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result(s) for
"Yuan, Hua"
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Ultrahigh–energy density lead-free dielectric films via polymorphic nanodomain design
Dielectric capacitors with ultrahigh power densities are fundamental energy storage components in electrical and electronic systems. However, a long-standing challenge is improving their energy densities. We report dielectrics with ultrahigh energy densities designed with polymorphic nanodomains. Guided by phase-field simulations, we conceived and synthesized lead-free BiFeO₃-BaTiO₃-SrTiO₃ solid-solution films to realize the coexistence of rhombohedral and tetragonal nanodomains embedded in a cubic matrix. We obtained minimized hysteresis while maintaining high polarization and achieved a high energy density of 112 joules per cubic centimeter with a high energy efficiency of ~80%. This approach should be generalizable for designing high-performance dielectrics and other functional materials that benefit from nanoscale domain structure manipulation.
Journal Article
Giant energy density and high efficiency achieved in bismuth ferrite-based film capacitors via domain engineering
Developing high-performance film dielectrics for capacitive energy storage has been a great challenge for modern electrical devices. Despite good results obtained in lead titanate-based dielectrics, lead-free alternatives are strongly desirable due to environmental concerns. Here we demonstrate that giant energy densities of ~70 J cm
−3
, together with high efficiency as well as excellent cycling and thermal stability, can be achieved in lead-free bismuth ferrite-strontium titanate solid-solution films through domain engineering. It is revealed that the incorporation of strontium titanate transforms the ferroelectric micro-domains of bismuth ferrite into highly-dynamic polar nano-regions, resulting in a ferroelectric to relaxor-ferroelectric transition with concurrently improved energy density and efficiency. Additionally, the introduction of strontium titanate greatly improves the electrical insulation and breakdown strength of the films by suppressing the formation of oxygen vacancies. This work opens up a feasible and propagable route, i.e., domain engineering, to systematically develop new lead-free dielectrics for energy storage.
Dielectrics with high capacitive energy storage density are essential for modern electrical devices and pulsed power systems. Here, the authors realised superior energy storage performance in lead-free bismuth ferrite-based relaxor ferroelectric films through domain engineering.
Journal Article
Phase-field modeling and machine learning of electric-thermal-mechanical breakdown of polymer-based dielectrics
Understanding the breakdown mechanisms of polymer-based dielectrics is critical to achieving high-density energy storage. Here a comprehensive phase-field model is developed to investigate the electric, thermal, and mechanical effects in the breakdown process of polymer-based dielectrics. High-throughput simulations are performed for the P(VDF-HFP)-based nanocomposites filled with nanoparticles of different properties. Machine learning is conducted on the database from the high-throughput simulations to produce an analytical expression for the breakdown strength, which is verified by targeted experimental measurements and can be used to semiquantitatively predict the breakdown strength of the P(VDF-HFP)-based nanocomposites. The present work provides fundamental insights to the breakdown mechanisms of polymer nanocomposite dielectrics and establishes a powerful theoretical framework of materials design for optimizing their breakdown strength and thus maximizing their energy storage by screening suitable nanofillers. It can potentially be extended to optimize the performances of other types of materials such as thermoelectrics and solid electrolytes.
Polymer dielectrics are promising for high-density energy storage but dielectric breakdown is poorly understood. Here, a phase-field model is developed to investigate electric, thermal, and mechanical effects in the breakdown process for a range of polymer dielectrics, and analytical expression for breakdown strength is provided by machine learning.
Journal Article
Complex electronic structure and compositing effect in high performance thermoelectric BiCuSeO
BiCuSeO oxyselenides are promising thermoelectric materials, yet further thermoelectric figure of merit ZT improvement is largely limited by the inferior electrical transport properties. The established literature on these materials shows only one power factor maximum upon carrier concentration optimization, which is typical for most thermoelectric semiconductors. Surprisingly, we found three power factor maxima when doping Bi with Pb. Based on our first-principles calculations, numerical modeling, and experimental investigation, we attribute the three maxima to the Fermi energy optimization, band convergence, and compositing effect due to in situ formed PbSe precipitates. Consequently, three ZT peaks of 0.9, 1.1, and 1.3 at 873 K are achieved for 4, 10, and 14 at.% Pb-doped samples, respectively, revealing the significance of complex electronic structure and multiple roles of Pb in BiCuSeO. The results establish an accurate band structure characterization for BiCuSeO and identify the role of band convergence and nanoprecipitation as the driving mechanism for high ZT.
Though BiCuSeO is a promising thermoelectric material, further study of its electronic structure-property relationship and compositing effect is required to optimize the performance. Here, the authors observe three power factor maxima in BiCuSeO with the increasing Pb-doping content.
Journal Article
Controllable photomechanical bending of metal-organic rotaxane crystals facilitated by regioselective confined-space photodimerization
Molecular machines based on mechanically-interlocked molecules (MIMs) such as (pseudo) rotaxanes or catenates are known for their molecular-level dynamics, but promoting macro-mechanical response of these molecular machines or related materials is still challenging. Herein, by employing macrocyclic cucurbit[8]uril (CB[8])-based pseudorotaxane with a pair of styrene-derived photoactive guest molecules as linking structs of uranyl node, we describe a metal-organic rotaxane compound, U-CB[8]-MPyVB, that is capable of delivering controllable macroscopic mechanical responses. Under light irradiation, the ladder-shape structural unit of metal-organic rotaxane chain in U-CB[8]-MPyVB undergoes a regioselective solid-state [2 + 2] photodimerization, and facilitates a photo-triggered single-crystal-to-single-crystal (SCSC) transformation, which even induces macroscopic photomechanical bending of individual rod-like bulk crystals. The fabrication of rotaxane-based crystalline materials with both photoresponsive microscopic and macroscopic dynamic behaviors in solid state can be promising photoactuator devices, and will have implications in emerging fields such as optomechanical microdevices and smart microrobotics.
The preparation of materials that display macro-mechanical responses to external stimuli is challenging. Here, the authors synthesize metal-organic rotaxane frameworks that contain photoactive axles as linkers; light irradiation triggers photodimerization of the ligands, which leads to macroscopic photomechanical bending of individual bulk crystals.
Journal Article
Compositing effects for high thermoelectric performance of Cu2Se-based materials
Thermoelectric materials can realize direct conversion between heat and electricity, showing excellent potential for waste heat recovery. Cu
2
Se is a typical superionic conductor thermoelectric material having extraordinary
ZT
values, but its superionic feature causes poor service stability and low mobility. Here, we reported a fast preparation method of self-propagating high-temperature synthesis to realize in situ compositing of BiCuSeO and Cu
2
Se to optimize the service stability. Additionally, using the interface design by introducing graphene in these composites, the carrier mobility could be obviously enhanced, and the strong phonon scatterings could lead to lower lattice thermal conductivity. Ultimately, the Cu
2
Se-BiCuSeO-graphene composites presented excellent thermoelectric properties with a
ZT
max
value of ~2.82 at 1000 K and a
ZT
ave
value of ~1.73 from 473 K to 1000 K. This work provides a facile and effective strategy to largely improve the performance of Cu
2
Se-based thermoelectric materials, which could be further adopted in other thermoelectric systems.
Here, the authors devise a synthesis strategy to optimize the stability and thermoelectric performance of Cu
2
Se-based materials. They obtain a maximum
ZT
value of ~2.82 at 1000 K on Cu
2
Se-BiCuSeO-graphene composites.
Journal Article
High-performance Raman quantum memory with optimal control in room temperature atoms
Quantum memories are essential for quantum information processing. Techniques have been developed for quantum memory based on atomic ensembles. The atomic memories through optical resonance usually suffer from the narrow-band limitation. The far off-resonant Raman process is a promising candidate for atomic memories due to broad bandwidths and high speeds. However, to date, the low memory efficiency remains an unsolved bottleneck. Here, we demonstrate a high-performance atomic Raman memory in
87
Rb vapour with the development of an optimal control technique. A memory efficiency of above 82.0% for 6 ns~20 ns optical pulses is achieved. In particular, an unconditional fidelity of up to 98.0%, significantly exceeding the no-cloning limit, is obtained with the tomography reconstruction for a single-photon level coherent input. Our work marks an important advance of atomic memory towards practical applications in quantum information processing.
Storage and retrieval of memory is important for applications in quantum information processing. Here the authors demonstrate an efficient quantum Raman memory protocol by preparing hot rubidium atoms in specific states using control pulse scheme.
Journal Article