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We fabricated memristive devices using focused electron beam-induced deposition (FEBID) as a direct-writing technique employing a Pt/TiO2/Pt sandwich layer device configuration. Pinching in the measured current-voltage characteristics (i-v), the characteristic fingerprint of memristive behavior was clearly observed. The temperature dependence was measured for both high and low resistive states in the range from 290 K down to about 2 K, showing a stretched exponential behavior characteristic of Mott-type variable-range hopping. From this observation, a valence change mechanism of the charge transport inside the TiO2 layer can be deduced.
Focused electron-beam-induced deposition (FEBID) is a highly versatile direct-write approach with particular strengths in the 3D nanofabrication of functional materials. Despite its apparent similarity to other 3D printing approaches, non-local effects related to precursor depletion, electron scattering and sample heating during the 3D growth process complicate the shape-true transfer from a target 3D model to the actual deposit. Here, we describe an efficient and fast numerical approach to simulate the growth process, which allows for a systematic study of the influence of the most important growth parameters on the resulting shape of the 3D structures. The precursor parameter set derived in this work for the precursor Me3PtCpMe enables a detailed replication of the experimentally fabricated nanostructure, taking beam-induced heating into account. The modular character of the simulation approach allows for additional future performance increases using parallelization or drawing on the use of graphics cards. Ultimately, beam-control pattern generation for 3D FEBID will profit from being routinely combined with this fast simulation approach for optimized shape transfer.
We present experimental results and theoretical simulations of the adsorption behavior of the metal–organic precursor Co2(CO)8 on SiO2 surfaces after application of two different pretreatment steps, namely by air plasma cleaning or a focused electron beam pre-irradiation. We observe a spontaneous dissociation of the precursor molecules as well as autodeposition of cobalt on the pretreated SiO2 surfaces. We also find that the differences in metal content and relative stability of these deposits depend on the pretreatment conditions of the substrate. Transport measurements of these deposits are also presented. We are led to assume that the degree of passivation of the SiO2 surface by hydroxyl groups is an important controlling factor in the dissociation process. Our calculations of various slab settings, using dispersion-corrected density functional theory, support this assumption. We observe physisorption of the precursor molecule on a fully hydroxylated SiO2 surface (untreated surface) and chemisorption on a partially hydroxylated SiO2 surface (pretreated surface) with a spontaneous dissociation of the precursor molecule. In view of these calculations, we discuss the origin of this dissociation and the subsequent autocatalysis.
Vanadium and Manganese Carbonyls as Precursors in Electron-Induced and Thermal Deposition Processes
(2022)
The material composition and electrical properties of nanostructures obtained from focused electron beam-induced deposition (FEBID) using manganese and vanadium carbonyl precursors have been investigated. The composition of the FEBID deposits has been compared with thin films derived by the thermal decomposition of the same precursors in chemical vapor deposition (CVD). FEBID of V(CO)6 gives access to a material with a V/C ratio of 0.63–0.86, while in CVD a lower carbon content with V/C ratios of 1.1–1.3 is obtained. Microstructural characterization reveals for V-based materials derived from both deposition techniques crystallites of a cubic phase that can be associated with VC1−xOx. In addition, the electrical transport measurements of direct-write VC1−xOx show moderate resistivity values of 0.8–1.2 × 103 µΩ·cm, a negligible influence of contact resistances and signatures of a granular metal in the temperature-dependent conductivity. Mn-based deposits obtained from Mn2(CO)10 contain ~40 at% Mn for FEBID and a slightly higher metal percentage for CVD. Exclusively insulating material has been observed in FEBID deposits as deduced from electrical conductivity measurements. In addition, strong tendencies for postgrowth oxidation have to be considered.