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New-phase retention in colloidal core/shell nanocrystals via pressure-modulated phase engineering.

ABSTRACT: Core/shell nanocrystals (NCs) integrate collaborative functionalization that would trigger advanced properties, such as high energy conversion efficiency, nonblinking emission, and spin-orbit coupling. Such prospects are highly correlated with the crystal structure of individual constituents. However, it is challenging to achieve novel phases in core/shell NCs, generally non-existing in bulk counterparts. Here, we present a fast and clean high-pressure approach to fabricate heterostructured core/shell MnSe/MnS NCs with a new phase that does not occur in their bulk counterparts. We determine the new phase as an orthorhombic MnP structure (B31 phase), with close-packed zigzagged arrangements within unit cells. Encapsulation of the solid MnSe nanorod with an MnS shell allows us to identify two separate phase transitions with recognizable diffraction patterns under high pressure, where the heterointerface effect regulates the wurtzite → rocksalt → B31 phase transitions of the core. First-principles calculations indicate that the B31 phase is thermodynamically stable under high pressure and can survive under ambient conditions owing to the synergistic effect of subtle enthalpy differences and large surface energy in nanomaterials. The ability to retain the new phase may open up the opportunity for future manipulation of electronic and magnetic properties in heterostructured nanostructures.

SUBMITTER: Wang Y

PROVIDER: S-EPMC8133026 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Hollow and concave nanoparticles via preferential oxidation of the core in colloidal core/shell nanocrystals.

Project description:Hollow and concave nanocrystals find applications in many fields, and their fabrication can follow different possible mechanisms. We report a new route to these nanostructures that exploits the oxidation of Cu(2-x)Se/Cu(2-x)S core/shell nanocrystals with various etchants. Even though the Cu(2-x)Se core is encased in a thick Cu(2-x)S shell, the initial effect of oxidation is the creation of a void in the core. This is rationalized in terms of diffusion of Cu(+) ions and electrons from the core to the shell (and from there to the solution). Differently from the classical Kirkendall effect, which entails an imbalance between in-diffusion and out-diffusion of two different species across an interface, the present mechanism can be considered as a limiting case of such effect and is triggered by the stronger tendency of Cu(2-x)Se over Cu(2-x)S toward oxidation and by fast Cu(+) diffusion in copper chalcogenides. As the oxidation progresses, expansion of the inner void erodes the entire Cu(2-x)Se core, accompanied by etching and partial collapse of the shell, yielding Cu(2-x)S(y)Se(1-y) concave particles.

| S-EPMC4073830 | biostudies-other

Galvanic Exchange in Colloidal Metal/Metal-Oxide Core/Shell Nanocrystals.

Project description:While galvanic exchange is commonly applied to metallic nanoparticles, recently its applicability was expanded to metal-oxides. Here the galvanic exchange is studied in metal/metal-oxide core/shell nanocrystals. In particular Sn/SnO2 is treated by Ag(+), Pt(2+), Pt(4+), and Pd(2+). The conversion dynamics is monitored by in situ synchrotron X-ray diffraction. The Ag(+) treatment converts the Sn cores to the intermetallic Ag x Sn (x ? 4) phase, by changing the core's crystal structure. For the analogous treatment by Pt(2+), Pt(4+), and Pd(2+), such a galvanic exchange is not observed. This different behavior is caused by the semipermeability of the naturally formed SnO2 shell, which allows diffusion of Ag(+) but protects the nanocrystal cores from oxidation by Pt and Pd ions.

| S-EPMC5018861 | biostudies-literature

Mapping the Atomistic Structure of Graded Core/Shell Colloidal Nanocrystals.

Project description:Engineering the compositional gradient for core/shell semiconductor nanocrystals improves their optical properties. To date, however, the structure of graded core/shell nanocrystal emitters has only been qualitatively described. In this paper, we demonstrate an approach to quantify nanocrystal structure, selecting graded Ag-In-Se/ZnSe core/shell nanocrystals as a proof-of-concept material. A combination of multi-energy small-angle X-ray scattering and electron microscopy techniques enables us to establish the radial distribution of ZnSe with sub-nanometer resolution. Using ab initio shape-retrieval analysis of X-ray scattering spectra, we further determine the average shape of nanocrystals. These results allow us to generate three-dimensional, atomistic reconstructions of graded core/shell nanocrystals. We use these reconstructions to calculate solid-state Zn diffusion in the Ag-In-Se nanocrystals and the lattice mismatch between nanocrystal monolayers. Finally, we apply these findings to propose design rules for optimal shell structure and record-luminescent core/shell nanocrystals.

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Giant five-photon absorption from multidimensional core-shell halide perovskite colloidal nanocrystals.

Project description:Multiphoton absorption processes enable many technologically important applications, such as in vivo imaging, photodynamic therapy and optical limiting, and so on. Specifically, higher-order nonlinear absorption such as five-photon absorption offers significant advantages of greater spatial confinement, increased penetration depth, reduced autofluorescence, enhanced sensitivity and improved resolution over lower orders in bioimaging. Organic chromophores and conventional semiconductor nanocrystals are leaders in two-/three-photon absorption applications, but face considerable challenges from their small five-photon action cross-sections. Herein, we reveal that the family of halide perovskite colloidal nanocrystals transcend these constraints with highly efficient five-photon-excited upconversion fluorescence-unprecedented for semiconductor nanocrystals. Amazingly, their multidimensional type I (both conduction and valence band edges of core lie within bandgap of shell) core-shell (three-dimensional methylammonium lead bromide/two-dimensional octylammonium lead bromide) perovskite nanocrystals exhibit five-photon action cross-sections that are at least 9 orders larger than state-of-the-art specially designed organic molecules. Importantly, this family of halide perovskite nanocrystals may enable fresh approaches for next-generation multiphoton imaging applications.

| S-EPMC5437305 | biostudies-other

Control of electronic band profiles through depletion layer engineering in core-shell nanocrystals.

Project description:Fermi level pinning in doped metal oxide (MO) nanocrystals (NCs) results in the formation of depletion layers, which affect their optical and electronic properties, and ultimately their application in smart optoelectronics, photocatalysis, or energy storage. For a precise control over functionality, it is important to understand and control their electronic bands at the nanoscale. Here, we show that depletion layer engineering allows designing the energetic band profiles and predicting the optoelectronic properties of MO NCs. This is achieved by shell thickness tuning of core-shell Sn:In2O3-In2O3 NCs, resulting in multiple band bending and multi-modal plasmonic response. We identify the modification of the band profiles after the light-induced accumulation of extra electrons as the main mechanism of photodoping and enhance the charge storage capability up to hundreds of electrons per NC through depletion layer engineering. Our experimental results are supported by theoretical models and are transferable to other core-multishell systems as well.

| S-EPMC8795196 | biostudies-literature

Crystal Phase Transitions in the Shell of PbS/CdS Core/Shell Nanocrystals Influences Photoluminescence Intensity.

Project description:We reveal the existence of two different crystalline phases, i.e., the metastable rock salt and the equilibrium zinc blende phase within the CdS-shell of PbS/CdS core/shell nanocrystals formed by cationic exchange. The chemical composition profile of the core/shell nanocrystals with different dimensions is determined by means of anomalous small-angle X-ray scattering with subnanometer resolution and is compared to X-ray diffraction analysis. We demonstrate that the photoluminescence emission of PbS nanocrystals can be drastically enhanced by the formation of a CdS shell. Especially, the ratio of the two crystalline phases in the shell significantly influences the photoluminescence enhancement. The highest emission was achieved for chemically pure CdS shells below 1 nm thickness with a dominant metastable rock salt phase fraction matching the crystal structure of the PbS core. The metastable phase fraction decreases with increasing shell thickness and increasing exchange times. The photoluminescence intensity depicts a constant decrease with decreasing metastable rock salt phase fraction but shows an abrupt drop for shells above 1.3 nm thickness. We relate this effect to two different transition mechanisms for changing from the metastable rock salt phase to the equilibrium zinc blende phase depending on the shell thickness.

| S-EPMC4311954 | biostudies-literature

Energy Transfer between Conjugated Colloidal Ga?O? and CdSe/CdS Core/Shell Nanocrystals for White Light Emitting Applications.

Project description:Developing solid state materials capable of generating homogeneous white light in an energy efficient and resource-sustainable way is central to the design of new and improved devices for various lighting applications. Most currently-used phosphors depend on strategically important rare earth elements, and rely on a multicomponent approach, which produces sub-optimal quality white light. Here, we report the design and preparation of a colloidal white-light emitting nanocrystal conjugate. This conjugate is obtained by linking colloidal Ga?O? and II-VI nanocrystals in the solution phase with a short bifunctional organic molecule (thioglycolic acid). The two types of nanocrystals are electronically coupled by Förster resonance energy transfer owing to the short separation between Ga?O? (energy donor) and core/shell CdSe/CdS (energy acceptor) nanocrystals, and the spectral overlap between the photoluminescence of the donor and the absorption of the acceptor. Using steady state and time-resolved photoluminescence spectroscopies, we quantified the contribution of the energy transfer to the photoluminescence spectral power distribution and the corresponding chromaticity of this nanocrystal conjugate. Quantitative understanding of this new system allows for tuning of the emission color and the design of quasi-single white light emitting inorganic phosphors without the use of rare-earth elements.

| S-EPMC5302483 | biostudies-literature

Rh@Au Core-Shell Nanocrystals with the Core in Tensile Strain and the Shell in Compressive Strain.

Project description:Bimetallic nanocrystals provide a versatile platform for utilizing the desired characteristics of two different elements within one particle. Core-shell nanocrystals, in particular, have found widespread use in catalysis by providing an ability to leverage the strains arising from the lattice mismatch between the core and the shell. However, large (>5%) lattice mismatch tends to result in nonepitaxial growth and lattice defects in an effort to release the strain. Herein, we report the epitaxial growth of Au on Rh cubic seeds under mild reaction conditions to generate Rh@Au truncated octahedra featuring a lattice mismatch of 7.2%. Key to the success was the use of small (4.5 nm) Rh cubes as seeds, which could homogeneously distribute the tensile strain arising from the epitaxial growth of a conformal, compressively strained Au shell. Further, delicate tuning of kinetic parameters through the introduction of NaOH and KBr into the synthesis allowed for a unique nucleation pattern that led to centrally located cores and a narrow size distribution for the product. A thorough investigation of the various possible highly strained morphologies was conducted to gain a full understanding of the system.

| S-EPMC10823532 | biostudies-literature

PbSe-Based Colloidal Core/Shell Heterostructures for Optoelectronic Applications.

Project description:Lead-based (IV-VI) colloidal quantum dots (QDs) are of widespread scientific and technological interest owing to their size-tunable band-gap energy in the near-infrared optical region. This article reviews the synthesis of PbSe-based heterostructures and their structural and optical investigations at various temperatures. The review focuses on the structures consisting of a PbSe core coated with a PbSexS1-x (0 ≤ x ≤ 1) or CdSe shell. The former-type shells were epitaxially grown on the PbSe core, while the latter-type shells were synthesized using partial cation-exchange. The influence of the QD composition and the ambient conditions, i.e., exposure to oxygen, on the QD optical properties, such as radiative lifetime, Stokes shift, and other temperature-dependent characteristics, was investigated. The study revealed unique properties of core/shell heterostructures of various compositions, which offer the opportunity of fine-tuning the QD electronic structure by changing their architecture. A theoretical model of the QD electronic band structure was developed and correlated with the results of the optical studies. The review also outlines the challenges related to potential applications of colloidal PbSe-based heterostructures.

| S-EPMC5512633 | biostudies-other

Epitaxial Core/Shell Nanocrystals of (Europium-Doped) Zirconia and Hafnia.

Project description:A careful design of the nanocrystal architecture can strongly enhance the nanocrystal function. So far, this strategy has faced a synthetic bottleneck in the case of refractory oxides. Here we demonstrate the epitaxial growth of hafnia shells onto zirconia cores and pure zirconia shells onto europium-doped zirconia cores. The core/shell structures are fully crystalline. Upon shelling, the optical properties of the europium dopant are dramatically improved (featuring a more uniform coordination and a longer photoluminescence lifetime), indicating the suppression of nonradiative pathways. These results launch the stable zirconium and hafnium oxide hosts as alternatives for the established NaYF4 systems.

| S-EPMC11295171 | biostudies-literature

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