductionmentioning

confidence: 99%

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Crystal structure prediction of (quasi-)two-dimensional lead halide perovskites

Ovčar¹,

Grisanti²,

Bruno³

et al. 2022

Preprint

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Two-dimensional lead halide perovskites are promising materials for optoelectronics due to the tunability of their properties with the number of lead halide layers and the choice of an organic spacer. Physical understanding for the rational design of materials primarily requires knowledge of crystal structure. 2D lead halide perovskites are usually prepared in the form of films complicating the experimental determination of structure.To enable theoretical studies of experimentally unresolvable structures as well as highthroughput virtual screening, we present an algorithm for crystal structure prediction of lead halide perovskites. Using automatically prepared classical potential we show that our algorithm enables fast access to a structure that can be used for further firstprinciples studies.

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Section: (4amp)pbbrsupporting

confidence: 70%

Section: Discussionmentioning

confidence: 99%

Section: Potentials For Iodine and Mixed Halide Systemsmentioning

confidence: 99%

Section: (4amp)pbbrmentioning

confidence: 99%

“…Aditionally, we have extended the method to predict an unknown Q2DP structure containing mixed-halide perovskite octahedra PbBr 3 I 3 . 22…”

Section: Introductionmentioning

confidence: 99%

See 3 more Smart Citations

Crystal structure prediction of (quasi-)two-dimensional lead halide perovskites

Ovčar¹,

Grisanti²,

Bruno³

et al. 2022

Preprint

Self Cite

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Homogeneous Phase Distribution in Q‐2D Perovskites via Co‐Assembly of Spacer Cations for Efficient Light‐Emitting Diodes

Guo

Yin

et al. 2023

Advanced Materials

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Quasi‐2D (Q‐2D) perovskites are promising candidates to apply in light‐emitting diodes (LEDs). However, delicate control on crystallization kinetics is needed to suppress severe phase segregation. Here, the crystallization kinetics of Q‐2D perovskites are investigated via in situ absorbance spectroscopy and for the first time find the multiphase distribution is governed by the arrangement, rather than diffusion, of spacer cations at the nucleation stage, which associate with its assembling ability determined by molecular configuration. A “co‐assembly” strategy is conceived by combining co‐cations with different configuration characteristics, where bulky cations disturb the assembling between slender cations and lead–bromide sheet, contributing to homogeneous emitting phase with effective passivation. Correspondingly, in the phenylethylammonium (PEA+)‐based Q‐2D perovskites (<n> = 3), homogeneous phase distribution is achieved by incorporating co‐cation triphenylmethaneammonium (TPMA+), the branching terminals of which suppress cations assembling into low‐n phases and afford adequate cations as passivating ligands. Therefore, the champion external quantum efficiency of the LED device reaches 23.9%, which is among the highest performance of green Q‐2D perovskite LEDs. This work reveals that the arrangement of spacer cations determines the crystallization kinetics in Q‐2D perovskites, providing further guidance on the molecular design and phase modulation of Q‐2D perovskites.

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Molecular Structure Tailoring of Organic Spacers for High-Performance Ruddlesden–Popper Perovskite Solar Cells

Liu,

Li,

Cai

et al. 2024

Nano-Micro Lett.

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Layer-structured Ruddlesden–Popper (RP) perovskites (RPPs) with decent stability have captured the imagination of the photovoltaic research community and bring hope for boosting the development of perovskite solar cell (PSC) technology. However, two-dimensional (2D) or quasi-2D RP PSCs are encountered with some challenges of the large exciton binding energy, blocked charge transport and poor film quality, which restrict their photovoltaic performance. Fortunately, these issues can be readily resolved by rationally designing spacer cations of RPPs. This review mainly focuses on how to design the molecular structures of organic spacers and aims to endow RPPs with outstanding photovoltaic applications. We firstly elucidated the important roles of organic spacers in impacting crystallization kinetics, charge transporting ability and stability of RPPs. Then we brought three aspects to attention for designing organic spacers. Finally, we presented the specific molecular structure design strategies for organic spacers of RPPs aiming to improve photovoltaic performance of RP PSCs. These proposed strategies in this review will provide new avenues to develop novel organic spacers for RPPs and advance the development of RPP photovoltaic technology for future applications.

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Mixed Halide Ordering as a Tool for the Stabilization of Ruddlesden–Popper Structures

Cited by 10 publications

References 108 publications

Crystal structure prediction of (quasi-)two-dimensional lead halide perovskites

Crystal structure prediction of (quasi-)two-dimensional lead halide perovskites

Homogeneous Phase Distribution in Q‐2D Perovskites via Co‐Assembly of Spacer Cations for Efficient Light‐Emitting Diodes

Molecular Structure Tailoring of Organic Spacers for High-Performance Ruddlesden–Popper Perovskite Solar Cells

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