Jing Zhang

Quasi-1D antimony chalcogenides are promising light-absorbing materials that demand a (001) crystallographic orientation for optimal performance in device applications. This study links substrate nanostructure to thin film orientation in quasi-1D materials. Here, exceptionally highly (001) oriented Sb₂Se₃ layers are achieved using substrate nanostructure engineering to “filter out” undesirable (hk0) crystals, and select (001), in the early growth stage.

Abstract

Antimony chalcogenide, Sb₂X₃ (X = S, Se), applications greatly benefit from efficient charge transport along covalently bonded (001) oriented (Sb₄X₆) _n ribbons, making thin film orientation control highly desirable – although particularly hard to achieve experimentally. Here, it is shown for the first time that substrate nanostructure plays a key role in driving the growth of (001) oriented antimony chalcogenide thin films. Vapor Transport Deposition of Sb₂Se₃ thin films is conducted on ZnO substrates whose morphology is tuned between highly nanostructured and flat. The extent of Sb₂Se₃ (001) orientation is directly correlated to the degree of substrate nanostructure. These data showcase that nanostructuring a substrate is an effective tool to control the orientation and morphology of Sb₂Se₃ films. The optimized samples demonstrate high (001) crystallographic orientation. A growth mechanism for these films is proposed, wherein the substrate physically restricts the development of undesirable crystallographic orientations. It is shown that the surface chemistry of the nanostructured substrates can be altered and still drive the growth of (001) Sb₂Se₃ thin films – not limiting this phenomenon to a particular substrate type. Insights from this work are expected to guide the rational design of Sb₂X₃ thin film devices and other low-dimensional crystal-structured materials wherein performance is intrinsically linked to morphology and orientation.

Nature, Published online: 31 May 2023; doi:10.1038/s41586-023-06074-9

The cycles of laser light have been used to advance transmission electron microscopy to attosecond time resolution, revealing the interactions between light and matter in terms of their fundamental dimensions in space and time.

Nature Communications, Published online: 30 May 2023; doi:10.1038/s41467-023-38431-7

Trivalent lanthanides are typically described using an ionic picture that leads to localized magnetic moments. Here authors show that the “textbook” description of lanthanides fails for Pr4+ ions where the hierarchy of single-ion energy scales can be tailored to explore correlated phenomena in quantum materials.

Crystalline silicon nano/micro membrane sheets from a single <111> mother wafer generated by multiple transfer printing method have thicknesses ranging from 300 nm to 13 µm and high areal density of over 90%. Two types of applications (photovoltaic device and transistor array) based on the silicon nano/micro membrane sheets demonstrate applicability in flexible electronics.

Abstract

Ultrathin crystalline silicon is widely used as an active material for high-performance, flexible, and stretchable electronics, from simple passive and active components to complex integrated circuits, due to its excellent electrical and mechanical properties. However, in contrast to conventional silicon wafer-based devices, ultrathin crystalline silicon-based electronics require an expensive and rather complicated fabrication process. Although silicon-on-insulator (SOI) wafers are commonly used to obtain a single layer of crystalline silicon, they are costly and difficult to process. Therefore, as an alternative to SOI wafers-based thin layers, here, a simple transfer method is proposed for printing ultrathin multiple crystalline silicon sheets with thicknesses between 300 nm to 13 µm and high areal density (>90%) from a single mother wafer. Theoretically, the silicon nano/micro membrane can be generated until the mother wafer is completely consumed. In addition, the electronic applications of silicon membranes are successfully demonstrated through the fabrication of a flexible solar cell and flexible NMOS transistor arrays.

Nature Photonics, Published online: 29 May 2023; doi:10.1038/s41566-023-01217-w

Optical analogues of electronic memristors are desirable for applications including photonic artificial intelligence and computing platforms. Here, recent progress on integrated optical memristors is reviewed.

A simple sprinkling of Se nanopowders onto sliding Mo and W thin films leads to the tribochemical in operando formation of lubricious 2D selenides. Due to the thermal and vacuum stability of the Se nanopowders they can be used to replenish sliding components with solid lubricants, avoiding the long-lasting problem of transition metal dichalcogenidelubricity degradation caused by environmental molecules.

Abstract

Transition metal dichalcogenide (TMD) coatings have attracted enormous scientific and industrial interest due to their outstanding tribological behavior. The paradigmatic example is MoS₂, even though selenides and tellurides have demonstrated superior tribological properties. Here, an innovative in operando conversion of Se nanopowders into lubricious 2D selenides, by sprinkling them onto sliding metallic surfaces coated with Mo and W thin films, is described. Advanced material characterization confirms the tribochemical formation of a thin tribofilm containing selenides, reducing the coefficient of friction down to below 0.1 in ambient air, levels typically reached using fully formulated oils. Ab initio molecular dynamics simulations under tribological conditions reveal the atomistic mechanisms that result in the shear-induced synthesis of selenide monolayers from nanopowders. The use of Se nanopowder provides thermal stability and prevents outgassing in vacuum environments. Additionally, the high reactivity of the Se nanopowder with the transition metal coating in the conditions prevailing in the contact interface yields highly reproducible results, making it particularly suitable for the replenishment of sliding components with solid lubricants, avoiding the long-lasting problem of TMD-lubricity degradation caused by environmental molecules. The suggested straightforward approach demonstrates an unconventional and smart way to synthesize TMDs in operando and exploit their friction- and wear-reducing impact.

The amino-As based synthesis of InAs@ZnSe core@shell nanocrystals with shell thickness up to seven monolayers is reported. The InAs@ZnSe nanocrystals exhibit photoluminescence quantum yields up to 70%, a record value for such system, thanks to an InZnSe interlayer featuring a structure similar to that of In₂ZnSe₄, which dampens the strain between the InAs core and the ZnSe shell.

Abstract

InAs-based nanocrystals can enable restriction of hazardous substances (RoHS) compliant optoelectronic devices, but their photoluminescence efficiency needs improvement. We report an optimized synthesis of InAs@ZnSe core@shell nanocrystals allowing to tune the ZnSe shell thickness up to seven mono-layers (ML) and to boost the emission, reaching a quantum yield of ≈70% at ≈900 nm. It is demonstrated that a high quantum yield can be attained when the shell thickness is at least ≈3ML. Notably, the photoluminescence lifetimeshows only a minor variation as a function of shell thickness, whereas the Auger recombination time (a limiting aspect in technological applications when fast) slows down from 11 to 38 ps when increasing the shell thickness from 1.5 to 7MLs. Chemical and structural analyses evidence that InAs@ZnSe nanocrystals do not exhibit any strain at the core-shell interface, likely due to the formation of an InZnSe interlayer. This is supported by atomistic modeling, which indicates the interlayer as being composed of In, Zn, Se and cation vacancies, alike to the In₂ZnSe₄ crystal structure. The simulations reveal an electronic structure consistent with that of type-I heterostructures, in which localized trap states can be passivated by a thick shell (>3ML) and excitons are confined in the core.

Biomanufacturing of high-purity rare earth (RE) materials is achieved by establishing a microbial synthesis system. RE bioproducts can be extracellularly collected from RE tailings by microbial in situ synthesis. A series of RE-biosorbent columns with high affinity are developed by immobilizing specifically designed proteins with an agarose matrix. Moreover, the lanthanide-immobilized methanol dehydrogenase is biofabricated for high-value utilization of RE.

Abstract

Rare earth materials play an irreplaceable role in biomedical and high technology fields. However, typical mining and extraction approaches to rare earth elements (REEs) often lead to severe environmental problems and resource wastage due to the involvement of hazardous chemicals. Although biomining shows elegant alternatives, there are still grand challenges to sustainably isolate and recover REEs in nature because of insufficient metal-extracting microbes and RE-scavenging macromolecular tools. To obtain high-performance rare earth materials directly from rare earth ore, a new generation of biological synthesis strategies needs to be developed for the efficient preparation of REEs. The microbial synthesis system established here has achieved active biomanufacturing of high-purity rare earth products. Further, through employing robust affinity columns bioconjugated with structurally engineered proteins, outstanding separation of Eu/Lu and Dy/La is acquired with the purity of 99.9% (Eu), 97.1% (La), and 92.7% (Dy). More importantly, in situ one-pot synthesis of lanthanide-dependent methanol dehydrogenase is well harnessed and exclusively adsorbs La, Ce, Pr, and Nd in RE tailing for advanced biocatalysis, indicating high value-added application. Therefore, this novel biosynthetic platform provides an insightful roadmap to expand the scope of chassis engineering in terms of biofoundry and to manufacture valuable bioproducts related to REEs.

Nature Communications, Published online: 27 May 2023; doi:10.1038/s41467-023-38852-4

Flexible thermoelectric generators can use body heat to power electronic wearables but are often limited by a trade-off between flexibility and output performance. Here, authors demonstrate a scalable, lightweight, elastic, and high-performing network-based Ag2Se thermoelectric generator.

A simple yet robust template-free strategy is developed to yield azobenzene-dangled covalent organic frameworks (Azo-COFs), whose crystallinity and morphology can be conveniently tailored by changing the ratio of amine to aldehyde. The adsorption capacity of Azo-COFs toward organic dyes is increased by 3.7-fold when irradiated with ultraviolet light, which is ascribed to the photoisomerization of azobenzene moieties in the Azo-COF pores.

Abstract

Covalent organic frameworks (COFs) containing azobenzene building blocks carry great potential for use in intelligent storage, separation, chemical sensing, and catalysis due to their intriguing photo-responsiveness. However, azobenzene units are often exploited as the linkers to form the framework of COFs, thereby restricting their molecular motion and photoisomerization. Herein, a simple yet robust template-free solvothermal strategy is reported to yield azobenzene-dangled COFs (Azo-COFs) with their azobenzene moieties suspending within the pores. The crystallinity, specific surface area, and morphology of Azo-COFs can be conveniently tailored by changing the ratio of amine to aldehyde monomers. Notably, the Azo-COFs provide sufficient free space for the reversible trans-to-cis isomerization of the dangled azobenzene units inside the pores, thus reversibly regulating surface wettability of Azo-COFs. The adsorption capacity of Azo-COFs toward organic dye molecules is increased by 3.7-fold when irradiated with ultraviolet light, which can be ascribed to the intelligent closing/opening of molecular gates rendered by photoisomerization of azobenzene moieties. As such, the ability to photoregulate the adsorption of Azo-COFs highlights their significance in functioning as smart porous nanomaterials for applications in cargo release, molecular sieves, ion transport, energy conversion systems, and environmental remediation.

Atomic scale epitaxy enables realization of artificial lattice structures unattainable in nature. Particularly, artificial 4d and 5d perovskite oxide superlattices, in which the finite spin–orbit coupling gives rise to novel functionalities, frequently exhibiting correlated quantum phenomena with practical controllability. The review summarizes the versatile correlated quantum functionalities of ruthenate and iridate based oxide superlattices in terms of the growth, underlying physics, and promising applications.

Abstract

Unexpected, yet useful functionalities emerge when two or more materials merge coherently. Artificial oxide superlattices realize atomic and crystal structures that are not available in nature, thus providing controllable correlated quantum phenomena. This review focuses on 4d and 5d perovskite oxide superlattices, in which the spin–orbit coupling plays a significant role compared with conventional 3d oxide superlattices. Modulations in crystal structures with octahedral distortion, phonon engineering, electronic structures, spin orderings, and dimensionality control are discussed for 4d oxide superlattices. Atomic and magnetic structures, J _eff = 1/2 pseudospin and charge fluctuations, and the integration of topology and correlation are discussed for 5d oxide superlattices. This review provides insights into how correlated quantum phenomena arise from the deliberate design of superlattice structures that give birth to novel functionalities.

Taking layered perovskite oxide thin films (RP-SrX, X= 25, 50, 75) as the model system, the critical impact of oxygen activity modulation on the switch of OER mechanism and the enhancement of intrinsic electrocatalytic activity via the combination of advanced spectroscopic techniques and density functional theory calculations is demonstrated.

Abstract

Developing high-performance oxygen evolution reaction (OER) catalysts are critical for the practical application of many electrochemical energy devices. In this study, taking layered perovskite oxide thin films as the model system, it is demonstrated that the OER pathway can be effectively shifted by activating lattice oxygen, leading to strongly enhanced intrinsic activity. The OER performance of Ruddlesden-Popper (RP)-phase cobaltite is significantly enhanced as Sr doping at the A site increases, which is attributed to the shift of the reaction pathway from adsorbate evolution mechanism (AEM) to lattice oxygen-mediated mechanism (LOM). Advanced spectroscopic techniques and density functional theory calculations reveal that the Sr dopant effectively facilitates oxygen ligand hole formation, charge transfer from the oxygen sites, and the formation and migration of oxygen vacancy, hence promoting lattice oxygen to participate in surface reactions. The results provide critical insight into the role of oxygen activity and offer a potential way for constructing highly active electrocatalysts.

Nature Communications, Published online: 26 May 2023; doi:10.1038/s41467-023-38792-z

Insect-scale untethered micro aerial vehicles such as artificial dandelion devices suffer from high flight randomness and inadequate controllability. Chen et al. design and fabricate an untethered dandelion-inspired microflier, which is spatially and temporally controlled by an ultralight and supersensitive light-driven bimorph soft actuator.

A full-diffraction-based 4f-less optical pattern recognition (OPR) method is proposed using a single complex amplitude modulating metasurface in the THz band, which is valid for systems with large Fresnel numbers. Moreover, a laser-induced graphene technique is applied for processing the device. A 15 mm × 15 mm metasurface can be fabricated by one-step laser writing in 34 s.

Abstract

Optical pattern recognition (OPR) has the advantage of single intensity detection ability for low-cost terahertz (THz) systems of imaging or security checks. However, conventional 4f-system-based OPR is limited by the paraxial approximation and bulky device volumes for THz applications. Here, a full-diffraction-based 4f-less OPR method is proposed using a single complex-amplitude-modulating metasurface, which is valid for systems with large Fresnel numbers. Moreover, a laser-induced graphene technique is applied for processing the device. A 15 mm × 15 mm metasurface can be fabricated by one-step laser writing in 34 s, indicating the potential of the proposed method in developing THz OPR systems with miniaturization, fast fabrication, and low-cost.

2D Metal Oxides

In article number 2207774, Ye Zhou and co-workers summarize the recent advances on the synthesis of 2D metal oxides and their electronic applications. The tunable physical properties and advanced synthesis methods are discussed. Various roles of 2D metal oxides in widespread applications are presented. An outlook of existing challenges and future opportunities in 2D metal oxides is also proposed.

Exotic functionalities of transition metal oxides are appealing to multifunctional devices if integrated with low-dimensional materials on Si-based platforms. In this study, heterostructures of MoS₂ and magnetic Sr-doped LaMnO₃ are achieved on Si using a freestanding form of Sr-doped LaMnO₃. The multifunctionality of the heterostructures is demonstrated based on three applications, including field-effect transistors, photodiodes, and magnetoresponsive heterostructure devices.

Abstract

Correlated oxides and related heterostructures are intriguing for developing future multifunctional devices by exploiting their exotic properties, but their integration with other materials, especially on Si-based platforms, is challenging. Here, van der Waals heterostructures of La_0.7Sr_0.3MnO₃ (LSMO) , a correlated manganite perovskite, and MoS₂ are demonstrated on Si substrates with multiple functions. To overcome the problems due to the incompatible growth process, technologies involving freestanding LSMO membranes and van der Waals force-mediated transfer are used to fabricate the LSMO-MoS₂ heterostructures. The LSMO-MoS₂ heterostructures exhibit a gate-tunable rectifying behavior, based on which metal-semiconductor field-effect transistors (MESFETs) with on-off ratios of over 10⁴ can be achieved. The LSMO-MoS₂ heterostructures can function as photodiodes displaying considerable open-circuit voltages and photocurrents. In addition, the colossal magnetoresistance of LSMO endows the LSMO-MoS₂ heterostructures with an electrically tunable magnetoresponse at room temperature. This work not only proves the applicability of the LSMO-MoS₂ heterostructure devices on Si-based platform but also demonstrates a paradigm to create multifunctional heterostructures from materials with disparate properties.

12-nm layers of silver deposited on the commercial optical adhesive NOA63 serve as ultrasmooth, haze-free transparent electrodes for optoelectronics that exhibit high resilience to bending. The electrodes may be readily patterned by selectively etching the NOA63 substrate with an oxygen plasma prior to metal deposition, with the silver forming continuous, conducting regions above unetched NOA63 and fragmented, highly insulating regions above etched NOA63.

Abstract

Template-patterned, flexible transparent electrodes (TEs) formed from an ultrathin silver film on top of a commercial optical adhesive – Norland Optical Adhesive 63 (NOA63) – are reported. NOA63 is shown to be an effective base-layer for ultrathin silver films that advantageously prevents coalescence of vapor-deposited silver atoms into large, isolated islands (Volmer-Weber growth), and so aids the formation of ultrasmooth continuous films. 12 nm silver films on top of free-standing NOA63 combine high, haze-free visible-light transparency (T ≈ 60% at 550 nm) with low sheet-resistance (Rs${\mathcal{R}}_s$ ≈ 16 Ω sq⁻¹), and exhibit excellent resilience to bending, making them attractive candidates for flexible TEs. Etching the NOA63 base-layer with an oxygen plasma before silver deposition causes the silver to laterally segregate into isolated pillars, resulting in a much higher sheet resistance (Rs${\mathcal{R}}_{s}$ > 8 × 10⁶ Ω sq^-1) than silver grown on pristine NOA63 . Hence, by selectively etching NOA63 before metal deposition, insulating regions may be defined within an otherwise conducting silver film, resulting in a differentially conductive film that can serve as a patterned TE for flexible devices. Transmittance may be increased (to 79% at 550 nm) by depositing an antireflective layer of Al₂O₃ on the Ag layer at the cost of reduced flexibility.

In this work, high bias-stress stability p-type GaSb nanowire (NW) field-effectr-transistors (FETs) are successfully constructed by configuring solution-processed oxide dielectric shell on the surface of GaSb NWs. Furthermore, benefiting from the excellent bias-stress stability, the as-constructed GaSb NWFETs demonstrate desirable stability and gate-controlled photodetection behaviors, along with excellent gate-controlled near-infrared photodetection imaging and photocommunication ability.

Abstract

The bias-stress instability of nanowires (NWs) field-effect-transistors (FETs), originated from the surface trappings, are challenging greatly the functionalization of III-V group semiconductors in next-generation electronics and optoelectronics. In this study, the solution-processed high-κ oxide dielectric shell is configured uniformly onto the surface of GaSb NWs, contributing to the excellent bias-stress stability of as-constructed p-type NWFETs. Owing to the interdiffusion between Al and Ga, the oxide dielectric shell is Ga-AlO_x. With an optimal oxide dielectric shell, the as-constructed p-type GaSb NWFETs show an insignificant attenuation of on-state current (within 10%) and a negligible negative shift of threshold voltage under 60 min continuous gate bias, which is far better than that of pristine GaSb NWFETs, resulting from the electric double layer effect. Benefiting from the excellent bias-stress stability, when configured into the near-infrared photodetector, NWFET exhibits desirable stability and gate-controlled photodetection behaviors. I_dark and I_light are effectively modulated by gate voltage, resulting in gate-controlled responsivity and gain under the illumination of 1550 nm laser. In the end, the as-constructed bias-stress stability NWFET demonstrates expected gate-controlled photodetection imaging and photocommunication ability. The strategy of solution-processed oxide dielectric shell promises high bias-stress stability NWFETs for gate-controlled photodetection and photocommunication.

A simple and robust strategy for fabricating dynamic hierarchical surface wrinkles is realized by the bilayer wrinkling system comprising the gelatin/polystyrene particles film and polydimethylsiloxane. Hierarchical surface wrinkles can be regulated by the different humidity sensitivity of the gelatin in the rigid exposed regions and the soft unexposed regions.

Abstract

Hierarchical stimuli-responsive surface pattern, which can realize the responsive surface with the dynamically tunable structures and on-demand properties, is the key to realize smart materials and devices, yet its fabrication remains challenging. This study presents a simple and robust fabrication strategy for creating a dynamic hierarchical surface wrinkle using a bilayer wrinkling system. This system consists of a hard and thin skin film made of gelatin containing polystyrene (PS) particles and a soft and thick substrate of polydimethylsiloxane. Based on the buckling deformation caused by stress instability in bilayer wrinkling system, the hierarchical surface wrinkles with random distribution of PS microparticles can be realized. By controlling the humidity in the environment and leveraging the different sensitivity of the exposed regions with high modulus and the soft unexposed regions, various dynamic hierarchical structures can be achieved. This wrinkled surface is a promising candidate for applications such as dynamic displays, optical smart windows, and anti-counterfeiting due to the strong light scattering effect of the surface wrinkles.

Two-dimensional Ruddlesden–Popper polycrystalline perovskite (BA)₂(MA)₃Pb₄I₁₃ film with excellent crystal orientation is fabricated by hot-casting deposition, and pyro-phototronic effect is proposed in such (BA)₂(MA)₃Pb₄I₁₃ photodetectors. The pyro-phototronic effect can increase the energy conversion efficiency and greatly improve the photodetector performance via coupling multiple energies.

Abstract

Two-dimensional (2D) Ruddlesden–Popper (RP) layered halide perovskite has attracted wide attentions due to its unique structure and excellent optoelectronic properties. With inserting organic cations, inorganic octahedrons are forced to extend in a certain direction, resulting in an asymmetric 2D perovskite crystal structure and causing spontaneous polarization. The pyroelectric effect resulted from spontaneous polarization exhibits a broad prospect in the application of optoelectronic devices. Herein, 2D RP polycrystalline perovskite (BA)₂(MA)₃Pb₄I₁₃ film with excellent crystal orientation is fabricated by hot-casting deposition, and a class of 2D hybrid perovskite photodetectors (PDs) with pyro-phototronic effect is proposed, achieving temperature and light detection with greatly improved performance by coupling multiple energies. Because of the pyro-phototronic effect, the current is ≈35 times to that of the photovoltaic effect current under 0 V bias. The responsivity and detectivity are 12.7 mA W⁻¹ and 1.73 × 10¹¹ Jones, and the on/off ratio can reach 3.97 × 10³. Furthermore, the influences of bias voltage, light power density, and frequency on the pyro-phototronic effect of 2D RP polycrystalline perovskite PDs are explored. The coupling of spontaneous polarization and light facilitates photo-induced carrier dissociation and tunes the carrier transport process, making 2D RP perovskites a competitive candidate for next-generation photonic devices.

A thermoelectric alloy achieves high performance in electronic cooling

Surface facet plays an essential role in affecting the surface stability of layered cathodes. It is revealed that the oblique surface facets show higher stability than that of the perpendicular ones due to the geometrical effect and chemical passivation, which can be utilized to prevent the cycling induced surface degradation, improving the cycling stability of layered cathodes.

Abstract

High chemical and mechanical stability of cathode surface are the prerequisites enabling high-performance rechargeable battery. Surface facet is among the surface properties that dictate surface stability and cycling performance, while its underlying mechanism remains elusive. Herein, it is reported that surface stability is closely related to the surface facet for a variety of layered cathodes. The investigation shows that surface structure of P2 layered cathode undergoes sequential transformation upon cycling, which results in severe surface degradation. This study finds that the surface facets perpendicular to the (002) planes experience severe cracking and corrosion, while other surface facets are much more stable. The surface stability difference mainly comes from a geometric effect on strain release, which determines the mechanical stability of surface. Chemically, transition metal condensation forms a passivation layer to effectively prevent the inward propagation of surface degradation. Therefore, the surface facets oblique to the layered-planes are intrinsically more resistant to mechanical cracking and chemical corrosion, which is further verified as a common effect in several O3-type layered cathodes. This work not only deepens the understanding of the mechanism how surface facet affects surface stability, but also validates surface facet regulation can be a promising strategy for optimizing battery materials.

Nature, Published online: 24 May 2023; doi:10.1038/s41586-023-05925-9

The authors introduce a single-molecule DNA-barcoding method, resolution enhancement by sequential imaging, that improves the resolution of fluorescence microscopy down to the Ångström scale using off-the-shelf fluorescence microscopy hardware and reagents.

A flexible dielectric capacitor is inkjet printed based on all-aqueous functional inks including conductive carbon nanotube inks and dielectric polyvinylidene fluoride latex and boron nitride inks. The origin ink formulations coupled with printed heterostructures allows for a high energy storage density, which is superior to most of the state-of-the-art dielectrics printed from solvent-based formulations.

Abstract

Due to the low energy density of commercial printable dielectrics, printed capacitors occupy a significant printing area and weight in printed electronics. It has long remained challenging to develop novel dielectric materials with printability and high-energy storage density. Herein, a novel strategy for inkjet printing of all aqueous colloidal inks to dielectric capacitors composed of carbon nanotube electrodes and polyvinylidene fluoride (PVDF)-based dielectrics is presented. The formulated dielectric ink is composed of negatively charged PVDF latex nanoparticles complexed with cationic chitosan molecules. Beyond the isoelectric point, the PVDF@Chitosan particles demonstrate excellent printability and film-forming properties. Chitosan serves as a strong binder to improve the printed film quality yet it introduces charged species. To mitigate the transport of mobile charges, the printed PVDF@Chitosan film is interlayered with a layer of boron nitride nanosheets. This layer is perpendicular to the electric field and serves as an efficient barrier to block the transport and the avalanche of charges, eventually leading to a recoverable energy density of 15 J cm⁻³ at 610 MV m⁻¹. This energy density represents the highest value among the waterborne dielectrics. It is also superior to most of the state-of-the-art dielectric materials printed from solvent-based formulations.