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Sc-doped aluminum nitride is emerging as a new piezoelectric material which can substitute undoped aluminum nitride (AlN) in radio-frequency MEMS applications, thanks to its demonstrated enhancement of the piezoelectric coefficients. Furthermore, the recent demonstration of the ferroelectric-switching capability of the material gives AlScN the possibility to integrate memory functionalities in RF components. However, its high-coercive field and high-leakage currents are limiting its applicability. Residual stress, growth on different substrates, and testing-temperature have already been demonstrated as possible knobs to flatten the energy barrier needed for switching, but no investigation has been reported yet on the whole impact on the dielectric and ferroelectric dynamic behavior of a single process parameter. In this context, we analyze the complete spectrum of variations induced by the applied substrate-RF, from deposition characteristics to dielectric and ferroelectric properties, proving its effect on all of the material attributes. In particular, we demonstrate the possibility of engineering the AlScN lattice cell to properly modify leakage, breakdown, and coercive fields, as well as polarization charge, without altering the crystallinity level, making substrate-RF an effective and efficient fabrication knob to ease the limitations the material is facing.more » « less
Uniformly acceptor doped Pb(Zr 0.48 Ti 0.52 )O 3 (PZT) films with 2 mol. % Mg or Fe prepared by chemical solution deposition exhibited decreased dielectric constants and remanent polarizations relative to undoped PZT. For highly accelerated lifetime testing (HALT) at 200 °C and an electric field of 300 kV/cm in the field up direction, the HALT lifetimes (t 50 ) for undoped, Mg-doped, and Fe-doped PZT films were shortened from 2.81 ± 0.1 to 0.21 ± 0.1 and 0.54 ± 0.04 h, respectively. Through thermally stimulated depolarization current measurement, significant [Formula: see text] electromigration was found in homogeneously Mg-doped PZT thin films, a major factor in their short HALT lifetime. Because the concentration of oxygen vacancies increases with uniform acceptor doping, the lifetime decreases. In contrast, when a thin layer of Mg-doped or Fe-doped PZT was deposited on undoped PZT or Nb-doped PZT (PNZT), the HALT lifetimes were longer than those of pure PZT or PNZT films. This confirms prior work on PNZT films with a Mn-doped top layer, demonstrating that the HALT lifetime increases for composite films when a layer with multivalent acceptors is present near the negative electrode during HALT. In that case, the compensating electrons are trapped, presumably on the multivalent acceptors, thus increasing the lifetime.more » « less
Periodically poled second-order nonlinear materials with submicrometer periods are important for the development of quasi-phase matched backward-wave nonlinear optical processes. Interactions involving counter-propagating waves exhibit many unique properties and enable devices such as backward second harmonic generators, mirrorless optical parametric oscillators, and narrow-band quantum entangled photon sources. Fabrication of dense ferroelectric domain gratings in lithium niobate remains challenging, however, due to lateral domain spreading and merging. Here, we report submicrometer periodic poling of ion-sliced x-cut magnesium oxide doped lithium niobate thin films. Electric-field poling is performed using multiple bipolar preconditioning pulses that improve the poling yield and domain uniformity. The internal field is found to decrease with each preconditioning poling cycle. The poled domains are characterized by piezoresponse force microscopy. A fundamental period of 747 nm is achieved.
Harnessing the exotic properties of molecular level nanostructures to produce novel sensors, metamaterials, and futuristic computer devices can be technologically transformative. In addition, connecting the molecular nanostructures to ferromagnetic electrodes bring the unprecedented opportunity of making spin property based molecular devices. We have demonstrated that magnetic tunnel junction based molecular spintronics device (MTJMSD) approach to address numerous technological hurdles that have been inhibiting this field for decades (P. Tyagi, J. Mater. Chem., Vol. 21, 4733). MTJMSD approach is based on producing a capacitor like a testbed where two metal electrodes are separated by an ultrathin insulator and subsequently bridging the molecule nanostructure across the insulator to transform a capacitor into a molecular device. Our prior work showed that MTJMSDs produced extremely intriguing phenomenon such as room temperature current suppression by six orders, spin photovoltaic effect, and evolution of new forms of magnetic metamaterials arising due to the interaction of the magnetic a molecule with two ferromagnetic thin films. However, making robust and reproducible electrical connections with exotic molecules with ferromagnetic electrodes is full of challenges and requires attention to MTJMSD structural stability. This paper focuses on MTJMSD stability by describing the overall fabrication protocol and the associated potential threat to reliability. MTJMSD is based on microfabrication methods such as (a) photolithography for patterning the ferromagnetic electrodes, (b) sputtering of metallic thin films and insulator, and (c) at the end electrochemical process for bridging the molecules between two ferromagnetic films separated by ∼ 2nm insulating gap. For the successful MTJMSD fabrication, the selection of ferromagnetic metal electrodes and thickness was found to be a deterministic factor in designing the photolithography, thin film deposition strategy, and molecular bridging process. We mainly used isotropic NiFe soft magnetic material and anisotropic Cobalt (Co) with significant magnetic hardness. We found Co was susceptible to chemical etching when directly exposed to photoresist developer and aged molecular solution. However, NiFe was very stable against the chemicals we used in the MTJMSD fabrication. As compared to NiFe, the Co films with > 10nm thickness were susceptible to mechanical stress-induced nanoscale deformities. However, cobalt was essential to produce (a) low leakage current before transforming the capacitor from the magnetic tunnel junction into molecular devices and (b) tailoring the magnetic properties of the ferromagnetic electrodes. This paper describes our overall MTJMSD fabrication scheme and process optimization to overcome various challenges to produce stable and reliable MTJMSDs. We also discuss the role of mechanical stresses arising during the sputtering of the ultrathin insulator and how to overcome that challenge by optimizing the insulator growth process. This paper will benefit researchers striving to make nanoscale spintronics devices for solving grand challenges in developing advanced sensors, magnetic metamaterials, and computer devices.
Ferroelectric films suffer from both aging and degradation under high ac‐field drive conditions due to loss of polarization with time. In this study, the roles of defect chemistry and internal electric fields on the long‐term stability of the properties of piezoelectric films were explored. For this purpose, lead zirconate titanate (PZT) films with a Zr/Ti ratio of 52/48 doped with Mn‐ (PMZT) or Nb‐ (PNZT) were deposited on Pt coated Si substrates by the sol‐gel method. It was demonstrated that the magnitude of the internal field is much higher in PMZT films compared to PNZT films after poling in the temperature range of 25‐200°C under an electric field of −240 kV/cm. The development of the internal field is thermally activated, with activation energies from 0.5 ± 0.06 to 0.8 ± 0.1 eV in Mn doped films and from 0.8 ± 0.1 to 1.2 ± 0.2 eV in Nb doped films. The different activation energies for imprint suggests that the physical mechanism underlying the evolution of the internal field in PMZT and PNZT films differs; the enhanced internal field upon poling is attributed to (a) alignment of oxygen vacancy—acceptor ion defect dipoles (
, ) in PMZT films, and (b) thermionic injection of electron charges and charge trapping in PNZT films. In either case, the internal field reduces back switching, enhances the remanent piezoelectric properties, and dramatically improves the aging behavior. PMZT films exhibited the greatest enhancement, with reduced high temperature (180°C) aging rates of 2%‐3%/decade due to improved stability of the poled state. In contrast, PNZT films showed significantly larger high temperature aging rates (15.5%/decade) in the piezoelectric coefficient, demonstrating that the fully poled state was not retained with time.