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1.
Nano Lett ; 24(1): 466-471, 2024 Jan 10.
Artigo em Inglês | MEDLINE | ID: mdl-38150569

RESUMO

Contemporary quantum plasmonics capture subtle corrections to the properties of plasmonic nano-objects in equilibrium. Here, we demonstrate non-equilibrium spill-out redistribution of the electronic density at the ultrafast time scale. As revealed by time-resolved 2D spectroscopy of nanoplasmonic Fe/Au bilayers, an injection of the laser-excited non-thermal electrons induces transient electron spill-out thus changing the plasma frequency. The response of the local electronic density switches the electronic density behavior from spill-in to strong (an order of magnitude larger) spill-out at the femtosecond time scale. The superdiffusive transport of hot electrons and the lack of a direct laser heating indicate significantly non-thermal origin of the underlying physics. Our results demonstrate an ultrafast and non-thermal way to control surface plasmon dispersion through transient variations of the spatial electron distribution at the nanoscale. These findings expand quantum plasmonics into previously unexplored directions by introducing ultrashort time scales in the non-equilibrium electronic systems.

2.
Artigo em Inglês | MEDLINE | ID: mdl-35482521

RESUMO

Strain NGK65T, a novel hexadecane degrading, non-motile, Gram-positive, rod-to-coccus shaped, aerobic bacterium, was isolated from plastic polluted soil sampled at a landfill. Strain NGK65T hydrolysed casein, gelatin, urea and was catalase-positive. It optimally grew at 28 °C, in 0-1% NaCl and at pH 7.5-8.0. Glycerol, d-glucose, arbutin, aesculin, salicin, potassium 5-ketogluconate, sucrose, acetate, pyruvate and hexadecane were used as sole carbon sources. The predominant membrane fatty acids were iso-C16:0 followed by iso-C17:0 and C18:1 ω9c. The major polar lipids were phosphatidylglycerol, phosphatidylethanolamine, phosphatidylinositol and hydroxyphosphatidylinositol. The cell-wall peptidoglycan type was A3γ, with ll-diaminopimelic acid and glycine as the diagnostic amino acids. MK 8 (H4) was the predominant menaquinone. Phylogenetic analysis based on 16S rRNA gene sequences indicated that strain NGK65T belongs to the genus Nocardioides (phylum Actinobacteria), appearing most closely related to Nocardioides daejeonensis MJ31T (98.6%) and Nocardioides dubius KSL-104T (98.3%). The genomic DNA G+C content of strain NGK65T was 68.2%. Strain NGK65T and the type strains of species involved in the analysis had average nucleotide identity values of 78.3-71.9% as well as digital DNA-DNA hybridization values between 22.5 and 19.7%, which clearly indicated that the isolate represents a novel species within the genus Nocardioides. Based on phenotypic and molecular characterization, strain NGK65T can clearly be differentiated from its phylogenetic neighbours to establish a novel species, for which the name Nocardioides alcanivorans sp. nov. is proposed. The type strain is NGK65T (=DSM 113112T=NCCB 100846T).


Assuntos
Actinomycetales , Nocardioides , Alcanos , Técnicas de Tipagem Bacteriana , Composição de Bases , DNA Bacteriano/genética , Ácidos Graxos/química , Filogenia , Plásticos , RNA Ribossômico 16S/genética , Análise de Sequência de DNA , Microbiologia do Solo
3.
Artigo em Inglês | MEDLINE | ID: mdl-35467502

RESUMO

Strain NGK35T is a motile, Gram-stain-negative, rod-shaped (1.0-2.1 µm long and 0.6-0.8 µm wide), aerobic bacterium that was isolated from plastic-polluted landfill soil. The strain grew at temperatures between 6 and 37 °C (optimum, 28 °C), in 0-10 % NaCl (optimum, 1 %) and at pH 6.0-9.5 (optimum, pH 7.5-8.5). It was positive for cytochrome c oxidase, catalase as well as H2S production, and hydrolysed casein and urea. It used a variety of different carbon sources including citrate, lactate and pyruvate. The predominant membrane fatty acids were C16 : 1 cis9 and C16 : 0, followed by C17 : 0 cyclo and C18 : 1 cis11. The major polar lipids were phosphatidylglycerol and phosphatidylethanolamine, followed by diphosphatidyglycerol. The only quinone was ubiquinone Q-8. Phylogenetic analysis based on 16S rRNA gene sequences indicated that strain NGK35T belongs to the genus Paenalcaligenes (family Alcaligenaceae), appearing most closely related to Paenalcaligenes hominis CCUG 53761AT (96.90 %) and Paenalcaligenes suwonensis ABC02-12T (96.94 %). The genomic DNA G+C content of strain NGK35T was 52.1 mol %. Genome-based calculations (genome-to-genome distance, average nucleotide identity and DNA G+C content) clearly indicated that the isolate represents a novel species within the genus Paenalcaligenes. Based on phenotypic and molecular characterization, strain NGK35T can clearly be differentiated from its phylogenetic neighbours establishing a novel species, for which the name Paenalcaligenes niemegkensis sp. nov. is proposed. The type strain is NGK35T (=DSM 113270T=NCCB 100854T).


Assuntos
Alcaligenaceae , Plásticos , Técnicas de Tipagem Bacteriana , Composição de Bases , DNA Bacteriano/genética , Ácidos Graxos/química , Filogenia , RNA Ribossômico 16S/genética , Análise de Sequência de DNA , Ubiquinona/química
4.
Nanotechnology ; 32(9): 095709, 2021 Feb 26.
Artigo em Inglês | MEDLINE | ID: mdl-33207326

RESUMO

The structural, optical, and mechanical properties of TiO2 nanolaminate films grown by plasma-enhanced atomic layer deposition are discussed. Several TiO2/Al2O3 and TiO2/SiO2 compositions have been investigated to study the effect of the relative number of ALD oxide cycles on the film properties to obtain a high refractive index coating with low optical losses, low roughness, and low mechanical stress. The formation of crystalline TiO2 observed at high deposition temperature, or film thickness was inhibited by periodically introducing ultra-thin amorphous layers into the film. Only 4 ALD cycles of Al2O3 (corresponding to ca. 0.5 nm) between 335 ALD cycles of TiO2 (ca. 11 nm) form a closed, distinct layer suppressing the crystallization in TiO2 film. Consequently, the roughness of the pure TiO2 film is reduced from ca. 20 nm rms to 1 nm rms in the 335/4 nanolaminate, with only a slight decrease of the refractive index from 2.46 to 2.44 in 100 nm pure TiO2 and the nanolaminate, respectively. The refractive indices of the nanolaminates in various compositions vary between 2.38 and 2.50 at 632 nm, and the corresponding optical losses from the films are low. The mechanical stress was reduced to about 140 MPa in several TiO2/Al2O3 nanolaminates; however, lower mechanical stress has not been obtained with the studied compositions. The nanolaminate structure is preserved up to 600 °C annealing temperature. After annealing at 800 °C, the individual layers interdiffuse into each other so that no distinct nanolaminate structure is detected. By using TiO2/Al2O3 nanolaminates with reduced mechanical stress, a narrow bandpass filter was realized on various substrates, including half-ball and aspherical lenses.

5.
J Am Chem Soc ; 141(51): 20037-20042, 2019 Dec 26.
Artigo em Inglês | MEDLINE | ID: mdl-31825615

RESUMO

Synthesis of nanoscale metal-organic frameworks (MOFs) is a highly challenging task because conventional soluble metal salt precursors are not easy to manipulate spatially, thus normally leading to bulk MOFs. In the present work, V2CTx MXene is demonstrated for the first time as a metal precursor to fabricate two-dimensional (2D) MOF nanosheets, whose thickness (6 to 18 nm) can be tuned by varying the reaction temperature. The highly electronegative surface atoms of MXene and sufficient accessible attacking sites for ligands are responsible for the evolution of 2D MOF nanosheets. Moreover, highly oriented and smooth MOF thin films have been grown based on these nanosheets using a convenient spin coating process. With the impregnation of nonvolatile H3PO4, the MOF thin film exhibits a proton-conducting property. This study demonstrates that high-quality 2D MOF sheets and thin films are enabled by 2D MXene precursors. We believe that the high-quality MOF films prepared in this study pave the way for many device applications.

6.
Phys Rev Lett ; 119(1): 017202, 2017 Jul 07.
Artigo em Inglês | MEDLINE | ID: mdl-28731774

RESUMO

Using the sensitivity of optical second harmonic generation to currents, we demonstrate the generation of 250-fs long spin current pulses in Fe/Au/Fe/MgO(001) spin valves. The temporal profile of these pulses indicates ballistic transport of hot electrons across a sub-100 nm Au layer. The pulse duration is primarily determined by the thermalization time of laser-excited hot carriers in Fe. Considering the calculated spin-dependent Fe/Au interface transmittance we conclude that a nonthermal spin-dependent Seebeck effect is responsible for the generation of ultrashort spin current pulses. The demonstrated rotation of spin polarization of hot electrons upon interaction with noncollinear magnetization at Au/Fe interfaces holds high potential for future spintronic devices.

7.
Macromol Rapid Commun ; 37(21): 1742-1747, 2016 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-27717056

RESUMO

The development of a straightforward method is reported to form hybrid polymer/gold planet-satellite nanostructures (PlSNs) with functional polymer. Polyacrylate type polymer with benzyl chloride in its backbone as a macromolecular tracer is synthesized to study its localization within PlSNs by analyzing the elemental distribution of chlorine. The functionalized nanohybrid structures are analyzed by scanning transmission electron microscopy, electron energy loss spectroscopy, and spectrum imaging. The results show that the RAFT (reversible addition-fragmentation chain transfer) polymers' sulfur containing end groups are colocalized at the gold cores, both within nanohybrids of simple core-shell morphology and within higher order PlSNs, providing microscopic evidence for the affinity of the RAFT group toward gold surfaces.


Assuntos
Ouro/química , Substâncias Macromoleculares/química , Nanoestruturas/química , Polímeros/química , Tamanho da Partícula , Polímeros/síntese química , Propriedades de Superfície
8.
Sci Technol Adv Mater ; 16(1): 015001, 2015 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-27877751

RESUMO

Highly textured thin films with small grain boundary regions can be used as model systems to directly measure the bulk conductivity of oxygen ion conducting oxides. Ionic conducting thin films and epitaxial heterostructures are also widely used to probe the effect of strain on the oxygen ion migration in oxide materials. For the purpose of these investigations a good lattice matching between the film and the substrate is required to promote the ordered film growth. Moreover, the substrate should be a good electrical insulator at high temperature to allow a reliable electrical characterization of the deposited film. Here we report the fabrication of an epitaxial heterostructure made with a double buffer layer of BaZrO3 and SrTiO3 grown on MgO substrates that fulfills both requirements. Based on such template platform, highly ordered (001) epitaxially oriented thin films of 15% Sm-doped CeO2 and 8 mol% Y2O3 stabilized ZrO2 are grown. Bulk conductivities as well as activation energies are measured for both materials, confirming the success of the approach. The reported insulating template platform promises potential application also for the electrical characterization of other novel electrolyte materials that still need a thorough understanding of their ionic conductivity.

9.
Phys Chem Chem Phys ; 16(19): 8837-42, 2014 May 21.
Artigo em Inglês | MEDLINE | ID: mdl-24676033

RESUMO

The reaction mechanism occurring during the (de)intercalation of sodium into the host olivine FePO4 structure is thoroughly analysed through a combination of structural and electrochemical methods. In situ XRD experiments have confirmed that the charge and discharge reaction mechanisms are different and have revealed the existence of a solid solution domain from 1 < x < 2/3 in Na(x)FePO4 upon charge. The second part of the charge proceeds through a 2-phase reaction between Na(2/3)FePO4 and FePO4 with strongly varying solubility limits. The strong cell mismatch between Na(2/3)FePO4 and FePO4 enhances the effects of the diffuse interface and therefore varying solubility limits are first observed here in micrometric materials.

10.
ACS Nano ; 18(14): 10124-10132, 2024 Apr 09.
Artigo em Inglês | MEDLINE | ID: mdl-38511608

RESUMO

MXenes are 2D transition metal carbides, nitrides, and/or carbonitrides that can be intercalated with cations through chemical or electrochemical pathways. While the insertion of alkali and alkaline earth cations into Ti3C2Tx MXenes is well studied, understanding of the intercalation of redox-active transition metal ions into MXenes and its impact on their electronic and electrochemical properties is lacking. In this work, we investigate the intercalation of Cu ions into Ti3C2Tx MXene and its effect on its electronic and electrochemical properties. Using X-ray absorption spectroscopy (XAS) and ab initio molecular dynamics (AIMD), we observe an unusual phenomenon whereby Cu2+ ions undergo partial reduction upon intercalation from the solution into the MXene. Furthermore, using in situ XAS, we reveal changes in the oxidation states of intercalated Cu ions and Ti atoms during charging. We show that the pseudocapacitive response of Cu-MXene originates from the redox of both the Cu intercalant and Ti3C2Tx host. Despite highly reducing potentials, Cu ions inside the MXene show an excellent stability against full reduction upon charging. Our findings demonstrate how electronic coupling between Cu ions and Ti3C2Tx modifies electrochemical and electronic properties of the latter, providing the framework for the rational design and utilization of transition metal intercalants for tuning the properties of MXenes for various electrochemical systems.

11.
J Am Chem Soc ; 135(33): 12313-23, 2013 Aug 21.
Artigo em Inglês | MEDLINE | ID: mdl-23862668

RESUMO

A novel clathrate phase, Ba8Au16P30, was synthesized from its elements. High-resolution powder X-ray diffraction and transmission electron microscopy were used to establish the crystal structure of the new compound. Ba8Au16P30 crystallizes in an orthorhombic superstructure of clathrate-I featuring a complete separation of gold and phosphorus atoms over different crystallographic positions, similar to the Cu-containing analogue, Ba8Cu16P30. Barium cations are trapped inside the large polyhedral cages of the gold-phosphorus tetrahedral framework. X-ray diffraction indicated that one out of 15 crystallographically independent phosphorus atoms appears to be three-coordinate. Probing the local structure and chemical bonding of phosphorus atoms with (31)P solid-state NMR spectroscopy confirmed the three-coordinate nature of one of the phosphorus atomic positions. High-resolution high-angle annular dark-field scanning transmission electron microscopy indicated that the clathrate Ba8Au16P30 is well-ordered on the atomic scale, although numerous twinning and intergrowth defects as well as antiphase boundaries were detected. The presence of such defects results in the pseudo-body-centered-cubic diffraction patterns observed in single-crystal X-ray diffraction experiments. NMR and resistivity characterization of Ba8Au16P30 indicated paramagnetic metallic properties with a room-temperature resistivity of 1.7 mΩ cm. Ba8Au16P30 exhibits a low total thermal conductivity (0.62 W m(-1) K(-1)) and an unprecedentedly low lattice thermal conductivity (0.18 W m(-1) K(-1)) at room temperature. The values of the thermal conductivity for Ba8Au16P30 are significantly lower than the typical values reported for solid crystalline compounds. We attribute such low thermal conductivity values to the presence of a large number of heavy atoms (Au) in the framework and the formation of multiple twinning interfaces and antiphase defects, which are effective scatterers of heat-carrying phonons.

12.
Nanoscale ; 15(27): 11592-11602, 2023 Jul 13.
Artigo em Inglês | MEDLINE | ID: mdl-37377085

RESUMO

Processes of self-organization play a key role in the development of innovative functional nanocomposites, allowing, in particular, the transformation of metastable solid solutions into multilayers by activating spinodal decomposition instead of layer-by-layer film growth. We report the formation of strained layered (V,Ti)O2 nanocomposites in thin polycrystalline films using a spinodal decomposition. Already during the growth of V0.65Ti0.35O2 films, spinodal decomposition was detected while producing atomic-scale disordered V- and Ti-rich phases. Post-growth annealing enhances compositional modulation, arranges the local atomic structures of the phases, and yields periodically layered nanostructures that resemble superlattices. The coherent interfacing of the V- and Ti-rich layers results in the compression of the V-rich phase along the c-axis of the rutile structure and enables strain-enhanced thermochromism. The latter is characterized by a simultaneous decrease in the temperature and width of the metal-insulator transition in the V-rich phase. Our results provide proof-of-concept for an alternative strategy to develop VO2-based thermochromic coatings by introducing strain-enhanced thermochromism into polycrystalline thin films.

13.
Nanomaterials (Basel) ; 13(21)2023 Nov 03.
Artigo em Inglês | MEDLINE | ID: mdl-37947741

RESUMO

Superlattices (SLs) comprising layers of a soft ferromagnetic metal La2/3Sr1/3MnO3 (LSMO) with in-plane (IP) magnetic easy axis and a hard ferromagnetic insulator La2MnCoO6 (LMCO, out-of-plane anisotropy) were grown on SrTiO3 (100)(STO) substrates by a metalorganic aerosol deposition technique. Exchange spring magnetic (ESM) behavior between LSMO and LMCO, manifested by a spin reorientation transition of the LSMO layers towards perpendicular magnetic anisotropy below TSR = 260 K, was observed. Further, 3ω measurements of the [(LMCO)9/(LSMO)9]11/STO(100) superlattices revealed extremely low values of the cross-plane thermal conductivity κ(300 K) = 0.32 Wm-1K-1. Additionally, the thermal conductivity shows a peculiar dependence on the applied IP magnetic field, either decreasing or increasing in accordance with the magnetic disorder induced by ESM. Furthermore, both positive and negative magnetoresistance were observed in the SL in the respective temperature regions due to the formation of 90°-Néel domain walls within the ESM, when applying IP magnetic fields. The results are discussed in the framework of electronic contribution to thermal conductivity originating from the LSMO layers.

14.
ACS Appl Mater Interfaces ; 15(18): 22626-22636, 2023 May 10.
Artigo em Inglês | MEDLINE | ID: mdl-37097287

RESUMO

Heterostructures increasingly attracted attention over the past several years to enable various optoelectronic and photonic applications. In this work, atomically thin interfaces of Ir/Al2O3 heterostructures compatible with micro-optoelectronic technologies are reported. Their structural and optical properties were determined by spectroscopic and microscopic techniques (XRR, XPS, HRTEM, spectroscopic ellipsometry, and UV/vis/NIR spectrophotometry). The XRR and HRTEM analyses reveal a layer-by-layer growth mechanism of Ir in atomic scale heterostructures, which is different from the typical island-type growth of metals on dielectrics. Alongside, XPS investigations imply the formation of Ir-O-Al bonding at the interfaces for lower Ir concentrations, in contrast to the nanoparticle core-shell structure formation. Precisely tuning the ratio of the constituents ensures the control of the dispersion profile along with a transition from effective dielectric to metallic heterostructures. The Ir coating thickness was varied ranging from a few angstroms to films of about 7 nm in the heterostructures. The transition has been observed in the structures containing individual Ir coating thicknesses of about 2-4 nm. Following this, we show epsilon-near-zero metamaterials with tunable dielectric constants by precisely varying the composition of such heterostructures. Overall, a comprehensive study on structural and optical properties of the metal-dielectric interfaces of Ir/Al2O3 heterostructures was addressed, indicating an extension of the material portfolio available for novel optical functionalities.

15.
Nanomaterials (Basel) ; 12(3)2022 Jan 26.
Artigo em Inglês | MEDLINE | ID: mdl-35159753

RESUMO

Electron overcharge causes rapid luminescence quenching in the quantum dot (QD) emission layer in QD light-emitting diodes (QD-LEDs), resulting in low device performance. In this paper we describe the application of different aromatic thiol ligands and their influence on device performance as well as their behavior in combination with an electron blocking material (EBM). The three different ligands, 1-octanethiol (OcSH), thiophenol (TP), and phenylbutan-1-thiol (PBSH), were introduced on to InP/ZnSe/ZnS QDs referred to as QD-OcSH, QD-TP, and QD-PBSH. PBSH is in particular applied as a ligand to improve QD solubility and to enhance the charge transport properties synergistically with EBM probably via π-π interaction. We synthesized poly-[N,N-bis[4-(carbazolyl)phenyl]-4-vinylaniline] (PBCTA) and utilized it as an EBM to alleviate excess electrons in the active layer in QD-LEDs. The comparison of the three QD systems in an inverted device structure without the application of PBCTA as an EBM shows the highest efficiency for QD-PBSH. Moreover, when PBCTA is introduced as an EBM in the active layer in combination with QD-PBSH in a conventional device structure, the current efficiency shows a twofold increase compared to the reference device without EBM. These results strongly confirm the role of PBCTA as an EBM that effectively alleviates excess electrons in the active layer, leading to higher device efficiency.

16.
Nanoscale ; 14(4): 1492-1504, 2022 Jan 27.
Artigo em Inglês | MEDLINE | ID: mdl-35024718

RESUMO

Upconverting nanoparticles (UCNPs) are well-known for their capacity to convert near-infrared light into UV/visible light, benefitting various applications where light triggering is required. At the nanoscale, loss of luminescence intensity is observed and thus, a decrease in photoluminescence quantum yield (PLQY), usually ascribed to surface quenching. We evaluate this by measuring the PLQY of NaGdF4:Er3+,Yb3+ UCNPs as a function of size (ca. 15 to 100 nm) and shape (spheres, cubes, hexagons). Our results show that the PLQY of α-phase NaGdF4 Er3+,Yb3+ surpasses that of ß-NaGdF4 for sizes below 20 nm, an observation related to distortion of the crystal lattice when the UCNPs become smaller. The present study also underlines that particle shape must not be neglected as a relevant parameter for PLQY. In fact, based on a mathematical nucleus/hull volumetric model, shape was found to be particularly relevant in the 20 to 60 nm size range of the investigated UCNPs.

17.
Phys Rev Lett ; 107(7): 076601, 2011 Aug 12.
Artigo em Inglês | MEDLINE | ID: mdl-21902412

RESUMO

Hot carrier-induced spin dynamics is analyzed in epitaxial Au/Fe/MgO(001) by a time domain approach. We excite a spin current pulse in Fe by 35 fs laser pulses. The transient spin polarization, which is probed at the Au surface by optical second harmonic generation, changes its sign after a few hundred femtoseconds. This is explained by a competition of ballistic and diffusive propagation considering energy-dependent hot carrier relaxation rates. In addition, we observe the decay of the spin polarization within 1 ps, which is associated with the hot carrier spin relaxation time in Au.

18.
Small Methods ; 5(9): e2100464, 2021 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-34928052

RESUMO

The rich phase diagram of bulk Pr1-x Cax MnO3 resulting in a high tunability of physical properties gives rise to various studies related to fundamental research as well as prospective applications of the material. Importantly, as a consequence of strong correlation effects, electronic and lattice degrees of freedom are vigorously coupled. Hence, it is debatable whether such bulk phase diagrams can be transferred to inherently strained epitaxial thin films. In this paper, the structural orthorhombic to pseudo-cubic transition for x = 0.1 is studied in ion-beam sputtered thin films and differences to the respective bulk system are pointed out by employing in situ heating nano-beam electron diffraction to follow the temperature dependence of lattice constants. In addition, it is demonstrated that controlling the environment during heating, that is, preventing oxygen loss, is crucial in order to avoid irreversible structural changes, which is expected to be a general problem of compounds containing volatile elements under non-equilibrium conditions.

19.
ACS Appl Mater Interfaces ; 13(20): 24013-24023, 2021 May 26.
Artigo em Inglês | MEDLINE | ID: mdl-34000195

RESUMO

A series of bimagnetic heterostructured nanocrystals having an antiferromagnetic NiO core and a ferrimagnetic MnxNi1-xO and/or FiM Mn3O4 island nanophase overgrowth has been synthesized under varying aqueous solution pH conditions. The two-step self-assembly process employs a thermal decomposition method to synthesize NiO nanoparticles, followed by growth of the MnxNi1-xO and/or Mn3O4 nanophase over the NiO core using hydrothermal synthesis at pH values ranging from 2.4-7.0. The environmentally benign hydrothermal process involves pH control of the protonation vs hydroxylation reactions occurring at the nanoparticle surface. TEM analysis and Rietveld refinement of XRD data show that three distinct types of heterostructured nanocrystals occur: NiO/MnxNi1-xO core-shell-like heterostructures at the pH of 2.4, mixed NiO/MnxNi1-xO and/or/Mn3O4 core-overgrowth structures for 2.4 < pH < 4.5, and predominantly NiO/Mn3O4 core-island structures for pH > 4.5. The magnetic coercivity and exchange bias of the heterostructured nanocrystals vary systematically with the pH of the aqueous solution used to synthesize the samples. The temperature-dependent magnetization and hysteresis loop data are consistent with the nature of overlayer coverage of the NiO core. Our DFT based calculations show that the MnxNi1-xO phase has ferrimagnetic properties with a stable spin orientation along the ⟨111⟩ orientation. Furthermore, the calculations show that the magnetic anisotropy constant (K1) of the Mn3O4 phase is considerably larger than that of the MnxNi1-xO phase, which is confirmed by our experimental results. The coercivity and exchange bias field are the largest for the NiO/Mn3O4 core-island nanocrystals, synthesized at a pH value of 5.0, with robust values of nearly 6 kOe and 3 kOe, respectively. This work demonstrates the tunability of hydrothermal deposition, and concomitant magnetic coercivity and exchange bias properties, of MnxNi1-xO and/or Mn3O4 nanophase overgrowth over a NiO core with pH, that makes these heterostructured nanocrystals potentially useful for magnetic device, biomedical, and other applications.

20.
Biosensors (Basel) ; 11(12)2021 Dec 14.
Artigo em Inglês | MEDLINE | ID: mdl-34940272

RESUMO

The imagination of clearly separated core-shell structures is already outdated by the fact, that the nanoparticle core-shell structures remain in terms of efficiency behind their respective bulk material due to intermixing between core and shell dopant ions. In order to optimize the photoluminescence of core-shell UCNP the intermixing should be as small as possible and therefore, key parameters of this process need to be identified. In the present work the Ln(III) ion migration in the host lattices NaYF4 and NaGdF4 was monitored. These investigations have been performed by laser spectroscopy with help of lanthanide resonance energy transfer (LRET) between Eu(III) as donor and Pr(III) or Nd(III) as acceptor. The LRET is evaluated based on the Förster theory. The findings corroborate the literature and point out the migration of ions in the host lattices. Based on the introduced LRET model, the acceptor concentration in the surrounding of one donor depends clearly on the design of the applied core-shell-shell nanoparticles. In general, thinner intermediate insulating shells lead to higher acceptor concentration, stronger quenching of the Eu(III) donor and subsequently stronger sensitization of the Pr(III) or the Nd(III) acceptors. The choice of the host lattice as well as of the synthesis temperature are parameters to be considered for the intermixing process.


Assuntos
Elementos da Série dos Lantanídeos , Nanopartículas , Transferência de Energia , Íons
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