Film Heterostructures Research Articles

On Model of Manufacturing of a Band-Pass Filter to Increase Integration Rate of Field-Effect Heterotransistors

In the present time several actual problems of the solid state electronics (such as increasing of performance, reliability and density of elements of integrated circuits: diodes, field-effect and bipolar transistors) are intensively solving. To increase the performance of these devices it is attracted an interest determination of materials with higher values of charge carriers mobility. One way to decrease dimensions of elements of integrated circuits is manufacturing them in thin film heterostructures. In this paper we introduce an approach to increase density of field-effect transistors in the framework of a metal-oxidesemiconductor field-effect transistor filter. In the framework of the approach we consider manufacturing of the above filter in a heterostructure with specific configuration. Several appropriate areas of the considered heterostructure should be doped by diffusion or by ion implantation. After the doping the considered dopant and radiation defects should be annealed in the framework oh the recently considered optimized scheme. We also consider an approach to decrease value of mismatch-induced stress in the considered heterostructure. The decreasing of the mismatch-induced stress could be decreased by radiation processing of appropriate areas of heterostructure. We introduce an analytical approach to analyze mass and heat transport in heterostructures during manufacturing of integrated circuits with account mismatch-induced stress.

Evolution of Phases at the Surface and Interface of Mn Based Spinel Cathode with Coating Layer - a Spectroscopic Investigation

Surface modifications, commonly termed coatings or artificial interphases, are known to mitigate secondary reactions of charged cathodes with organic electrolyte and limit surface reconstruction. As a result, better electrochemical stability has been observed for coated cathodes in both liquid and solid electrolyte-based Li ion batteries (LIBs). However, these coatings, in contact with electrolyte, can be dynamic and evolve during processing stages or electrochemical cycling.In this work we investigate the interphases between spinel cathodes and two coating layers, LiNbO3 and Al2O3. The spinel LiMn2O4 (LMO) cathode and its doped variant LiMn1.5Ni0.5O4 (LMNO), owing to their three-dimensional structure, have high-rate and high-power capability with moderate energy density. With conventional electrolytes, the surface transition metal undergoes reduction forming thin binary or layered ternary oxides when charged beyond 4.2V (vs Li), restricting Li ion transport, and thereby compromising accessible capacity. This along with dissolution of manganese by HF (generated at the liquid electrolyte-electrode interface) restricts long-term applicability in practical LIBs thus necessitating surface coating or doping. In our experiments we choose epitaxial thin-film cathodes and thin-film coating materials. These provide large interface, and hence interphase areas, of well-defined crystal orientation, facilitating characterisation to deepen our understanding of the surface reactions occurring. We form an epitaxial film of cathode material using pulsed laser deposition (PLD) followed by controlled deposition of Al2O3 via atomic layer deposition (ALD) or LiNbO3 via PLD.We will present the detailed characterisation analysis of coated and uncoated spinel thin films. The epitaxial nature and crystal structure of deposited thin films are confirmed using thin film X-ray diffraction. Structurally, the phase diagram of Li-Mn(Ni)-O is complicated with many possible crystal structures with varying lithium content as well as different oxidation states of manganese. Hence, we employ a combination of X-ray absorption and photoelectron spectroscopies (XAS/XPS) to look at the chemical states of Mn ion in the cathode and Nb and Al ions in LiNbO3 and Al2O3 coating layers. For the as deposited fresh samples, the effect of deposition conditions is evaluated using XAS of the Mn L-edge and Al K-edge. XPS depth profiles of elemental distribution in the thin film heterostructures are obtained at three different incident X-ray energies (up to 6.6 kV) – thus providing chemical information from the surface, coating and at the interface of coating and cathode layers. Subsequently we electrochemically cycled these films in organic electrolyte against Li metal anode and further spectroscopic investigations were carried out. The effect of Al2O3 vs LiNbO3 coatings on retaining the structure of cathode material is probed and we will discuss the understanding thereby developed.

Bi2O3/ZnO heterostructured semiconductor nanocomposites: synthesis, characterization and its visible light-induced degradation of methylene blue dye

Abstract In this study, we describe the creation of linked semiconductor nanomaterials, which represents a significant development for photocatalytic applications. A Bi2O3–ZnO hetrostructured thin film was created using the SILAR-CBD deposition technique. In comparison to pure ZnO and Bi2O3, the produced heterostructured thin film showed greater photocatalytic (PCD) activity for the degradation of methylene blue (MB) dye under UV light. The formation of Bi2O3 (monoclinic lattice phase) and ZnO (hexagonal wurtzite phase) are the heterostructured nanomaterials that were generated, according to a powder XRD inspection. An image taken with HR-TEM demonstrates the mixing of nanoparticles and nanorod formations in the Bi2O3/ZnO. The vectorial movement of electrons (e−) and holes (h+) between ZnO and Bi2O3 is responsible for the boosted photocatalytic efficiency, which is in turn, accountable for the enhanced photocatalytic activities.

Impedance spectroscopy studies revealing the influence of ZnO-rGO heterojunction interface on NO2 sensing

Heterojunction interfaces play a very important role in improving the gas sensing properties. In our previous study through direct current (dc) measurements we showed that a synergetic balance of depletion width at ZnO-rGO interface with the Debye length leads to the improved selective NO2 response. In this paper, impedance spectroscopy is used to probe the NO2 sensing behaviour of ZnO-rGO heterostructure films as the processes of different time constants in gas/ solid interactions can be distinguished by varying the AC frequency. The Nyquist plots for ZnO-rGO films measured under ambient as well as after NO2 exposure shows that sensor response is governed by the variation in potential barrier of depletion region formed at the p-n junction between ZnO and rGO. To understand the adsorption mechanism, experimental response data measured at different NO2 concentrations were fitted using suitable adsorption kinetic models. Elovich model is found to be apt for lower concentrations where energetically different sites are involved in the adsorption process while higher concentrations are better modelled with pseudo first order kinetics that is independent of the surface coverage.

Identification of electronic dimensionality reduction in semiconductor quantum well structures

Two-dimensional (2D) systems, such as high-temperature superconductors, surface states of topological insulators, and layered materials, have been intensively studied using vacuum-ultraviolet (VUV) angle-resolved photoemission spectroscopy (ARPES). In semiconductor films (heterostructures), quantum well (QW) states arise due to electron/hole accumulations at the surface (interface). The quantized states due to quantum confinement can be observed by VUV-ARPES, while the periodic intensity modulations along the surface normal (kz) direction of these quantized states are also observable by varying incident photon energy, resembling three-dimensional (3D) band dispersion. We have conducted soft X-ray (SX) ARPES measurements on thick and ultrathin III-V semiconductor InSb(001) films to investigate the electronic dimensionality reduction in semiconductor QWs. In addition to the dissipation of the kz dispersion, the SX-ARPES observations demonstrate the changes of the symmetry and periodicity of the Brillouin zone in the ultrathin film as 2D QW compared with these of the 3D bulk one, indicating the electronic dimensionality reduction of the 3D bulk band dispersion caused by the quantum confinement. The results provide a critical diagnosis using SX-ARPES for the dimensionality reduction in semiconductor QW structures.

Piezo-phototronic effect modulated optoelectronic artificial synapse based on a-Ga2O3/ZnO heterojunction

Amorphous gallium oxide (a-Ga2O3) based optoelectronic devices responds to deep ultraviolet (DUV), which triggers their potential applications for simulating biological vision system. However, there is still lack of research on the influence of multiple stimuli on regulating synaptic plasticity in artificial synapse. Herein, we reported a flexible a-Ga2O3/ZnO film heterostructure with tunable DUV photoresponse, serving as a promising platform for artificial optoelectronic synapse. Based on persistent photoconductivity effect under 265 nm illumination, basic synaptic functions have been mimicked. Notably, the strain-induced piezo-phototronic effect of the heterojunction enables the modulation of synaptic plasticity, playing a role analogous to neuromodulator interaction with biological synapse activity. Strain-evoked an additional degree of freedom controls synapse weight-update rate during learning process and synapse weight-decay during forgetting process. The underlying mechanism is attributed to energy band bending tailored by strain-induced piezo-potential that determines carrier separation/transport and the recombination reaction of ionized oxygen vacancy. The recognition accuracy of MNIST images is as high as 92.31% in the artificial neural network constructed by the heterojunction devices. This work not only exhibits the application prospect of ultra-wide bandgap semiconductor-based heterojunction in artificial optoelectronic synapse, but also opens up a new avenue for multiple stimuli modulating synaptic plasticity.

Al-doped ZnO/WO3 heterostructure films prepared by magnetron sputtering for isopropanol sensors

Al-doped ZnO/WO3 heterostructure films prepared by magnetron sputtering for isopropanol sensors

Accelerated design of stable halide perovskite heterostructure film in hostile condition via surface modifier

The bulk halide perovskite heterostructure has been adopted for perovskite-based optoelectronic devices owing to their interesting interfacial phenomena; however, most of them are unstable in hostile condition and the extremely large virtual design space causes problems for traditional trial-and-error methods to optimize them. In this study, we combine photoelectrochemical experiments, machine learning and first-principles calculations (Exp + ML + DFT) to accelerate the design of halide perovskite heterostructures in aqueous solution, in an effort to improve stability of halide perovskite materials in hostile condition (prototypical CH3NH3PbI3 quickly deactivates in water within seconds). The optimization of halide perovskite heterojunction with surface modifier is speeded up via machine learning using extra tree algorithm, and a large virtual design space consisting of halide perovskite heterostructure composites is predicted. Five new water-stable perovskite heterostructure candidates predicted via machine learning are experimentally validated, and the first-principles calculations reveal the detailed atomic and electronic structures of an exemplar stable heterostructure candidate. This study demonstrates the effectiveness of machine learning to accelerate the design of stable halide perovskite heterostructure materials in hostile condition.

AlScN-on-SiC Diaphragm Multimode Micromechanical Resonators for High-Temperature Sensing Applications

We demonstrate circular diaphragm multimode micromechanical resonators made of heterostructure thin film of aluminum scandium nitride (AlScN) sputtered on cubic silicon carbide (3C-SiC). We systematically characterize the multimode resonators from room temperature up to 600ºC high-temperature environment. We observe clear consistency in resonances measured in heating up and cooling down processes, validating that the AlScN/SiC diaphragm resonators can operate robustly in high-temperature environment up to 600°C without observable degradation. Raman spectroscopy results indicate that the turning points of the peak positions of the longitudinal optical (LO) phonon modes of both 3C-SiC and AlScN occur in almost the same temperature region where the turning point of temperature coefficient of resonance frequency (TCf) is observed. We calibrate the device temperature by measuring Raman peak of the silicon (Si) substrate of the chip, yielding a crystal lattice temperature of 410ºC at the heater setting temperature being 600ºC. The heating efficiency can be improved by clamping the chip using a clip or jig with lower thermal conductivity.

A flexible magnetic detector based on transferred ferroelectric/ferromagnetic thin film heterostructure

A flexible magnetic detector based on ferroelectric/ferromagnetic (PZT/Metglas) thin film heterostructure is developed by using etching and transferring technique. The transferred PZT film still exhibits (001)-oriented or very highly textured structure with good ferroelectricity (P r = 50 μC cm−2 and E c = 150 kV cm−1). Magnetoelectric (ME) voltage coefficient of the PZT/Metglas film heterostructure approaches 5.1 V cm−1 Oe at resonance frequency (57.5 kHz). The flexible detector has a sensitivity of AC 0.3 nT and DC 1 Oe with high stability for magnetic field detection. Our demonstration provides a viable approach for realizing ME thin film transfer technology, which is of great significance for future applications on flexible magnetic detectors.

Interface modification of MoS2/ZnO heterojunction for controllable electron flow and fabrication of high-performance UV photodetectors with fast response/recovery speed

Hetero-structured thin films, MoS2/ZnO thin films, were fabricated by adding MoS2 films under the ZnO thin films via sol-gel spin-coating method; ZnO nanoparticles were observed on the surface of sol-gel spin-coated ZnO thin films. Although ZnO nanoparticles were observed on the surface of hetero-structured thin films, the surface area of the hetero-structured thin films was higher than ZnO thin films owing to the high surface roughness of the MoS2 films. Three diffraction peaks were observed in the hetero-structured thin films at 31.74°, 34.38°, and 36.22°, which indicates heterostructure was polycrystalline, and the heterostructure was formed successfully. When the UV photodetector was fabricated by using hetero-structured thin films, the enhanced values of photocurrent, photoresponsivity and photosensitivity were observed. In addition, the hetero-structured thin films exhibited a faster response/recovery speed because the move of electrons and holes during UV illumination. Thus, it was concluded that the interface modification of the MoS2/ZnO heterojunction is an effective solution for overcoming the drawbacks of ZnO-based UV photodetectors. This approach can be considered a novel method for high-performance optoelectronics with fast response speed applicable to various fields.

Heterogeneous Ti3C2Tx MXene-MWCNT@MoS2 Film for Enhanced Long-Term Electromagnetic Interference Shielding in the Moisture Environment.

MXene, as a novel two-dimensional (2D) material, has unique inherent features such as lightweight, flexibility, high electrical conductivity, customizable surface chemistry, and facile solution processability. However, utilizing MXene (Ti3C2Tx) films for long-term electromagnetic interference (EMI) shielding poses challenges, as they are susceptible to chemical deterioration through oxidation into TiO2. In this work, an ultrathin heterogeneous film of Ti3C2Tx MXene integrated with multiwalled carbon nanotubes supporting MoS2 clusters (MXene/MWCNT@MoS2) was developed. The heterogeneous film with 15 wt % of MWCNT@MoS2 clusters exhibited improved EMI shielding performance such as the highest EMI shielding effectiveness of 50 dB and the specific shielding effectiveness of 20,355 dB cm2 g -1, mainly attributed to the excellent electrical conductivity, distinctive porous structure, and multiple interfacial interactions. The heterogeneous films underwent extended exposure to a moisture environment (35 days), and their structural stability and EMI shielding performance were enhanced by the integration of MWCNT@MoS2 clusters. As a result, the engineered heterostructure of multilayered hybrid films holds promise as a viable option for improving the EMI shielding effectiveness and stability of Ti3C2Tx MXene.

Revealing enhanced X-Ray radiation shielding of 2D layered materials and their laminar heterostructures

This paper demonstrates a new concept of using two-dimensional (2D) layered materials and their heterostructures for enhanced X-ray radiation shielding. This phenomenon is revealed by characterization on the X-ray shielding performances of several 2D materials with high atomic numbers (Z), including MoS2, antimonene (Sb), and MXene prepared as multi-layered and heterostructure films by assembly their few-layer sheets. Results showed considerable X-ray shielding enhancement of (40–50%) at 30 kVp for individual 2D multi-layered films compared with their bulk structures of these materials. Furthermore, when these multi-layered films were combined into laminar heterostructures structures (e.g., MoS2 + MXene), further enhancement of 60% was achieved. The mechanism of the observed X-ray shielding enhancement by these multi-layered 2D structures is not clear at this stage. It is postulated to be the result of an additional multiple scattering and reflections of photons between multiple layers of 2D crystals inside the film, which does not occur in their uniform bulk materials. The presented results suggest that multi-layered 2D materials with high atomic numbers (Z) and their laminar heterostructures could offer a new and promising strategy for designing of a new generation of Pb-free radiation-shielding materials, which is urgently needed across broad sectors.Graphical abstract

A Novel Strategy for the Synthesis of High Stability of Luminescent Zero Dimensional-Two Dimensional CsPbBr3 Quantum Dot/1,4-bis(4-methylstyryl)benzene Nanoplate Heterostructures at an Atmospheric Condition.

Perovskite quantum dots (QDs), emerging with excellent bright-green photoluminescence (PL) and a large absorption coefficient, are of great potential for the fabrication of light sources in underwater optical wireless communication systems. However, the instability caused by low formation energy and abundant surface traps is still a major concern for perovskite-based light sources in underwater conditions. Herein, we propose ultra-stable zero dimensional-two dimensional (0D-2D) CsPbBr3 QD/1,4-bis(4-methylstyryl)benzene (p-MSB) nanoplate (NP) heterostructures synthesized via a facile approach at room temperature in air. CsPbBr3 QDs can naturally nucleate on the p-MSB NP toluene solution, and the radiative combination is drastically intensified owing to the electron transfer within the typical type-II heterostructures, leading to a sharply increased PLQY of the heterostructure thin films up to 200% compared with the pristine sample. The passivation of defects within CsPbBr3 QDs can be effectively realized with the existence of p-MSB NPs, and thus the obviously improved PL is steadily witnessed in an ambient atmosphere and thermal environment. Meanwhile, the enhanced humidity stability and a peak EQE of 9.67% suggests a synergetic strategy for concurrently addressing the knotty problems on unsatisfied luminous efficiency and stability of perovskites for high-performance green-emitting optoelectronic devices in underwater applications.

Modulation-doping a correlated electron insulator

Correlated electron materials (CEMs) host a rich variety of condensed matter phases. Vanadium dioxide (VO2) is a prototypical CEM with a temperature-dependent metal-to-insulator (MIT) transition with a concomitant crystal symmetry change. External control of MIT in VO2—especially without inducing structural changes—has been a long-standing challenge. In this work, we design and synthesize modulation-doped VO2-based thin film heterostructures that closely emulate a textbook example of filling control in a correlated electron insulator. Using a combination of charge transport, hard X-ray photoelectron spectroscopy, and structural characterization, we show that the insulating state can be doped to achieve carrier densities greater than 5 × 1021 cm−3 without inducing any measurable structural changes. We find that the MIT temperature (TMIT) continuously decreases with increasing carrier concentration. Remarkably, the insulating state is robust even at doping concentrations as high as ~0.2 e−/vanadium. Finally, our work reveals modulation-doping as a viable method for electronic control of phase transitions in correlated electron oxides with the potential for use in future devices based on electric-field controlled phase transitions.

Stack growth of wafer-scale van der Waals superconductor heterostructures.

Two-dimensional (2D)van der Waals (vdW) heterostructures have attracted considerable attention in recent years1-5. The most widely used method of fabrication is to stack mechanically exfoliated micrometre-sized flakes6-18, but this process is not scalable for practical applications. Despite thousands of 2D materials being created, using various stacking combinations1-3,19-21, hardly any large 2D superconductors can be stacked intact into vdW heterostructures, greatly restricting the applications for such devices. Here we report a high-to-low temperature strategy for controllably growing stacks of multiple-layered vdW superconductor heterostructure (vdWSH) films at a wafer scale. The number of layers of 2D superconductors in the vdWSHs can be precisely controlled, and we have successfully grown 27double-block, 15 triple-block, 5 four-block and 3 five-block vdWSH films(where one block represents one 2D material). Morphological, spectroscopic and atomic-scale structural analyses reveal the presence of parallel, clean and atomicallysharp vdW interfaces on a large scale, with very little contamination between neighbouring layers. The intact vdW interfaces allow us to achieve proximity-induced superconductivity and superconducting Josephson junctions on a centimetre scale. Our process for making multiple-layered vdWSHs can easily be generalized to other situations involving 2D materials, potentially accelerating the design of next-generation functional devices and applications22-24.

On-chip all-electrical determination of the magnetoelastic coupling constant of magnetic heterostructures

We have developed an approach to determine the magnetoelastic coupling constant of magnetic layers in thin film heterostructures. The film is formed on a piezoelectric substrate between two interdigital transducers (IDTs), a platform often used to construct a surface acoustic wave device. With the substrate piezoelectricity, strain is induced into the film by applying a dc voltage to the IDTs. The strain causes changes in the magnetization direction of the magnetic layer, which is probed by measuring changes, if any, in the transverse resistance of the heterostructure. We find that the extracted magnetoelastic coupling constant of the magnetic layer (CoFeB) depends on the film stacking. Such change can be accounted for provided that the elastic properties of the layers that constitute the heterostructures are taken into account. The on-chip all-electrical approach described here provides a versatile means to quantitatively assess the magnetoelastic coupling constant of thin film heterostructures.

Solar Cell Application of 1D Heterostructure Based on Single-Walled CNT

The experimental synthesis of one-dimensional (1D) van der Waals heterostructures, first introduced in 2020 [1], has attracted much research attention. Discussions upon this coaxial stack of different atomic layers are not only limited to synthesis and characteristics, but also extended to applications. Many unique properties of the 1D van der Waals heterostructures, such as the adjustable band gap, strong quenching of photoluminescence of MoS2 by inner single-walled CNT, enable this structure to be a potential active layer material for solar cells [2].For the synthesis of 1D van der Waals heterostructures, we first use dispersed high-purity semiconducting single-walled carbon nanotubes (s-SWCNT) solution obtained from Kataura group [3] as inner tube material. With an anodic aluminum oxide (AAO) membrane filter and HCl, we managed to fabricate a free-standing s-SWCNT film [4]. Then following our established CVD process [5], we are wrapping this inner s-SWCNT tube with an insulating boron nitride layer, and a semiconducting MoS2 layer. After that, the as-prepared 1D van der Waals heterostructures film will be utilized for solar cell fabrication.The solar cell is adopting an n-i-p structure, in the order of glass-ITO-SnO2-Active layer-Spiro-Au. After spin-coating and annealing SnO2 (electron transporting layer) onto ITO-patterned glass, the 1D van der Waals heterostructure film is laminated on the SnO2 layer. Spiro (hole transporting layer) will be then spin-coated onto the film. Finally, gold is vapor-deposited onto the device in a vacuum chamber, as the top electrode [6].Through photocurrent measurement of 1D van der Waals structure film using Esko film, a mixture of metallic-SWCNT and s-SWCNT, we found it is photosensitive with exposure to light and laser. The 1D van der Waals structure film using high-purity s-SWCNT is then expected to generate higher photocurrent, the experimental result will be updated in the future. By the IV measurement of the solar cell, we observed the photovoltaic effect of the device. Moreover, this new conceptual solar cell is believed to possess many advantages at the same time, such as flexibility, durability, non-toxicity, and sustainability [2]. However, further research on the choices of materials and optimizations of device parameters is still required in order to reach sufficient power conversion efficiency as a photovoltaic device.[1] R. Xiang et al., Science 367, 537–542 (2020)[2] R. Xiang et al., Natl Sci Open 1, 3 (2022)[3] J. Cui et al., ACS Appl. Nano Mater 2, 1, 343–350 (2019)[4] C. Zhang et al., ACS Nano 16, 11, 18630–18636 (2022)[5] M. Liu et al., ACS Nano 15, 5, 8418–8426 (2021)[6] J.-M. Choi et al, Adv. Funct. Mater. 32, 2204594 (2022)

Phase change, tuning of optical and dielectric parameters in Bi/S-Se-Sb heterostructure film upon thermal annealing: An experimental and computational approach

The study is based on annealing-induced Bi diffusion into Se30S30Sb40 sites that bring modification in its linear-nonlinear optical, structural, and dielectric properties. The Bi/Se30S30Sb40 heterostructure film was annealed at 100,150,200 and 250 °C. The Bi2Se3 and Sb2Se3 phase formation was confirmed from the X-ray diffraction as well as from the Raman study. The morphology has been studied by the field emission scanning electron microscopy images with increased particle size upon annealing. The uniformity and homogeneity of the film were noticed from the energy dispersive X-ray analysis elemental mapping. The bandgap decreased from 1.461 eV (as-prepared Bi/Se30S30Sb40) to 1.258 eV (250 °C annealed) with an increment in static refractive index from 2.864 to 3.114 which was noticed from the optical study. The linear optical parameters were tuned with annealing conditions and such changes were understood from the concept of density of states and defects in the film. The increase in dielectric loss factor and decrease in quality factor with annealing is accompanied by the increase in both electronic and optical conductivity. The plasma frequency decreased and optical electronegativity reduced from 1.728 (as-prepared Bi/Se30S30Sb40) to 1.692 (250 °C annealed) with annealing. The value of 3rd-order nonlinear susceptibility and non-linear refractive index gets almost doubled (i.e. 1.838 × 10−11 to 3.913 × 10−11 esu and 2.419 × 10−10 to 4.735 × 10−10 esu respectively) with annealing with an increase in the nonlinear absorption coefficient. The hydrophilic nature of the films with annealing was observed from the surface wettability study. The computational study by density functional theory provided the necessary idea for structural and physical parameters of the films.

Modulation of polarization behavior in Na0.5Bi0.5(Ti,Fe)O3-based heterostructure thin films for dielectric energy storage: Defect engineering study via an artificial aging process

Na0.5Bi0.5TiO3 (NBT)-based thin films are highly desired for energy storage owing to their high intrinsic polarization and Curie temperature under the current trend of electronic device integration and portability. However, the low energy density originating from the inferior anti-breakdown ability (EBD), as well as the limited space for improvement of the gap between maximum polarization and remanent polarization (Pm–Pr) is the main challenge for practical applications. Here, we propose a strategy to modulate polarization behavior of NBT-based heterostructure thin films. Na0.5Bi0.5(Ti0.97Fe0.03)O3 (NBFT) is taken as the basic component. Na0.5Bi0.5(Ti0.98Zr0.02)O3 (NBZT) and (Ba1-xSrx)TiO3 (BSxT, where x is set with gradient characteristics of 0, 0.1 and 0.2, respectively from near to far substrate ends) are chosen to fabricate NBFT/BSxT and (NBFT/NBZT)5/NBFT heterostructure thin films. Artificial aging process is carried out for modulating polarization behavior of both the heterostructure thin films. Time-dependent strain and defect migration are observed and analyzed, reflecting the structural relaxation characteristics of the thin films. After aging with treating, the recoverable energy storage density (Wrec) of NBFT/BSxT and (NBFT/NBZT)5/NBFT are increased from 46.78 to 66.95 J/cm3 and 66.57–67.64 J/cm3, respectively, with energy storage efficiency (η) increasing from 68.46% to 75.65% and 64.33%–70.76%, respectively at 20 kHz and room temperature. This research provides a new route to take usages of aging process for designing NBT-based thin film for dielectric energy storage.