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Register a new userNanoscale reversal of stable room temperature ferroelectric polarization in organic croconic acid thin films
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It was discovered in 2010 that Croconic Acid, in its crystal form, has the highest polarization among organic ferroelectrics. In the context of eliminating toxic substances from electronic devices, Croconic Acid has a great potential as a sublimable lead-free ferroelectric. However, studies on ferroelectric properties of its thin films are only in their early stages and its capability to be incorporated in nanoscale devices is unknown. In this work, we demonstrate, upon ferroelectric switching at the nanoscale, stable and enduring room temperature polarization with no leakage current in Croconic Acid thin films. We thus show that it is a promising lead-free organic ferroelectric toward integration in nanoscale devices. The challenging switching current and polarization reversal characterization at the nanoscale was done using a unique combination of piezoresponse force microscopy, polarization switching current spectroscopy and the concurrent electromechanical strain response. Indeed, this combination can help to rationalize otherwise asymmetric polarization-voltage data and distorted hysteresis due to current jumps below the background noise, which are statistically washed away in macrojunctions but become prevalent at the nanoscale. These results are valid irrespective of the ferroelectrics nature, organic or inorganic. Beyond the potential of Croconic Acid as an ecological ferroelectric material in devices, our detection of a clear nanoscopic polarization switching current thus paves the way for a fundamental understanding and technological applications of the polarization reversal mechanism at the nanoscale.
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Ferroelectricity at room temperature has been demonstrated in nanometer-thin quasi 2D croconic acid thin films, by the polarization hysteresis loop measurements in macroscopic capacitor geometry, along with observation and manipulation of the nanoscale domain structure by piezoresponse force microscopy. The fabrication of continuous thin films of the hydrogen-bonded croconic acid was achieved by the suppression of the thermal decomposition using low evaporation temperatures in high vacuum, combined with growth conditions far from thermal equilibrium. For nominal coverages >=20 nm, quasi 2D and polycrystalline films, with an average grain size of 50-100 nm and 3.5 nm roughness, can be obtained. Spontaneous ferroelectric domain structures of the thin films have been observed and appear to correlate with the grain patterns. The application of this solvent-free growth protocol may be a key to the development of flexible organic ferroelectric thin films for electronic applications.
Magnetic skyrmions have attracted considerable interest, especially after their recent experimental demonstration at room temperature in multilayers. The robustness, nanoscale size and non-volatility of skyrmions have triggered a substantial amount of research on skyrmion-based low-power, ultra-dense nanocomputing and neuromorphic systems such as artificial synapses. Room-temperature operation is required to integrate skyrmionic synapses in practical future devices. Here, we numerically propose a nanoscale skyrmionic synapse composed of magnetic multilayers that enables room-temperature device operation tailored for optimal synaptic resolution. We demonstrate that when embedding such multilayer skyrmionic synapses in a simple spiking neural network (SNN) with unsupervised learning via the spike-timing-dependent plasticity rule, we can achieve only a 78% classification accuracy in the MNIST handwritten data set under realistic conditions. We propose that this performance can be significantly improved to about 98.61% by using a deep SNN with supervised learning. Our results illustrate that the proposed skyrmionic synapse can be a potential candidate for future energy-efficient neuromorphic edge computing.
The ferroelectric polarization switching in ferroelectric hafnium zirconium oxide (Hf0.5Zr0.5O2, HZO) in the HZO/Al2O3 ferroelectric/dielectric stack is investigated systematically by capacitance-voltage and polarization-voltage measurements. The thickness of dielectric layer is found to have a determinant impact on the ferroelectric polarization switching of ferroelectric HZO. A suppression of ferroelectricity is observed with thick dielectric layer. In the gate stacks with thin dielectric layers, a full polarization switching of the ferroelectric layer is found possible by the proposed leakage-current-assist mechanism through the ultrathin dielectric layer. Theoretical simulation results agree well with experimental data. This work clarifies some of the critical parts of the long-standing confusions and debating related to negative capacitance field-effect transistors (NC-FETs) concepts and experiments.
The discovery of stable room temperature ferroelectricity in Croconic Acid, an organic ferroelectric material, with polarization values on par with those found in inorganic ferroelectric materials and highest among organic ferroelectric materials, has opened up possibilities to realize myriads of nano-electronic and spintronic devices based on organic ferroelectrics. Such possibilities require an adequate understanding of the ferroelectric properties of Croconic Acid grown on surfaces that are commonly employed in device fabrication. While several macroscopic studies on relatively larger crystals of Croconic Acid have been performed, studies on thin films are only in their early stages. We have grown thin films of Croconic Acid on gold and cobalt surfaces, which are commonly used in spintronic devices as metallic electrodes, and studied the ferroelectric response of the films using ex-situ Piezoresponse Force Microscopy at room temperature. We show that the polarization reversal in Croconic Acid domains is sensitive to the substrate surface. Using the same experimental protocol, we observe the robust polarization reversal of a single, mostly in-plane electrical domain for a cobalt substrate, whereas polarization reversal is hardly observed for a gold substrate. We attribute this difference to the influence of substrates on the Croconic Acid molecular networks. Our study suggests that to realize devices one has to take care about the substrate on which Croconic Acid will be deposited. The fact that polarization switching is robust on cobalt surface can be used to fabricate multifunctional devices that utilize the cobalt-Croconic Acid interface.
The coherent manipulation of acoustic waves on the nanoscale usually requires multilayers with thicknesses and interface roughness defined down to the atomic monolayer. This results in expensive devices with predetermined functionality. Nanoscale mesoporous materials present high surface-to-volume ratio and tailorable mesopores, which allow the incorporation of chemical functionalization to nanoacoustics. However, the presence of pores with sizes comparable to the acoustic wavelength is intuitively perceived as a major roadblock in nanoacoustics. Here we present multilayered nanoacoustic resonators based on mesoporous SiO$_2$ thin-films showing acoustic resonances in the 5-100 GHz range. We characterize the acoustic response of the system using coherent phonon generation experiments. Despite resonance wavelengths comparable to the pore size, we observe for the first time unexpectedly well-defined acoustic resonances with Q-factors around 10. Our results open the path to a promising platform for nanoacoustic sensing and reconfigurable acoustic nanodevices based on soft, inexpensive fabrication methods.
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