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1.
Nanomaterials (Basel) ; 12(17)2022 Sep 03.
Artigo em Inglês | MEDLINE | ID: mdl-36080096

RESUMO

Despite the great potential of Hf0.5Zr0.5O2 (HZO) ferroelectrics, reliability issues, such as wake-up, fatigue, endurance limitations, imprint and retention loss, impede the implementation of HZO to nonvolatile memory devices. Herein, a study of the reliability properties in HZO-based stacks with the conventional TiN top electrode and Ru electrode, which is considered a promising alternative to TiN, is performed. An attempt to distinguish the mechanisms underlying the wake-up, fatigue and retention loss in both kinds of stacks is undertaken. Overall, both stacks show pronounced wake-up and retention loss. Moreover, the fatigue and retention loss were found to be worsened by Ru implementation. The huge fatigue was suggested to be because Ru does not protect HZO against oxygen vacancies generation during prolonged cycling. The vacancies generated in the presence of Ru are most likely deeper traps, as compared to the traps formed at the interface with the TiN electrode. Implementing the new procedure, which can separate the depolarization-caused retention loss from the imprint-caused one, reveal a rise in the depolarization contribution with Ru implementation, accompanied by the maintenance of similarly high imprint, as in the case with the TiN electrode. Results show that the mechanisms behind the reliability issues in HZO-based capacitors are very electrode dependent and simple approaches to replacing the TiN electrode with the one providing, for example, just higher remnant polarization or lower leakages, become irrelevant on closer examination.

2.
Light Sci Appl ; 11(1): 92, 2022 Apr 11.
Artigo em Inglês | MEDLINE | ID: mdl-35410998

RESUMO

Carbon dots (CDs) are light-emitting nanoparticles that show great promise for applications in biology and medicine due to the ease of fabrication, biocompatibility, and attractive optical properties. Optical chirality, on the other hand, is an intrinsic feature inherent in many objects in nature, and it can play an important role in the formation of artificial complexes based on CDs that are implemented for enantiomer recognition, site-specific bonding, etc. We employed a one-step hydrothermal synthesis to produce chiral CDs from the commonly used precursors citric acid and ethylenediamine together with a set of different chiral precursors, namely, L-isomers of cysteine, glutathione, phenylglycine, and tryptophan. The resulting CDs consisted of O,N-doped (and also S-doped, in some cases) carbonized cores with surfaces rich in amide and hydroxyl groups; they exhibited high photoluminescence quantum yields reaching 57%, chiral optical signals in the UV and visible spectral regions, and two-photon absorption. Chiral signals of CDs were rather complex and originated from a combination of the chiral precursors attached to the CD surface, hybridization of lower-energy levels of chiral chromophores formed within CDs, and intrinsic chirality of the CD cores. Using DFT analysis, we showed how incorporation of the chiral precursors at the optical centers induced a strong response in their circular dichroism spectra. The optical characteristics of these CDs, which can easily be dispersed in solvents of different polarities, remained stable during pH changes in the environment and after UV exposure for more than 400 min, which opens a wide range of bio-applications.

3.
Nanomaterials (Basel) ; 12(3)2022 Feb 05.
Artigo em Inglês | MEDLINE | ID: mdl-35159888

RESUMO

Carbon dots (CDs) with an emission in the near infrared spectral region are attractive due to their promising applications in bio-related areas, while their fabrication still remains a challenging task. Herein, we developed a template-assisted method using porous silica microspheres for the formation of CDs with optical transitions in the near infrared. Two organic dyes, Rhodamine 6G and IR1061 with emission in the yellow and near infrared spectral regions, respectively, were used as precursors for CDs. Correlation of morphology and chemical composition with optical properties of obtained CDs revealed the origin of their emission, which is related to the CDs' core optical transitions and dye-derivatives within CDs. By varying annealing temperature, different kinds of optical centers as derivatives of organic dyes are formed in the microsphere's pores. The template-assisted method allows us to synthesize CDs with an emission peaked at 1085 nm and photoluminescence quantum yield of 0.2%, which is the highest value reported so far for CDs emitting at wavelengths longer than 1050 nm.

4.
Nanomaterials (Basel) ; 11(11)2021 Nov 18.
Artigo em Inglês | MEDLINE | ID: mdl-34835874

RESUMO

The development of new strategies for the mass synthesis of SiC nanocrystals with high structure perfection and narrow particle size distribution remains in demand for high-tech applications. In this work, the size-controllable synthesis of the SiC 3C polytype, free of sp2 carbon, with high structure quality nanocrystals, was realized for the first time by the pyrolysis of organosilane C12H36Si6 at 8 GPa and temperatures up to 2000 °C. It is shown that the average particle size can be monotonically changed from ~2 nm to ~500 nm by increasing the synthesis temperature from 800 °C to 1400 °C. At higher temperatures, further enlargement of the crystals is impeded, which is consistent with the recrystallization mechanism driven by a decrease in the surface energy of the particles. The optical properties investigated by IR transmission spectroscopy, Raman scattering, and low-temperature photoluminescence provided information about the concentration and distribution of carriers in nanoparticles, as well as the dominant type of internal point defects. It is shown that changing the growth modes in combination with heat treatment enables control over not only the average crystal size, but also the LO phonon-plasmon coupled modes in the crystals, which is of interest for applications related to IR photonics.

5.
Nanoscale ; 13(17): 8058-8066, 2021 May 06.
Artigo em Inglês | MEDLINE | ID: mdl-33956931

RESUMO

Since chirality is one of the phenomena often occurring in nature, optically active chiral compounds are important for applications in the fields of biology, pharmacology, and medicine. With this in mind, chiral carbon dots (CDs), which are eco-friendly and easy-to-obtain light-emissive nanoparticles, offer great potential for sensing, bioimaging, enantioselective synthesis, and development of emitters of circularly polarized light. Herein, chiral CDs have been produced via two synthetic approaches using a chiral amino acid precursor l/d-cysteine: (i) surface modification treatment of achiral CDs at room temperature and (ii) one-pot carbonization in the presence of chiral precursor. The chiral signal in the absorption spectra of synthesized CDs originates not only from the chiral precursor but from the optical transitions attributed to the core and surface states of CDs. The use of chiral amino acid molecules in the CD synthesis through carbonization results in a substantial (up to 8 times) increase in their emission quantum yield. Moreover, the synthesized CDs show two-photon absorption which is an attractive feature for their potential bioimaging and sensing applications.


Assuntos
Nanopartículas , Pontos Quânticos , Carbono , Cisteína , Estereoisomerismo , Temperatura
6.
Nanoscale ; 13(5): 3070-3078, 2021 Feb 07.
Artigo em Inglês | MEDLINE | ID: mdl-33522554

RESUMO

The optical properties of chemically synthesized carbon dots (CDs) can be widely tuned via doping and surface modification with heteroatoms such as nitrogen, which results in a range of potential applications. Herein, two most commonly used synthesis approaches, namely, solvothermal and microwave-assisted thermal treatments, have been used for the preparation of CDs from phloroglucinol using three different nitrogen containing solvents, namely, ethylenediamine, dimethylformamide, and formamide. Based on the analysis of the morphology and optical properties, we demonstrate the tenability of the CD appearance from amorphous or well-carbonized spherical particles to onion-like ones, which is controlled by solvent polarity, whereas the thermal treatment conditions mostly influence the degree of N-doping and the nature of emissive centers of CDs formed. The findings of this study expand the toolkit of the available CDs with variable morphology and energy structure.

7.
ACS Appl Mater Interfaces ; 12(49): 55331-55341, 2020 Dec 09.
Artigo em Inglês | MEDLINE | ID: mdl-33190485

RESUMO

Resistive switching (RS) device behavior is highly dependent on both insulator and electrode material properties. In particular, the bottom electrode (BE) surface morphology can strongly affect RS characteristics. In this work, Ru films with different thicknesses grown on a TiN layer by radical-enhanced atomic layer deposition (REALD) are used as an inert BE in TaOx-based RS structures. The REALD Ru surface roughness is found to increase by more than 1 order of magnitude with the increase in the reaction cycle number. Simultaneously, a wide range of RS parameters, such as switching voltage, resistance both in low and high resistance states, endurance, and so forth, monotonically change. A simplified model is proposed to explain the linkage between RS properties and roughness of the Ru surface. The field distribution was simulated based on the observed surface morphologies, and the resulting conducting filament formation was anticipated based on the local field enhancement. Conductive atomic force microscopy confirmed the theoretical expectations.

8.
J Phys Condens Matter ; 33(3): 035001, 2020 Oct 20.
Artigo em Inglês | MEDLINE | ID: mdl-33078711

RESUMO

Technological applications involving 2D MoS2 require transfer of chemical vapor deposition (CVD) grown material from its original substrate and subsequent lithographic processes. Inevitably, those steps contaminate the surface of the 2D material with polymeric residues affecting the electronic and optical properties of the MoS2. Annealing in forming gas is considered an efficient treatment to partially remove such residues. However, hydrogen also interacts with MoS2 creating or saturating sulfur vacancies. Sulfur vacancies are known to be at the origin of n-doping evident in the majority of as-grown MoS2 samples. In this context, investigating the impact of thermal annealing in forming gas on the electronic and optical properties of MoS2 monolayer is technologically important. In order to address this topic, we have systematically studied the evolution of CVD grown MoS2 monolayer using Raman spectroscopy, photoluminescence, x-ray photoelectron spectroscopy and transport measurements through a series of thermal annealing in forming gas at temperatures up to 500 °C. Efficient removal of the polymeric residues is demonstrated at temperatures as low as 200 °C. Above this value, carrier density modulation is identified by photoluminescence, x-ray photoelectron spectroscopy and electrical characterization and is correlated to the creation of sulfur vacancies. Finally, the degradation of the MoS2 single layer is verified with annealing at or above 350 °C through Raman and photocurrent measurements.

9.
Artigo em Inglês | MEDLINE | ID: mdl-33017817

RESUMO

Technological applications involving 2D MoS2 require transfer of CVD grown material from its original substrate and subsequent lithographic processes. Inevitably, those steps contaminate the surface of the 2D material with polymeric residues affecting the electronic and optical properties of the MoS2. Annealing in forming gas is considered an efficient treatment to partially remove such residues. However, hydrogen also interacts with MoS2 creating or saturating sulfur vacancies. Sulfur vacancies are known to be at the origin of n-doping evident in the majority of as-grown MoS2 samples. In this context, investigating the impact of thermal annealing in forming gas on the electronic and optical properties of MoS2 monolayer is technologically important. In order to address this topic, we have systematically studied the evolution of CVD grown MoS2 monolayer using Raman spectroscopy, photoluminescence, x-ray photoelectron spectroscopy and transport measurements through a series of thermal annealing in forming gas at temperatures up to 500 °C. Efficient removal of the polymeric residues is demonstrated at temperature as low as 200 °C. Above this value, carrier density modulation is identified by photoluminescence, x-ray photoelectron spectroscopy and electrical characterization and is correlated to the creation of sulfur vacancies. Finally, the degradation of the MoS2 single layer is verified with annealing at or above 350 °C through Raman and photocurrent measurements.

10.
ACS Appl Energy Mater ; 2(12): 8747-8756, 2019 Dec 23.
Artigo em Inglês | MEDLINE | ID: mdl-31894204

RESUMO

The combination of oxide and heavier chalcogenide layers in thin film photovoltaics suffers limitations associated with oxygen incorporation and sulfur deficiency in the chalcogenide layer or with a chemical incompatibility which results in dewetting issues and defect states at the interface. Here, we establish atomic layer deposition (ALD) as a tool to overcome these limitations. ALD allows one to obtain highly pure Sb2S3 light absorber layers, and we exploit this technique to generate an additional interfacial layer consisting of 1.5 nm ZnS. This ultrathin layer simultaneously resolves dewetting and passivates defect states at the interface. We demonstrate via transient absorption spectroscopy that interfacial electron recombination is one order of magnitude slower at the ZnS-engineered interface than hole recombination at the Sb2S3/P3HT interface. The comparison of solar cells with and without oxide incorporation in Sb2S3, with and without the ultrathin ZnS interlayer, and with systematically varied Sb2S3 thickness provides a complete picture of the physical processes at work in the devices.

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