Polar Alternating Cations Intercalated Hybrid Perovskite with Iodine‐Substituted Spacers Toward Efficient Passive X‐Ray Detection

Advanced Functional Materials, Год журнала: 2024, Номер unknown

Опубликована: Июль 30, 2024

Abstract 2D hybrid perovskites, with their high X‐ray absorption and extended carrier transport, present excellent promise for efficient direct detection. However, most of the current devices require external bias voltage, which results in need significant energy consumption severe ion migration, therefore, it is urgent to develop new types materials achieving passive Herein, two novel chiral polar alternating cations intercalation (ACI)‐type perovskite materials, named ( R / S ‐PPA)(IEA)PbBr 4 1‐ , )‐PPA = ‐1‐phenylpropylamine; IEA iodoethylamine), are constructed by integrating aromatic spacer ‐PPA iodine‐substituted IEA. Various intermolecular interactions, such as I···I, C─H···I, π···π introduced due introduction I‐substituted chain amines, effectively suppresses migration thus lead improved operational stability. The device along axis displays superior detection performance, relatively sensitivity an ultra‐low limit (LoD) 3.0 nGy s −1 making first ACI‐type material realizing Furthermore, also presents low dark drift exceptional irradiation This work provides thought using high‐performance

Язык: Английский

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Quasi‐CW Amplified Spontaneous Emission in Air‐Processed Quasi‐2D Perovskite Thin Films with High Stability

Advanced Functional Materials, Год журнала: 2024, Номер 34(23)

Опубликована: Янв. 18, 2024

Abstract Due to the hydrophobic organic cations, quasi‐two‐dimensional (quasi‐2D) lead halide perovskite materials have shown better moisture resistance. However, inappropriate multiphase structure in quasi‐2D films seriously affects efficient transport of energy from low‐n domains high‐n domains, especially when prepared air. Herein, study develops 30% ± 10% humidity and studies their amplified spontaneous emission (ASE) properties. It can be seen that phase disproportionation air is greatly suppressed by manipulating crystallization kinetics via using additive benzimidazole (BI), thereby enabling a narrowed distribution. improvement transfer efficiency, surface roughness, stability, ASE with low threshold 13.4 µJ cm −2 realized under quasi‐continuous pumping condition, which significantly <28.8 pristine film. Furthermore, introduction BI enhanced number peak intensity half‐decay pulses as high 5.6 × 10 7 , indicating good operating stability BI‐treated films. This work suggests provide possibility for preparing high‐performance lasers

Язык: Английский

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Precursor Engineering Induced High-Efficiency Electroluminescence of Quasi-Two-Dimensional Perovskites: A Synergistic Defect Inhibition and Passivation Approach

Nano Letters, Год журнала: 2024, Номер 24(13), С. 3952 - 3960

Опубликована: Март 25, 2024

Despite light-emitting diodes (LEDs) based on quasi-two-dimensional (Q-2D) perovskites being inexpensive and exhibiting high performance, defects still limit the improvement of electroluminescence efficiency stability by causing nonradiative recombination. Here, an organic molecule, 1-(o-tolyl) biguanide, is used to simultaneously inhibit passivate Q-2D via in situ synchronous crystallization. This molecule not only prevents surface bromine vacancies from forming through hydrogen bonding with intermediaries but also passivates its interaction uncoordinated Pb. Via combination defect inhibition passivation, trap density perovskite films can be significantly reduced, emission film improved. Consequently, corresponding LED shows external quantum 24.3%, operational has been increased nearly 15 times.

Язык: Английский

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Multiple Interlayer Interactions Enable Highly Stable X-ray Detection in 2D Hybrid Perovskites

JACS Au, Год журнала: 2024, Номер 4(6), С. 2393 - 2402

Опубликована: Июнь 10, 2024

Metal halide perovskites have outperformed conventional inorganic semiconductors in direct X-ray detection due to their ease of synthesis and intriguing photoelectric properties. However, the operational instability caused by severe ion migration under a high external electric field is still big concern for practical application perovskite detectors. Here, we report 2D (BPEA)2PbI4 (BPEA = R-1-(4-bromophenyl)ethylammonium) with Br-substituted aromatic spacer capable introducing abundant interactions, e.g., molecular electrostatic forces between Br atoms rings halogen bonds Br–I, interlayer space, which effectively suppresses thus enables superior stability. Constructing detectors based on high-quality single crystals results sensitivity 1,003 μC Gy–1 cm–2, low limit 366 nGy s–1, an ultralow baseline drift 3.48 × 10–8 nA cm–1 s–1 V–1 at 80 V bias. More strikingly, it also exhibits exceptional stability flux, long-time irradiation, large working voltage. This work shows integration multiple interactions stabilize detectors, providing new insights into future design optoelectronic devices toward application.

Язык: Английский

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Boosted Chirality Transfer in 2D Perovskites through Structural Isomer‐Driven Halogen–Halogen Interaction

Advanced Functional Materials, Год журнала: 2024, Номер unknown

Опубликована: Авг. 11, 2024

Abstract Chiral perovskites are promising materials due to their unique ability interact with circularly polarized light (CPL), offering great potential in advanced photonic and spintronic applications. However, specific design principles for highly chiroptically active chiral remain unclear, hindering practical exploitation. In this study, cation fluorinated isomerization approach is employed enhance the chiroptical response of perovskites. Specifically, it systematically discovered that incorporating ortho ‐fluorinated cations instead para induces a strong organic–inorganic halogen–halogen interaction spatial arrangement. This boosted chirality transfer, mediated by interaction, resulting fivefold improvement circular dichroism compared its para‐fluorinated counterpart. Consequently, CPL photodetector utilizing perovskite exhibited superior distinguishability 0.288, highest value among 2D lead‐iodide perovskite‐based devices. Furthermore, these structural isomers demonstrated extended operational stability as well high photodetecting performance.

Язык: Английский

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Strategic regulation of crystallization kinetics to achieve efficient pure-red quasi-2D perovskite light-emitting diodes

Chemical Engineering Journal, Год журнала: 2025, Номер unknown, С. 160278 - 160278

Опубликована: Фев. 1, 2025

Язык: Английский

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Suppressing Nonradiative Recombination in Pure Red Perovskites Toward Efficient Hybrid Perovskite/Organic Tandem White Light‐Emitting Diodes

Advanced Functional Materials, Год журнала: 2025, Номер unknown

Опубликована: Фев. 9, 2025

Abstract Perovskite light‐emitting diodes (PeLEDs) have recently attracted great interest for their superior electroluminescent properties. However, the development of pure red (620–660 nm) PeLEDs as an essential component display applications continues to be hampered by severe nonradiative recombination. Particularly, solution fabrication process perovskites poses a challenge in white PeLEDs, which further hinders commercialization. Herein, novel design is reported high‐efficiency hybrid perovskite/organic tandem (POTWLEDs) integrating bottom (640 PeLED units with top blue OLED units. To optimize device performance, 5‐Bromo‐2‐fluoropyridine (PD) introduced, featuring strong electronegative groups C─N and C─F, pyridine passivator into inhibit recombination passivating defects improving phase purity perovskite films, promotes maximum external quantum efficiency (EQE) 20.4%. By optimized units, efficient POTWLEDs are obtained high EQE values 25.9 23.7% CIE coordinates (0.279 0.339) (0.310 0.330), respectively. These represent highest efficiencies perovskite‐based (WLEDs), illustrating potential solid‐state lighting applications.

Язык: Английский

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Pressure-Driven Circularly Polarized Luminescence Enhancement and Chirality Amplification

Journal of the American Chemical Society, Год журнала: 2025, Номер unknown

Опубликована: Март 11, 2025

Achieving ultrahigh-color-purity circularly polarized luminescence (CPL) in low-dimensional chiral perovskites is challenging due to strong electron–phonon coupling caused by lead halide octahedral distortion. Herein, the piezoluminescence behaviors of six novel perovskites, (S/R-3-XPEA)2PbBr4 (PEA = phenethylamine; X F, Cl, Br), were systematically investigated. Upon compression, (S/R-3-ClPEA)2PbBr4 exhibits significant piezofluorochromic behaviors, transforming from yellow CPL deep-blue CPL. At 2.5 GPa, intensity increases an order magnitude and its asymmetry factors (glum) are amplified initial ±0.03 ±0.1. (S/R-3-BrPEA)2PbBr4 presents a similar piezochromic response, realizing at 1.7 while (S/R-3-FPEA)2PbBr4 retains under high pressure. High-pressure structural characterization theoretical calculations confirm that pressure-enhanced halogen bonds reduce penetration depth S/R-3-BrPEA+ S/R-3-ClPEA+ into [PbBr6]4– frameworks, significantly suppressing increasing magnetic transition dipole moment (S/R-3-ClPEA)2PbBr4, which responsible for ultrahigh-purity chirality amplification, respectively.

Язык: Английский

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2D Multilayered Perovskite Ferroelectric with Halogen Bond Induced Interlayer Locking Structure toward Efficient Self‐Powered X‐Ray Detection

Small, Год журнала: 2025, Номер unknown

Опубликована: Март 24, 2025

Abstract 2D Ruddlesden‐Popper (RP) hybrid perovskite ferroelectrics have emerged as a promising class of direct X‐ray detection materials. However, their intrinsic van der Waals gaps result in weak interlayer interactions that destabilize the layered motifs impacting stability detector. Thus, it is crucial but remains toughly challenge to enhance exploring stable RP ferroelectric detectors. Here, halogen bond proposed obtaining trilayered ferroelectric, (BrPA) 2 (EA) Pb 3 Br 10 ( BEPB , BrPA = 3‐bromopropylaminium; EA ethylammonium). Strikingly, strong Br···Br bonds lock cations inorganic skeletons, and C─H···Br hydrogen bridge adjacent spacing sheets, which effectively improves structural suppresses ion migration. The typical P‐E hysteresis loops reveal its concrete behaviors, giving large polarization ≈7.3 µC cm −2 . Consequently, ‐based detector results high sensitivity 562.6 Gy −1 at 0 V bias, most importantly, exhibits low baseline drift exceptional environmental stability. As far known, strengthening multilayered achieve efficient unprecedented, sheds light on future design optoelectronic devices toward practical applications.

Язык: Английский

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Multiple Interactions in Polar Lead‐Free Perovskites toward Highly Stable X‐Ray Detection

Advanced Science, Год журнала: 2025, Номер unknown

Опубликована: Апрель 3, 2025

Lead-free halide perovskites have emerged as a promising class of high-performance "green" X-ray detecting semiconductors due to their nontoxicity and strong absorption. However, ion migration caused by high operating electric field remains bottleneck limiting the long-term stability perovskite detectors. Herein, introducing multiple halogen interactions in lead-free perovskites, stable detection is successfully realized. Specifically, 0D polar bismuth (R/S-BPEA)4Bi2I10 (1R/1S, R/S-BPEA = R/S-1-(4-bromophenyl)ethylammonium) are designed Br-substituted chiral organic cation BPEA, which exists with molecular electrostatic forces between Br atom neighboring benzene ring interaction Br···I. Notably, introduction improves activation energy migration, makes dark current drift detector low 3.25 × 10-8 nA cm-1 s-1 V-1 at 2500 V cm-1. Furthermore, excellent operational under prolonged irradiation unchanged device sensitivity after 90 days exposure air, further demonstrates improved perovskites. Meanwhile, chiral-polar characteristic 1R/1S gives them potential for self-powered detection, limit 183 nGy zero bias single-crystal devices. This study opens new avenues future development "green", highly stable, radiation

Язык: Английский

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