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Title: High Layer Number (n = 1–6) 2D Ruddlesden–Popper Lead Bromide Perovskites: Nanosheets, Crystal Structure, and Optoelectronic Properties

Journal Article · · ACS Materials Letters

2D Ruddlesden–Popper (RP) lead halide perovskites have highly tunable structures, compositions, and properties that enable their promising optoelectronic applications. Among various 2D halide perovskites, the materials chemistry and fundamental optoelectronic properties of high layer number (n) lead-bromide RP perovskites, where n refers to the number of inorganic octahedra layers, have been less studied. Here, we report the synthesis of thin nanosheets of (PEA)2Csn–1PbnBr3n+1 (n = 1–6, PEA = phenylethylammonium) perovskites and study the optical properties, assigning photoluminescence emissions of 486, 496, and 505 nm to n = 4–6 phases, respectively, and reporting the photoluminescence lifetimes. Furthermore, the crystal structure of (PEA)2Cs2Pb3Br10 was determined to reveal minimal octahedral structural distortions. Ultraviolet photoelectron spectroscopy measurements reveal the positioning of the valence and conduction bands for n = 1–3 phases and confirm the type-I band alignment for the (PEA)2Csn–1PbnBr3n+1 series, laying the foundation for rational heterostructure device design in the future.

Research Organization:
University of Kentucky, Lexington, KY (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
SC0018208; SC0002162
OSTI ID:
2205086
Journal Information:
ACS Materials Letters, Journal Name: ACS Materials Letters Journal Issue: 11 Vol. 5; ISSN 2639-4979
Publisher:
ACS PublicationsCopyright Statement
Country of Publication:
United States
Language:
English

References (51)

Layer-by-layer anionic diffusion in two-dimensional halide perovskite vertical heterostructures journal February 2021
Valence and Conduction Band Densities of States of Metal Halide Perovskites: A Combined Experimental–Theoretical Study journal June 2016
Halide Perovskites: Is It All about the Interfaces? journal March 2019
Structural Descriptors to Correlate Pb Ion Displacement and Broadband Emission in 2D Halide Perovskites journal October 2022
Structure‐Property Relationships and Idiosyncrasies of Bulk, 2D Hybrid Lead Bromide Perovskites journal October 2021
Metal halide perovskite nanostructures for optoelectronic applications and the study of physical properties journal February 2019
Intrinsic Halide Immiscibility in 2D Mixed-Halide Ruddlesden–Popper Perovskites journal September 2022
From bulk to molecularly thin hybrid perovskites journal March 2020
Tunable White-Light Emission in Single-Cation-Templated Three-Layered 2D Perovskites (CH 3 CH 2 NH 3 ) 4 Pb 3 Br 10– x Cl x journal August 2017
Control of n-Phase Distribution in Quasi Two-Dimensional Perovskite for Efficient Blue Light-Emitting Diodes journal February 2023
Single-crystal microplates of two-dimensional organic–inorganic lead halide layered perovskites for optoelectronics journal January 2017
Ruddlesden–Popper Hybrid Lead Iodide Perovskite 2D Homologous Semiconductors journal April 2016
Uniaxial Expansion of the 2D Ruddlesden–Popper Perovskite Family for Improved Environmental Stability journal March 2019
Stable room-temperature continuous-wave lasing in quasi-2D perovskite films journal September 2020
Controlling the formation energy of perovskite phase via surface polarity of substrate for efficient pure-blue light-emitting diodes journal May 2023
Multicolor Heterostructures of Two-Dimensional Layered Halide Perovskites that Show Interlayer Energy Transfer journal October 2018
How To Correctly Determine the Band Gap Energy of Modified Semiconductor Photocatalysts Based on UV–Vis Spectra journal December 2018
A Layered Solution Crystal Growth Technique and the Crystal Structure of (C6H5C2H4NH3)2PbCl4 journal July 1999
Suppressing the Formation of High n-Phase and 3D Perovskites in the Fabrication of Ruddlesden–Popper Perovskite Thin Films by Bulky Organic Cation Engineering journal March 2022
Molecularly thin two-dimensional hybrid perovskites with tunable optoelectronic properties due to reversible surface relaxation journal September 2018
Direct Characterization of Type‐I Band Alignment in 2D Ruddlesden–Popper Perovskites journal September 2022
Domain Distribution Management of Quasi‐2D Perovskites toward High‐Performance Blue Light‐Emitting Diodes journal May 2023
Toward Continuous-Wave Pumped Metal Halide Perovskite Lasers: Strategies and Challenges journal May 2022
Recent progress in two-dimensional Ruddlesden–Popper perovskite based heterostructures journal February 2021
High-efficiency two-dimensional Ruddlesden–Popper perovskite solar cells journal July 2016
Color-Pure Violet-Light-Emitting Diodes Based on Layered Lead Halide Perovskite Nanoplates journal June 2016
The Unprecedented Highest‐Layer‐Number Ferroelectric Semiconductor of 2D Homologous Single‐Phase Perovskites Tailored by Regulating Thickness of Inorganic Frameworks journal August 2022
Organic–Inorganic Perovskites: Structural Versatility for Functional Materials Design journal March 2016
Perovskite energy funnels for efficient light-emitting diodes journal June 2016
Scaling law for excitons in 2D perovskite quantum wells journal June 2018
Color-stable highly luminescent sky-blue perovskite light-emitting diodes journal August 2018
Metal halide perovskites for light-emitting diodes journal September 2020
Narrowing the Phase Distribution of Quasi‐2D Perovskites for Stable Deep‐Blue Electroluminescence journal July 2022
High Members of the 2D Ruddlesden-Popper Halide Perovskites: Synthesis, Optical Properties, and Solar Cells of (CH 3 (CH 2 ) 3 NH 3 ) 2 (CH 3 NH 3 ) 4 Pb 5 I 16 journal March 2017
Two-dimensional halide perovskite nanomaterials and heterostructures journal January 2018
Shedding Light on the Stability and Structure–Property Relationships of Two-Dimensional Hybrid Lead Bromide Perovskites journal June 2021
Semiconductor physics of organic–inorganic 2D halide perovskites journal December 2020
Discerning between Exciton and Free-Carrier Behaviors in Ruddlesden–Popper Perovskite Quantum Wells through Kinetic Modeling of Photoluminescence Dynamics journal July 2020
Deterministic fabrication of arbitrary vertical heterostructures of two-dimensional Ruddlesden–Popper halide perovskites journal November 2020
Two-Dimensional Hybrid Perovskite-Type Ferroelectric for Highly Polarization-Sensitive Shortwave Photodetection journal January 2019
Synthetic Variation and Structural Trends in Layered Two-Dimensional Alkylammonium Lead Halide Perovskites journal July 2019
Tuning the Luminescence of Layered Halide Perovskites journal January 2019
The 2D Halide Perovskite Rulebook: How the Spacer Influences Everything from the Structure to Optoelectronic Device Efficiency journal January 2021
Tailored Engineering of an Unusual (C 4 H 9 NH 3 ) 2 (CH 3 NH 3 ) 2 Pb 3 Br 10 Two-Dimensional Multilayered Perovskite Ferroelectric for a High-Performance Photodetector journal September 2017
Lead halide perovskite nanowire lasers with low lasing thresholds and high quality factors journal April 2015
2D Homologous Perovskites as Light-Absorbing Materials for Solar Cell Applications journal June 2015
Vibrational relaxation dynamics in layered perovskite quantum wells journal June 2021
Structural and thermodynamic limits of layer thickness in 2D halide perovskites journal December 2018
Bilayered Hybrid Perovskite Ferroelectric with Giant Two-Photon Absorption journal April 2018
High-performance quasi-2D perovskite light-emitting diodes: from materials to devices journal March 2021
Spectrally Resolved Ultrafast Exciton Transfer in Mixed Perovskite Quantum Wells journal January 2019