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1.
Adv Sci (Weinh) ; 11(32): e2401973, 2024 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-39189467

RESUMO

Precise control of quantum structures in hybrid nanocrystals requires advancements in scientific methodologies. Here, on the design of tunable CsPbBr3/Cs4PbBr6 quantum dots are reported by developing a unique discrete phase transformation approach in Cs4PbBr6 nanocrystals. Unlike conventional hybrid systems that emit solely in the green region, this current strategy produces adjustable luminescence in the blue (450 nm), cyan (480 nm), and green (510 nm) regions with high photoluminescence quantum yields up to 45%, 60%, and 85%, respectively. Concentration-dependent studies reveal that phase transformation mechanisms and the factors that drive CsBr removal occur at lower dilutions while the dissolution-recrystallization process dominates at higher dilutions. When the polymer-CsPbBr3/Cs4PbBr6 integrated into a field-effected transistor the resulting phototransistors featured enhanced photosensitivity exceeding 105, being the highest reported for an n-type phototransistor, while maintaining good transistor performances as compared to devices consisting of polymer-CsPbBr3 NCs.

2.
Adv Sci (Weinh) ; 11(35): e2404465, 2024 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-38995100

RESUMO

Low-dimensional lead halide perovskites demonstrate remarkable nonlinear optical characteristics attributed to their distinctive physical structures and electronic properties. Nevertheless, the investigation into their nonlinear optical properties remains in its incipient stages. This study addresses this gap by precisely controlling solvent volumes to synthesize both 0D Cs4PbBr6 and Cs4PbBr6/CsPbBr3 perovskites. Remarkably, as saturable absorbers, both pure Cs4PbBr6 and Cs4PbBr6/CsPbBr3 composites exhibit favorable nonlinear optical properties within the C-band, showcasing modulation depths of 9.22% and 16.83%, respectively. Moreover, for the first time, Cs4PbBr6 and Cs4PbBr6/CsPbBr3 composites have been successfully integrated into erbium-doped fiber lasers to realize the mode-locking operations. The utilization of the Cs4PbBr6/CsPbBr3 composites as a saturable absorber that enables the generation of conventional soliton mode-locked laser pulses with a pulse duration of 688 fs, and a repetition frequency of 10.947 MHz at a central wavelength of 1557 nm. Cs4PbBr6 is instrumental in generating laser pulses at a frequency of 10.899 MHz, producing pulse widths of 642 fs at the central wavelength of 1531.2 nm and 1.02 ps at the central wavelength of 1565.3 nm, respectively. The findings of this investigation underscore the potential utility of 0D Cs4PbBr6 and Cs4PbBr6/CsPbBr3 composites as promising materials for optical modulation within fiber laser applications.

3.
Small ; : e2404044, 2024 Jul 22.
Artigo em Inglês | MEDLINE | ID: mdl-39036834

RESUMO

Often deemed the "natural nemesis" of perovskites, water molecules have been largely circumvented by the majority of researchers in the field of perovskite solar cells. This has resulted in significant hurdles in investigating the beneficial impacts of water molecules on perovskite crystallization. Herein, it is found that by utilizing ethanol with minimal water content and subjecting all-inorganic perovskite to three distinct annealing temperatures within the same solvent, the residual CsBr can be effectively removed, and the formation of the Cs4PbBr6 phase can be curtailed. By selecting an optimal water content, substantial improvements are observed in the crystalline quality of CsPbBr3, the perovskite/carbon interface, and the mesoporous filling effect. The Urbach energy (Eu) is reduced from 38.96 to 35.59 meV, and the defect density decreased from 4.16 × 1014 to 3.39 × 1014 cm-3. As a result, the power conversion efficiency (PCE) improved from 7.55% in the control group to 9.37%. Under severe environmental conditions with a temperature (T) of 85 °C and a relative humidity (RH) of 40%, tracking tests over 1200 h retained 89.3% of the initial PCE. This research signifies a breakthrough in the fabrication of highly stable and efficient all-inorganic printable mesoscopic perovskite solar cells.

4.
Spectrochim Acta A Mol Biomol Spectrosc ; 316: 124379, 2024 Aug 05.
Artigo em Inglês | MEDLINE | ID: mdl-38692106

RESUMO

Metal halide perovskites are promising optoelectronic materials due to their outstanding luminescent properties. However, the instability of perovskites has long been the bottleneck to their practical applications. Here Cs4PbBr6 nanocrystals based glass composite (Cs4PbBr6 NCs@glass) are successfully prepared, which displays green emission color (520 nm), narrow bandwidth (23 nm) and a near-unity photoluminescence quantum yield (PLQY). The H2O molecules permeating in the lattice of Cs4PbBr6 were found to be a crucial role in the subband energy emission. The Cs4PbBr6 NCs@glass has excellent emission stability; maintains 93 % of initial PL intensity after ultraviolet light irradiation for over 5000 h. In addition, by adjusting the halogen content, we have achieved tunable emission color from blue (450 nm) to green (520 nm) and red (670 nm) on Cs4PbX6 NCs@glass (X = Cl, Br, I), which covers up to 127 % of the National Television Systems Board (NTSC) standard system. Our finding indicates the commercial applications of perovskite materials in lighting and display.

5.
ACS Appl Mater Interfaces ; 16(9): 11704-11714, 2024 Mar 06.
Artigo em Inglês | MEDLINE | ID: mdl-38406990

RESUMO

The microscale flow preparation scheme has been widely used in the preparation of inorganic perovskite nanocrystals (NCs). It is considered to be the most promising method for large-scale production. Recently, it has been suggested that increasing the precursor concentration can further improve efficiency, but there is still a lack of understanding of high-concentration synthesis. Here, we develop a microscale flow synthesis scheme using high-concentration precursors, and the typical concentration value in the reaction phase reaches 0.035 mol/L using cesium acetate. The CsPbBr3 NCs with sharp photoluminescence (PL) at 515.7 nm can be obtained, and their PL quantum yield after post-treatment exceeds 90%. The effect of the molar ratio of Pb/Cs (Rm), reaction time, reaction temperature, and excess ligands on this flow reaction is studied. Several new phenomena are observed in our experiment. At 120 °C, some Cs4PbBr6 NCs exist in addition to the usual CsPbBr3 nanoplatelets. Excess ligands lead to the formation of numerous Cs4PbBr6 NCs with a bright green PL, and these NCs will spontaneously transform into a nonemission form in the film. Moreover, mixed-halide CsPbBrxI3-x NCs and CsPbI3 NCs are also prepared in this scheme, and then they are used to obtain LEDs in a range of colors.

6.
Small ; 20(22): e2309107, 2024 May.
Artigo em Inglês | MEDLINE | ID: mdl-38145322

RESUMO

Synthesis of upconversion nanoparticles (UCNPs)-metal halide perovskites (MHPs) heterostructure is garnered immense attentions due to their unparalleled photophysical properties. However, the obvious difference in their structural forms makes it a huge challenge. Herein, hexagonal ß-NaYF4 and hexagonal Cs4PbBr6 are filtrated to construct the UCNP/MHP heterostructural luminescent material. The similarity in their crystal structures facilitate the heteroepitaxial growth of Cs4PbBr6 on the surface of ß-NaYF4 NPs, leading to the formation of high-quality ß-NaYF4:Yb,Tm/Cs4PbBr6 core/shell nanocrystals (NCs). Interestingly, this heterostructure endows the core/shell NCs with typically narrow-band green emission centered at 524 nm under 980 nm excitation, which should be attributed to the Förster resonance energy transfer (FRET) from Tm3+ to Cs4PbBr6. It is noteworthy that the FRET efficiency of ß-NaYF4:Yb,Tm/Cs4PbBr6 core/shell NCs (58.33%) is much higher than that of the physically mixed sample (1.84%). In addition, the reduced defect density, lattice anchoring effect, as well as diluted ionic bonding proportion induced by the core/shell structure further increase the excellent water-resistance and thermal cycling stability of Cs4PbBr6. These findings open up a new way to construct UCNP/MHP heterostructure with better multi-code luminescence performance and stability and promote its wide optoelectronic applications.

7.
ACS Appl Mater Interfaces ; 15(34): 40762-40771, 2023 Aug 30.
Artigo em Inglês | MEDLINE | ID: mdl-37595125

RESUMO

Despite the great success of hybrid CH3NH3PbI3 perovskite in photovoltaics, ascribed to its excellent optical absorption properties, its instability toward moisture is still an insurmountable drawback. All-inorganic perovskites are much less sensitive to humidity and have potential interest for solar cell applications. Alternative strategies have been developed to design novel materials with appealing properties, which include different topologies for the octahedral arrangements from three-dimensional (3D, e.g., CsPbBr3 perovskite) or two-dimensional (2D, e.g., CsPb2Br5) to zero-dimensional (0D, i.e., without connection between octahedra), as the case of Cs4PbX6 (X = Br, I) halides. The crystal structure of these materials is complex, and their thermal evolution is unexplored. In this work, we describe the synthesis of Cs4PbBr6-xIx (x = 0, 2, 4, 6) halides by mechanochemical procedures with green credentials; these specimens display excellent crystallinity enabling a detailed structural investigation from synchrotron X-ray powder diffraction (SXRD) data, essential to revisit some features in the temperature range of 90-298 K. In all this regime, the structure is defined in the trigonal R3̅c space group (#167). The presence of Cs and X vacancies suggests some ionic mobility into the crystal structure of these 0D halides. Bond valence maps (BVMs) are useful in determining isovalent surfaces for both Cs4PbBr6 and Cs4PbI6 phases, unveiling the likely ionic pathways for cesium and bromide ions and showing a full 3D connection in the bromide phase, in contrast to the iodide one. On the other hand, the evolution of the anisotropic displacement parameters is useful to evaluate the Debye temperatures, confirming that Cs atoms have more freedom to move, while Pb is more confined at its site, likely due to a higher covalency degree in Pb-X bonds than that in Cs-X bonds. Diffuse reflectance ultraviolet-visible (UV-vis) spectroscopy shows that the optical band gap can be tuned depending on iodine content (x) in the range of 3.6-3.06 eV. From density functional theory (DFT) simulations, the general trend of reducing the band gap when Br is replaced by I is well reproduced.

8.
Nanomaterials (Basel) ; 13(2)2023 Jan 15.
Artigo em Inglês | MEDLINE | ID: mdl-36678108

RESUMO

Inorganic lead halide perovskite is one of the most excellent fluorescent materials, and it plays an essential role in high-definition display and visible light communication (VLC). Its photochromic properties and stability determine the final performance of light-emitting devices. However, efficiently synthesizing perovskite with high quality and stability remains a significant challenge. Here, we develop a facile and environmentally friendly method for preparing high-stability and strong-emission CsPbBr3/Cs4PbBr6 composites using ultrasonication and liquid paraffin. Tuning the contents of liquid paraffin, bright-emission CsPbBr3/Cs4PbBr6 composite powders with a maximum PLQY of 74% were achieved. Thanks to the protection of the Cs4PbBr6 matrix and liquid paraffin, the photostability, thermostability, and polar solvent stability of CsPbBr3/Cs4PbBr6-LP are significantly improved compared to CsPbBr3 quantum dots and CsPbBr3/Cs4PbBr6 composites that were prepared without liquid paraffin. Moreover, the fabricated CsPbBr3/Cs4PbBr6-LP-based WLEDs show excellent luminescent performance with a power efficiency of 129.5 lm/W and a wide color gamut, with 121% of the NTSC and 94% of the Rec. 2020, demonstrating a promising candidate for displays. In addition, the CsPbBr3/Cs4PbBr6-LP-based WLEDs were also demonstrated in a VLC system. The results suggested the great potential of these high-performance WLEDs as an excitation light source to achieve VLC.

9.
Adv Mater ; 34(31): e2203226, 2022 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-35679199

RESUMO

The 0D cesium lead halide perovskite Cs4 PbBr6 has drawn remarkable interest due to its highly efficient robust green emission compared to its 3D CsPbBr3 counterpart. However, seizing the advantages of the superior photoluminescence properties for practical light-emitting devices remains elusive. To date, Cs4 PbBr6 has been employed only as a higher-bandgap nonluminescent matrix to passivate or provide quantum/dielectric confinement to CsPbBr3 in light-emitting devices and to enhance its photo-/thermal/environmental stability. To resolve this disparity, a novel solvent engineering method to incorporate highly luminescent 0D Cs4 PbBr6 nanocrystals (perovskite nanocrystals (PNCs)) into a 3D CsPbBr3 film, forming the active emissive layer in single-layer perovskite light-emitting electrochemical cells (PeLECs) is designed. A dramatic increase of the maximum external quantum efficiency and luminance from 2.7% and 6050 cd m-2 for a 3D-only PeLEC to 8.3% and 11 200 cd m-2 for a 3D-0D PNC device with only 7% by weight of 0D PNCs is observed. The majority of this increase is driven by the efficient inherent emission of the 0D PNCs, while the concomitant morphology improvement also contributes to reduced leakage current, reduced hysteresis, and enhanced operational lifetime (half-life of 129 h), making this one of the best-performing LECs reported to date.

10.
Polymers (Basel) ; 14(3)2022 Jan 19.
Artigo em Inglês | MEDLINE | ID: mdl-35160370

RESUMO

All-inorganic metal halide perovskite nanocrystals (IPeNCs) have become one of the most promising luminescent materials for next-generation display and lighting technology owing to their excellent color expression ability. However, research on IPeNCs with stable blue emission is limited. In this paper, we report stable blue emissive all-bromide IPeNCs obtained through a modified ligand-assisted reprecipitation method using an ultraviolet (UV)-curable prepolymer as the anti-solvent at a low temperature. We found that the blue emission originates from quantum-confined CsPbBr3 nanoparticles formed together with the colorless wide-bandgap Cs4PbBr6 nanocrystals. When the temperature of the prepolymer was increased from 0 to 50 °C, CsPbBr3 nanoparticles became larger and more crystalline, thereby altering their emission color from blue to green. The synthesized all-bromide blue-emitting IPeNC solution remained stable for over 1 h. It also remained stable when it was mixed with the green-emitting IPeNC solution. By simply exposing the as-synthesized IPeNC-prepolymer solutions to UV light, we formed water-stable composite films that emitted red, green, blue, and white colors. We believe that this synthetic method can be used to develop color-emitting composite materials that are highly suitable for application as the color conversion films of full-color liquid crystal display backlight systems and lighting applications.

11.
Front Chem ; 10: 828322, 2022.
Artigo em Inglês | MEDLINE | ID: mdl-35127638

RESUMO

Recently, perovskite light-emitting diodes (PeLEDs) have drew widespread attention due to their high efficiencies. However, because of the sensitivity to moisture and oxygen, perovskite luminescent layers are usually prepared in high-purity nitrogen environment, which increases the cost and process complexity of device preparation and seriously hindrances its commercialization of PeLED in lighting and display application. Herein, dual-phase all-inorganic composite CsPbBr3-Cs4PbBr6 films are fabricated from CsBr-rich perovskite solutions by a simple one-step spin-coating method in the air with high humidity. Compared with the pure CsPbBr3 film, the composite CsPbBr3-Cs4PbBr6 film has much stronger photoluminescence emission and longer fluorescence lifetime, accompanied by increased photoluminescence quantum yield (33%). As a result, we obtained green PeLED devices without hole transport layer exhibiting a maximum brightness of 72,082 cd/m2 and a maximum external quantum efficiency of about 2.45%, respectively. More importantly, the champion device shows excellent stability with operational half-lifetime exceeding 1,000 min under continuous operation in the air. The dual-phase all-inorganic composite CsPbBr3-Cs4PbBr6 film shows attractive prospect for advanced light emission applications.

12.
ACS Appl Mater Interfaces ; 13(28): 33199-33208, 2021 Jul 21.
Artigo em Inglês | MEDLINE | ID: mdl-34233117

RESUMO

Perovskite light-emitting devices (PeLEDs) have drawn a great deal of attention because of their exceptional optical and electrical properties. However, as for the blue PeLEDs based on low-dimensional (LD) CsPbBr3, the low conductivity of the widely used organic spacers as well as the difficulty of forming pure and uniform LD CsPbBr3 phase have severely inhibited the device performance such as stability and efficiency. In this work, we report an effective strategy to obtain high-quality LD CsPbBr3 by using a novel spacer of inorganic Cs4PbBr6 instead of the common long-chain ammonium halides. We found that a 3-amino-1-propanol (3AP)-modified PEDOT:PSS was helpful to stimulate the formation of the LD blue emissive CsPbBr3:Cs4PbBr6 composite. We also revealed that an additive of poly(vinylpyrrolidone) (PVP) in the precursor can limit further growth of LD perovskite phase into 3D perovskite phase upon annealing, thus resulting in a uniformly distributed LD perovskite with high color stability. Consequently, efficient blue PeLEDs @ 485 nm with a brightness of 2192 cd/m2, current efficiency of 2.68 cd/A, and external quantum efficiency of 2.3% was successfully achieved. More importantly, the device showed much improved working stability compared to those with the spacer of organic ammonium halides. Our results provide some helpful insights into developing efficient and stable blue PeLEDs.

13.
Luminescence ; 36(3): 631-641, 2021 May.
Artigo em Inglês | MEDLINE | ID: mdl-33171538

RESUMO

Due to indispensable ligands, polluted organic solution, or complex vapour deposition, stable CsPbBr3 film is hard to be prepared directly using a simple and environmentally friendly method. To improve the stability of CsPbBr3 film and its synthesis methods, the double-films solid phase reaction was developed, and Cs4 PbBr6 /CsPbBr3 composites were designed. Although the synthesized particle had a size of 2-5 µm, much larger than that of quantum dots, in ambient conditions the composites films still showed good photoluminescence properties, with the highest photoluminescence quantum yield of 80%. It had good stability against air, temperature and humidity, and even had interesting fluorescence-enhanced phenomenon after about 4 days.


Assuntos
Pontos Quânticos , Fluorescência
14.
Polymers (Basel) ; 12(2)2020 Feb 13.
Artigo em Inglês | MEDLINE | ID: mdl-32070002

RESUMO

Composite materials with different concentration ratios of a hybrid of zero-dimensional (0-D) Cs4PbBr6 perovskite, which acts as a donor (D), and poly[2-methoxy-5-(2-ethylhexyloxy)-1,4-phenylenevinylene] (MEH-PPV), which acts as an acceptor (A), were successfully prepared via a solution blending method prior to being deposited onto glass substrates by a spin-coating technique. The influence of acceptor content on the structural, optical, and energy transfer properties of the donor was investigated. The perovskite nanocrystals formed thin films without any chemical interactions within a matrix of MEH-PPV in the blend. The possibility of dipole-dipole (non-radiative) energy transfer from the 0-D Cs4PbBr6 to the MEH-PPV was proven. The energy transfer parameters such as Ro (critical distance of the energy transfer), kapp (apparent quenching constant), ∅DA (quantum yield of D in the presence of A), τDA (lifetime of D in the presence of A), PDA (probability of energy transfer), η (efficiency of energy transfer), RDA (energy transfer radius), kET (energy transfer rate constant), TDR (total decay rate), Ao (critical concentration of A), and Aπ (conjugation length) were calculated based on the absorption and emission measurements.

15.
ACS Nano ; 14(5): 5183-5193, 2020 May 26.
Artigo em Inglês | MEDLINE | ID: mdl-31774652

RESUMO

Halide perovskite (HP) nanocrystals (NCs) have recently shown great potential for X-ray detection and imaging. However, the practical application still has a long way to go with many technical requirements waiting to be fulfilled, including structure optimization, stability enhancement, and cost reduction. A design principle in this beginning stage is urgently needed but still lacking. Herein, with an "emitter-in-matrix" principle refined from commercial scintillators, CsPbBr3@Cs4PbBr6 with emissive CsPbBr3 NCs embedded inside a solid-state Cs4PbBr6 host is subjected to X-ray sensing and imaging. The Cs4PbBr6 matrix not only enhances the attenuation of X-rays but also dramatically improves the stability of CsPbBr3 NCs. A favorable optical design with the Cs4PbBr6 matrix being transparent to the emission from CsPbBr3 NCs enables efficient light output. As a result, stable and sensitive scintillation response to X-ray signals is demonstrated with superior linearity and ultrahigh time resolution. In order to show the huge potential for practical applications, X-ray imaging using a large-area film (360 mm × 240 mm) by the blade-coating technique is carried out to obtain a high-quality image of interior structures invisible to the human eye. In addition to the above advantages in optics, CsPbBr3@Cs4PbBr6 also enjoys facile solution synthesis with large scalability, excellent repeatability, and low cost.

16.
Nanomaterials (Basel) ; 9(9)2019 Sep 11.
Artigo em Inglês | MEDLINE | ID: mdl-31514284

RESUMO

All-inorganic cesium lead halide perovskite CsPbX3 (X = Cl, Br, I) nanocrystals (NCs) have attracted significant attention owing to their fascinating electronic and optical properties. However, researchers still face challenges to achieve highly stable and photoluminescent CsPbX3 NCs at room temperature by the direct-synthesis method. Herein, we synthesize CsPbX3 NCs by a facile and environmentally friendly method, which uses an aqueous solution of metal halides to react with Cs4PbBr6 NCs via interfacial anion exchange reactions and without applying any pretreatment. This method produces monodisperse and air-stable CsPbX3 NCs with tunable spectra covering the entire visible range, narrow photoluminescence emission bandwidth, and high photoluminescence quantum yield (PL QY, 80%). In addition, the chemical transformation mechanism between Cs4PbBr6 NCs and CsPbX3 NCs was investigated. The Cs4PbBr6 NCs were converted to CsPbBr3 NCs first by stripping CsBr, and then, the as-prepared CsPbBr3 NCs reacted with metal halides to form CsPbX3 NCs. This work takes advantage of the chemical transformation mechanism of Cs4PbBr6 NCs and provides an efficient and environmentally friendly way to synthesize CsPbX3 NCs.

17.
J Colloid Interface Sci ; 554: 133-141, 2019 Oct 15.
Artigo em Inglês | MEDLINE | ID: mdl-31295685

RESUMO

Here, Cs4PbBr6 microcrystals (MCs) are synthesized using a two-phase liquid-liquid immiscible method. In order to unravel the bright green photoluminescence (PL) mechanism for in-situ Cs4PbBr6 MCs, the thermal stability of PL spectra for the supernatant and precipitate of reactants is investigated comparatively. Exciton binding energy, exciton-phonon (EP) coefficient and PL lifetime all indicate that the PL of the precipitate has similar temperature dependence as that of the supernatant. It is found that, according to its structural and optical characteristics, the supernatant of the reactants is CsPbBr3 nanocrystals (NCs). We also find that the bright green PL from the precipitate of the reactants is due to CsPbBr3 NCs embedded into Cs4PbBr6 MCs. Experimental results further reveal the size of CsPbBr3 NCs embedded into Cs4PbBr6 MCs is larger than that of CsPbBr3 NCs in the supernatant. The surface passivation of the composites can thus help to suppress the thermal quenching of PL for CsPbBr3 NCs, which opens a new avenue for enhancing the thermal stability of PL for perovskite NCs.

18.
Adv Mater ; 31(24): e1900606, 2019 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-31058382

RESUMO

All-inorganic cesium lead halide perovskite nanocrystals (NCs) with different dimensionalities have recently fascinated the research community due to their extraordinary optoelectronic performance such as tunable bandgaps over the entire visible spectral region. However, compared to well-developed 3D CsPbX3 perovskites (X = Cl, Br, and I), the bandgap tuning in 0D Cs4 PbX6 perovskite NCs remains an arduous task. Herein, a simple but valid strategy is proposed to tailor the insulator bandgap (≈3.96 eV) of Cs4 PbBr6 NCs to the blue spectral region by changing the local coordination environment of isolated [PbBr6 ]4- octahedra in the Cs4 PbBr6 crystal through Sn cation doping. Benefitting from the unique Pb2+ -poor and Br- -rich reaction environment, the Sn cation is successfully introduced into the Cs4 PbBr6 NCs, forming coexisting point defects comprising substitutional SnPb and interstitial Bri , thereby endowing these theoretically nonluminescent Cs4 PbBr6 NCs with an ultranarrow blue emission at ≈437 nm (full width at half maximum, ≈12 nm). By combining the experimental results with first-principles calculations, an unusual electronic dual-bandgap structure, comprising the newly emerged semiconducting bandgap of ≈2.87 eV and original insulator bandgap of ≈3.96 eV, is found to be the underlying fundamental reason for the ultranarrow blue emission.

19.
Beilstein J Nanotechnol ; 10: 666-676, 2019.
Artigo em Inglês | MEDLINE | ID: mdl-30931208

RESUMO

We demonstrate an ultrasonication-assisted synthesis without polar solvent of CsPbBr3 and Cs4PbBr6 perovskite nanocrystals (PNCs) and their reversible transformation. The as-prepared CsPbBr3 PNCs and Cs4PbBr6 PNCs exhibit different optical properties that depend on their morphology, size, and structure. The photoluminescence (PL) emission and quantum yield (QY) of the CsPbBr3 PNCs can be tuned by changing the ultrasound power, radiation time, and the height of the vibrating spear. The optimized CsPbBr3 PNCs show a good stability and high PL QY of up to 85%. In addition, the phase transformation between CsPbBr3 PNCs and Cs4PbBr6 PNCs can be obtained through varying the amount of oleylamine (OAm) and water. The mechanism of this transformation between the CsPbBr3 PNCs and Cs4PbBr6 PNCs and their morphology change are studied, involving ions equilibrium, anisotropic growth kinetics, and CsBr-stripping process.

20.
ACS Appl Mater Interfaces ; 11(3): 3351-3359, 2019 Jan 23.
Artigo em Inglês | MEDLINE | ID: mdl-30592200

RESUMO

Although all-inorganic CsPbX3 (X = Cl, Br, I) nanocrystals (NCs) have been considered as a promising material for photoelectronic devices, their applications are still limited because of their poor stability and the lack of in-depth understanding. Here, we demonstrate a post-treatment method for the preparation of ultrathin CsPbX3 nanowires (NWs) by treating CsPbBr3 nanocubes with thiourea solution. A systematic study showed a consecutive interfacial transformation process, in which CsPbBr3 nanocubes were first converted to Cs4PbBr6 NCs in the presence of thiourea, followed by a further transformation to CsPbBr3 NCs through an interfacial CsX-stripping process. To reduce the surface energy, an oriented attachment process has been realized and CsPbBr3 NCs aggregated to form ultrathin NWs. The ultrathin CsPbBr3 NWs exhibited high photoluminescence quantum yield (up to 60%) and high resistance to water treatment, which can be attributed to the surface passivation by thiourea. In addition to thiourea, cysteine and thioacetamide that contain the thiol group can also be used to trigger this transformation. This work can not only offer a facile method for the synthesis of efficient and stable ultrathin CsPbBr3 NWs but also help to reveal the in-depth mechanisms which may be very useful in the field of metal halide perovskite NCs.

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