Efficient Lone-Pair-Driven Luminescence: Structure–Property Relationships in Emissive 5s² Metal Halides

ACS Materials Letters, Journal Year: 2020, Volume and Issue: 2(9), P. 1218 - 1232

Published: Aug. 4, 2020

Low-dimensional metal halides have been the focus of intense investigations in recent years following success hybrid lead halide perovskites as optoelectronic materials. In particular, light emission low-dimensional based on 5s2 cations Sn2+ and Sb3+ has found utility a variety applications complementary to those three-dimensional because its unusual properties such broadband character highly temperature-dependent lifetime. These derive from exceptional chemistry lone pair, but terminology explanations given for vary widely, hampering efforts build cohesive understanding these materials that would development efficient devices. this Perspective, we provide structural overview with dynamics driven by stereoactivity pair identify features enable strong emission. We unite different theoretical models able explain bright centers into framework, which is then applied array compounds recently developed our group other researchers, demonstrating generating holistic picture field point view chemist. highlight state-of-the-art demonstrate unique capabilities versatile emissive promising future directions halides.

Language: Английский

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Sb³⁺‐Doping in Cesium Zinc Halides Single Crystals Enabling High‐Efficiency Near‐Infrared Emission

Advanced Functional Materials, Journal Year: 2021, Volume and Issue: 31(40)

Published: July 10, 2021

Abstract Luminescent metal halide materials with flexible crystallography/electronic structures and tunable emission have demonstrated broad application prospects in the visible light region. However, designing near‐infrared (NIR) light‐emitting halides remains a challenge. Here, an enlightening prototype is proposed to explore high‐efficiency broadband NIR systems by incorporating Sb 3+ into Cs 2 ZnCl 4 matrix. Combined experimental analysis density functional theory calculations reveal modified self‐trapped excitons model elaborate emission. The high photoluminescence quantum yield of 69.9% peaking at 745 nm large full width half maximum 175 nm, along excellent air/thermal stability, show unique advantages lead‐free :Sb as source. substitution Cl − Br further enables red‐shift peak from 823 nm. diode device based on demonstrates potential non‐visible source night vision. This study puts forward effective strategy design novel eco‐friendly emissive provides guidance for expanding scope luminescent halides.

Language: Английский

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Bright Blue and Green Luminescence of Sb(III) in Double Perovskite Cs₂MInCl₆ (M = Na, K) Matrices

Chemistry of Materials, Journal Year: 2020, Volume and Issue: 32(12), P. 5118 - 5124

Published: June 8, 2020

The vast structural and compositional space of metal halides has recently become a major research focus for designing inexpensive versatile light sources; in particular, applications displays, solid-state lighting, lasing, etc. Compounds with isolated ns2-metal halide centers often exhibit bright broadband emission that stems from self-trapped excitons (STEs). Sb(III) are attractive STE emitters due to their low toxicity oxidative stability; however, coupling these features an appropriately robust, fully inorganic material containing Sb3+ octahedral environment proven be challenge. Here, we investigate as dopant solution-grown double perovskite (DP) matrix, namely Cs2MInCl6:xSb (M = Na, K, x 0-100%). Cs2KInCl6 is found crystallize the tetragonal DP phase, unlike Cs2NaInCl6 adopts traditional cubic structure. This difference results distinct colors, Cs2NaInCl6:xSb Cs2KInCl6:xSb compounds blue green emissions, respectively, photoluminescence quantum yields (PLQYs) up 93%. Spectroscopic computational investigations confirm this efficient originates Sb(III)-hosted STEs. These demonstrate can incorporated emissive center stable lighting applications.

Language: Английский

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Lead‐Free Double Perovskite Cs₂AgBiBr₆: Fundamentals, Applications, and Perspectives

Advanced Functional Materials, Journal Year: 2021, Volume and Issue: 31(49)

Published: Sept. 5, 2021

Abstract Cs 2 AgBiBr 6 , as a benchmark lead‐free double perovskite, has emerged promising alternative to lead‐based perovskites because of its high stability, non‐toxicity, exceptional optoelectronic properties, and multifunctionality. To encourage further research on broad applications, in this review, fundamental properties including the structure‐property relation, synthesis, origin absorption photoluminescence, electron‐phonon coupling, role defects, charge carrier dynamics, bandgap modulation are comprehensively emphasized. The recent progress wide applications solar cells, light/X‐ray detectors, ferroelectric/magnetic devices highlighted. Moreover, challenges materials related discussed perspectives provided for guiding future development area.

Language: Английский

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Broad-band emission in metal halide perovskites: Mechanism, materials, and applications

Materials Science and Engineering R Reports, Journal Year: 2020, Volume and Issue: 141, P. 100548 - 100548

Published: March 20, 2020

Language: Английский

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ns² Electron (Bi³⁺ and Sb³⁺) Doping in Lead-Free Metal Halide Perovskite Derivatives

Chemistry of Materials, Journal Year: 2020, Volume and Issue: 32(24), P. 10255 - 10267

Published: Dec. 3, 2020

Bi3+ and Sb3+ doping (and codoping with lanthanides) in Cs2SnCl6 vacancy ordered perovskites Cs2MInCl6 (M = Na, K, Ag) double has been shown to open up new opportunities for solid state lighting. ns2 outer electronic configuration can tailor both optical absorption emission properties phosphor-converted light emitting diode (pc-LEDs) applications. Therefore, the s-electron dopants (Bi3+ Sb3+) act as sensitizers emitters. This is because dopant s-electrons contribute near band edges of host, unlike cases d- f-electron dopants. Consequently, also a sensitizer lanthanide luminescence systems like Bi3+-Ln3+ codoped Cs2AgInCl6, where Ln Er, Yb, Tb. In this perspective, we provide insights on tailoring by electron doping. These are then connected rational design hosts, dopants, codopants, their potential Finally, discuss challenges future research.

Language: Английский

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Photoluminescence of Singlet/Triplet Self‐Trapped Excitons in Sb³⁺‐Based Metal Halides

Advanced Optical Materials, Journal Year: 2021, Volume and Issue: 9(8)

Published: Feb. 18, 2021

Abstract Emerging lead‐free metal halides with low toxicity and unparalleled optoelectronic properties have attracted growing research interests, also demonstrating extensive application potentials. Among these, Sb 3+ ‐based all‐inorganic/organic–inorganic hybrid become a vital group due to the special energy level distribution along diverse optical properties. However, there remains gap in understanding relationship between crystal structure radiation process of involved emission. Herein, existing reports about luminescent are revisited their structure–luminescence–application is explored, it further established that triplet self‐trapped excitons (STEs) emission varies different crystallographic environments endows tunable performance. This work aims provide constructive strategies exploitation halides, guides structural design photoluminescence tuning doped halide materials.

Language: Английский

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Efficient White Photoluminescence from Self-Trapped Excitons in Sb³⁺/Bi³⁺-Codoped Cs₂NaInCl₆ Double Perovskites with Tunable Dual-Emission

ACS Energy Letters, Journal Year: 2021, Volume and Issue: 6(9), P. 3343 - 3351

Published: Aug. 30, 2021

Efficient and stable inorganic lead-free halide perovskites have attracted tremendous attention for next-generation solid-state lighting. However, single perovskite phosphors with strong, tunable-color-temperature white-light emission are rare. Here, a doping strategy was developed to incorporate Sb3+ Bi3+ ions into Cs2NaInCl6 crystals. Blue yellow white light 77% quantum yield observed. The dual-emission originates from different [SbCl6]3– octahedron-related self-trapped excitons (STEs). blue is attributable limited Jahn–Teller deformation doping. Large-radii increase the level of octahedron, enhancing STE emission. Density functional theory calculations indicated that forms sub-band level, which produces Tuning between warm cold can be realized by changing Sb3+/Bi3+ ratio, suggests unique interaction mechanism dopants, as well Bi3+-induced lattice distortion in double perovskites.

Language: Английский

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Boosting triplet self-trapped exciton emission in Te(IV)-doped Cs2SnCl6 perovskite variants

Nano Research, Journal Year: 2020, Volume and Issue: 14(5), P. 1551 - 1558

Published: Nov. 19, 2020

Language: Английский

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Efficient Energy Transfer in Te⁴⁺-Doped Cs₂ZrCl₆ Vacancy-Ordered Perovskites and Ultrahigh Moisture Stability via A-Site Rb-Alloying Strategy

The Journal of Physical Chemistry Letters, Journal Year: 2021, Volume and Issue: 12(7), P. 1829 - 1837

Published: Feb. 12, 2021

As an effective method to improve the optical properties and stability of perovskite matrix, doped halide perovskites have attracted extensive attention in field optoelectronic applications. Herein, a series all inorganic lead-free Te4+-doped Cs2ZrCl6 vacancy-ordered were successfully synthesized with different Te-doping concentrations by solvothermal method, deliberate Te4+-doping results green-yellow triplet self-trapped exciton (STE) emission high photoluminescence quantum yield (PLQY) 49.0%. The efficient energy transfer was observed from singlet emission. Further, effects A-site Rb alloying on investigated. We found that C-site cohalogenation did not change luminescence Te4+, but addition small amount Rb+ can PL intensity moisture stability. Our provide physical insights into nS2 Te4+-ion-doping-induced emissive mechanism shed light improving environmental for further

Language: Английский

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