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1.
Nano Lett ; 24(31): 9683-9690, 2024 Aug 07.
Artigo em Inglês | MEDLINE | ID: mdl-39052088

RESUMO

I-III-VI type semiconductor nanocrystals (NCs) have attracted considerable attention due to their environmental friendly nature and large-scale tunable emission. Herein, we report the successful synthesis of full-spectrum (470 to 614 nm) Ag-In-Ga-Zn-S (AIGZS) NCs by precisely regulating the In/Ga ratios using a facile one-pot method. Intriguingly, the photoluminescence (PL) peak width exhibits a continuous narrowing trend with extended reaction time, ultimately reaching a full width at half-maximum (fwhm) of 34 nm for green AIGZS NCs. Furthermore, the exciton relaxation dynamics of AIGZS NCs were systematically investigated using time-resolved photoluminescence and femtosecond transient absorption spectroscopy. Remarkably, we successfully fabricated blue, green, and red quantum-dot light-emitting diodes (QLEDs), forecasting the potential of AIGZS NCs with high color purity for applications in full-spectrum QLEDs.

2.
ACS Nano ; 18(32): 21523-21533, 2024 Aug 13.
Artigo em Inglês | MEDLINE | ID: mdl-39058309

RESUMO

Short-wave infrared (SWIR) light-emitting diodes (LEDs) have emerged as promising technologies for diverse applications such as optical communication, biomedical imaging, surveillance, and machine vision. Colloidal quantum dots (QDs) are particularly attractive for SWIR LEDs due to their solution processability, compatibility with flexible substrates, and tunable absorption and luminescence. However, the presence of toxic elements or precious metals in most SWIR-emitting QDs poses health, environmental, and cost challenges. In this context, CuInS2 (CIS) QDs are known for low toxicity, cost-effective fabrication, and SWIR-light emitting capability. However, CIS QDs have not yet been directly utilized to fabricate SWIR LEDs to date, which is due to low particle stability, inefficient charge carrier recombination, and significantly blue-shifted luminescence after integrating into LED devices. To address challenges, we propose a dual-passivation strategy using ZnI2 as a chemical additive to enhance both the optical property of plain CIS QDs and charge carrier recombination upon LED device implementation. The resulting CIS-QD-based LEDs exhibit a stable SWIR electroluminescence (EL) peak (over 1000 nm) with a high EL radiance and a record external quantum efficiency in the SWIR region. Our study represents a significant step forward in SWIR-QLED technology, offering a pathway for the development of high-performance, low-cost, and nontoxic SWIR light sources.

3.
J Phys Chem Lett ; 15(29): 7516-7523, 2024 Jul 25.
Artigo em Inglês | MEDLINE | ID: mdl-39023013

RESUMO

The utility of semiconductor nanocrystals (NCs) in light-emitting diodes (LED) has shown great potential in the field of display, whereas the challenge remains in developing efficient and stable cadmium-free blue-emitting LED devices due to the poor photophysical properties of blue-emitting NCs. Herein, we develop a controllable synthesis of Cu-Ga-Zn-S (CGZS) semiconductor NCs that show blue light emission with a relative photoluminescence quantum yield exceeding 90%. Furthermore, we have successfully fabricated a solution-processed quantum-dot LED (QLED) using CGZS NCs, achieving a notable maximum external quantum efficiency (EQE) of 1.00% at a luminance of 100 cd/m2. Our work lays a foundational framework for advancing cadmium-free blue-emitting QLEDs and facilitates the development of quantum dot electroluminescent panchromatic displays.

4.
ACS Nano ; 18(27): 17715-17724, 2024 Jul 09.
Artigo em Inglês | MEDLINE | ID: mdl-38916440

RESUMO

Colloidal nanoparticles offer unique photoelectric properties, making them promising for functional applications. Multiparticle systems exhibit synergistic effects on the functional properties of their individual components. However, precisely controlled assembly of multiparticles to form patterned building blocks for solid-state devices remains challenging. Here, we demonstrate a versatile multiparticle synergistic electrophoretic deposition (EPD) strategy to achieve controlled assembly, high-efficiency, and high-resolution patterns. Through elaborate surface design and charge regulation of nanoparticles, we achieve precise control over the particle distribution (gradient or homogeneous structure) in multiparticle films using the EPD technique. The multiparticle system integrates silicon oxide and titanium oxide nanoparticles, synergistically enhancing the emission efficiency of quantum dots to a high level in the field. Furthermore, we demonstrate the superiority of our strategy to integrate multiparticle into large-area full-color display panels with a high resolution over 1000 pixels per inch. The results suggest great potential for developing multiparticle systems and expanding diverse functional applications.

5.
ACS Appl Mater Interfaces ; 16(22): 28845-28852, 2024 Jun 05.
Artigo em Inglês | MEDLINE | ID: mdl-38776522

RESUMO

Perovskites have made remarkable advancements in optoelectronics owing to their high light absorption coefficient, tunable bandgap, and long charge diffusion. Nonetheless, the practical applications of Pb-based perovskites have been hindered by the instability and toxicity of Pb, especially in flexible electronics, which require high biosecurity and low toxicity. Hence, the development of stable Pb-free perovskite materials has gained increasing attention. In this study, we synthesized stable CsBi3I10 Pb-free perovskites outside the glovebox and improved the optoelectronic and mechanical performances of the CsBi3I10-based flexible devices through polyvinylcarbazole (PVK) doping. Flexible photodetectors with the device structure of PET/ITO/PEDOT:PSS/CsBi3I10:PVK/Au was fabricated. The results indicated that the introduction of poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) reduced the surface roughness of the flexible PET substrate, while PVK doping further improved the surface smoothness of CsBi3I10 thin films, thereby enhancing the interfacial charge transportation. Moreover, PEDOT:PSS and PVK acted as stepwise hole transport layers in the photodetectors. The device demonstrated a maximum responsivity of 0.3 A/W, detectivity of 2.6 × 1011 Jones, and a response time of 102 µs at 650 nm. After subjecting it to 1000 bending tests, the light current retained 80% of its initial value. This study presents a universally applicable method for controlling the surface morphology of a flexible perovskite thin film.

6.
Opt Lett ; 49(8): 1896-1899, 2024 Apr 15.
Artigo em Inglês | MEDLINE | ID: mdl-38621033

RESUMO

Next-generation display and lighting based on quantum dot light-emitting diodes (QLEDs) require a balanced electron injection of electron transport layers (ETLs). However, classical ZnO nanoparticles (NPs) as ETLs face inherent defects such as excessive electron injection and positive aging effects, urgently requiring the development of new types of ETL materials. Here, we show that high stability SnO2 NPs as ETL can significantly improve the QLED performance to 100567 cd·m-2 luminance, 14.3% maximum external quantum efficiency, and 13.1 cd·A-1 maximum current efficiency using traditional device structures after optimizing the film thickness and annealing the temperature. Furthermore, experimental tests reveal that by doping Zr4+ ions, the size of SnO2 NPs will reduce, dispersion will improve, and energy level will shift up. As expected, when using Zr-SnO2 NPs as the ETL, the maximum external quantum efficiency can reach 16.6%, which is close to the state-of-the-art QLEDs based on ZnO ETL. This work opens the door for developing novel, to the best of our knowledge, type ETLs for QLEDs.

7.
Small ; 20(26): e2310226, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38308112

RESUMO

Organic afterglow materials have significant applications in information security and flexible electronic devices with unique optical properties. It is vital but challenging to develop organic afterglow materials possessing controlled output with multi-stimuli-responsive capacity. Herein, dimethyl terephthalate (DTT) is introduced as a strong proton acceptor. The migration direction of N─H protons on two compounds Hs can be regulated by altering the excitation wavelength (Ex) or amine stimulation, thereby achieving dual-stimuli-responsive afterglow emission. When the Ex is below 300 nm, protons migrate to S1-2 DTT, where strong interactions induce phosphorescent emission of Hs, resulting in afterglow behavior. Conversely, when the Ex is above 300 nm, protons interact with the S0 DTT weakly and the afterglow disappears. In view of amine-based compounds with higher proton accepting capabilities, it can snatch proton from S1-2 DTT and redirect the proton flow toward amine, effectively suppressing the afterglow but obtaining a new redshifted fluorescence emission with Δλ over 200 nm due to the high polarity of amine. Moreover, it is successfully demonstrated that the applications of dual-stimuli-responsive organic afterglow materials in information encryption based on the systematic excitation-wavelength-dependent (Ex-De) behavior and amine selectivity detection.

8.
Nanoscale ; 16(9): 4591-4599, 2024 Feb 29.
Artigo em Inglês | MEDLINE | ID: mdl-38356393

RESUMO

Silver-based I-III-VI-type semiconductor nanocrystals have received extensive attention due to their narrow-band luminescence properties. Herein, we demonstrated a seed-mediated growth of quaternary Ag-In-Ga-S (AIGS) nanocrystals (NCs) with narrow-band luminescence. By conducting partial cation exchange with In3+ and Ga3+ based on Ag2S NCs and controlling the Ag/In feeding ratios (0.25 to 2) of Ag-In-S seeds as well as the inventory of 1-dodecanethiol, we achieved optimized luminescence performance in the synthesized AIGS NCs, characterized by a narrow full width at half maximum of less than 40 nm. Meanwhile, narrow-band luminescent AIGS NCs exhibit a tetragonal AgGaS2 crystal structure and a gradient alloy structure, rather than a core-shell structure. Most importantly, the kinetics decay curves of time-resolved photoluminescence and the ground state bleaching in transient absorption generally agree with each other regarding the lifetime of the second decay component, which indicates that the narrow-band luminescence is due to the slow radiative recombination between trapped electrons and trapped holes located at the edge of the conduction band and the deep silver-related trap states (e.g., silver vacancy), respectively. This study provides new insights into the correlation between the narrow-band luminescence properties and the structural characteristics of AIGS NCs.

9.
Small ; : e2307115, 2023 Dec 07.
Artigo em Inglês | MEDLINE | ID: mdl-38059744

RESUMO

The imbalance of charge injection is considered to be a major factor that limits the device performance of cadmium-free quantum-dot light-emitting diodes (QLEDs). In this work, high-performance cadmium-free Cu─In─Zn─S(CIZS)-based QLEDs are designed and fabricated through tailoring interfacial energy level alignment and improving the balance of charge injection. This is achieved by introducing a bilayered hole-injection layer (HIL) of Cu-doped NiOx (Cu─NiOx )/Poly(3,4-ethylenedioxythiophene): poly (styrene sulfonate) (PEDOT:PSS). High-quality Cu─NiOx film is prepared through a novel and straightforward sol-gel procedure. Multiple experimental characterizations and theoretical calculations show that the incorporation of Cu2+ ions can regulate the energy level structure of NiOx and enhance the hole mobility. The state-of-art CIZS-based QLEDs with Cu─NiOx /PEDOT:PSS bilayered HIL exhibit the maximum external quantum efficiency of 6.04% and half-life time of 48 min, which is 1.3 times and four times of the device with only PEDOT:PSS HIL. The work provides a new pathway for developing high-performance cadmium-free QLEDs.

10.
Nanomaterials (Basel) ; 13(22)2023 Nov 13.
Artigo em Inglês | MEDLINE | ID: mdl-37999290

RESUMO

Organometal halide perovskites have achieved great success in solution-processed photovoltaics. The explorations quickly expanded into other optoelectronic applications, including light-emitting diodes, lasers, and photodetectors. An in-depth analysis of the special scale effects is essential to understand the working mechanisms of devices and optimize the materials towards an enhanced performance. Generally speaking, organometal halide perovskites can be classified in two ways. By controlling the morphological dimensionality, 2D perovskite nanoplatelets, 1D perovskite nanowires, and 0D perovskite quantum dots have been studied. Using appropriate organic and inorganic components, low-dimensional organic-inorganic metal halide hybrids with 2D, quasi-2D, 1D, and 0D structures at the molecular level have been developed and studied. This provides opportunities to investigate the scale-dependent properties. Here, we present the progress on the characteristics of scale effects in organometal halide perovskites in these two classifications, with a focus on carrier diffusion, excitonic features, and defect properties.

11.
Cancer Med ; 12(19): 19595-19606, 2023 10.
Artigo em Inglês | MEDLINE | ID: mdl-37740601

RESUMO

BACKGROUND: Studies exploring whether metastatic organotropism and risk in gastric cancer (GC) differ by primary anatomical site are scarce. METHODS: This study included 15,260 and 1623 patients diagnosed with GC from the Surveillance, Epidemiology, and End Results (SEER) registry database and the Nanfang Hospital in China, respectively. Patients were stratified according to primary site of GC, and the incidence of metastasis to different organs was used to determine the metastatic organotropism for each GC subsite. Finally, the metastatic organotropism and risk were compared among the different subsite groups. RESULTS: Liver metastasis was the most common metastasis site in cardia GC, whereas other-site metastases were more common in the body, antrum, overlapping lesions, and unspecified GCs. Liver and other-site metastases were also frequently observed in the fundus, pylorus, lesser curvature, and greater curvature GCs. Patients with GC with definite primary tumor sites in the SEER and validation Nanfang hospital cohorts were compared by grouping as proximal and distal GCs for further analysis. In the SEER cohort, the top three metastatic sites of proximal GC were liver (21.4%), distant lymph node (LN) (14.6%), and other-site (mainly peritoneum, 11.9%), whereas those of distal GC were other-site (mainly peritoneum, 19.5%), liver (11.8%), and distant LN (9.5%). The incidence of metastasis to the liver, distant LN, lung, and brain was significantly higher in patients with proximal GC than in those with distal GC in both the SEER and Nanfang cohorts (p < 0.05). However, metastasis to other-site/peritoneum was significantly lower in patients with proximal GC compared to those with distal GC in the Nanfang Hospital and SEER cohorts, respectively (p < 0.05). CONCLUSION: Liver and distant LN are the preferred metastatic sites for proximal GC, whereas peritoneal metastasis is more common in distal GC. Proximal GC has a higher risk of lymphatic and hematogenous metastases, and a lower risk of transcoelomic metastasis than distal GC. Our findings highlight the need to stratify GC by its primary subsite to aid in planning and decision-making related to metastatic management in clinical practice.


Assuntos
Neoplasias Gástricas , Humanos , Estudos de Coortes , População do Leste Asiático , Prognóstico , Sistema de Registros/estatística & dados numéricos , Programa de SEER/estatística & dados numéricos , Neoplasias Gástricas/epidemiologia , Neoplasias Gástricas/patologia , Estados Unidos/epidemiologia , China
12.
Adv Mater ; 35(19): e2211235, 2023 May.
Artigo em Inglês | MEDLINE | ID: mdl-36906925

RESUMO

Lead-free double perovskites have emerged as a promising class of materials with potential to be integrated into a wide range of optical and optoelectronic applications. Herein, the first synthesis of 2D Cs2 AgInx Bi1- x Cl6 (0 ≤ x ≤ 1) alloyed double perovskite nanoplatelets (NPLs) with well controlled morphology and composition is demonstrated. The obtained NPLs show unique optical properties with the highest photoluminescence quantum yield of 40.1%. Both temperature dependent spectroscopic studies and density functional theory calculation results reveal that the morphological dimension reduction and In-Bi alloying effect together boost the radiative pathway of the self-trapped excitons of the alloyed double perovskite NPLs. Moreover, the NPLs exhibit good stability under ambient conditions and against polar solvents, which is ideal for all solution-processing of the materials in low-cost device manufacturing. The first solution-processed light-emitting diodes is demonstrated using the Cs2 AgIn0.9 Bi0.1 Cl6 alloyed double perovskite NPLs as the sole emitting component, showing luminance maximum of 58 cd m-2 and peak current efficiency of 0.013 cd A-1 . This study sheds light on morphological control and composition-property relationships of double perovskite nanocrystals, paving the way toward ultimate utilizations of lead-free perovskite materials in diverse sets of real-life applications.

13.
BMJ Case Rep ; 16(1)2023 Jan 12.
Artigo em Inglês | MEDLINE | ID: mdl-36634987

RESUMO

Vitamin B12 deficiency is a significant public health problem globally. Although it is a well-known cause of macrocytic anaemia and in advanced cases, pancytopenia, there remains a relative paucity of cases reported in pregnancy. It is associated with an increased risk of pregnancy complications and adverse birth outcomes such as neural tube defects, preterm birth, low birth weight, neurological sequelae and intrauterine death. It has a predilection for individuals aged >60 years. It has been implicated in a spectrum of neuropsychiatric disorders and it may also exert indirect cardiovascular effects. Severe vitamin B12 deficiency may present with haematological abnormalities that mimic thrombotic microangiopathy such as HELLP syndrome (haemolysis, elevated liver enzymes and low platelets) or it may present as pseudothrombotic microangiopathy (Moschcowitz syndrome) characterised by anaemia, thrombocytopenia and schistocytosis. It can also closely mimic thrombotic thrombocytopenia purpura, hence posing a diagnostic challenge to the unwary physician. Serological measurement of vitamin B12 levels confirms the diagnosis. Oral supplementation with vitamin B12 remains a safe and effective treatment. The authors describe the case of a multiparous woman in her late 20s presenting with a plethora of non-specific symptoms at 29+5 weeks' gestation. Her haemoglobin was 45 g/L, platelets 32×109/L, vitamin B12 <150 ng/L and serum folate <2 µg/L. She was not a vegetarian, but her diet lacked nutrition. Following parenteral B12 supplementation, her haematological parameters improved. The pregnancy was carried to term. Due to the plethora of non-specific symptoms, the diagnosis can be challenging to establish. Adverse maternal or fetal outcomes may occur. Folic acid supplementation may mask an occult vitamin B12 deficiency and further exacerbate or initiate neurological disease.


Assuntos
Pancitopenia , Complicações na Gravidez , Nascimento Prematuro , Púrpura Trombocitopênica Trombótica , Deficiência de Vitamina B 12 , Recém-Nascido , Gravidez , Feminino , Humanos , Vitamina B 12/uso terapêutico , Pancitopenia/complicações , Deficiência de Vitamina B 12/complicações , Deficiência de Vitamina B 12/diagnóstico , Deficiência de Vitamina B 12/tratamento farmacológico , Púrpura Trombocitopênica Trombótica/diagnóstico , Complicações na Gravidez/diagnóstico , Vitaminas , Ácido Fólico/uso terapêutico
14.
J Phys Chem Lett ; 13(51): 11857-11863, 2022 Dec 29.
Artigo em Inglês | MEDLINE | ID: mdl-36520488

RESUMO

I-III-VI type semiconductor nanocrystals (NCs) have attracted considerable attention in the display field. Herein, we realized the synthesis of narrow-bandwidth blue-emitting Ag-Ga-Zn-S (AGZS) NCs via a facile one-pot method. Intriguingly, the Ag/Zn feeding ratio and Ag/Ga feeding ratio are crucial for the realization of narrow-bandwidth AGZS NCs. By choosing a Ag/Zn feeding ratio of 4:1 and Ag/Ga feeding ratio of 1:8, AGZS NCs demonstrate a typical blue emission at 470 nm with a narrow full width at half-maximum (fwhm) of 48 nm, which is mainly generated from the band-to-hole recombination rather than the donor-acceptor pair (DAP) recombination. Furthermore, a solution-processed quantum-dot light-emitting device based on AGZS NCs exhibits a narrow electroluminescent bandwidth of 53 nm and high luminance over 123.1 cd m-2, as well as a high external quantum efficiency (EQE) of 0.40%. Our work highlights AGZS NCs with high color purity as an important candidate for blue-light-emitting devices.

15.
Opt Lett ; 47(11): 2722-2725, 2022 Jun 01.
Artigo em Inglês | MEDLINE | ID: mdl-35648914

RESUMO

A high color rendering index (CRI) and stable spectra under different voltages are important parameters for large-area planar light sources. However, the spectrum of most electroluminescent white light-emitting diodes (el-WLEDs) with a single emissive layer (EML) varies with a changing voltage. Herein, an el-WLED is fabricated based on Cd-free Cu-In-Zn-S (CIZS)/ZnS nanocrystals (NCs) and poly [(9,9-dioctylfluorenyl-2,7-diyl)-co-(4,4'-(N-(p-butylphenyl))diphenylamine)] (TFB) as double EMLs, which exhibit white-light emission with a high CRI value of 91 and commission internationale de l'éclairage (CIE) color coordinates of (0.33, 0.33). Meanwhile, it has a stable spectrum under voltage up to 7 V and a maximum luminance up to 679 cd/m2 with a low turn-on voltage of 2.2 V. This work provides a foundation for Cd-free el-WLEDs with high CRI and stable spectra.

16.
J Phys Chem Lett ; 13(22): 4856-4863, 2022 Jun 09.
Artigo em Inglês | MEDLINE | ID: mdl-35617309

RESUMO

Ternary Pb-free Cs-Cu-I perovskites have attracted widespread attention because of their excellent optical properties and environmentally friendly advantages. Herein, two different Pb-free ternary Cs3Cu2I5 nanocrystals (NCs) and CsCu2I3 microrods (MRs) were synthesized via a heating method. The phase and morphology transition from blue emission of Cs3Cu2I5 NCs to yellow emission of CsCu2I3 MRs could be tuned effectively by manipulating the reaction temperature, decreasing the maximum photoluminescence quantum yields (PLQYs) from 82.7% to ∼10%. More interestingly, the Cs3Cu2I5 NCs could self-assemble into stacking chains, which exhibited a strong dependence on the polarity of solvents. In addition, it was demonstrated that the rapid phase transition and luminescence tuning between Cs3Cu2I5 and CsCu2I3 films took only a few seconds by direct heating or exposure to the polar solvent. This work may deepen the understanding of the phase transition process in Cu-based perovskites and provide a fluorescence material with a short switching time for anticounterfeiting applications.

17.
J Phys Chem Lett ; 12(50): 12107-12113, 2021 Dec 23.
Artigo em Inglês | MEDLINE | ID: mdl-34910877

RESUMO

Monochromaticity for light-emitting diodes (LEDs) is an important parameter. However, carbon dots-based light-emitting diodes (CDs-LEDs) usually suffer from broad emission, which limits the development of this material. In this work, high-quality carbon dots (CDs) with a quantum yield of 16.2% were synthesized. When they were mixed with poly(N-vinyl carbazole) (PVK) to form a homogeneous film, the solid-state fluorescence of CDs was realized. After fabrication and systematic optimization of the device, the full width at half-maximum (fwhm) of EL spectra could be narrowed to 64 nm in comparison with the fwhm of 77 nm for PL, demonstrating that structural engineering is an effective approach for improving the color purity of CDs-LEDs. Meanwhile, the performance of the devices is improving. The obtained CDs-LEDs display high monochromaticity with a maximum luminance of 681 cd/m2. This work provides a new way to optimize the monochromaticity and performance of CDs-LEDs.

18.
J Phys Chem Lett ; 12(30): 7113-7119, 2021 Aug 05.
Artigo em Inglês | MEDLINE | ID: mdl-34296612

RESUMO

Combination of the merit of inorganic nanocrystals (NCs) and solution-processed conjugated polymer is a convenient strategy to obtain stable and efficient electroluminescent white-light-emitting diodes (el-WLEDs). In this work, an el-WLED was fabricated on the basis of Cd-free Cu-In-Zn-S (CIZS)/ZnS NCs blending with polyfluorene derivative poly[4-(octyloxy)-9,9-diphenylfluoren-2,7-diyl]-co-[5-(octyloxy)-9,9-diphenylfluoren-2,7-diyl] (PODPF), which exhibited a stable white light emission with a color rendering index value of 85. Meanwhile, it had a stable spectrum under high voltage due to the extremely weak energy transfer between PODPF and CIZS/ZnS NCs. To further improve the device performance, PC9O4 was used to replace PODPF, which presented better solubility and smoother film-forming properties. Thus, the maximum external quantum efficiency (EQE) of the optimized el-WLED was increased by 221% while maintaining a stable spectrum under high voltage. This work may provide a great foundation on color mixing cadmium-free el-WLEDs.

19.
Nano Lett ; 21(4): 1620-1627, 2021 Feb 24.
Artigo em Inglês | MEDLINE | ID: mdl-33570415

RESUMO

Morphology control represents an important strategy for the development of functional nanomaterials and has yet to be achieved in the case of promising lead-free double perovskite materials so far. In this work, high-quality Cs2AgBiX6 (X = Cl, Br, I) two-dimensional nanoplatelets were synthesized through a newly developed synthetic procedure. By analyzing the optical, morphological, and structural evolutions of the samples during synthesis, we elucidated that the growth mechanism of lead-free double perovskite nanoplatelets followed a lateral growth process from mono-octahedral-layer (half-unit-cell in thickness) cluster-based nanosheets to multilayer (three to four unit cells in thickness) nanoplatelets. Furthermore, we demonstrated that Cs2AgBiBr6 nanoplatelets possess a better performance in photocatalytic CO2 reduction compared with their nanocube counterpart. Our work demonstrates the first example with two-dimensional morphology of this important class of lead-free perovskite materials, shedding light on the synthetic manipulation and the application integration of such promising materials.

20.
ACS Energy Lett ; 5(6): 1840-1847, 2020 Jun 12.
Artigo em Inglês | MEDLINE | ID: mdl-33344767

RESUMO

We devised a hot-injection synthesis to prepare colloidal double-perovskite Cs2NaBiCl6 nanocrystals (NCs). We also examined the effects of replacing Na+ with Ag+ cations by preparing and characterizing Cs2Na1-x Ag x BiCl6 alloy NCs with x ranging from 0 to 1. Whereas Cs2NaBiCl6 NCs were not emissive, Cs2Na1-x Ag x BiCl6 NCs featured a broad photoluminescence band at ∼690 nm, Stokes-shifted from the respective absorption by ≥1.5 eV. The emission efficiency was maximized for low Ag+ amounts, reaching ∼3% for the Cs2Na0.95Ag0.05BiCl6 composition. Density functional theory calculations coupled with spectroscopic investigations revealed that Cs2Na1-x Ag x BiCl6 NCs are characterized by a complex photophysics stemming from the interplay of (i) radiative recombination via trapped excitons localized in spatially connected AgCl6-BiCl6 octahedra; (ii) surface traps, located on undercoordinated surface Bi centers, behaving as phonon-assisted nonradiative decay channels; and (iii) a thermal equilibrium between trapping and detrapping processes. These results offer insights into developing double-perovskite NCs with enhanced optoelectronic efficiency.

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