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1.
Nat Commun ; 15(1): 860, 2024 Jan 29.
Article in English | MEDLINE | ID: mdl-38287021

ABSTRACT

HfO2-based thin films hold huge promise for integrated devices as they show full compatibility with semiconductor technologies and robust ferroelectric properties at nanometer scale. While their polarization switching behavior has been widely investigated, their electromechanical response received much less attention so far. Here, we demonstrate that piezoelectricity in Hf0.5Zr0.5O2 ferroelectric capacitors is not an invariable property but, in fact, can be intrinsically changed by electrical field cycling. Hf0.5Zr0.5O2 capacitors subjected to ac cycling undergo a continuous transition from a positive effective piezoelectric coefficient d33 in the pristine state to a fully inverted negative d33 state, while, in parallel, the polarization monotonically increases. Not only can the sign of d33 be uniformly inverted in the whole capacitor volume, but also, with proper ac training, the net effective piezoresponse can be nullified while the polarization is kept fully switchable. Moreover, the local piezoresponse force microscopy signal also gradually goes through the zero value upon ac cycling. Density functional theory calculations suggest that the observed behavior is a result of a structural transformation from a weakly-developed polar orthorhombic phase towards a well-developed polar orthorhombic phase. The calculations also suggest the possible occurrence of a non-piezoelectric ferroelectric Hf0.5Zr0.5O2. Our experimental findings create an unprecedented potential for tuning the electromechanical functionality of ferroelectric HfO2-based devices.

2.
ACS Appl Electron Mater ; 5(3): 1478-1488, 2023 Mar 28.
Article in English | MEDLINE | ID: mdl-37012903

ABSTRACT

The wake-up behavior and ON/OFF current ratio of TiN-Al2O3-Hf0.5Zr0.5O2-W ferroelectric tunnel junction (FTJ) devices were investigated for different wake-up voltage waveforms. We studied triangular and square waves, as well as square pulse trains of equal or unequal voltage amplitudes for positive and negative polarities. We find that the wake-up behavior in these FTJ stacks is highly influenced by the field cycling waveform. A square waveform is observed to provide wake-up with the lowest number of cycles, concomitantly resulting in higher remnant polarization and a higher ON/OFF ratio in the devices, compared to a triangular waveform. We further show that wake-up is dependent on the number of cycles rather than the total time of the applied electric field during cycling. We also demonstrate that different voltage magnitudes are necessary for positive and negative polarities during field cycling for efficient wake-up. Utilizing an optimized waveform with unequal magnitudes for the two polarities during field cycling, we achieve a reduction in wake-up cycles and a large enhancement of the ON/OFF ratio from ∼5 to ∼35 in our ferroelectric tunnel junctions.

3.
Nanotechnology ; 34(24)2023 Mar 29.
Article in English | MEDLINE | ID: mdl-36806199

ABSTRACT

Conductive bridge random access memory devices such as Cu/SiO2/W are promising candidates for applications in neuromorphic computing due to their fast, low-voltage switching, multiple-conductance states, scalability, low off-current, and full compatibility with advanced Si CMOS technologies. The conductance states, which can be quantized, originate from the formation of a Cu filament in the SiO2electrolyte due to cation-migration-based electrochemical processes. A major challenge related to the filamentary nature is the strong variability of the voltage required to switch the device to its conducting state. Here, based on a statistical analysis of more than hundred fifty Cu/SiO2/W devices, we point to the key role of the activation energy distribution for copper ion diffusion in the amorphous SiO2. The cycle-to-cycle variability is modeled well when considering the theoretical energy landscape for Cu diffusion paths to grow the filament. Perspectives of this work point to developing strategies to narrow the distribution of activation energies in amorphous SiO2.

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