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Register a new userRoom Temperature Ferroelectricity in Continuous Croconic Acid Thin Films
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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.
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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.
We investigated the ferroelectric properties of strontium titanate (STO) thin films deposited on SrTiO3 (001) substrate with SrRuO3 electrodes. The STO layer was grown coherently on the SrTiO3 substrate without in-plane lattice relaxation, but its out-of-plane lattice constant increased with a decrease in the oxygen pressure during deposition. Using piezoresponse force microscopy and P-V measurements, we showed that our tetragonal STO films possess room-temperature ferroelectricity. We discuss the possible origins of the observed ferroelectricity.
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.
We have studied ferroelectricity and photovoltaic effects in atomic layer deposited (ALD) 40-nm thick SnTiO$_{x}$ films deposited directly onto p-type (001)Si substrate. These films showed well-saturated, square and repeatable hysteresis loops with remnant polarization of 1.5 $mu$C/cm$^{2}$ at room temperature, as detected by out-of-plane polarization versus electric field (P-E) and field cycling measurements. A photo-induced enhancement in ferroelectricity was also observed as the spontaneous polarization increased under white-light illumination. The ferroelectricity exhibits relaxor characteristics with dielectric peak shifting from ca. T = 600 K at f = 1 MHz to ca. 500 K at 100 Hz. Moreover, our films showed ferroelectric photovoltaic behavior under the illumination of a wide spectrum of light, from visible to ultraviolet regions. A combination of experiment and theoretical calculation provided optical band gap of SnTiO$_{x}$ films which lies in the visible range of white light spectra. Our study leads a way to develop green ferroelectric SnTiO$_{x}$ thin films, which are compatible to semiconducting processes, and can be used for various ferroelectric and dielectric applications.
Layered iridates have been the subject of intense scrutiny on account of their unusually strong spin-orbit coupling, which opens up a narrow gap in a material that would otherwise be a metal. This insulating state is very sensitive to external perturbations. Here, we show that vertical compression at the nanoscale, delivered using the tip of a standard scanning probe microscope, is capable of inducing a five orders of magnitude change in the room temperature resistivity of Sr2IrO4. The extreme sensitivity of the electronic structure to anisotropic deformations opens up a new angle of interest on this material, and the giant and fully reversible perpendicular piezoresistance makes iridates a promising material for room temperature piezotronic devices.
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