Activation of Self‐Trapped Emission in Stable Bismuth‐Halide Perovskite by Suppressing Strong Exciton–Phonon Coupling

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

Published: June 10, 2021

Abstract All‐inorganic bismuth‐halide perovskites are promising alternatives for lead halide due to their admirable chemical stability and optoelectronic properties; however, these materials deliver inferior photoluminescence (PL) properties, severely hindering prospects in lighting applications. Here, a novel air‐stable but non‐emissive perovskite Rb 3 BiCl 6 is synthesized, the material used as prototype uncover origin of poor optical performance perovskite. It found that extremely strong exciton–phonon interactions with large coupling constant up 693 meV leads seriously nonradiative recombination, which, can be effectively suppressed 347 by introducing Sb 3+ ions. As result, ‐doped exhibits stable yellow emission unprecedented PL quantum yield 33.6% from self‐trapped excitons. Systematic spectroscopic characterizations theoretical calculations carried out unveil intriguing photophysical mechanisms. This work reveals effect interaction, often underemphasized, on material's properties.

Language: Английский

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Ultra‐Sensitive, Selective and Repeatable Fluorescence Sensor for Methanol Based on a Highly Emissive 0D Hybrid Lead‐Free Perovskite

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(35)

Published: June 7, 2022

A convenient and rapid detection method for methanol in ethanol remains a major challenge due to their indistinguishable physical properties. Herein, novel fluorescence probe based on perovskite was successfully designed overcome this bottleneck. We report new zero-dimensional (0D) hybrid of [MP]2 Inx Sb1-x Cl7 ⋅ 6 H2 O (MP=2-methylpiperazine) displaying an unusual green light emission with near-unity photoluminescence quantum yield. Remarkably, 0D exhibits reversible methanol-response luminescence switching between yellow color but fail any other organic vapors. Even blended alcohol solutions, the luminescent excellent sensing performance multiple superiorities response time (30 s) ultra-low limit (40 ppm), etc. Therefore, can be utilized as perfect detect traces from ultrahigh sensitivity, selectivity repeatability. To best our knowledge, work represents first wide potential environmental monitoring detection,

Language: Английский

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Structural Dimensionality Modulation toward Enhanced Photoluminescence Efficiencies of Hybrid Lead‐Free Antimony Halides

Advanced Optical Materials, Journal Year: 2021, Volume and Issue: 9(19)

Published: June 3, 2021

Abstract Rationally optimizing the photoluminescence performance via accurate structural modulation is one of most important and challenging issues for hybrid halides. Herein, a viable crystal dimensional reduction strategy proposed to reasonably enhance quantum yield (PLQY) antimony halide. Specifically, synthetic technique developed new 1D [DMPZ]SbCl 5 ∙ H 2 O (DP‐SbCl ) sliced 0D [DMPZ] SbCl 6 Cl (H O) with from infinite [SbCl ] 2− chain discrete 3− octahedron. Comparing nonluminescent DP‐SbCl , displays highly efficient broadband yellow light emission enhanced PLQY up 75.94%. First‐principles calculation demonstrates that features more flat narrow band structure, which promotes photoelectron localization increases confinement, finally boosts luminescence efficiency. Together ultra‐stable enable as excellent down‐conversion phosphor successfully fabricate white emitting diodes high color rendering index 92. This work provides novel rationally optimize PL metal

Language: Английский

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Hybrid 0D Antimony Halides as Air‐Stable Luminophores for High‐Spatial‐Resolution Remote Thermography

Advanced Materials, Journal Year: 2021, Volume and Issue: 33(9)

Published: Jan. 22, 2021

Abstract Luminescent organic–inorganic low‐dimensional ns 2 metal halides are of rising interest as thermographic phosphors. The intrinsic nature the excitonic self‐trapping provides for reliable temperature sensing due to existence a range, typically 50–100 K wide, in which luminescence lifetimes (and quantum yields) steeply temperature‐dependent. This sensitivity range can be adjusted from cryogenic temperatures above room by structural engineering, thus enabling diverse thermometric and applications ranging protein crystallography diagnostics microelectronics. Owing stable oxidation state Sb 3+ , Sb(III)‐based far more attractive than all major non‐heavy‐metal alternatives (Sn‐, Ge‐, Bi‐based halides). In this work, relationship between characteristics crystal structure microstructure TPP SbBr 5 (TPP = tetraphenylphosphonium) is established, then its potential showcased environmentally robust phosphor remote thermography. material easily processable into thin films, highly beneficial high‐spatial‐resolution particular, compelling combination high spatial resolution (1 µ m) precision (high specific sensitivities 0.03–0.04 −1 ) demonstrated fluorescence‐lifetime imaging heated resistive pattern on flat substrate, covered with solution‐spun film .

Language: Английский

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Bright Green Emission from Self-Trapped Excitons Triggered by Sb³⁺ Doping in Rb₄CdCl₆

Chemistry of Materials, Journal Year: 2022, Volume and Issue: 34(12), P. 5717 - 5725

Published: June 10, 2022

Sb3+ with stereochemically active lone pair 5s2 electrons is overwhelming in the doping engineering of luminescent metal halides, and it usually leads to extrinsic self-trapped excitons (STEs) tunable emissions. However, photoluminescence enhancement mechanism doped halides compared pristine host remains unclear. Herein, we into all-inorganic non-emissive Rb4CdCl6, realizing bright green emission peaking at 525 nm a quantum yield 70.2%. A comparison Raman spectra, as well Debye temperature, was utilized elucidate STEs mechanism, verifying that softens structural lattice. Thus, strong electron–phonon interactions enable highly efficient originating from Rb4CdCl6:Sb3+. This work demonstrates solid evidence emissions can be triggered by doping, design principle involved will guide future studies for emerging luminescence material exploration.

Language: Английский

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Strong Self‐Trapped Exciton Emissions in Two‐Dimensional Na‐In Halide Perovskites Triggered by Antimony Doping

Angewandte Chemie International Edition, Journal Year: 2021, Volume and Issue: 60(14), P. 7587 - 7592

Published: Jan. 15, 2021

Abstract Soft lattice and strong exciton–phonon coupling have been demonstrated in layered double perovskites (LDPs) recently; therefore, LDPs represents a promising class of compounds as excellent self‐trapped exciton (STE) emitters for applications solid‐state lighting. However, few with outstanding STE emissions discovered, their optoelectronic properties are still unclear. Based on the three‐dimensional (3D) Cs 2 NaInCl 6 , we synthesized two 2D derivatives (PEA) 4 8 :Sb (PEA=phenethylamine) CsNaInCl 7 monolayer bilayer inorganic sheets by combination dimensional reduction Sb‐doping. Bright broadband were obtained first time under ambient temperature pressure, photoluminescence quantum efficiency (PLQE) 48.7 % (monolayer) 29.3 (bilayer), superior to current known LDPs. Spectroscopic characterizations first‐principles calculations excited state indicate originate from STEs trapped at introduced [SbCl ] 3− octahedron.

Language: Английский

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Highly efficient Sb3+ emitters in 0D cesium indium chloride nanocrystals with switchable photoluminescence through water-triggered structural transformation

Nano Today, Journal Year: 2022, Volume and Issue: 44, P. 101460 - 101460

Published: March 21, 2022

Language: Английский

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Efficient Near‐Infrared Luminescence in Lanthanide‐Doped Vacancy‐Ordered Double Perovskite Cs₂ZrCl₆ Phosphors via Te⁴⁺ Sensitization

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(26)

Published: April 19, 2022

All-inorganic lead-free perovskite-derivative metal halides have shown great promise in optoelectronics, however, it remains challenging to realize efficient near-infrared (NIR) luminescence these materials. Herein, we report a novel strategy based on Te4+ /Ln3+ (Ln=Er, Nd, and Yb) co-doping achieve NIR vacancy-ordered double perovskite Cs2 ZrCl6 phosphors, which are excitable by low-cost near-ultraviolet light-emitting diode (LED) chip. Through sensitization the spin-orbital allowed 1 S0 →3 P1 transition of , intense multi-wavelength originating from 4f→4f transitions Er3+ Nd3+ Yb3+ was acquired, with quantum yield 6.1 % for emission. These findings provide general approach emission through ns2 -metal lanthanide ion co-doping, thereby opening up new avenue exploring NIR-emitting derivatives towards versatile applications such as NIR-LEDs bioimaging.

Language: Английский

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Highly Distorted Antimony(III) Chloride [Sb₂Cl₈]²⁻ Dimers for Near‐Infrared Luminescence up to 1070 nm

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(33)

Published: June 23, 2022

Zero-dimensional (0D) hybrid metal halides with unique compositional and structural tunability appear as an emerging class of luminescent materials, but near-infrared (NIR) emitters therein are largely unexplored to date. This study presents three novel 0D antimony chlorines edge-sharing [Sb2 Cl8 ]2- dimers, showing unusual room-temperature broadband NIR emission the maximum wavelength up 1070 nm. Photoluminescence studies density functional theory calculation demonstrate that emissions originate from highly localized excitons, confined dimers in these structures show low symmetry a large degree freedom. These expand range new materials halides.

Language: Английский

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Regulating the Singlet and Triplet Emission of Sb³⁺ Ions to Achieve Single-Component White-Light Emitter with Record High Color-Rendering Index and Stability

Nano Letters, Journal Year: 2022, Volume and Issue: 22(12), P. 5046 - 5054

Published: May 17, 2022

The rapid development of solid-state lighting technology has attracted much attention for searching efficient and stable luminescent materials, especially the single-component white-light emitter. Here, we adopt a facile ion-doping to synthesize vacancy-ordered double perovskite Cs2ZrCl6:Sb. introduction Sb3+ ions with 5s2 active lone pair into Cs2ZrCl6 host stimulates singlet (blue) triplet (orange) states emission ions, their relative intensity can be tuned through energy transfer from states. Benefiting dual-band as perfect complementary colors, optimum Cs2ZrCl6:1.5%Sb exhibits high-quality white color-rendering index 96. By employing down-conversion phosphor, light-emitting diodes record half-lifetime 2003 h were further fabricated. This study puts forward an effective strategy design emitter, making practical applications them in technologies real possibility.

Language: Английский

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