Achieving Near‐unity Photoluminescence Quantum Yields in Organic‐Inorganic Hybrid Antimony (III) Chlorides with the [SbCl₅] Geometry

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(10)

Published: Jan. 9, 2023

Hybrid organic-inorganic antimony halides have attracted increasing attention due to the non-toxicity, stability, and high photoluminescence quantum yield (PLQY). To shed light on structural factors that contribute PLQY, five pairs of with general formula A2 SbCl5 Sb2 Cl8 are synthesized via two distinct methods characterized. The type adopts square pyramidal [SbCl5 ] geometry near-unity while seesaw dimmer [Sb2 PLQY≈0 %. Through combined data analysis literature, we found series generally has much longer Sb⋅⋅⋅Sb distances, leading more expressed lone SbIII . Additional including Sb-Cl distance stability chlorides may also affect PLQY. Our targeted synthesis correlated insights provide efficient tools precisely form highly emissive materials for optoelectronic applications.

Language: Английский

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Multiple Stimuli‐Responsive Luminescent Chiral Hybrid Antimony Chlorides for Anti‐Counterfeiting and Encryption Applications

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(36)

Published: July 18, 2023

Stimuli-responsive circularly polarized luminescence (CPL) materials are ideal for information anti-countering applications, but the best-performing have not yet been identified. This work presents enantiomorphic hybrid antimony halides R-(C5 H12 NO)2 SbCl5 (1) and S-(C5 (2) showing mirror-imaged CPL activity with a dissymmetry factor of 1.2×10-3 . Interestingly, DMF-induced structural transformation is realized to obtain non-emissive ⋅ DMF (3) (4) upon exposure vapor. The process reversed heating. DFT calculations showed that DMF-induced-quenched-luminescence attributed intersection ground excited state curves on configuration coordinates. Unexpectedly, nanocrystals chiral 1 2 were prepared indicate excellent solution performance. reversible PL switching gives system applications in technology, anti-counterfeiting, encryption-decryption, logic gates.

Language: Английский

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Photophysical studies for Cu(i)-based halides: broad excitation bands and highly efficient single-component warm white-light-emitting diodes

Chemical Science, Journal Year: 2023, Volume and Issue: 14(20), P. 5415 - 5424

Published: Jan. 1, 2023

Designing and synthesizing cuprous halide phosphors unifying efficient low-energy emission a broad excitation band is still great challenge. Herein, by rational component design, three novel Cu(i)-based metal halides, DPCu4X6 [DP = (C6H10N2)4(H2PO2)6; X Cl, Br, I], were synthesized reacting p-phenylenediamine with (CuX), they show similar structures, consisting of isolated [Cu4X6]2- units separated organic layers. Photophysical studies uncover that the highly localized excitons rigid environment give rise to yellow-orange photoluminescence in all compounds spanning from 240 450 nm. The bright PL (X Br) originates self-trapped due strong electron-phonon coupling. Intriguingly, DPCu4I6 features dual-band emissive characteristic, attributed synergistic effect halide/metal-to-ligand charge-transfer (X/MLCT) triplet cluster-centered (3CC) excited states. Benefiting broadband excitation, high-performance white-light emitting diode (WLED) high color rendering index 85.1 was achieved using single-component phosphor. This work not only unveils role halogens photophysical processes but also provides new design principles for WLEDs.

Language: Английский

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Highly Bright and Stable Lead‐Free Double Perovskite White Light‐Emitting Diodes

Advanced Materials, Journal Year: 2023, Volume and Issue: 36(4)

Published: Nov. 2, 2023

Lead-free double perovskites (DPs) are emerging highly stable emitters with efficient broadband self-trapped exciton (STE) photoluminescence (PL), but their low electroluminescent (EL) efficiency is a critical shortcoming. This work promotes the external quantum (EQE) and luminance of DP-based white light-emitting diode (wLED) normal device structure to 0.76% 2793 cd m

Language: Английский

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Modulating Inorganic Dimensionality of Ultrastable Lead Halide Coordination Polymers for Photocatalytic CO2 Reduction to Ethanol

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(16)

Published: Feb. 22, 2024

Lead halide hybrids have shown great potentials in CO

Language: Английский

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Efficient Red Light Emitting Diodes Based on a Zero‐Dimensional Organic Antimony Halide Hybrid

Advanced Materials, Journal Year: 2022, Volume and Issue: 35(9)

Published: Dec. 16, 2022

Zero-dimensional (0D) organic metal halide hybrids (OMHHs) have recently emerged as a new class of light emitting materials with exceptional color tunability. While near-unity photoluminescence quantum efficiencies (PLQEs) are routinely obtained for large number 0D OMHHs, it remains challenging to apply them emitter electrically driven diodes (LEDs), largely due the low conductivity wide bandgap cations. Here, development OMHH, triphenyl(9-phenyl-9H-carbazol-3-yl) phosphonium antimony bromide (TPPcarzSbBr4 ), efficient LEDs, which consists semiconducting cations (TPPcarz+ ) and anions (Sb2 Br82- is reported. By replacing one phenyl groups in well-known tetraphenylphosphonium cation (TPP+ an electroactive phenylcarbazole group, TPPcarz+ developed preparation red TPPcarzSbBr4 single crystals high PLQE 93.8%. With solution processed thin films (PLQE 86.1%) layer, LEDs fabricated exhibit external efficiency (EQE) 5.12%, peak luminance 5957 cd m-2 , current 14.2 A-1 best values reported date electroluminescence devices based on OMHHs.

Language: Английский

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Realizing High-Efficiency Yellow Emission of Organic Antimony Halides via Rational Structural Design

ACS Applied Materials & Interfaces, Journal Year: 2022, Volume and Issue: 14(40), P. 45611 - 45620

Published: Sept. 30, 2022

Zero-dimensional (0D) organic metal halides have captured extensive attention for their various structures and distinguished optical characteristics. However, achieving efficient emission through rational crystal structure design remains a great challenge, how the affects photophysical properties of 0D is currently unclear. Herein, regulation strategy in Sb(III)-based proposed to realize near-unity photoluminescence quantum yield (PLQY). Specifically, two compounds with different coordination configurations, namely, (C25H22P)2SbCl5 (C25H22P)SbCl4 (C25H22P+ = benzyltriphenylphosphonium), were successfully obtained by precisely controlling ratio initial raw materials. adopts an octahedral geometry shows highly broadband yellow PLQY 98.6%, while exhibits seesaw-shaped [SbCl4]- cluster does not emit light under photoexcitation. Theoretical calculations reveal that, rationally structure, indirect bandgap can be converted direct (C25H22P)2SbCl5, thus ultimately boosting intensity. Together outstanding stability high-performance white-light emitting diode (WLED) high luminous efficiency 31.2 lm W-1 demonstrated. Our findings provide novel regulate crystals, so as optimize luminescence halides.

Language: Английский

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Stepwise Crystalline Structural Transformation in 0D Hybrid Antimony Halides with Triplet Turn-on and Color-Adjustable Luminescence Switching

Research, Journal Year: 2023, Volume and Issue: 6

Published: Jan. 1, 2023

Intelligent stimuli-responsive fluorescence materials are extremely pivotal for fabricating luminescent turn-on switching in solid-state photonic integration technology, but it remains a challenging objective typical 3-dimensional (3D) perovskite nanocrystals. Herein, by fine-tuning the accumulation modes of metal halide components to dynamically control carrier characteristics, novel triple-mode photoluminescence (PL) was realized 0D through stepwise single-crystal (SC-SC) transformation. Specifically, family hybrid antimony halides designed exhibit three distinct types PL performance including nonluminescent [Ph 3 EtP] 2 Sb Cl 8 ( 1 ), yellow-emissive SbCl 5 ·EtOH and red-emissive ). Upon stimulus ethanol, successfully converted SC-SC transformation with enhanced quantum yield from ~0% 91.50% acting as “turn-on” switching. Meanwhile, reversible luminescence between can be also achieved ethanol impregnation–heating process vapochromism As consequence, new triple-model color-adjustable off–on I –on II halides. Simultaneously, wide advanced applications were anti-counterfeiting, information security, optical logic gates. This photon engineering strategy is expected deepen understanding dynamic mechanism guide development smart cutting-edge switchable device.

Language: Английский

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0D Hybrid Cuprous Halide as an Efficient Light Emitter and X‐Ray Scintillator

Laser & Photonics Review, Journal Year: 2023, Volume and Issue: 17(12)

Published: Aug. 24, 2023

Abstract Despite the extraordinary X‐ray scintillation performance of three‐dimensional (3D) lead perovskite nanocrystals (PNCs), serious biotoxicity Pb 2+ and luminescent instability in water remain insurmountable obstacles for their applications medical imaging. To address these drawbacks, herein, study demonstrates one new lead‐free zero‐dimensional (0D) hybrid cuprous halide single‐crystalline [BzTPP] 2 Cu I 4 (BzTPP = Benzyltriphenylphosphonium) as a satisfactory scintillator. displays broadband yellowish‐green light emission with high photoluminescent quantum yield (PLQY) 44.2% large Stokes shift 167 nm upon UV excitation. High PLQY negligible self‐absorption enable to display impressive excited by 27 706 photons MeV ‐1 low detection limit 0.352 µ Gy s −1 , surpassing typical 3D PNCs. More importantly, represents structural stability at least month. The excellent stable radioluminescence well solution growth method ensure ‐based screen fine‐resolution imaging potential radiography inspection. This work highlights multiple merits low‐toxicity cost, yield, long‐term water‐stability 0D halides highly desirable scintillators.

Language: Английский

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Stable Organic Antimony Halides with Near‐Unity Photoluminescence Quantum Yield for X‐Ray Imaging

Laser & Photonics Review, Journal Year: 2023, Volume and Issue: 17(7)

Published: Feb. 19, 2023

Abstract X‐ray imaging technology has been widely used in the fields of environmental monitoring, safety inspection, nondestructive examination, space exploration, and medical diagnosis, among which scintillation materials play a vital role indirectly converting to visible photons. Here, zero‐dimensional organic–inorganic hybrid halide C 50 H 44 P 2 SbCl 5 crystal is prepared via facile antisolvent precipitation method at room temperature. The single displays strong yellow broadband emission centered 592 nm with near‐unity photoluminescence quantum yield 98.42%. Importantly, crystals show great stability irradiation stability. Radioluminescence characterization indicates that exhibit good linear response dose rates along an excellent light 460 photons MeV −1 , surpassing commercial inorganic LuAG:Ce scintillator. spatial resolution ‐based scintillating screen determined be 8.2 lp mm . In conjunction polymer thin film, feature halides offers exciting opportunities for achieving high‐quality flexible imaging.

Language: Английский

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