An official website of the United States government
Abstract Achieving substantial electrostrain alongside a large effective piezoelectric strain coefficient (d33*) in piezoelectric materials remains a formidable challenge for advanced actuator applications. Here, a straightforward approach to enhance these properties by strategically designing the domain structure and controlling the domain switching through the introduction of arrays of ordered {100}<100> dislocations is proposed. This dislocation engineering yields an intrinsic lock‐in steady–state electrostrain of 0.69% at a low field of 10 kV cm−1without external stress and an output strain energy density of 5.24 J cm−3in single‐crystal BaTiO3, outperforming the benchmark piezoceramics and relaxor ferroelectric single‐crystals. Additionally, applying a compression stress of 6 MPa fully unlocks electrostrains exceeding 1%, yielding a remarkabled33* value over 10 000 pm V−1and achieving a record‐high strain energy density of 11.67 J cm−3. Optical and transmission electron microscopy, paired with laboratory and synchrotron X‐ray diffraction, is employed to rationalize the observed electrostrain. Phase‐field simulations further elucidate the impact of charged dislocations on domain nucleation and domain switching. These findings present an effective and sustainable strategy for developing high‐performance, lead‐free piezoelectric materials without the need for additional chemical elements, offering immense potential for actuator technologies.
more »
« less
High Velocity, Low‐Voltage Collective In‐Plane Switching in (100) BaTiO 3 Thin Films
Abstract Ferroelectrics are being increasingly called upon for electronic devices in extreme environments. Device performance and energy efficiency is highly correlated to clock frequency, operational voltage, and resistive loss. To increase performance it is common to engineer ferroelectric domain structure with highly‐correlated electrical and elastic coupling that elicit fast and efficient collective switching. Designing domain structures with advantageous properties is difficult because the mechanisms involved in collective switching are poorly understood and difficult to investigate. Collective switching is a hierarchical process where the nano‐ and mesoscale responses control the macroscopic properties. Using chemical solution synthesis, epitaxially nearly‐relaxed (100) BaTiO3films are synthesized. Thermal strain induces a strongly‐correlated domain structure with alternating domains of polarization along the [010] and [001] in‐plane axes and 90° domain walls along the [011] or [01] directions. Simultaneous capacitance–voltage measurements and band‐excitation piezoresponse force microscopy revealed strong collective switching behavior. Using a deep convolutional autoencoder, hierarchical switching is automatically tracked and the switching pathway is identified. The collective switching velocities are calculated to be ≈500 cm s−1at 5 V (7 kV cm−1), orders‐of‐magnitude faster than expected. These combinations of properties are promising for high‐speed tunable dielectrics and low‐voltage ferroelectric memories and logic.
more »
« less
- Award ID(s):
- 1839234
- PAR ID:
- 10376415
- Publisher / Repository:
- Wiley Blackwell (John Wiley & Sons)
- Date Published:
- Journal Name:
- Advanced Science
- Volume:
- 9
- Issue:
- 29
- ISSN:
- 2198-3844
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
-
-
Abstract Multifunctionality as a paradigm requires materials exhibiting multiple superior properties. Integrating second‐order optical nonlinearity and large bandgap with piezoelectricity can, for example, enable broadband, strain‐tunable photonics. Though very different phenomena at distinct frequencies, both second‐order optical nonlinearity and piezoelectricity are third‐rank polar tensors present only in acentric crystal structures. However, simultaneously enhancing both phenomena is highly challenging since it involves competing effects with tradeoffs. Recently, a large switchable ferroelectric polarization of ≈80 μC cm−2was reported in Zn1‐xMgxO films. Here, ferroelectric Zn1‐xMgxO is demonstrated to be a platform that hosts simultaneously a 30% increase in the electronic bandgap, a 50% enhancement in the second harmonic generation (SHG) coefficients, and a near 200% improvement in the piezoelectric coefficients over pure ZnO. These enhancements are shown to be due to a 400% increase in the electronic anharmonicity and a ≈200% decrease in the ionic anharmonicity with Mg substitution. Precisely controllable periodic ferroelectric domain gratings are demonstrated down to 800 nm domain width, enabling ultraviolet quasi‐phase‐matched optical harmonic generation as well as domain‐engineered piezoelectric devices.more » « less
-
Abstract The hafnate perovskites PbHfO3(antiferroelectric) and SrHfO3(“potential” ferroelectric) are studied as epitaxial thin films on SrTiO3(001) substrates with the added opportunity of observing a morphotropic phase boundary (MPB) in the Pb1−xSrxHfO3system. The resulting (240)‐oriented PbHfO3(Pba2) films exhibited antiferroelectric switching with a saturation polarization ≈53 µC cm−2at 1.6 MV cm−1, weak‐field dielectric constant ≈186 at 298 K, and an antiferroelectric‐to‐paraelectric phase transition at ≈518 K. (002)‐oriented SrHfO3films exhibited neither ferroelectric behavior nor evidence of a polarP4mmphase . Instead, the SrHfO3films exhibited a weak‐field dielectric constant ≈25 at 298 K and no signs of a structural transition to a polar phase as a function of temperature (77–623 K) and electric field (–3 to 3 MV cm−1). While the lack of ferroelectric order in SrHfO3removes the potential for MPB, structural and property evolution of the Pb1−xSrxHfO3(0 ≤x < 1) system is explored. Strontium alloying increased the electric‐breakdown strength (EB) and decreased hysteresis loss, thus enhancing the capacitive energy storage density (Ur) and efficiency (η). The composition, Pb0.5Sr0.5HfO3produced the best combination ofEB = 5.12 ± 0.5 MV cm−1,Ur = 77 ± 5 J cm−3, and η = 97 ± 2%, well out‐performing PbHfO3and other antiferroelectric oxides.more » « less
-
Neutrons generated through charge-exchange9Be (p; ni)9Be reactions, with energies ranging from 0–33 MeV and an average energy of ∼9.8 MeV were used to irradiate conventional Schottky Ga2O3rectifiers and NiO/Ga2O3p-n heterojunction rectifiers to fluences of 1.1–2.2 × 1014cm−2. The breakdown voltage was improved after irradiation for the Schottky rectifiers but was highly degraded for their NiO/Ga2O3counterparts. This may be a result of extended defect zones within the NiO. After irradiation, the switching characteristics were degraded and irradiated samples of both types could not survive switching above 0.7 A or 400 V, whereas reference samples were robust to 1 A and 1 kV. The carrier removal rate in both types of devices was ∼45 cm−1. The forward currents and on-state resistances were only slightly degraded by neutron irradiation.more » « less
-
Abstract Strain engineering in perovskite oxides provides for dramatic control over material structure, phase, and properties, but is restricted by the discrete strain states produced by available high‐quality substrates. Here, using the ferroelectric BaTiO3, production of precisely strain‐engineered, substrate‐released nanoscale membranes is demonstrated via an epitaxial lift‐off process that allows the high crystalline quality of films grown on substrates to be replicated. In turn, fine structural tuning is achieved using interlayer stress in symmetric trilayer oxide‐metal/ferroelectric/oxide‐metal structures fabricated from the released membranes. In devices integrated on silicon, the interlayer stress provides deterministic control of ordering temperature (from 75 to 425 °C) and releasing the substrate clamping is shown to dramatically impact ferroelectric switching and domain dynamics (including reducing coercive fields to <10 kV cm−1and improving switching times to <5 ns for a 20 µm diameter capacitor in a 100‐nm‐thick film). In devices integrated on flexible polymers, enhanced room‐temperature dielectric permittivity with large mechanical tunability (a 90% change upon ±0.1% strain application) is demonstrated. This approach paves the way toward the fabrication of ultrafast CMOS‐compatible ferroelectric memories and ultrasensitive flexible nanosensor devices, and it may also be leveraged for the stabilization of novel phases and functionalities not achievable via direct epitaxial growth.more » « less
