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Title: Phase Transition Control for High Performance Ruddlesden-Popper Perovskite Solar Cells

Journal Article · · Advanced Materials
 [1];  [2];  [3];  [3]; ORCiD logo [4]; ORCiD logo [4];  [3];  [3];  [5];  [6]; ORCiD logo [4];  [3];  [2];  [1]
  1. Shaanxi Normal Univ., Xi'an (China); Chinese Academy of Sciences, Dalian (China)
  2. King Abdullah Univ. of Science and Technology (KAUST), Thuwal (Saudi Arabia)
  3. Shaanxi Normal Univ., Xi'an (China)
  4. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  5. Cornell Univ., Ithaca, NY (United States). Cornell High Energy Synchrotron Source (CHESS)
  6. Northwestern Univ., Evanston, IL (United States)

Ruddlesden–Popper reduced-dimensional hybrid perovskite (RDP) semiconductors have attracted significant attention recently due to their promising stability and excellent optoelectronic properties. Here, the RDP crystallization mechanism in real time from liquid precursors to the solid film is investigated, and how the phase transition kinetics influences phase purity, quantum well orientation, and photovoltaic performance is revealed. An important template-induced nucleation and growth of the desired (BA)2(MA)3Pb4I13 phase, which is achieved only via direct crystallization without formation of intermediate phases, is observed. As such, the thermodynamically preferred perpendicular crystal orientation and high phase purity are obtained. At low temperature, the formation of intermediate phases, including PbI2 crystals and solvate complexes, slows down intercalation of ions and increases nucleation barrier, leading to formation of multiple RDP phases and orientation randomness. These insights enable to obtain high quality (BA)2(MA)3Pb4I13 films with preferentially perpendicular quantum well orientation, high phase purity, smooth film surface, and improved optoelectronic properties. The resulting devices exhibit high power conversion efficiency of 12.17%. This work should help guide the perovskite community to better control Ruddlesden–Popper perovskite structure and further improve optoelectronic and solar cell devices.

Research Organization:
Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
Sponsoring Organization:
National Science Foundation (NSF); USDOE
Grant/Contract Number:
89233218CNA000001
OSTI ID:
1558068
Report Number(s):
LA-UR-19-22960
Journal Information:
Advanced Materials, Vol. 30, Issue 21; ISSN 0935-9648
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 117 works
Citation information provided by
Web of Science

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Impact of the Solvation State of Lead Iodide on Its Two‐Step Conversion to MAPbI 3 : An In Situ Investigation journal January 2019
Introduction of Hydrophobic Ammonium Salts with Halogen Functional Groups for High‐Efficiency and Stable 2D/3D Perovskite Solar Cells journal January 2019
Solution‐Processable Perovskite Solar Cells toward Commercialization: Progress and Challenges journal April 2019
Layered Ruddlesden–Popper Efficient Perovskite Solar Cells with Controlled Quantum and Dielectric Confinement Introduced via Doping journal May 2019
Merits and Challenges of Ruddlesden-Popper Soft Halide Perovskites in Electro-Optics and Optoelectronics journal October 2018
Kinetic Stabilization of the Sol-Gel State in Perovskites Enables Facile Processing of High-Efficiency Solar Cells journal June 2019
Compositional Control in 2D Perovskites with Alternating Cations in the Interlayer Space for Photovoltaics with Efficiency over 18% journal September 2019
Fine Multi‐Phase Alignments in 2D Perovskite Solar Cells with Efficiency over 17% via Slow Post‐Annealing journal September 2019
Controlling Spatial Crystallization Uniformity and Phase Orientation of Quasi‐2D Perovskite‐Based Light‐Emitting Diodes Using Lewis Bases journal December 2019
Management of Crystallization Kinetics for Efficient and Stable Low-Dimensional Ruddlesden-Popper (LDRP) Lead-Free Perovskite Solar Cells journal November 2018
Benefiting from Spontaneously Generated 2D/3D Bulk‐Heterojunctions in Ruddlesden−Popper Perovskite by Incorporation of S‐Bearing Spacer Cation journal May 2019
Ruddlesden–Popper Perovskites: Synthesis and Optical Properties for Optoelectronic Applications journal October 2019
High‐Performance Perovskite Solar Cells with Enhanced Environmental Stability Based on a ( p ‐FC 6 H 4 C 2 H 4 NH 3 ) 2 [PbI 4 ] Capping Layer journal January 2019
Compositional and Solvent Engineering in Dion-Jacobson 2D Perovskites Boosts Solar Cell Efficiency and Stability journal January 2019
Ruddlesden–Popper 2D Component to Stabilize γ‐CsPbI 3 Perovskite Phase for Stable and Efficient Photovoltaics journal September 2019
Enhanced Charge Transport by Incorporating Formamidinium and Cesium Cations into Two‐Dimensional Perovskite Solar Cells journal July 2019
Pressure‐Induced Emission (PIE) and Phase Transition of a Two‐dimensional Halide Double Perovskite (BA) 4 AgBiBr 8 (BA=CH 3 (CH 2 ) 3 NH 3 + ) journal October 2019
Pressure‐Induced Emission (PIE) and Phase Transition of a Two‐dimensional Halide Double Perovskite (BA) 4 AgBiBr 8 (BA=CH 3 (CH 2 ) 3 NH 3 + ) journal October 2019
Bismuth‐Based Perovskite‐Inspired Solar Cells: In Situ Diagnostics Reveal Similarities and Differences in the Film Formation of Bismuth‐ and Lead‐Based Films journal May 2019
Origin and Suppression of the Graded Phase Distribution in Ruddlesden‐Popper Perovskite Films for Photovoltaic Application journal March 2019
Manipulating the Phase Distributions and Carrier Transfers in Hybrid Quasi‐Two‐Dimensional Perovskite Films journal February 2019
Oriented and Uniform Distribution of Dion–Jacobson Phase Perovskites Controlled by Quantum Well Barrier Thickness journal May 2019
Recent advances in controlling the crystallization of two-dimensional perovskites for optoelectronic device journal May 2019
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Synergistic enhancement of Cs and Br doping in formamidinium lead halide perovskites for high performance optoelectronics journal January 2018
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Enhanced V OC of two-dimensional Ruddlesden–Popper perovskite solar cells using binary synergetic organic spacer cations journal January 2020
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Engineering the underlying surface to manipulate the growth of 2D perovskites for highly efficient solar cells journal January 2019
Asymmetric alkyl diamine based Dion–Jacobson low-dimensional perovskite solar cells with efficiency exceeding 15% journal January 2020
Enhanced Charge Transport by Incorporating Formamidinium and Cesium Cations into Two-Dimensional Perovskite Solar Cells journal July 2019
Synthetic control over orientational degeneracy of spacer cations enhances solar cell efficiency in two-dimensional perovskites text January 2019
Templated growth of oriented layered hybrid perovskites on 3D-like perovskites journal January 2020
Efficient lateral-structure perovskite single crystal solar cells with high operational stability journal January 2020
Single Source Thermal Evaporation of Two-dimensional Perovskite Thin Films for Photovoltaic Applications journal November 2019