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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Multiexcitonic Emission in Zero-Dimensional Cs₂ZrCl₆:Sb³⁺ Perovskite Crystals

Journal of the American Chemical Society, Journal Year: 2021, Volume and Issue: 143(42), P. 17599 - 17606

Published: Oct. 13, 2021

Metal halide perovskites are highly attractive for lighting applications, but the multiexcitonic emission processes in these crystals largely unexplored. This study presents an investigation of Sb3+-doped Cs2ZrCl6 perovskite that display double luminescence due to intrinsic host self-trapped excitons (denoted as STEs) and dopant-induced extrinsic dopant STEs), respectively. Steady-state transient-state spectroscopy reveal STEs can be independently charged at specific energies. Density functional theory calculations confirm stems from minimal interactions between zero-dimensional crystal lattice. By selective excitation different through precise control wavelength, we further demonstrate dynamic color tuning Cs2ZrCl6:Sb3+ crystals. The kinetic feature offers exciting opportunities constructing multicolor light-emitting devices encrypting multilevel optical codes.

Language: Английский

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Sb³⁺–Er³⁺‐Codoped Cs₂NaInCl₆for Emitting Blue and Short‐Wave Infrared Radiation

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(32)

Published: April 11, 2022

Cs2 NaInCl6 double perovskite is stable, environmentally benign and easy to prepare. But it has a wide band gap (5.1 eV), therefore, does not show optical optoelectronic properties in the visible short-wave infrared (SWIR) region. Here we introduce such functionalities by codoping Sb3+ (s-electron doping) Er3+ (f-electron ions. doping introduces optically allowed 5s2→ 5s1 5p1 electronic absorption at sub-band level, which then emits blue photoluminescence with ≈93 % quantum yield. f-f of parity forbidden. Codoping -Er3+ , leads transfer excitation energy from yielding SWIR emission 1540 nm. Temperature (6 300 K) dependent measurements elucidate mechanism. A phosphor converted light emitting diode (pc-LED) fabricated using codoped sample stable radiation over prolonged (84 hours) operation 5.1 V.

Language: Английский

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Ultrafast Dynamics of Self-Trapped Excitons in Lead-Free Perovskite Nanocrystals

The Journal of Physical Chemistry Letters, Journal Year: 2021, Volume and Issue: 12(34), P. 8256 - 8262

Published: Aug. 23, 2021

Lead-free halide perovskite nanocrystals (NCs) have received increasing attention owing to their low toxicity and high stability. Localized charge distribution strong carrier–phonon coupling in lead-free NCs facilitates the formation of self-trapped excitons (STEs), which typically give a broadband photoluminescence (PL) emission with large Stokes shift. In this Perspective, we highlight how PL modulations can rise an efficient white-light by understanding tuning ultrafast dynamics STEs NCs. We then present exciton energy transfer mediated provide thermally activated delayed fluorescence dopant PL. also illustrate promising directions for future applications based on STEs. hope that Perspective new viewpoint researchers understand promote optoelectronic applications.

Language: Английский

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Sb-Doped Metal Halide Nanocrystals: A 0D versus 3D Comparison

ACS Energy Letters, Journal Year: 2021, Volume and Issue: 6(6), P. 2283 - 2292

Published: May 27, 2021

We synthesize colloidal nanocrystals (NCs) of Rb3InCl6, composed isolated metal halide octahedra ("0D"), and Cs2NaInCl6 Cs2KInCl6 double perovskites, where all share corners are interconnected ("3D"), with the aim to elucidate compare their optical features once doped Sb3+ ions. Our computational analyses evidence that photoluminescence quantum yield (PLQY) these systems is consistently lower than corresponding bulk materials due presence deep surface traps from under-coordinated Also, Sb-doped "0D" Rb3InCl6 NCs exhibit a higher PLQY "3D" NCs, most likely because excitons responsible for PL emission migrate faster in 3D 0D NCs. also observe feature large Stokes shift (varying system system), should be interest applications photon management scintillation technologies. Scintillation properties evaluated via radioluminescence experiments, re-absorption-free waveguiding performance large-area plastic scintillators assessed using Monte Carlo ray-tracing simulations.

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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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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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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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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Dual‐Band‐Tunable White‐Light Emission from Bi³⁺/Te⁴⁺ Emitters in Perovskite‐Derivative Cs₂SnCl₆ Microcrystals

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(9)

Published: Jan. 4, 2022

Luminescent metal halides have attracted considerable attention in next-generation solid-state lighting because of their superior optical properties and easy solution processibility. Herein, we report a new class highly efficient dual-band-tunable white-light emitters based on Bi3+ /Te4+ co-doped perovskite derivative Cs2 SnCl6 microcrystals. Owing to the strong electron-phonon coupling energy transfer from Te4+ , microcrystals exhibited broad dual-band emission originating inter-configurational 3 P0,1 →1 S0 transitions with good stability high photoluminescence (PL) quantum yield up 68.3 %. Specifically, remarkable transition -PL lifetime milliseconds at 10 K microseconds 300 was observed, as solid evidence for isolated emission. These findings provide not only insights into excited-state dynamics but also general approach achieve single-composition lead-free through ns2 -metal ion co-doping.

Language: Английский

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