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1.
Nucl Med Biol ; 84-85: 102-110, 2020.
Artigo em Inglês | MEDLINE | ID: mdl-32334356

RESUMO

INTRODUCTION: Porous silicon (PSi) nanoparticles are capable of delivering therapeutic payloads providing targeted delivery and sustained release of the payloads. In this work we describe the development and proof-of-concept in vivo evaluation of thermally hydrocarbonized porous silicon (PSi) nanoparticles that are implanted with radioactive 155Tb atoms and coated with red blood cell (RBC) membrane (155Tb-THCPSi). The developed nanocomposites can be utilized as an intravenous delivery platform for theranostic radionuclides. METHODS: THCPSi thin films were implanted with 155Dy ions that decay to 155Tb at the ISOLDE radioactive ion-beam (RIB) facility at CERN. The films were processed to nanoparticles by ball-milling and sonication, and subsequently coated with either a solid lipid and RBC membrane or solely with RBC membrane. The nanocomposites were evaluated in vitro for stability and in vivo for circulation half-life and ex vivo for biodistribution in Balb/c mice. RESULTS: Nanoporous THCPSi films were successfully implanted with 155Tb and processed to coated nanoparticles. The in vitro stability of the particles in plasma and buffer solutions was not significantly different between the particle types, and therefore the RBC membrane coated particles with less laborious processing method were chosen for the biological evaluation. The RBC membrane coating enhanced significantly the blood half-life compared to bare THCPSi particles. In the ex vivo biodistribution study a pronounced accumulation to the spleen was found, with lower uptake in the liver and a minor uptake in the lung, gall bladder and bone marrow. CONCLUSIONS: We have demonstrated, using 155Tb RIB-implanted PSi nanoparticles coated with mouse RBC membranes, the feasibility of using such a theranostic nanosystem for the delivery of RIB based radionuclides with prolonged circulation time. ADVANCES IN KNOWLEDGE AND IMPLICATIONS FOR PATIENT CARE: For the first time, the RIB implantation technique has been utilized to produce PSi nanoparticle with a surface modified for better persistence in circulation. When optimized, these particles could be used in targeted radionuclide therapy with a combination of chemotherapeutic payload within the PSi structure.

2.
Nanotechnology ; 2020 Jan 24.
Artigo em Inglês | MEDLINE | ID: mdl-31978899

RESUMO

Amorphous SiO2-Nb2O5 nanolaminates and mixture films were grown by atomic layer deposition. The films were grown at 300 oC from Nb(OC2H5)5, Si2(NHC2H5)6, and O3 to thicknesses ranging from 13 to 130 nm. The niobium to silicon atomic ratio was varied in the range of 0.11-7.20. After optimizing the composition, resistive switching properties could be observed in the form of characteristic current-voltage behavior. Switching parameters in the conventional regime were well defined only in a SiO2:Nb2O5 mixture at certain, optimized, composition with Nb:Si atomic ratio of 0.13, whereas low-reading voltage measurements allowed recording memory effects in a wider composition range.

3.
ACS Omega ; 4(6): 11205-11214, 2019 Jun 30.
Artigo em Inglês | MEDLINE | ID: mdl-31460221

RESUMO

Herein, we report an atomic layer deposition (ALD) process for Cu2O thin films using copper(II) acetate [Cu(OAc)2] and water vapor as precursors. This precursor combination enables the deposition of phase-pure, polycrystalline, and impurity-free Cu2O thin films at temperatures of 180-220 °C. The deposition of Cu(I) oxide films from a Cu(II) precursor without the use of a reducing agent is explained by the thermally induced reduction of Cu(OAc)2 to the volatile copper(I) acetate, CuOAc. In addition to the optimization of ALD process parameters and characterization of film properties, we studied the Cu2O films in the fabrication of photoconductor devices. Our proof-of-concept devices show that approximately 20 nm thick Cu2O films can be used for photodetection in the visible wavelength range and that the thin film photoconductors exhibit improved device characteristics in comparison to bulk Cu2O crystals.

4.
Nanoscale Res Lett ; 14(1): 55, 2019 Feb 12.
Artigo em Inglês | MEDLINE | ID: mdl-30747362

RESUMO

In this work, we report the successful growth of high-quality SiO2 films by low-temperature plasma-enhanced atomic layer deposition using an oxidant which is compatible with moisture/oxygen sensitive materials. The SiO2 films were grown at 90 °C using CO2 and Bis(tertiary-butylamino)silane as process precursors. Growth, chemical composition, density, optical properties, and residual stress of SiO2 films were investigated. SiO2 films having a saturated growth-per-cycle of ~ 1.15 Å/cycle showed a density of ~ 2.1 g/cm3, a refractive index of ~ 1.46 at a wavelength of 632 nm, and a low tensile residual stress of ~ 30 MPa. Furthermore, the films showed low impurity levels with bulk concentrations of ~ 2.4 and ~ 0.17 at. % for hydrogen and nitrogen, respectively, whereas the carbon content was found to be below the measurement limit of time-of-flight elastic recoil detection analysis. These results demonstrate that CO2 is a promising oxidizing precursor for moisture/oxygen sensitive materials related plasma-enhanced atomic layer deposition processes.

5.
Angew Chem Int Ed Engl ; 57(44): 14538-14542, 2018 Oct 26.
Artigo em Inglês | MEDLINE | ID: mdl-30048031

RESUMO

Rhenium is both a refractory metal and a noble metal that has attractive properties for various applications. Still, synthesis and applications of rhenium thin films have been limited. We introduce herein the growth of both rhenium metal and rhenium nitride thin films by the technologically important atomic layer deposition (ALD) method over a wide deposition temperature range using fast, simple, and robust surface reactions between rhenium pentachloride and ammonia. Films are grown and characterized for compositions, surface morphologies and roughnesses, crystallinities, and resistivities. Conductive rhenium subnitride films of tunable composition are obtained at deposition temperatures between 275 and 375 °C, whereas pure rhenium metal films grow at 400 °C and above. Even a just 3 nm thick rhenium film is continuous and has a low resistivity of about 90 µΩ cm showing potential for applications for which also other noble metals and refractory metals have been considered.

6.
Adv Mater ; 30(24): e1703622, 2018 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-29315833

RESUMO

2D materials research is advancing rapidly as various new "beyond graphene" materials are fabricated, their properties studied, and materials tested in various applications. Rhenium disulfide is one of the 2D transition metal dichalcogenides that has recently shown to possess extraordinary properties such as that it is not limited by the strict monolayer thickness requirements. The unique inherent decoupling of monolayers in ReS2 combined with a direct bandgap and highly anisotropic properties makes ReS2 one of the most interesting 2D materials for a plethora of applications. Here, a highly controllable and precise atomic layer deposition (ALD) technique is applied to deposit ReS2 thin films. Film growth is demonstrated on large area (5 cm × 5 cm) substrates at moderate deposition temperatures between 120 and 500 °C, and the films are extensively characterized using field emission scanning electron microscopy/energy-dispersive X-ray spectroscopy, X-ray diffractometry using grazing incidence, atomic force microscopy, focused ion beam/transmission electron microscopy, X-ray photoelectron spectroscopy, and time-of-flight elastic recoil detection analysis techniques. The developed ReS2 ALD process highlights the potential of the material for applications beyond planar structure architectures. The ALD process also offers a route to an upgrade to an industrial scale.

7.
Langmuir ; 32(41): 10559-10569, 2016 Oct 18.
Artigo em Inglês | MEDLINE | ID: mdl-27673703

RESUMO

Nucleation and conformality are important issues, when depositing thin films for demanding applications. In this study, iridium and iridium dioxide (IrO2) films were deposited by atomic layer deposition (ALD), using five different processes. Different reactants, namely, O2, air, consecutive O2 and H2 (O2 + H2), and consecutive O3 and H2 (O3 + H2) pulses were used with iridium acetylacetonate [Ir(acac)3] to deposit Ir, while IrO2 was deposited using Ir(acac)3 and O3. Nucleation was studied using a combination of methods for film thickness and morphology evaluation. In conformality studies, microscopic lateral high-aspect-ratio (LHAR) test structures, specifically designed for accurate and versatile conformality testing of ALD films, were used. The order of nucleation, from the fastest to the slowest, was O2 + H2 > air ≈ O2 > O3 > O3 + H2, whereas the order of conformality, from the best to the worst, was O3 + H2 > O2 + H2 > O2 > O3. In the O3 process, a change in film composition from IrO2 to metallic Ir was seen inside the LHAR structures. Compared to the previous reports on ALD of platinum-group metals, most of the studied processes showed good to excellent results.

8.
Nanotechnology ; 26(26): 265304, 2015 Jul 03.
Artigo em Inglês | MEDLINE | ID: mdl-26062985

RESUMO

A focused ion beam (FIB) is otherwise an efficient tool for nanofabrication of silicon structures but it suffers from the poor thermal stability of the milled surfaces caused by segregation of implanted gallium leading to severe surface roughening upon already slight annealing. In this paper we show that selective etching with KOH:H2O2 solutions removes the surface layer with high gallium concentration while blocking etching of the surrounding silicon and silicon below the implanted region. This remedies many of the issues associated with gallium FIB nanofabrication of silicon. After the gallium removal sub-nm surface roughness is retained even during annealing. As the etching step is self-limited to a depth of 25-30 nm for 30 keV ions, it is well suited for defining nanoscale features. In what is essentially a reversal of gallium resistless lithography, local implanted areas can be prepared and then subsequently etched away. Nanopore arrays and sub-100 nm trenches can be prepared this way. When protective oxide masks such as Al2O3 grown with atomic layer deposition are used together with FIB milling and KOH:H2O2 etching, ion-induced amorphization can be confined to sidewalls of milled trenches.

9.
Phys Chem Chem Phys ; 17(16): 10838-48, 2015 Apr 28.
Artigo em Inglês | MEDLINE | ID: mdl-25815628

RESUMO

Ar ion irradiation-induced changes in the morphology of bare and 1-dodecanethiol self-assembled monolayer (SAM) covered Au(111) surfaces have been investigated systematically. The changes were followed by scanning tunneling microscopy (STM) and X-ray photoelectron spectroscopy (XPS) measurements while varying the ion charge (Ar(+),Ar(4+)), energy (10-40 keV) and fluency (10(12)-10(13) ions per cm(2)). The impact of flame-annealing of the Au(111) surface on subsequent ion bombardment was considered and more prominent related surface morphology changes were noted. The irradiation of Au(111) surfaces generated Au vacancy and adatom islands and caused roughening of step edges. The size and abundance of these islands and the level of deformation on the step edges depended strongly on the ion energy and fluency. In case of the SAM functionalized surface, the gold vacancy islands present on the surface already from the SAM formation were modified, step edges roughened and gold adatom islands formed. Similarly to the bare surface, the level of surface deformation increased as a function of ion energy and fluency. The Ar(4+) irradiation caused on the average slightly larger vacancy islands on the SAM modified surfaces than the Ar(+) irradiation. Irradiation to fluency of 10(12) ions per cm(2) mostly maintained standing-up orientation of the thiolates whereas irradiation to higher fluency resulted in reduced surface coverage and flat-lying molecules. As a general trend the DDT covered surfaces were more susceptible for irradiation-induced surface morphology changes than the unmodified Au surfaces.

10.
Nanotechnology ; 26(13): 134004, 2015 Mar 27.
Artigo em Inglês | MEDLINE | ID: mdl-25764569

RESUMO

In this work we report on the influence of nitrogen ambient thermal effects on the performance of Pt/Al2O3/Si3N4/SiO2/Si memory capacitors. Two post deposition annealing (PDA) furnace steps were employed, at 850 and 1050 °C both for 15 min. The alumina films were deposited by atomic layer deposition using TMA/H2O at 250 °C. The structural characteristics of the stacks were evaluated by transmission electron microscopy and x-ray reflectivity measurements. The memory performance of the stacks was evaluated by write/erase and erase/write measurements, endurance and retention testing. It was found that in as-deposited state the Al2O3 layer is defective resulting in strong leakage currents, controlled by deep defects states. Thus, this behavior inhibits the memory functionality of the stacks. PDA crystallizes and condenses the Al2O3 transforming the layer from amorphous to polycrystalline. During this transformation the Al2O3 electrical quality improves greatly indicating that a significant number of these deep defects have been removed during annealing. Physical reasoning implies that the most plausible origin of these deep defects is hydrogen. However, the polycrystalline Al2O3 films showed inferior retention characteristics which are attributed to grain boundary related shallow defects. The findings of this work could pave the way for more efficient annealing schemes, in which an important factor is the time interval for hydrogen out-diffusion from the Al2O3 layer.

11.
J Phys Chem A ; 119(11): 2298-306, 2015 Mar 19.
Artigo em Inglês | MEDLINE | ID: mdl-25105932

RESUMO

Bi2Te3 thin films were deposited by atomic layer deposition (ALD) from BiCl3 and (Et3Si)2Te at 160-300 °C. The process was studied in detail, and growth properties typical of ALD were verified. Films were stoichiometric with low impurity content. The film thickness was easily controlled with the number of deposition cycles. Properties of the ALD Bi2Te3 thin films were found to be comparable to those reported in literature for Bi2Te3 films made by other methods. Films crystallized to a rhombohedral phase, and there was a preferred orientation to the growth. Electrical and thermoelectric properties were also determined to be comparable to literature values.

12.
Biointerphases ; 9(3): 031008, 2014 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-25280849

RESUMO

Nanocrystalline hydroxyapatite thin films were fabricated on silicon and titanium by atomic layer deposition (ALD) of CaCO3 and its subsequent conversion to hydroxyapatite by diammonium hydrogen phosphate (DAP) solution. The effects of conversion process parameters to crystallinity and morphology of the films were examined. DAP concentration was found to be critical in controlling the crystal size and homogeneity of the films. The hydroxyapatite phase was identified by XRD. ToF-elastic recoil detection analysis studies revealed that the films are calcium deficient in relation to hydroxyapatite with a Ca/P ratio of 1.39 for films converted with 0.2 M DAP at 95 °C. The coatings prepared on titanium conformally follow the rough surface topography of the substrate, verifying that the good step coverage of the ALD method was maintained in the conversion process. The dissolution tests revealed that the coating was nondissolvable in the cell culture medium. Annealing the coated sample at 700 °C for 1 h seemed to enhance its bonding properties to the substrate. Also, the biocompatibility of the coatings was confirmed by human bone marrow derived cells in vitro. The developed method provides a new possibility to produce thin film coatings on titanium implants with bone-type hydroxyapatite that is biocompatible with human osteoblasts and osteoclasts.


Assuntos
Carbonato de Cálcio/química , Durapatita/química , Nanopartículas/química , Humanos , Fosfatos/química , Solubilidade , Difração de Raios X
13.
J Phys Chem Lett ; 5(24): 4319-23, 2014 Dec 18.
Artigo em Inglês | MEDLINE | ID: mdl-26273981

RESUMO

The atomic layer deposition (ALD) method was applied to grow thin polycrystalline BiFeO3 (BFO) films on Pt/SiO2/Si substrates. The 50 nm thick films were found to exhibit high resistivity, good morphological integrity, and homogeneity achieved by the applied ALD technique. Magnetic characterization revealed saturated magnetization of 25 emu/cm(3) with temperature-dependent coercivity varying from 5 to 530 Oe within the temperature range from 300 to 2 K. Magnetism observed in the films was found to change gradually from ferromagnetic spin ordering to pinned magnetic domain interactions mixed with weak spin-glass-like behavior of magnetically frustrated antiferromagnetic/ferromagnetic (AFM-FM) spin ordering depending on the temperature and magnitude of the applied magnetic field. Antiferromagnetic order of spin cycloids was broken in polycrystalline films by crystal sizes smaller than the cycloid length (∼60 nm). Uncompensated spincycloids and magnetic domain walls were found to be the cause of the high magnetization of the BFO films.

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