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1.
Chem Commun (Camb) ; 60(55): 6988-6998, 2024 Jul 04.
Artigo em Inglês | MEDLINE | ID: mdl-38895748

RESUMO

Lead halide perovskite nanocrystals (PNCs) hold immense promise in high-performance light-emitting diodes (LEDs) for future high-definition displays. Their adjustable bandgaps, vivid colors, and good carrier mobility are key factors that make them a potential game-changer. However, to fully harness their potential, the efficiency and long-term stability of PNCs-based light-emitting diodes (PNC-LEDs) must be enhanced. Recent material research results have shed light on the leading cause of performance decline in PNC-LEDs, which is ionic migration linked to surface defects and grain boundary imperfections. This review aims to present recent advancements in the modification strategies of PNCs, focusing on obtaining high-quality PNCs for LEDs. The PNC modification strategies are first summarized, including crystal structure regulation, nanocrystal size tuning, ligand exchange, and surface passivation. Then, the effects of these material design aspects on LED device performances, such as efficiency, brightness, and stability, are presented. Based on the efficient modification strategies, we propose promising material design insights for efficient and stable PNC-LEDs.

2.
Nano Lett ; 24(20): 6084-6091, 2024 May 22.
Artigo em Inglês | MEDLINE | ID: mdl-38717110

RESUMO

Chiral perovskites play a pivotal role in spintronics and optoelectronic systems attributed to their chiral-induced spin selectivity (CISS) effect. Specifically, they allow for spin-polarized charge transport in spin light-emitting diodes (LEDs), yielding circularly polarized electroluminescence at room temperature without external magnetic fields. However, chiral lead bromide-based perovskites have yet to achieve high-performance green emissive spin-LEDs, owing to limited CISS effects and charge transport. Herein, we employ dimensional regulation and Sn2+-doping to optimize chiral bromide-based perovskite architecture for green emissive spin-LEDs. The optimized (PEA)x(S/R-PRDA)2-xSn0.1Pb0.9Br4 chiral perovskite film exhibits an enhanced CISS effect, higher hole mobility, and better energy level alignment with the emissive layer. These improvements allow us to fabricate green emissive spin-LEDs with an external quantum efficiency (EQE) of 5.7% and an asymmetry factor |gCP-EL| of 1.1 × 10-3. This work highlights the importance of tailored perovskite architectures and doping strategies in advancing spintronics for optoelectronic applications.

3.
Adv Mater ; : e2404815, 2024 May 08.
Artigo em Inglês | MEDLINE | ID: mdl-38719211

RESUMO

The solid electrolyte interphase (SEI) with lithium fluoride (LiF) is critical to the performance of lithium metal batteries (LMBs) due to its high stability and mechanical properties. However, the low Li ion conductivity of LiF impedes the rapid diffusion of Li ions in the SEI, which leads to localized Li ion oversaturation dendritic deposition and hinders the practical applications of LMBs at high-current regions (>3 C). To address this issue, a fluorophosphated SEI rich with fast ion-diffusing inorganic grain boundaries (LiF/Li3P) is introduced. By utilizing a sol electrolyte that contains highly dispersed porous LiF nanoparticles modified with phosphorus-containing functional groups, a fluorophosphated SEI is constructed and the presence of electrochemically active Li within these fast ion-diffusing grain boundaries (GBs-Li) that are non-nucleated is demonstrated, ensuring the stability of the Li || NCM811 cell for over 1000 cycles at fast-charging rates of 5 C (11 mA cm-2). Additionally, a practical, long cycling, and intrinsically safe LMB pouch cell with high energy density (400 Wh kg-1) is fabricated. The work reveals how SEI components and structure design can enable fast-charging LMBs.

4.
Angew Chem Int Ed Engl ; 63(17): e202400424, 2024 Apr 22.
Artigo em Inglês | MEDLINE | ID: mdl-38433094

RESUMO

Halide superionic conductors (SICs) are drawing significant research attention for their potential applications in all-solid-state batteries. A key challenge in developing such SICs is to explore and design halide structural frameworks that enable rapid ion movement. In this work, we show that the close-packed anion frameworks shared by traditional halide ionic conductors face intrinsic limitations in fast ion conduction, regardless of structural regulation. Beyond the close-packed anion frameworks, we identify that the non-close-packed anion frameworks have great potential to achieve superionic conductivity. Notably, we unravel that the non-close-packed UCl3-type framework exhibit superionic conductivity for a diverse range of carrier ions, including Li+, Na+, K+, and Ag+, which are validated through both ab initio molecular dynamics simulations and experimental measurements. We elucidate that the remarkable ionic conductivity observed in the UCl3-type framework structure stems from its significantly more distorted site and larger diffusion channel than its close-packed counterparts. By employing the non-close-packed anion framework as the key feature for high-throughput computational screening, we also identify LiGaCl3 as a promising candidate for halide SICs. These discoveries provide crucial insights for the exploration and design of novel halide SICs.

5.
Nanoscale ; 16(15): 7387-7395, 2024 Apr 18.
Artigo em Inglês | MEDLINE | ID: mdl-38545886

RESUMO

Inorganic cesium lead bromide nanocrystals (CsPbBr3 NCs) hold promising prospects for high performance green light-emitting diodes (LEDs) due to their exceptional color purity and high luminescence efficiency. However, the common ligands employed for passivating these indispensable NCs, such as long-chain organic ligands like oleic acid and oleylamine (OA/OAm), display highly dynamic binding and electronic insulating issues, thereby resulting in a low efficiency of the as-fabricated LEDs. Herein, we report a new zwitterionic short-branched alkyl sulfobetaine ligand, namely trioctyl(propyl-3-sulfonate) ammonium betaine (TOAB), to in situ passivate CsPbBr3 NCs via a feasible one-step solution synthesis, enabling efficiency improvement of CsPbBr3 NC-based LEDs. The zwitterionic TOAB ligand not only strengthened the surface passivation of CsPbBr3 NCs with a high photoluminescence quantum yield (PLQY) of 97%, but also enhanced the carrier transport in the fabricated CsPbBr3 NC thin films due to the short-branched alkyl design. Consequently, CsPbBr3 NCs passivated with TOAB achieved a green LED with an external quantum efficiency (EQE) of 7.3% and a maximum luminance of 5716 cd m-2, surpassing those of LEDs based on insulating long-chain ligand-passivated NCs. Our work provides an effective surface passivation ligand design to enhance the performance of CsPbBr3 NC-based LEDs.

6.
Adv Mater ; 36(15): e2310356, 2024 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-38232743

RESUMO

Li6PS5Cl (LPSC) is a very attractive sulfide solid electrolyte for developing high-performance all-solid-state lithium batteries. However, it cannot suppress the growth of lithium dendrites and then can only tolerate a small critical current density (CCD) before getting short-circuited to death. Learning from that a newly-developed LaCl3-based electrolyte (LTLC) can afford a very large CCD, a three-layer sandwich-structured electrolyte is designed by inserting LTLC inside LPSC. Remarkably, compared with bland LPSC, this hybrid electrolyte LPSC/LTLC/LPSC presents extraordinary performance improvements: the CCD gets increased from 0.51 to 1.52 mA cm-2, the lifetime gets prolonged from 7 h to >500 h at the cycling current of 0.5 mA cm-2 in symmetric cells, and the cyclability gets extended from 10 cycles to >200 cycles at the cycling rate of 0.5 C and 30 °C in Li|electrolyte|NCM721 full cells. The enhancing reasons are assigned to the capability of LTLC to scavenge lithium dendrites, forming a passive layer of Ta, La, and LiCl.

7.
Nat Commun ; 15(1): 251, 2024 Jan 04.
Artigo em Inglês | MEDLINE | ID: mdl-38177173

RESUMO

Colorful circularly polarized luminescence materials are desired for 3D displays, information security and asymmetric synthesis, in which single-emitted materials are ideal owing to self-absorption avoidance, evenly entire-visible-spectrum-covered photon emission and facile device fabrication. However, restricted by the synthesis of chiral broad-luminescent emitters, the realization and application of high-performing single-emitted full-color circularly polarized luminescence is in its infancy. Here, we disclose a single-emitted full-color circularly polarized luminescence system (spiral full-color emission generator), composed of whole-vis-spectrum emissive quantum dots and chiral liquid crystals. The system achieves a maximum luminescence dissymmetry factor of 0.8 and remains an order of 10-1 in visible region by tuning its photonic bandgap. We then expand it to a series of desired customized-color circularly polarized luminescence, build chiral devices and further demonstrate the working scenario in the photoinduced enantioselective polymerization. This work contributes to the design and synthesis of efficient chiroptical materials, device fabrication and photoinduced asymmetric synthesis.

8.
J Am Chem Soc ; 145(50): 27774-27787, 2023 Dec 20.
Artigo em Inglês | MEDLINE | ID: mdl-38079498

RESUMO

Solid electrolytes (SEs) are central components that enable high-performance, all-solid-state lithium batteries (ASSLBs). Amorphous SEs hold great potential for ASSLBs because their grain-boundary-free characteristics facilitate intact solid-solid contact and uniform Li-ion conduction for high-performance cathodes. However, amorphous oxide SEs with limited ionic conductivities and glassy sulfide SEs with narrow electrochemical windows cannot sustain high-nickel cathodes. Herein, we report a class of amorphous Li-Ta-Cl-based chloride SEs possessing high Li-ion conductivity (up to 7.16 mS cm-1) and low Young's modulus (approximately 3 GPa) to enable excellent Li-ion conduction and intact physical contact among rigid components in ASSLBs. We reveal that the amorphous Li-Ta-Cl matrix is composed of LiCl43-, LiCl54-, LiCl65- polyhedra, and TaCl6- octahedra via machine-learning simulation, solid-state 7Li nuclear magnetic resonance, and X-ray absorption analysis. Attractively, our amorphous chloride SEs exhibit excellent compatibility with high-nickel cathodes. We demonstrate that ASSLBs comprising amorphous chloride SEs and high-nickel single-crystal cathodes (LiNi0.88Co0.07Mn0.05O2) exhibit ∼99% capacity retention after 800 cycles at ∼3 C under 1 mA h cm-2 and ∼80% capacity retention after 75 cycles at 0.2 C under a high areal capacity of 5 mA h cm-2. Most importantly, a stable operation of up to 9800 cycles with a capacity retention of ∼77% at a high rate of 3.4 C can be achieved in a freezing environment of -10 °C. Our amorphous chloride SEs will pave the way to realize high-performance high-nickel cathodes for high-energy-density ASSLBs.

9.
Chem Soc Rev ; 52(16): 5516-5540, 2023 Aug 14.
Artigo em Inglês | MEDLINE | ID: mdl-37482807

RESUMO

Lead halide perovskite nanocrystals are promising for next-generation high-definition displays, especially in light of their tunable bandgaps, high color purities, and high carrier mobility. Within the past few years, the external quantum efficiency of perovskite nanocrystal-based light-emitting diodes has progressed rapidly, reaching the standard for commercial applications. However, the low operational stability of these perovskite nanocrystal-based light-emitting diodes remains a crucial issue for their industrial development. Recent experimental evidence indicates that the migration of ionic species is the primary factor giving rise to the performance degradation of perovskite nanocrystal-based light-emitting diodes, and ion migration is closely related to the defects on the surface of perovskite nanocrystals and at the grain boundaries of their thin films. In this review, we focus on the central idea of surface reconstruction of perovskite nanocrystals, discuss the influence of surface defects on halide ion migration, and summarize recent advances in resurfacing perovskite nanocrystal strategies toward mitigating halide ion migration to improve the stability of the as-fabricated light-emitting diode devices. From the perspective of perovskite nanocrystal resurfacing, we set out a promising research direction for improving both the spectral and operational stability of perovskite nanocrystal-based light-emitting diodes.

10.
Phys Chem Chem Phys ; 25(16): 11665-11672, 2023 Apr 26.
Artigo em Inglês | MEDLINE | ID: mdl-37051730

RESUMO

The possibility of controlling fragment branching in the dissociation and ionization channels of HD+ is theoretically explored by synthesized intense fields using 790 nm and 395 nm pulses. In the control scheme, the branching ratios of the fragments to different channels (H + D+, D + H+ and H+ + D+) are manipulated by regulating the relative phase and intensity between the 790 nm and 395 nm pulses. Altering the relative phase can induce constructive or destructive interference between the net two photon process and the direct one photon process, and the highest modulation reaches 80% between the two dissociation fragments (H + D+ and D + H+). The high selectivity of the ionization fragment (H+ + D+) is achieved by tuning the relative intensity, since the ionization rate is not only related to the internuclear distance, but also to the instantaneous intensity of field strength. The results demonstrate that the synthesized ω-2ω laser pulse can provide an efficient control over the strong-field fragments of HD+.

11.
Nano Lett ; 23(8): 3385-3393, 2023 Apr 26.
Artigo em Inglês | MEDLINE | ID: mdl-37052258

RESUMO

Lead halide perovskite nanocrystals (LHP NCs) are regarded as promising emitters for next-generation ultrahigh-definition displays due to their high color purity and wide color gamut. Recently, the external quantum efficiency (EQE) of LHP NC based light-emitting diodes (PNC LEDs) has been rapidly improved to a level required by practical applications. However, the poor operational stability of the device, caused by halide ion migration at the grain boundary of LHP NC thin films, remains a great challenge. Herein, we report a resurfacing strategy via pseudohalogen ions to mitigate detrimental halide ion migration, aiming to stabilize PNC LEDs. We employ a thiocyanate solution processed post-treatment method to efficiently resurface CsPbBr3 NCs and demonstrate that the thiocyanate ions can effectively inhibit bromide ion migration in LHP NC thin films. Owing to thiocyanate resurfacing, we fabricated LEDs with a high EQE of 17.3%, a maximum brightness of 48000 cd m-2, and an excellent operation half-life time.

12.
Nature ; 616(7955): 77-83, 2023 04.
Artigo em Inglês | MEDLINE | ID: mdl-37020008

RESUMO

Inorganic superionic conductors possess high ionic conductivity and excellent thermal stability but their poor interfacial compatibility with lithium metal electrodes precludes application in all-solid-state lithium metal batteries1,2. Here we report a LaCl3-based lithium superionic conductor possessing excellent interfacial compatibility with lithium metal electrodes. In contrast to a Li3MCl6 (M = Y, In, Sc and Ho) electrolyte lattice3-6, the UCl3-type LaCl3 lattice has large, one-dimensional channels for rapid Li+ conduction, interconnected by La vacancies via Ta doping and resulting in a three-dimensional Li+ migration network. The optimized Li0.388Ta0.238La0.475Cl3 electrolyte exhibits Li+ conductivity of 3.02 mS cm-1 at 30 °C and a low activation energy of 0.197 eV. It also generates a gradient interfacial passivation layer to stabilize the Li metal electrode for long-term cycling of a Li-Li symmetric cell (1 mAh cm-2) for more than 5,000 h. When directly coupled with an uncoated LiNi0.5Co0.2Mn0.3O2 cathode and bare Li metal anode, the Li0.388Ta0.238La0.475Cl3 electrolyte enables a solid battery to run for more than 100 cycles with a cutoff voltage of 4.35 V and areal capacity of more than 1 mAh cm-2. We also demonstrate rapid Li+ conduction in lanthanide metal chlorides (LnCl3; Ln = La, Ce, Nd, Sm and Gd), suggesting that the LnCl3 solid electrolyte system could provide further developments in conductivity and utility.

13.
Phys Rev Lett ; 130(11): 113201, 2023 Mar 17.
Artigo em Inglês | MEDLINE | ID: mdl-37001077

RESUMO

We report the ionization reduction of atoms in two-color femtosecond laser fields in this joint theoretical-experimental study. For the multiphoton ionization of atoms using a 400 nm laser pulse, the ionization probability is reduced if another relatively weak 800 nm laser pulse is overlapped. Such ionization reduction consistently occurs regardless of the relative phase between the two pulses. The time-dependent Schrödinger equation simulation results indicate that with the assisted 800 nm photons the electron can be launched to Rydberg states with large angular quantum numbers, which stand off the nuclei and thus are hard to be freed in the multiphoton regime. This mechanism works for hydrogen, helium, and probably some other atoms if two-color laser fields are properly tuned.

14.
Hereditas ; 160(1): 14, 2023 Mar 29.
Artigo em Inglês | MEDLINE | ID: mdl-36978173

RESUMO

BACKGROUND: Dongxiang group, as an important minority, resides in Gansu province which is located at the northwest China, forensic detection system with more loci needed to be studied to improve the application efficiency of forensic case investigation in this group. METHODS: A 60-plex system including 57 autosomal deletion/insertion polymorphisms (A-DIPs), 2 Y chromosome DIPs (Y-DIPs) and the sex determination locus (Amelogenin) was explored to evaluate the forensic application efficiencies of individual discrimination, kinship analysis and biogeographic origin prediction in Gansu Dongxiang group based on the 60-plex genotype results of 233 unrelated Dongxiang individuals. The 60-plex genotype results of 4582 unrelated individuals from 33 reference populations in five different continents were also collected to analyze the genetic background of Dongxiang group and its genetic relationships with other continental populations. RESULTS: The system showed high individual discrimination power, as the cumulative power of discrimination (CPD), cumulative power of exclusion (CPE) for trio and cumulative match probability (CMP) values were 0.99999999999999999999997297, 0.999980 and 2.7029E- 24, respectively. The system could distinguish 98.12%, 93.78%, 82.18%, 62.35% and 39.32% of full sibling pairs from unrelated individual pairs, when the likelihood ratio (LR) limits were set as 1, 10, 100, 1000 and 10,000 based on the simulated family samples, respectively. Additionally, Dongxiang group had the close genetic distances with populations in East Asia, especially showed the intimate genetic relationships with Chinese Han populations, which were concluded from the genetic affinities and genetic background analyses of Dongxiang group and 33 reference populations. In terms of the effectiveness of biogeographic origin inference, different artificial intelligent algorithms possessed different efficacies. Among them, the random forest (RF) and extreme gradient boosting (XGBoost) algorithm models could accurately predict the biogeographic origins of 99.7% and 90.59% of three and five continental individuals, respectively. CONCLUSION: This 60-plex system had good performance for individual discrimination, kinship analysis and biogeographic origin prediction in Dongxiang group, which could be used as a powerful tool for case investigation.


Assuntos
População do Leste Asiático , Genética Populacional , Humanos , China , População do Leste Asiático/genética , Frequência do Gene , Repetições de Microssatélites , Polimorfismo Genético , Grupos Minoritários
15.
J Am Chem Soc ; 2023 Feb 01.
Artigo em Inglês | MEDLINE | ID: mdl-36724236

RESUMO

Nations, industries, and aspects of everyday life have undergone forgery and counterfeiting ever since the emergence of commercialization. Securing documents and products with anticounterfeit additives shows promise for authentication, allowing one to combat ever-increasing global counterfeiting. One most-used effective encryption strategy is to combine with optical-security markers on the required protection objects; however, state-of-the-art labels still suffer from imitation due to their poor complexity and easy forecasting, as a result of deterministic production. Developing advanced anticounterfeiting tags with unusual optical characters and further incorporating complex security features are desired to achieve multimodal, unbreakable authentication capacity; unfortunately, this has not yet been achieved. Here, we prepare a series of stable circularly polarized luminescence (CPL) materials, composed of toxicity-free, high-quality-emitting inorganic quantum dots (QDs) and liquid crystals, using a designed helical-coassembly strategy. This CPL system achieves a figure of merit (FM, assessing the performance of both luminescence dissymmetry and quantum yield) value of 0.39, fulfilling practical demands for anticounterfeiting applications. Based on these CPL structures, we produce a type of multimodal-responsive security materials (MRSMs) that exhibits six different stimuli-responsive modes, including light activation, polarization, temperature, voltage, pressure, and view angle. Thus, we show a proof-of-principle blockchain-like integrated anticounterfeiting system, allowing multimodal-responsive, interactive/changeable information encryption-decryption. We further encapsulate the obtained security materials into a fiber to expand our materials to work on flexible fabrics, that is, building an intelligent textile with a color-adaptable function along with environmental change.

16.
Sci Adv ; 8(45): eabq2321, 2022 Nov 11.
Artigo em Inglês | MEDLINE | ID: mdl-36367940

RESUMO

Solution-processable all-inorganic CsPbI3-xBrx perovskite holds great potential for pure red light-emitting diodes. However, the widely existing defects in this mixed halide perovskite markedly limit the efficiency and stability of present light-emitting diode devices. We here identify that intragrain Ruddlesden-Popper planar defects are primary forms of such defects in the CsPbI3-xBrx thin film owing to the lattice strain caused by inhomogeneous halogen ion distribution. To eliminate these defects, we develop a stepwise metastable phase crystallization strategy to minimize the CsPbI3-xBrx perovskite lattice strain, which brings planar defect-free CsPbI3-xBrx thin film with improved radiative recombination, narrowed emission band, and enhanced spectral stability. Using these high-quality thin films, we fabricate spectrally stable pure red perovskite light-emitting diodes, showing 17.8% external quantum efficiency and 9000 candela meter-2 brightness with color coordinates required by Rec. 2020.

17.
Orthop J Sports Med ; 10(8): 23259671221115743, 2022 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-36051971

RESUMO

Background: Rotator cuff pathology is a common cause of pain and shoulder dysfunction. Several nonoperative treatment modalities have been developed for rotator cuff lesions, but their relative efficacy is not well-established. Purpose/Hypothesis: The purpose of this systematic review and meta-analysis was to evaluate the efficacy and safety of sodium hyaluronate (SH) in the treatment of patients with rotator cuff lesions. It was hypothesized that SH would be found to be more effective than other nonoperative regimens. Study Design: Systematic review; Level of evidence, 3. Methods: We searched various databases to identify eligible studies that evaluated the effects of SH on the pain and shoulder dysfunction attributed to rotator cuff lesions. Outcome measures were pain visual analog scale (VAS) score; Constant score; University of California, Los Angeles (UCLA) score; satisfaction rate; complications; and factors affecting the pain VAS score. Outcomes were reported as weighted mean difference (WMD) or risk ratio. Results: A total of 9 studies were identified for data analysis. Compared with patients treated with other nonoperative treatments (controls), those treated with SH had significantly improved pain VAS scores at 1 week (WMD = -0.95; 95% CI, -1.75 to -0.16; P = .019), 2 weeks (WMD = -1.05; 95% CI, -2.07 to -0.03; P = .044), 3 weeks (WMD = -1.49; 95% CI, -2.88 to -0.11; P = .035), and 4 weeks (WMD = -2.12; 95% CI, -4.05 to -0.19; P = .031). The Constant score was significantly improved in the SH group versus controls at 2 weeks (WMD = 3.25; 95% CI, 2.36 to 4.13; P < .001), 3 months (WMD = 20.28; 95% CI, 0.54 to 40.03; P = .044), and 6 months (WMD = 5.58; 95% CI, 0.94 to 10.21; P = .018). The UCLA score and satisfaction rate did not differ significantly between the 2 groups. No complications associated with SH were reported in the included studies. Metaregression analysis showed that, except for study design (coefficient = -1.64; 95% CI, -2.64 to -0.63; P = .002), none of the variables (sample size, tear type, control treatments) significantly predicted the difference in VAS pain score between SH and other treatments. Conclusion: The present meta-analysis demonstrated that SH was effective in treating patients with rotator cuff lesions.

18.
Plants (Basel) ; 11(15)2022 Aug 04.
Artigo em Inglês | MEDLINE | ID: mdl-35956523

RESUMO

Grassland is the dominant vegetation type in the Loess Plateau, and grassland productivity and processes are limited by nitrogen (N) and phosphorus (P). Studies have shown that productivity would change following fertilization in the grassland. The response of productivity to fertilization mainly depends on the dominant species traits. Trait-based methods provide a useful tool for explaining the variations in grassland productivity following fertilization. However, the relative contribution of plant functional traits to grassland productivity under N and P addition in the Loess Plateau is not clear. We measured aboveground biomass (AGB) and leaf N content (LN), leaf P content (LP), leaf N/P ratio (LN/P), specific leaf area (SLA), leaf tissue density (LTD), leaf dry matter content (LDMC), and maximum plant height (Hmax) to study how these plant functional traits regulate the relative biomass of different species and grassland productivity following fertilization. Our results showed, that under different nutrient addition levels, the linkages between plant functional traits and the relative biomass of different species were different. Community AGB was positively related to community-weighted mean LN (CWM_LN), CWM_LN/P, CWM_SLA, and CWM_Hmax, but negatively related to CWM_LTD and CWM_LDMC. Dominant species traits largely determined grassland productivity, in line with the mass ratio hypothesis. These findings further highlight the close linkages between community-level functional traits and grassland productivity. Our study contributes to the mechanisms underlying biodiversity-ecosystem function relationships and has significance for guiding semiarid grassland management.

19.
Angew Chem Int Ed Engl ; 61(38): e202208960, 2022 Sep 19.
Artigo em Inglês | MEDLINE | ID: mdl-35861476

RESUMO

Thermochromic phosphors are intriguing materials for realizing thermochromic behaviors of light-emitting diodes. Here a highly luminescent and stable thermochromic phosphor based on one-dimensional Cu4 I6 (4-dimethylamino-1-ethylpyridinium)2 is reported. This unique ionic copper-iodine chain-based hybrid exhibits near-unity photoluminescence efficiency owing to the through-space charge-transfer character of relevant electronic transitions. More importantly, an alternative mechanism of thermochromic phosphorescence was unraveled, supported by a first principles simulation of concerted copper atom migration in the copper-iodine chain. Furthermore, we successfully fabricate a bright thermochromic light-emitting diode using this Cu4 I6 (4-dimethylamino-1-ethylpyridinium)2 thermochromic phosphor. Our reported flexible ionic copper-iodine chain-based thermochromic luminescent material represents a new type of cost-effective functional phosphor.

20.
Nat Commun ; 13(1): 3339, 2022 06 09.
Artigo em Inglês | MEDLINE | ID: mdl-35680921

RESUMO

Hierarchically structured chiral luminescent materials hold promise for achieving efficient circularly polarized luminescence. However, a feasible chemical route to fabricate hierarchically structured chiral luminescent polycrystals is still elusive because of their complex structures and complicated formation process. We here report a biomimetic non-classical crystallization (BNCC) strategy for preparing efficient hierarchically structured chiral luminescent polycrystals using well-designed highly luminescent homochiral copper(I)-iodide hybrid clusters as basic units for non-classical crystallization. By monitoring the crystallization process, we unravel the BNCC mechanism, which involves crystal nucleation, nanoparticles aggregation, oriented attachment, and mesoscopic transformation processes. We finally obtain the circularly polarized phosphors with both high luminescent efficiency of 32% and high luminescent dissymmetry factor of 1.5 × 10-2, achieving the demonstration of a circularly polarized phosphor converted light emitting diode with a polarization degree of 1.84% at room temperature. Our designed BNCC strategy provides a simple, reliable, and large-scale synthetic route for preparing bright circularly polarized phosphors.


Assuntos
Biomimética , Medições Luminescentes , Cristalização , Luminescência
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