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Post-synthesis phase and shape evolution of CsPbBr3 colloidal nanocrystals: The role of ligands
摘要： The surface chemistry of colloidal cesium lead bromide (CsPbBr3) nanocrystals is decisive in determining the stability and the final morphology of this class of materials, characterized by ionic structure and a high defect tolerance factor. Here, the high sensitivity of purified colloidal nanocubes of CsPbBr3 to diverse environmental condition (solvent dilution, ageing, ligands post synthetic treatment) in ambient atmosphere is investigated by means of a comprehensive morphological (electron microscopy), structural (θ/2θ X-ray diffraction (XRD) and grazing incidence wide angle scattering (GIWAXS)), and spectroscopic chemical (1H nuclear magnetic resonance (NMR), nuclear Overhauser effect spectroscopy (NOESY), absorption and emission spectroscopy) characterization. The aging and solvent dilution contribute to modify the nanocrystal morphology, due to a modification of the ligand dynamic. Moreover, we establish the ability of aliphatic carboxylic acids and alkyl amines ligands to induce, even in a post preparative process at room temperature, structural, morphological and spectroscopic variations. Upon post synthesis alkyl amine addition, in particular of oleyl amine and octyl amine, the highly green emitting CsPbBr3 nanocubes effectively turn into one-dimensional (1D) thin tetragonal nanowires or lead halide deficient rhombohedral zero-dimensional (0D) Cs4PbBr6 structures with a complete loss of fluorescence. The addition of an alkyl carboxylic acid, as oleic and nonanoic acid, produces the transformation of nanocubes into still emitting orthorombic two-dimensional (2D) nanoplates. The acid/base equilibrium between the native and added ligands, the adsorbed/free ligands dynamic in solution and the ligand solubility in non-polar solvent contribute to render CsPbBr3 particularly sensitive to environmental and processing conditions and, therefore prone to undergo to structural, morphological and, hence spectroscopic, transformations.
关键词： lead halide perovskite nanocrystals,surface chemistry,ligands equilibria,long term stability
更新于2025-11-21 11:01:37
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Direct Hot-Injection Synthesis of Lead Halide Perovskite Nanocubes in Acrylic Monomers for Ultrastable and Bright Nanocrystal–Polymer Composite Films
摘要： In recent years, lead halide perovskite nanocrystals (NCs) have attracted significant attention in both fundamental research and commercial applications due to their excellent optical and optoelectrical properties. However, the protective ligands on the surface of the perovskites NCs could be easily removed after the tedious process of centrifugation, separation, and dispersion, which greatly hampers their stability against light, heat, moisture, and oxygen and limits their practical applications. Here we report a new post-processing-free strategy (i.e., without centrifugation, separation, and dispersion process) of using an UV-polymerizable acrylic monomer of lauryl methacrylate (LMA) as the solvent to synthesize CsPbBr3 NCs, and then adding polyester polyurethane acrylates oligomer, monomer (IBOA) and initiator for directly UV polymerization to fabricate NC-polymer composite films. These films exhibited an improved photoluminescence quantum yield (85-90%) than classic NC-film (40-50%), which were processed using octadecene (ODE) as the solvent for NC synthesis and post-processed for UV polymerization. Significantly, the as-fabricated films by post-processing-free strategy exhibited excellent photostability against strong Xe lamp illumination; while the other films using classic methods were quickly photo-degraded. Meanwhile, these NC-polymer composite films showed good stability against moisture and heating when aging in water at 50oC for over 200 hours. These films, along with K2SiF6:Mn4+ (KSF) phosphor emitters, were used as downconverters for blue LEDs in liquid crystal displays with a wide color gamut of 115% in the International Commission on Illumination (CIE) 1931 color space. This work provides a facile and effective strategy for the preparation of ultrastable and bright color-conversion NC films for the development of the next-generation wide color gamut displays.
关键词： display backlight,lead halide perovskite,colloidal nanocrystals,color-conversion optical films,photostability
更新于2025-11-14 17:03:37
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Cesium lead halide perovskite nanocrystals for ultraviolet and blue light blocking
摘要： Direct exposure to ultraviolet (UV) light is closely related to various harmful effects [1-3], ranging from skin injures to cancer originated from DNA damage. Recent years, some studies reported that blue light are also detrimental to humans [4,5], for example, the blue light could cause photochemical lesions to human retinal within the intensity range of the natural light [6]. Furthermore, blue light is responsible for the solar retinitis and may play a role in age-related macular degeneration. Importantly, the harmful effects of blue lights generated from the electronic display devices should also be careful [7]. Thus, the development of new UV and blue light shielding materials has been received much attention [8]. In the past few years, there has been an increased awareness of the importance to develop UV shielding materials. A variety of materials have been used to prevent UV lesions. Organic molecules like avobenzone or oxybenzone have been used as a UV absorber for many years, but the self-degradation limits their usage time. Inorganic materials such as zinc oxide (ZnO) and titanium oxide (TiO2) have been used intensively for UV shielding [9-12]. However, photocatalytic properties and self-degradations of the ZnO and TiO2 based absorbers also hindered their applications [13,14]. Other materials, e.g., graphene oxide-poly(vinyl alcohol) composite film and lanthanide complex functionalized cellulose nanopaper were also reported for UV shielding [15,16]. Whereas, the excellent UV-filtering capability of these films was obtained by sacrificing the visible light transmittance. Therefore, fabricating UV and blue light blocking materials with good photostability and high transparency to the rest of visible light still remains a challenge and is urgently needed to be developed. Recently, because of the outstanding performance in photovoltaic applications, lead halide perovskite APbX3 (where A = CH3NH3+, (NH2)2CH+ and Cs+, X = Cl?, Br? and I?) has become the most noticeable materials [17-22]. These perovskite nanocrystals exhibit intriguing features [23], such as easy tunable band gap, sharp optical absorption edges and high quantum efficiency with narrow emission spectra. These nanocrystals have been studied extensively for various optical applications, especially light emitting diodes and lasers [24-27]. Post modification of perovskite nanocrystals by anion exchange enables the absorbance band gap tuned from ultraviolet to near infrared spectra [28,29]. In addition, the perovskite nanocrystals show large absorption range, which offers the great potential for UV and blue light shielding applications. Although the tunable absorption-band edge of perovskite nanocrystals has already been realized, there have not been reports on developing UV and blue light blocking material with tunable absorption-band edge. Herein, we aim to the development of a simple and easy way to fabricate UV and blue light blocking material by mixing pervoskite nanocrystals and ethyl cellulose (EC). In this study, EC was used as a host material for the CsPb(Cl/Br)3 pervoskite nanocrystals. By tuning the ratio of Br to Cl, the blocked wavelength range could be easily controlled. Using the sharp absorption edges, the material possesses excellent light blocking ability in the range of 200-460 nm and maintains high transparency (95%) to visible light in the range beyond blue light.
关键词： UV blocking,Cesium lead halide nanocrystals,Blue light blocking,Tunable adsorption edge,Perovskite nanocrystals
更新于2025-09-23 15:23:52
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From Lead Iodide to Radical Form Lead-Iodide Superlattice: High Conductance Gain and Broader Band for Photoconductive Response
摘要： Superlattice materials offer new opportunities to modify optical and electrical properties of the recently emerging 2D materials. The insertion of tetraethylbenzidine into interlamination of the known 2D PbI2 semiconductor through a mild solution method yielded lead-iodide superlattice, EtDAB·4PbI2 (EtDAB = tetraethylbenzidine), with radical and non-radical forms. The non-radical form has a nonionic structure that differs from the common ionic structures for inorganic–organic hybrid lead halides. The radical form shows five orders of magnitude of conductance gain and broader photoconductive response range (UV–Vis → UV–Vis–IR), compared with pure PbI2 and the non-radical form.
关键词： Inorganic-organic hybrid,Photoconductive,Semiconductive,Lead halide,Superlattice
更新于2025-09-23 15:22:29
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From Lead Iodide to Radical Form Lead-Iodide Superlattice: High Conductance Gain and Broader Band for Photoconductive Response
摘要： Superlattice materials offer new opportunities to modify optical and electrical properties of the recently emerging 2D materials. The insertion of tetraethylbenzidine into interlamination of the known 2D PbI2 semiconductor through a mild solution method yielded lead-iodide superlattice, EtDAB·4PbI2 (EtDAB = tetraethylbenzidine), with radical and non-radical forms. The non-radical form has a nonionic structure that differs from the common ionic structures for inorganic–organic hybrid lead halides. The radical form shows five orders of magnitude of conductance gain and broader photoconductive response range (UV–Vis → UV–Vis–IR), compared with pure PbI2 and the non-radical form.
关键词： Inorganic-organic hybrid,Photoconductive,Semiconductive,Lead halide,Superlattice
更新于2025-09-23 15:22:29
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High performance and mechanism of the resistive switching device based on lead halide thin films
摘要： In this work, the lead halide was firstly applied in resistive random-access memory (RRAM) device with the structure of W/lead iodide/fluorine-doped tin oxide (FTO). The mechanism was investigated by reliable data fitting and the experiment of temperature influence, illustrating that the resistive switching phenomenon was origin from the filament. The iodide vacancies were considered as the main composition of the conductive filaments, which was verified by the first principle calculation and experimental verification. These performances were also found in device fabricated by other lead halide, such as PbBr2 and PbCl2. Moreover, they performed great potential as the non-volatile memory due to the excellent resistive switching properties. This work was of great significance for the expansion of RRAM material system.
关键词： conductive filaments,lead halide,resistive switching memory,first principle calculation
更新于2025-09-23 15:22:29
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Impact of Organic Spacers on the Carrier Dynamics in 2D Hybrid Lead-Halide Perovskites
摘要： We have carried out non-adiabatic molecular dynamics simulations combined with time-dependent density functional theory calculations to compare the properties of the two-dimensional (2D) (BA)2(MA)Pb2I7 and three-dimensional (3D) MAPbI3 (where MA = methylammonium and BA = butylammonium) materials. We evaluate the different impacts that the 2D-confined spacer layer of butylammonium cations and the 3D-confined methylammonium cations have on the charge carrier dynamics in the two systems. Our results indicate that while both the MA+ and BA+ cations play important roles in determining the carrier dynamics, the BA+ cations exhibit stronger non-adiabatic couplings with the 2D perovskite framework. The consequence is a faster hot-carrier decay rate in 2D (BA)2(MA)Pb2I7 than in 3D MAPbI3. Thus, tuning of the functional groups of the organic spacer cations in order to reduce the vibronic couplings between the cations and the Pb-I framework can offer the opportunity to slow down the hot-carrier relaxations and increase the carrier lifetimes in 2D lead-halide perovskites.
关键词： carrier dynamics,2D hybrid lead-halide perovskites,time-dependent density functional theory,non-adiabatic molecular dynamics,organic spacers
更新于2025-09-23 15:21:21
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Long Exciton Dephasing Time and Coherent Phonon Coupling in CsPbBr <sub/>2</sub> Cl Perovskite Nanocrystals
摘要： Fully-inorganic cesium lead halide perovskite nanocrystals (NCs) have shown to exhibit outstanding optical properties such as wide spectral tunability, high quantum yield, high oscillator strength as well as blinking-free single photon emission and low spectral diffusion. Here, we report measurements of the coherent and incoherent exciton dynamics on the 100 fs to 10 ns timescale, determining dephasing and density decay rates in these NCs. The experiments are performed on CsPbBr2Cl NCs using transient resonant three-pulse four-wave mixing (FWM) in heterodyne detection at temperatures ranging from 5 K to 50 K. We found a low-temperature exciton dephasing time of 24.5±1.0 ps, inferred from the decay of the photon-echo amplitude at 5 K, corresponding to a homogeneous linewidth (FWHM) of 54±5 μeV. Furthermore, oscillations in the photon-echo signal on a picosecond timescale are observed and attributed to coherent coupling of the exciton to a quantized phonon mode with 3.45 meV energy.
关键词： quantum dots,coherence,four wave mixing,nanocrystals,heterodyne detection,Perovskite,T2,lead halide,photon echo,phonons
更新于2025-09-23 15:21:21
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Ultrafast Interfacial Charge Transfer of Cesium Lead Halide Perovskite Films CsPbX3 (X = Cl, Br, I) with Different Halogen Mixing
摘要： Understanding the interfacial charge transfer of the photoinduced transients of all-inorganic cesium lead halide perovskites (CsPbX3; X = Cl, Br, I) is critical for their photovoltaic applications. Ultrafast dynamics can provide comprehensive information about the transient behavior of the carriers and their transfer mechanism in the materials. In this work, the interfacial charge transfer of CsPbX3 films assembled with TiO2 with different halogen doping ratios was studied using femtosecond transient absorption (TA) spectroscopy combined with global analysis. Four subsequent decay processes after photoexcitation were obtained, including hot carrier cooling, free exciton forming, electron transfer, and charge recombination. The results indicate that the time constant of the interfacial electron transfer varies with the location of the trap state of these perovskites and the relative energy of CBs in the perovskite and TiO2 and that the time constant of the charge recombination can be attributed to the electron–hole interactions. These interpretations are supported by calculations based on first-principles density functional theory (DFT). Greater iodine doping in such perovskite CsPbX3/TiO2 systems increases the time constants of the electron transfer and charge recombination, which suggests that all-inorganic perovskite CsPbX3 with a high iodine content is favorable for improving the power conversion efficiency of solar cells.
关键词： cesium lead halide perovskite,transient absorption,global analysis,interfacial charge transfer
更新于2025-09-23 15:21:01
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One-step Co-evaporation of All-Inorganic Perovskite Thin Films with Room Temperature Ultralow Amplified Spontaneous Emission Threshold and Air-stability
摘要： Inorganic cesium lead halide perovskite has been successfully applied in optoelectronic field due to its remarkable optical gain properties. Unfortunately, conventional solution-processed CsPbX3 films suffer unavoidable pinhole defects and poor surface morphology, severely limiting their performance on amplified spontaneous emission (ASE) and lasing application. Herein, a dual-source thermal evaporation approach is explored in our work to achieve a uniform and high-coverage CsPbX3 polycrystalline thin film. It is found that the one-step co-evaporated CsPbBr3 (OC-CsPbBr3) thin films without post-annealing exhibit an ultralow ASE threshold of ~ 3.3 μJ/cm2 and gain coefficient above 300 cm-1. The coexistence of cubic and orthorhombic phases in this materials naturally form an energy cascade for the exciton transfer process, which enables rapid accumulation of excitons. Stable ASE intensity without degradation for at least 7 hours is also realized from OC-CsPbBr3 thin films under continuous excitation, which is superior to that in the solution-processed CsPbBr3 thin film. Notably, a Fabry-Perot (F-P) cavity laser based on the OC-CsPbBr3 thin film is first achieved, featuring an ultralow lasing threshold (1.7 μJ/cm2) and directional output (beam divergence of ~ 3.8°). This work highlights the noteworthy optical properties of OC-CsPbBr3 thin films, leading to potential available applications in the integrated optoelectronic chips.
关键词： amplified spontaneous emission,Cesium lead halide perovskite,vapor deposition,long-term stability,thin films
更新于2025-09-23 15:21:01