Enhanced Absolute Recovered Energy under Low Electric Field in All-Inorganic 0-3 Nanocomposition Thick Films.

Inorganic thick-film dielectric capacitors with ultrahigh absolute recovered energy at low electric fields are extremely desired for their wide application in pulsed power systems. However, a long-standing technological bottleneck exists between high absolute energy and large recovered energy density. A new strategy is offered to fabricate selected all-inorganic 0-3 composite thick films up to 10 µm by a modified sol-slurry method. Here, the ceramic powder is dispersed into the sol-gel matrix to form a uniform suspension, assisted by powder, therefore, the 2 µm-thickness after single layer spin coating. To enhance the energy-storage performances, the composites process is thoroughly optimized by ultrafine powder (<50 nm) technique based on a low-cost coprecipitation method instead of the solid-state and sol-gel methods. 0D coprecipitation powder has a similar dielectric constant to the corresponding 3D films, thus uneven electrical field distributions is overcome. Moreover, the increase of interfacial polarization is realized due to the larger specific surface area. A maximum recoverable energy density of 14.62 J cm-3 is obtained in coprecipitation thick films ≈2.2 times that of the solid-state powder and ≈1.3 times for sol-gel powder. This study provides a new paradigm for further guiding the design of composite materials.

Photomodulated cryogenic temperature sensing through a photochromic reaction in Na0.5Bi2.5Ta2O9: Er/Yb multicolour upconversion.

Optical temperature sensing of the non-thermally coupled energy levels (N-TCLs) based on fluorescence intensity ratio (FIR) technologies has excellent temperature sensitivity and signal recognition properties. In this study, a novel strategy is established to enhance the low-temperature sensing properties by controlling photochromic reaction process in Na0.5Bi2.5Ta2O9: Er/Yb samples. The maximum relative sensitivity reaches up to 5.99% K-1 at cryogenic temperature of 153 K. After irradiation with commercial laser of 405 nm for 30 s, the relative sensitivity is increased to 6.81% K-1. The improvement is verified to originate from the coupling of optical thermometric and photochromic behaviour at the elevated temperatures. The strategy may open up a new avenue to improve the thermometric sensitivity in photo-stimuli response photochromic materials.

Enhanced Energy-Storage Performances in Sodium Bismuth Titanate-Based Relaxation Ferroelectric Ceramics with Optimized Polarization by Tuning Sintering Temperature.

Energy-storage capacitors based on relaxation ferroelectric ceramics have attracted a lot of interest in pulse power devices. How to improve the energy density by designing the structure of ceramics through simple approaches is still a challenge. Herein, enhanced energy-storage performances are achieved in relaxation ferroelectric 0.9 (0.94Na0.5Bi0.5TiO3-0.06BaTiO3)-0.1NaNbO3 (NBT-BT-NN) ceramics by tuning sintering temperature. The original observation based on Kelvin probe force microscopy (KPFM) presented that the sintering temperature has a key effect on the electrical homogeneousness of the ceramics. It is found that a high electrical homogeneousness can induce quick and active domain switching due to the weakening of the constraint from built-in fields, resulting in a big polarization difference. This work provides a feasible strategy to design high-performance energy-storage ceramic capacitors.

Large Room-Temperature Electrocaloric Response Realized in Potassium-Sodium Niobate by a Relaxor Enhancement Effect and Multilayer Ceramic Construct.

The development of high-performance electrocaloric (EC) materials is crucial for solid-state refrigeration applied in micro-electromechanical systems. Herein, a large room-temperature EC response is realized in (1 - x)(K0.49Na0.49Li0.02)(Nb0.8Ta0.2)O3-xCaZrO3 (KNLNT-xCZ) benefiting from a relaxor enhancement effect and multilayer ceramic construct. The relaxor enhancement effect is because the long-range order is broken by adding CaZrO3, which is in favor of enhancing the temperature change (ΔT) and broadening the temperature span (Tspan) at room temperature. A ΔT of 0.48 K in the KNLNT-12CZ ceramic is ∼5 times higher than that in the KNLNT-8CZ ceramic at 30 °C. KNLNT-12CZ also exhibits good temperature stability, and the Tspan is up to 65 K. In addition, the multilayer ceramic construct improves the breakdown electric field (Eb) through diminishing defects, leading to a booming ΔT of 3.2 K at 30 °C under 250 kV cm-1 via a direct measurement. The work proposes an avenue for developing high-performance EC materials with a large EC response and broad Tspan in solid-state refrigeration.

High-Performance Ferroelectric Electromagnetic Attenuation Materials with Multiple Polar Units Based on Nanodomain Engineering.

The multirelaxation behavior is promising for high-performance dielectric materials based on polarization-controllable high-efficiency electromagnetic attenuation. However, a single polar unit is the main problem that restricts the development of dielectric materials in the field. Herein, by constructing multiple polar units based on nanodomain engineering, enhanced electromagnetic attenuation properties are achieved in La doping BiFeO3 ferroelectric ceramics. A dual-band attenuation with a maximum reflection loss of -43.4 dB together with a wide effective bandwidth (<-10 dB) of 3.3 GHz in X-band, is acquired in Bi0.85 La0.15 FeO3 which just has a thickness of 1.54 mm. A systematic experimental analysis coupled with potential well modeling suggests that the miniaturization of the ferroelectric domain, from micron to nanoscale, induces an additional interface polarization that is capable of responding to microwave frequency, leading to the formation of dual dielectric relaxation. The way that intrinsic polar unit induces another polar unit through size effect to obtain multiple contributions of electromagnetic loss provides a feasible and universal strategy to design high-performance electromagnetic attenuation materials based on the ferroelectric family.

Enhanced energy-storage performance of an all-inorganic flexible bilayer-like antiferroelectric thin film via using electric field engineering.

A novel all-inorganic flexible bilayer-like Pb0.99Nb0.02(Zr0.55Sn0.40Ti0.05)0.98O3 (PNZSTBL) thin film with the same chemical composition is designed to enhance its energy-storage performance. The PNZSTBL thin film that consists of a large polarization (PNZSTLP) top layer and a high electric breakdown field (PNZSTHE) bottom layer are deposited on flexible mica by controlling the sputtering pressure. The dislocations in such a bilayer-like film can be repressed effectively owing to the identical chemical composition. Most importantly, the PNZSTBL exhibits the complementary advantages of the PNZSTHE and PNZSTLP films based on the electric field amplifying effect and interlayer coupling. An enhanced recoverable energy-storage density (Wrec) of 39.35 J cm-3 is achieved in the PNZSTBL thin film, which is 70% higher than that of the single-layer PNZSTLP. Meanwhile, the flexible PNZSTBL thin film enjoys an outstanding stability in terms of frequency (10-5000 Hz) and temperature (30-170 °C). In addition, the flexible PNZSTBL thin film shows a favorable mechanical cycling endurance after repeated bending 1200 times for a 3.5 mm tensile radius. This work offers a fresh strategy to design prospective bilayer-like dielectric thin films for optimizing the energy-storage performances of materials.

A high-performance triboelectric nanogenerator with improved output stability by construction of biomimetic superhydrophobic nanoporous fibers.

The utilization of nanoporous materials is an extremely effective approach to enhance the electrical performance of triboelectric nanogenerators (TENGs). However, existing methods for preparing nanoporous tribo-materials are not only complicated, costly and time-consuming, but also waste a lot of material. Meanwhile, fabricated nanoporous tribo-materials that have low roughness by nature possess poor surface hydrophobicity, causing low output stability in humid environments. Here, a bio-inspired petiole-like micron fiber-based tribo-material with inner nanopores, rough surface nanostructures and superhydrophobicity is first designed that uses an extraordinarily simple, ultralow-waste and efficient single-component electrospinning process. The petiole-like structures and superhydrophobicity endow the assembled triboelectric nanogenerator (PMF-TENG) with outstanding electrical performance and superior output stability under humid conditions. With a giant power density of 56.9 W m-2 and a high peak-to-peak output voltage of 2209 V, the optimized PMF-TENG can not only be used as a biomechanical energy harvester to directly drive 833 light-emitting-diodes and small electronics, but also serve as a self-powered sensor to detect body motions. Moreover, under a high relative humidity of 80%, the output retention rate of the optimized PMF-TENG is 1.7 and 2.2 times higher than the TENG assembled with the traditional smoother solid nanofiber-based tribo-material and the monolithic nanoporous tribo-material-based TENG, respectively. This work provides an easy-to-fabricate high-performance nanoporous material-based TENG with ultralow material waste and extends its potential for application in humid conditions.

Multifunctional All-Inorganic Flexible Capacitor for Energy Storage and Electrocaloric Refrigeration over a Broad Temperature Range Based on PLZT 9/65/35 Thick Films.

Multifunctional capacitors can efficiently integrate multiple functionalities into a single material to further down-scale state-of-the-art integrated circuits, which are urgently needed in new electronic devices. Here, an all-inorganic flexible capacitor based on Pb0.91La0.09 (Zr0.65Ti0.35)0.9775O3 (PLZT 9/65/35) relaxor ferroelectric thick film (1 µm) was successfully fabricated on LaNiO3/F-Mica substrate for application in electrostatic energy storage and electrocaloric refrigeration simultaneously. The flexible PLZT 9/65/35 thick film presents a desirable breakdown field of 1998 kV/cm, accompanied by a superior recoverable energy density (Wrec) of 40.2 J/cm3. Meanwhile, the thick film exhibits excellent stability of energy-storage performance, including a broad operating temperature (30-180 °C), reduplicative charge-discharge cycles (1 × 107 cycles), and mechanical bending cycles (2000 times). Moreover, a large reversible adiabatic temperature change (ΔT) of 18.0 °C, accompanied by an excellent electrocaloric strength (ΔT/ΔE) of 22.4 K cm/V and refrigerant capacity (RC) of 11.2 J/cm3, is obtained at 80 °C in the flexible PLZT 9/65/35 thick film under the moderate applied electric field of 850 kV/cm. All of these results shed light on a flexible PLZT 9/65/35 thick film capacitor that opens up a route to practical applications in microenergy-storage systems and on-chip thermal refrigeration of advanced electronics.

Tunable Luminescence Contrast of Na0.5Bi4.5Ti4O15:Re (Re = Sm, Pr, Er) Photochromics by Controlling the Excitation Energy of Luminescent Centers.

High luminescent switching contrast of photochromic materials is extremely important in improving the sensitivity and resolution of optical switches and high-density optical data storage devices. To date, conventional methods, such as tuning absorption and emission bands based on electron or resonance energy transfer mechanisms in well-known organic photochromic molecules or compounds, have routinely been adopted to tune luminescent switching behavior. However, these strategies and mechanisms are not effectively applied to luminescence switching in inorganic materials because their crystal structures differ strongly from those of organic materials. In this paper, we report a new method to significantly tune the luminescent switching contrast by modifying the excitation energy of luminescent centers in a newly synthesized photochromism material: Na0.5Bi4.5Ti4O15:Re (Re = Sm, Pr, Er). A significant enhancement of luminescence switching contrast was achieved when the luminescent centers were excited by low energy photons at a given irradiation wavelength, intensity, and time, compared with high excitation energy photons. The trend "the lower the excitation energy, the higher the luminescence switching contrast" is universal in different rare earth ion-doped Na0.5Bi4.5Ti4O15 ferroelectrics. The changes in the luminescent switching contrast based on excitation energy are ascribed to nonradiative energy transfer from the luminescent center to the color center by dipole-dipole interactions according to Dexter theory. This possible utilization of excitation energy at lower energy levels is usually less destructive to both information recording and the recording material itself during luminescent readout processes while achieving higher luminescence switching contrast.

Dual-Mode Luminescence Modulation upon Visible-Light-Driven Photochromism with High Contrast for Inorganic Luminescence Ferroelectrics.

A luminescence ferroelectric oxide, Na(0.5)Bi(2.5)Nb2O9 (NBN), system with bismuth layer structure introduced by lanthanide ion (Er(3+)) has been demonstrated to exhibit reversible, high-contrast luminescence modulation (95%) and excellent fatigue resistance based on visible-light-driven photochromism (407 nm or sunlight). The coloration and decoloration process can be effectively read out by dual modes, upconversion and downshifting, and reversibly converted between green and dark gray by alternating visible light or sunlight irradiation and thermal stimulus. The luminescence modulation degree upon photochromic reactions is strongly dependent upon irradiation light wavelength and irradiation time. After undergoing several cycles, there are no significant degradations, showing high reversibility. Considering its high-contrast photoswitchable luminescence feature and intrinsic ferroelectricity of NBN host, NBN-based multifunctional materials can be suggested as a promising candidate for new potentials in photonic storage and optoelectronic multifunctional devices.

Reversible Luminescence Modulation upon Photochromic Reactions in Rare-Earth Doped Ferroelectric Oxides by in Situ Photoluminescence Spectroscopy.

Reversible luminescence photoswitching upon photochromic reactions with excellent reproducibility is achieved in a new inorganic luminescence material: Na(0.5)Bi(2.5)Nb2O9: Pr(3+) (NBN:Pr) ferroelectric oxides. Upon blue light (452 nm) or sunlight irradiation, the material exhibits a reversible photochromism (PC) performance between dark gray and green color by alternating visible light and thermal stimulus without inducing any structure changes and is accompanied by a red emission at 613 nm. The coloration and decoloration process can be quantitatively evaluated by in situ photoluminescence spectroscopy. Meanwhile, the luminescence emission intensity based on PC reactions is effectively tuned by changing irradiation time and excitation wavelength, and the degree of luminescence modulation has no significant degradation after several periods, showing very excellent reproducibility. On the basis of the luminescence modulation behavior, a double-exponential relaxation model is proposed, and a combined equation is adopted to well describe the luminescence response to light irradiation, being in agreement with the experimental data.

Reversible photoresponsive switching in Bi(2.5)Na(0.5)Nb(2)O(9)-based luminescent ferroelectrics.

Reversible luminescence modulation upon photochromic reactions with excellent reproducibility was achieved from Eu(3+) doped Bi2.5Na0.5Nb2O9 multifunctional ferroelectrics. The material exhibits strong sensitivity to visible light or sunlight with fast response time without inducing any structural changes.

Energy-storage properties and electrocaloric effect of Pb(1-3x/2)LaxZr0.85Ti0.15O3 antiferroelectric thick films.

Antiferroelectric (AFE) thick (1 µm) films of Pb(1-3x/2)LaxZr0.85Ti0.15O3 (PLZT) with x = 0.08, 0.10, 0.12, and 0.14 were deposited on LaNiO3/Si (100) substrates by a sol-gel method. The dielectric properties, energy-storage performance, electrocaloric effect, and leakage current behavior were investigated in detail. With increasing La content, dielectric constant and saturated polarizations of the thick films were gradually decreased. A maximum recoverable energy-storage density of 38 J/cm(3) and efficiency of 71% were achieved in the thick films with x = 0.12 at room temperature. A large reversible adiabatic temperature change of ΔT = 25.0 °C was presented in the thick films with x = 0.08 at 127 °C at 990 kV/cm. Moreover, all the samples had a lower leakage current density below 10(-6) A/cm(2) at room temperature. These results indicated that the PLZT AFE thick films could be a potential candidate for applications in high energy-storage density capacitors and cooling devices.