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DOE OSTI2023

Boosting Piezoelectricity by 3D Printing PVDF‐MoS 2 Composite as a Conformal and High‐Sensitivity Piezoelectric Sensor

Abstract Additively manufactured flexible and high‐performance piezoelectric devices are highly desirable for sensing and energy harvesting of 3D conformal structures. Herein, the study reports a significantly enhanced piezoelectricity in polyvinylidene fluoride (PVDF) achieved through the in situ dipole alignment of PVDF within PVDF‐2D molybdenum disulfide (2D MoS 2 ) composite by 3D printing. The shear stress‐induced dipole poling of PVDF and 2D MoS 2 alignment are harnessed during 3D printing to boost piezoelectricity without requiring a post‐poling process. The results show a remarkable, more than the eight‐fold increment in the piezoelectric coefficient ( d 33 ) for 3D printed PVDF‐8wt.% MoS 2 composite over cast neat PVDF. The underlying mechanism of piezoelectric property enhancement is attributed to the increased volume fraction of β phase in PVDF, filler fraction, heterogeneous strain distribution around PVDF‐MoS 2 interfaces, and strain transfer to the nanofillers as confirmed by microstructural analysis and finite element simulation. These results provide a promising route to design and fabricate high‐performance 3D piezoelectric devices via 3D printing for next‐generation sensors and mechanical–electronic conformal devices.

2D MoS2↗

DOE OSTI2023

Piezoelectric Energy Harvesting Gyroscopes: Comparative Modeling and Effectiveness

Given its versatility in drawing power from many sources in the natural world, piezoelectric energy harvesting (PEH) has become increasingly popular. However, its energy harvesting capacities could be enhanced further. Here, a mathematical model that accurately simulates the dynamic behavior and energy harvested can facilitate further improvements in the performance of piezoelectric devices. One of the goals of this study is to create a dependable reduced-order model of a multi-purpose gyroscope. This model will make it possible to compute the harvested voltage and electrical power in a semi-analytical manner. The harvested voltage is often modeled as an average value across the whole electrode surface in piezoelectric devices. We propose a model which provides practical insights toward optimizing the performance of the system by considering a spatially varying electric field across the electrode surface length. Our framework allows investigation of the limits of applicability of the modeling assumptions across a range of load resistances. The differential quadrature method (DQM) provides the basis for the suggested numerical solution. The model is also employed to examine energy harvesting under various resistance loads. The newly developed spatially varying model is evaluated for open- and closed-circuit conditions and is proved to be accurate for various values of load resistance that have not previously been considered. The results show that using a spatially varying model is more versatile when modeling the performance of the piezoelectric multifunctional energy harvester. The performance may be accurately captured by the model for load resistances ranging between 103 Ω and 108 Ω. At optimum load resistance and near 65 KHz, the maximum power output predicted by the spatially varying (SV) model is 1.3 mV, 1.5 mV for the open-circuit (OC) model, and 2.1 mV for the closed circuit (CE) model. At a high-load resistance, the SV and OC models all predict the maximum power output to be 1.9 mV while the CE model predicted the maximum voltage to be 3 mV.

42 ENGINEERING↗

DOE OSTI2025

Ferroelectric materials toward next-generation electromechanical technologies

Ferroelectric materials have been widely used in various electromechanical devices, from ultrasonic transducers and actuators to mechanical energy harvesters. The key performance metrics of these devices, such as sensitivity, efficiency, and bandwidth of ultrasonic transducers, are largely determined by the piezoelectric properties. This Review highlights recent research progress in improving the piezoelectricity of ferroelectric materials and offers potential strategies for further enhancement to meet the ever-increasing demands for high-performance piezoelectric devices and systems. Here, it provides insights into the future development of ferroelectrics to address the increasing demands of emerging applications, including photoacoustic imaging and piezoelectric fans and motors in integrated circuit–enabled electronic devices. Additionally, it emphasizes the need to consider environmental impacts across the entire life cycle of ferroelectrics, from sourcing and manufacturing to usage and disposal.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Focusing transformers/filters in isotropic/anisotropic piezoelectrics

A focusing interdigital transducer (IDT) and corresponding single- and dual-port piezoelectric devices are disclosed. The focusing interdigital transducer, which generates Lamé acoustic waves, permits operation at significantly higher frequencies than those possible with traditional IDTs. The focusing IDT employs multiple arced fingers formed both above and below the piezoelectric layer to improve coupling efficiency by coupling through both the e31 and e33 piezoelectric coefficients to the piezoelectric layer. By optimizing both anchor design and location, acoustic wave losses are minimized, thereby improving the device's quality factor Q. Through proper bus design and selection of the number of IDT fingers, a device's impedance can be tuned for a given application. The focusing IDTs may be used in single-port filter devices and dual-port transformer devices. The single- and dual-port devices may operate at a single frequency, at two frequencies, or over a band of frequencies.

Siddiqui, Aleem↗

DOE OSTI2023

Large Enhancements in Optical and Piezoelectric Properties in Ferroelectric Zn 1- x Mg x O Thin Films through Engineering Electronic and Ionic Anharmonicities

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 –2 was reported in Zn 1-x Mg x O films. Here, ferroelectric Zn 1-x Mg x O 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.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Strain phase equilibria and phase‐field method of ferroelectric polydomain: A case study of monoclinic K x Na 1 − x NbO 3 thin films

Abstract Knowledge of the thermodynamic equilibria and domain structures of ferroelectrics is critical to establishing their structure–property relationships that underpin their applications from piezoelectric devices to nonlinear optics. Here, we establish the strain condition for strain phase separation and polydomain formation and analytically predict the corresponding domain volume fractions and wall orientations of, relatively low symmetry and theoretically more challenging, monoclinic ferroelectric thin films by integrating thermodynamics of ferroelectrics, strain phase equilibria theory, microelasticity, and phase‐field method. Using monoclinic K x Na 1 − x NbO 3 (0.5 < x < 1.0) thin films as a model system, we establish the polydomain strain–strain phase diagrams, from which we identify two types of monoclinic polydomain structures. The analytically predicted strain conditions of formation, domain volume fractions, and domain wall orientations for the two polydomain structures are consistent with phase‐field simulations and in good agreement with experimental results in the literature. The present study demonstrates a general, powerful analytical theoretical framework to predict the strain phase equilibria and domain wall orientations of polydomain structures applicable to both high‐ and low‐symmetry ferroelectrics and provide fundamental insights into the equilibrium domain structures of ferroelectric K x Na 1 − x NbO 3 thin films that are of technology relevance for lead‐free dielectric and piezoelectric applications.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Constructing Polymorphic Nanodomains in BaTiO 3 Films via Epitaxial Symmetry Engineering

Ferroelectric materials owning a polymorphic nanodomain structure usually exhibit colossal susceptibilities to external mechanical, electrical, and thermal stimuli, thus holding huge potential for relevant applications. Despite the success of traditional strategies by means of complex composition design, alternative simple methods such as strain engineering have been intensively sought to achieve a polymorphic nanodomain state in lead-free, simple-composition ferroelectric oxides in recent years. Here, a nanodomain configuration with morphed structural phases is realized in an epitaxial BaTiO3 film grown on a (111)-oriented SrTiO3 substrate. Using a combination of experimental and theoretical approaches, it is revealed that a threefold rotational symmetry element enforced by the epitaxial constraint along the [111] direction of BaTiO3 introduces considerable instability among intrinsic tetragonal, orthorhombic, and rhombohedral phases. Such phase degeneracy induces ultrafine ferroelectric nanodomains (1-10 nm) with low-angle domain walls, which exhibit significantly enhanced dielectric and piezoelectric responses compared to the (001)-oriented BaTiO3 film with uniaxial ferroelectricity. Therefore, the finding highlights the important role of epitaxial symmetry in domain engineering of oxide ferroelectrics and facilitates the development of dielectric capacitors and piezoelectric devices.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Anomalous elastic softening in ferroelectric hafnia under pressure

his study employs first-principles density-functional theory (DFT) calculations to explore the elastic and mechanical properties of ferroelectric hafnia (HfO 2 ) in its polar orthorhombic 𝑃⁢𝑐⁢𝑎⁢2 1 phase under varying hydrostatic pressure conditions up to 30 GPa. Utilizing a plane-wave basis set and Perdew-Burke-Ernzerhof generalized-gradient approximation for solids in our DFT calculations, we investigate both pure and yttrium-substituted HfO 2 . Our findings reveal an anomalous reduction in the 𝐶 33 component of the elastic tensor with increasing pressure, which becomes significant above 15 GPa and signals a potential pressure-driven structural phase transition at higher pressure. The analysis of atomic displacements under pressure sheds light on the unusual mechanical behavior and phase stability of this material. Additionally, we observe a transition from an indirect band gap to a direct band gap with increasing pressure, which could have significant implications for optical applications. Here, the effects of yttrium substitution on the mechanical and electronic properties are further examined, revealing that yttrium substitution softens the elastic response of this material and reduces the electronic band gap. These results enhance our understanding of elastic and mechanical responses of ferroelectric hafnia and its potential for applications in microelectronics, piezoelectric devices, and nonvolatile ferroelectric random-access memories. Further experimental validation is recommended to confirm our predictions and explore the practical implications of the observed phase transitions and electronic behavior of the ferroelectric hafnia under high-pressure conditions.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2021

Vibrational Energy Harvesting Using a Cantilever Model

Vibrational energy harvesting (VEH) is a method of capturing incidental mechanical vibrational energy and converting it to electrical energy. This is enabled by two technologies: Electromagnetic induction via a cantilever or piezoelectric devices. When designing a VEH system, a fast forward model is desired for response determination and optimal parameter estimation. An ordinary different equation (ODE) system model is developed for the cantilever system based upon the derivations of [1] and [2], and compared with a full electromechanical COMSOL model.

42 ENGINEERING↗

DOE OSTI2025

Observation of interface piezoelectricity in superconducting devices on silicon

The development of superconducting quantum processors relies on understanding and mitigating decoherence in superconducting qubits. Piezoelectric coupling contributes to decoherence by mediating energy exchange between microwave photons and acoustic phonons. Although bulk centrosymmetric materials like silicon and sapphire are non-piezoelectric and commonly used as qubit substrates, the lack of centrosymmetry at interfaces may induce piezoelectric losses. This effect was predicted decades ago but never experimentally observed in superconducting devices. Here, we report interface piezoelectricity at aluminum-silicon junctions and demonstrate it as a significant loss channel in superconducting devices. Using aluminum interdigital transducers on silicon, we observe piezoelectric transduction from room to millikelvin temperatures, with an effective electromechanical coupling factor K 2 ≈ (3 ± 0.4) × 10−5%, comparable to weakly piezoelectric substrates. Modeling shows this mechanism limits qubit quality factors to Q ~ 10 4 − 10 8 , depending on surface participation and mode matching. These findings reveal interface piezoelectricity as a major dissipation channel and highlight the need for heterostructure and phononic engineering in next-generation superconducting qubits.

Zhou, Haoxin [University of California, Berkeley, ↗

DOE OSTI2023

Piezoelectric deformable photonic devices

A CMOS-compatible actuator platform for implementing phase, amplitude, and frequency modulation in silicon nitride photonic integrated circuits via piezo-optomechanical coupling using tightly mechanically coupled aluminum nitride actuators is disclosed. The platform, which may be fabricated in a CMOS foundry, enables scalable active photonic integrated circuits for visible wavelengths, and the piezoelectric actuation functions without performance degradation down to cryogenic operating temperatures. A number of devices are possible, including ring modulator devices, phase shifter devices, Mach-Zehnder interferometer devices, directional coupler devices (including tunable directional coupler devices), and acousto-optic modulator and frequency shifter devices, each of which can employ the same AlN actuator platform. As all of these devices can be built on the same AlN actuator platform, numerous optical functions can be implemented on a single die.

Eichenfield, Matt↗

DOE OSTI2024

Integration of semiconductor membranes with piezoelectric substrates

Piezoelectrically actuated devices constructed from thin semiconductor membranes bonded directly to piezoelectric substrates are provided. Methods for fabricating these devices are also provided. The bonding of the semiconductor to the piezoelectric material does not require the use of any intermediate layers, such as bonding agents.

Lagally, Max G.↗

DOE OSTI2021

Hybrid printing of wearable piezoelectric sensors

Piezoelectricity provides an ideal electromechanical mechanism with emerging applications in wearable devices due to its simplicity and self-powered nature. However, the 3D printing of piezoelectric devices still faces many challenges, including material printability, high energy poling process, and low dimensional accuracy. This study demonstrates, for the first time, a tellurium nanowire-based piezoelectric device fabricated by a hybrid printing method integrating highly complementary aerosol jet printing and extrusion printing in a single printing platform. The aerosol-jet-printed tellurium nanowire demonstrates piezoelectric properties without the need for any poling processing due to the unique properties of the tellurium nanowires. The silver nanowire electrodes printed by aerosol jet printing demonstrate excellent conductivity and stretchability without the need for sintering. An extrusion method is employed to print the silicone films, which serve as the stretchable substrate and the electrical insulation layers between the printed tellurium and silver. The printed wearable piezoelectric devices were attached to a human wrist to detect different hand gestures and to a human neck to detect heartbeat without using an external power source. In conclusion, the fully printed, sintering-free and poling-free, and stretchable piezoelectric device opens enormous opportunities for facile integration with a broad range of printed electronics and wearable devices.

47 OTHER INSTRUMENTATION↗

DOE OSTI2024

Nuclear reactor radiation and temperature effects on piezoelectric surface acoustic wave devices

Surface acoustic wave (SAW) resonators were characterized in-situ in a nuclear reactor environment at high temperature. Devices based on lithium niobate (LiNbO 3 ), aluminum nitride (sc-AlN), and thin-film aluminum nitride on sapphire substrate (AlN/sapphire) were tested up to 400 °C temperature and 1.9 × 10 12 n/cm 2 s neutron flux. Shifts in device resonant frequency were detected in response to temperature and neutron flux. Devices undergo a frequency change when exposed to neutron flux. At 300 °C, AlN/sapphire produced the strongest neutron flux response about 1.02 ppm at 1.27 × 10 12 n/cm 2 s neutron flux (5.7 × 10 4 rad-Si/hr neutron dose rate), compared to 0.30 ppm for LiNbO 3 and 0.17 ppm for sc-AlN. While the transient kinetics in response to step change in neutron flux support the defect-accumulation mechanism, the concurrent measurement of device temperature using resistive temperature sensor suggests additional heating caused by absorption of gamma rays can also play a role. These results make SAW devices attractive candidates for sensor applications in extreme environments.

Aluminum nitride↗

DOE OSTI2023

Systems and methods for piezoelectric, electronic, and photonic devices with dual inversion layers

An apparatus comprising a substrate, one or more nanowire pillars, each having a base portion and a tip portion, a first electrode connected to the tip portions of the one or more nanowire pillars, an internal hollow cavity positioned between the substrate and the first electrode, such that at least a portion of each of the one or more nanowire pillars extend through the internal hollow cavity, and a second electrode proximate the first side of the substrate. High-performance broadband photodetectors and other optoelectronics for converting light to electricity with enhanced absorption and carrier collection.

30 DIRECT ENERGY CONVERSION↗

DOE OSTI2019

Mechanical Purcell filters for microwave quantum machines

In circuit quantum electrodynamics, measuring the state of a superconducting qubit introduces a loss channel, which can enhance spontaneous emission through the Purcell effect, thus decreasing the qubit lifetime. This decay can be mitigated by performing the measurement through a Purcell filter, which strongly suppresses signal propagation at the qubit transition frequency. If the filter is also well-matched at the readout cavity frequency, it will protect the qubit from decoherence channels without sacrificing measurement bandwidth. In this work, we propose and analyze design for a mechanical Purcell filter, which we also fabricate and characterize at room temperature. The filter is composed of an array of nanomechanical resonators in thin-film lithium niobate, connected in a ladder topology, with series and parallel resonances arranged to produce a bandpass response. Their modest footprint, steep band edges, and lack of cross talk make these filters an appealing alternative to analogous electromagnetic versions currently used in microwave quantum machines.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2023

Non-reciprocal acoustoelectric microwave amplifiers with net gain and low noise in continuous operation

Abstract Piezoelectric acoustic devices that are integrated with semiconductors can leverage the acoustoelectric effect, allowing functionalities such as gain and isolation to be achieved in the acoustic domain. This could lead to performance improvements and miniaturization of radio-frequency electronic systems. However, acoustoelectric amplifiers that offer a large acoustic gain with low power consumption and noise figure at microwave frequencies in continuous operation have not yet been developed. Here we report non-reciprocal acoustoelectric amplifiers that are based on a three-layer heterostructure consisting of an indium gallium arsenide (In 0.53 Ga 0.47 As) semiconducting film, a lithium niobate (LiNbO 3 ) piezoelectric film, and a silicon substrate. The heterostructure can continuously generate 28.0 dB of acoustic gain (4.0 dB net radio-frequency gain) for 1 GHz phonons with an acoustic noise figure of 2.8 dB, while dissipating 40.5 mW of d.c. power. We also create a device with an acoustic gain of 37.0 dB (11.3 dB net gain) at 1 GHz with 19.6 mW of d.c. power dissipation and a non-reciprocal transmission of over 55 dB.

42 ENGINEERING↗

DOE OSTI2026

Modulating surface acoustic wave generation through superconductivity

Surface acoustic waves (SAWs), with their five orders-of-magnitude slower propagation velocity, allow for considerably shorter wavelengths at the same frequency compared to electromagnetic waves. The short wavelengths allow for device miniaturization and on-chip integration. The generic design of these devices involves piezoelectric substrates with comb-like arrays of Al or Au electrodes known as interdigitated transducers (IDTs) deposited on the surface. However, Al and Au both have shortcomings at the cryogenic temperatures required for quantum applications, namely, the formation of two-level systems and the lack of superconductivity perpetuating Ohmic losses, respectively. In this work, SAWs are generated in the high-MHz to low-GHz range using niobium nitride (NbN) interdigitated transducers and Bragg reflectors. We demonstrate the fabrication of acoustic devices through photolithography and reactive ion etching. The sharp transition between superconducting and normal states and the corresponding change in SAW transmission allows for fine control of the “on” (superconducting) and “off” (normal) states of NbN, with a ΔT = 1 K separating the transmission minimum and maximum. We demonstrate a 16× difference in transmission between the “on” and “off” states of the device. The SAW transmission behavior mirrors the change in resistance of NbN at its T c . These findings open up new possibilities for the integration of NbN SAW resonators into existing quantum architectures based on NbN and a method for adjusting transmission properties independent of applied voltage.

36 MATERIALS SCIENCE↗