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By combining electrical, physical, and transport/atomistic modeling results, this study identifies critical conductive filament (CF) features controlling TiN/HfO2/TiN resistive memory (RRAM) operations. The leakage current through the dielectric is found to be supported by the oxygen vacancies, which tend to segregate at hafnia grain boundaries. We simulate the evolution of a current path during the forming operation employing the multiphonon trap-assisted tunneling (TAT) electron transport model. The forming process is analyzed within the concept of dielectric breakdown, which exhibits much shorter characteristic times than the electroforming process conventionally employed to describe the formation of the conductive filament. The resulting conductive filament is calculated to produce a non-uniform temperature profile along its length during the reset operation, promoting preferential oxidation of the filament tip. A thin dielectric barrier resulting from the CF tip oxidation is found to control filament resistance in the high resistive state. Field-driven dielectric breakdown of this barrier during the set operation restores the filament to its initial low resistive state. These findings point to the critical importance of controlling the filament cross section during forming to achieve low power RRAM cell switching.

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Resistive switching (RS) phenomenon in the HfO2 dielectric has been indirectly observed at device level in previous studies using metal-insulator-metal structures, but its origin remains unclear. In this work, using the enhanced conductive atomic force microscope (ECAFM), we have been able to obtain in situ direct observation of RS with nanometric resolution. The ECAFM measurements reveal that the conductive filaments exhibiting the RS are primarily formed at the grain boundaries, which were shown exhibiting especially low breakdown voltage due to their intrinsic high density of the oxygen vacancies.

Multilevel operation in resistive switching memory (RRAM) based on HfOx is demonstrated through variable sizes and orientations of the conductive filament. Memory states with the same resistance, but opposite orientation of defects, display a different response to an applied read voltage, therefore allowing an improvement of the information stored in each physical cell. The multilevel scheme allows a 50% increase (from 2 to 3 bits) of the stored information.

A side-by-side comparison of the TiO2 deposition kinetics and the corresponding microstructures was studied. The two precursors were titanium(IV) isopropoxide and anhydrous titanium(IV) nitrate, and all depositions were conducted at low pressures (<10-4 Torr) in an ultrahigh vacuum chemical vapor deposition reactor. For both precursors deposition kinetics were qualitatively similar and exhibited three distinct regimes as a function of temperature. At the lowest temperatures, growth was limited by the rate of precursor reaction on the substrate surface. At intermediate temperatures flux-limited growth was obtained, and at the highest temperatures the growth rates decreased with increasing temperatures. The overall behavior was modeled quantitatively for each precursor using a two-step mechanism involving reversible adsorption followed by irreversible reaction. Titanium(IV) nitrate exhibited a lower activation energy of reaction (E r = 98 kJ/mol) which allowed deposition at lower temperatures compared to titanium(IV) isopropoxide (E r = 135 kJ/mol). The film microstructures were examined using transmission and scanning electron microscopy and X-ray diffraction. Comparison of the microstructures of films deposited at similar temperatures revealed significant differences in the reaction rate-limited regime. As the growth rates of the two precursors converged in the flux-limited regime, the respective microstructures became indistinguishable. The importance of precursor surface coverage and diffusion on this effect is described.