Tunable and Non-Invasive Printing of Transmissive Interference Colors with 2D Material Inks.

Interference colors hold significant importance in optics and arts. Current methods for printing interference colors entail complex procedures and large-scale printing systems for the scarcity of inks that exhibit both sensitivity and tunability to external fields. The production of highly transparent inks capable of rendering transmissive colors has presented ongoing challenges. Here, a type of paramagnetic ink based on 2D materials that exhibit polychrome in one magnetic field is invented. By precisely manipulating the doping ratio of magnetic elements within titanate nanosheets, the magneto-optical sensitivity named Cotton-Mouton coefficient is engineerable from 728 to a record high value of 3272 m-1 T-2, with negligible influence on its intrinsic wide optical bandgap. Combined with the sensitive and controllable magneto-responsiveness of the ink, modulate and non-invasively print transmissive interference colors using small permanent magnets are precised. This work paves the way for preparing transmissive interference colors in an energy-saving and damage-free manner, which can expand its use in widespread areas.

Collective Behavior Induced Highly Sensitive Magneto-Optic Effect in 2D Inorganic Liquid Crystals.

Collective behavior widely exists in nature, ranging from the macroscopic cloud of swallows to the microscopic cloud of colloidal particles. The behavior of an individual inside the collective is distinctive from its behavior alone, as it follows its neighbors. The introduction of such collective behavior in two-dimensional (2D) materials may offer new degrees of freedom to achieve desired but unattained properties. Here, we report a highly sensitive magneto-optic effect and transmissive magneto-coloration via introduction of collective behavior into magnetic 2D material dispersions. The increase of ionic strength in the dispersion enhances the collective behavior of colloidal particles, giving rise to a magneto-optic Cotton-Mouton coefficient up to 2700 T-2 m-1 which is the highest value obtained so far, being 3 orders of magnitude larger than other known transparent media. We also reveal linear dependence of magneto-coloration on the concentration and hydration ratios of ions. Such linear dependence and the extremely large Cotton-Mouton coefficient cooperatively allow fabrication of giant magneto-birefringent devices for color-centered visual sensing.

High-efficiency inverted polymer solar cells controlled by the thickness of polyethylenimine ethoxylated (PEIE) interfacial layers.

In this work, we investigate the effect of the thickness of the polyethylenimine ethoxylated (PEIE) interface layer on the performance of two types of polymer solar cells based on inverted poly(3-hexylthiophene) (P3HT):phenyl C61-butryric acid methyl ester (PCBM) and thieno[3,4-b]thiophene/benzodithiophene (PTB7):[6,6]-phenyl C71-butyric acid methyl ester (PC71BM). Maximum power conversion efficiencies of 4.18% and 7.40% were achieved at a 5.02 nm thick PEIE interface layer, for the above-mentioned solar cell types, respectively. The optimized PEIE layer provides a strong enough dipole for the best charge collection while maintaining charge tunneling ability. Optical transmittance and atomic force microscopy measurements indicate that all PEIE films have the same high transmittance and smooth surface morphology, ruling out the influence of the PEIE layer on these two parameters. The measured external quantum efficiencies for the devices with thick PEIE layers are quite similar to those of the optimized devices, indicating the poor charge collection ability of thick PEIE layers. The relatively low performance of devices with a PEIE layer of thickness less than 5 nm is the result of a weak dipole and partial coverage of the PEIE layer on ITO.

On-demand engineerable visible spectrum by fine control of electrochemical reactions.

Tunability of optical performance is one of the key technologies for adaptive optoelectronic applications, such as camouflage clothing, displays, and infrared shielding. High-precision spectral tunability is of great importance for some special applications with on-demand adaptability but remains challenging. Here we demonstrate a galvanostatic control strategy to achieve this goal, relying on the finding of the quantitative correlation between optical properties and electrochemical reactions within materials. An electrochromic electro-optical efficiency index is established to optically fingerprint and precisely identify electrochemical redox reactions in the electrochromic device. Consequently, the charge-transfer process during galvanostatic electrochemical reaction can be quantitatively regulated, permitting precise control over the final optical performance and on-demand adaptability of electrochromic devices as evidenced by an ultralow deviation of <3.0%. These findings not only provide opportunities for future adaptive optoelectronic applications with strict demand on precise spectral tunability but also will promote in situ quantitative research in a wide range of spectroelectrochemistry, electrochemical energy storage, electrocatalysis, and material chemistry.

An Electro-Optical Kerr Device Based on 2D Boron Nitride Liquid Crystals for Solar-Blind Communications.

Achieving light modulation in the spectral range of 200-280 nm is a prerequisite for solar-blind ultraviolet communication, where current technologies are mainly based on the electro-luminescent self-modulation of the ultraviolet source. External light modulation through the electro-birefringence control of liquid crystal (LC) devices has shown success in the visible-to-infrared regions. However, the poor stability of conventional LCs against ultraviolet irradiation and their weak electro-optical response make it challenging to modulate ultraviolet light. Here, an external ultraviolet light modulator is demonstrated using two-dimensional boron nitride LC. It exhibits robust ultraviolet stability and a record-high specific electro-optical Kerr coefficient of 5.1 × 10⁻2 m V-2, being three orders of magnitude higher than those of other known electro-optical media that are transparent (or potentially transparent) in the ultraviolent spectral range. The sensitive response enables fabricating transmissive and stable ultraviolet-C electro-optical Kerr modulators for solar-blind ultraviolet light. An M-ary coding array with high transmission density is also demonstrated for solar-blind ultraviolet communication.

An inorganic liquid crystalline dispersion with 2D ferroelectric moieties.

Electro-optical effect-based liquid crystal devices have been extensively used in optical modulation techniques, in which the Kerr coefficient reflects the sensitivity of the liquid crystals and determines the strength of the device's operational electric field. The Peterlin-Stuart theory and the O'Konski model jointly indicate that a giant Kerr coefficient could be obtained in a material with both a large geometrical anisotropy and an intrinsic polarization, but such a material is not yet reported. Here we reveal a ferroelectric effect in a monolayer two-dimensional mineral vermiculite. A large geometrical anisotropy factor and a large inherent electric dipole together raise the record value of Kerr coefficient by an order of magnitude, till 3.0 × 10-4 m V-2. This finding enables an ultra-low operational electric field of 102-104 V m-1 and the fabrication of electro-optical devices with an inch-level electrode separation, which has not previously been practical. Because of its high ultraviolet stability (decay <1% under ultraviolet exposure for 1000 hours), large-scale production, and energy efficiency, prototypical displayable billboards have been fabricated for outdoor interactive scenes. This work provides new insights for both liquid crystal optics and two-dimensional ferroelectrics.

Electricity generated by upstream proton diffusion in two-dimensional nanochannels.

The movement of ions along the pressure-driven water flow in narrow channels, known as downstream ionic transport, has been observed since 1859 to induce a streaming potential and has enabled the creation of various hydrovoltaic devices. In contrast, here we demonstrate that proton movement opposing the water flow in two-dimensional nanochannels of MXene/poly(vinyl alcohol) films, termed upstream proton diffusion, can also generate electricity. The infiltrated water into the channel causes the dissociation of protons from functional groups on the channel surface, resulting in a high proton concentration inside the channel that drives the upstream proton diffusion. Combined with the particularly sluggish water diffusion in the channels, a small water droplet of 5 µl can generate a voltage of ~400 mV for over 330 min. Benefiting from the ultrathin and flexible nature of the film, a wearable device is built for collecting energy from human skin sweat.

Recent Advances for the Synthesis and Applications of 2-Dimensional Ternary Layered Materials.

Layered materials with unique structures and symmetries have attracted tremendous interest for constructing 2-dimensional (2D) structures. The weak interlayer interaction renders them to be readily isolated into various ultrathin nanosheets with exotic properties and diverse applications. In order to enrich the library of 2D materials, extensive progress has been made in the field of ternary layered materials. Consequently, many brand-new materials are derived, which greatly extend the members of 2D realm. In this review, we emphasize the recent progress made in synthesis and exploration of ternary layered materials. We first classify them in terms of stoichiometric ratio and summarize their difference in interlayer interaction, which is of great importance to produce corresponding 2D materials. The compositional and structural characteristics of resultant 2D ternary materials are then discussed so as to realize desired structures and properties. As a new family of 2D materials, we overview the layer-dependent properties and related applications in the fields of electronics, optoelectronics, and energy storage and conversion. The review finally provides a perspective for this rapidly developing field.

Coaxial Wet Spinning of Boron Nitride Nanosheet-Based Composite Fibers with Enhanced Thermal Conductivity and Mechanical Strength.

Hexagonal boron nitride nanosheets (BNNSs) exhibit remarkable thermal and dielectric properties. However, their self-assembly and alignment in macroscopic forms remain challenging due to the chemical inertness of boron nitride, thereby limiting their performance in applications such as thermal management. In this study, we present a coaxial wet spinning approach for the fabrication of BNNSs/polymer composite fibers with high nanosheet orientation. The composite fibers were prepared using a superacid-based solvent system and showed a layered structure comprising an aramid core and an aramid/BNNSs sheath. Notably, the coaxial fibers exhibited significantly higher BNNSs alignment compared to uniaxial aramid/BNNSs fibers, primarily due to the additional compressive forces exerted at the core-sheath interface during the hot drawing process. With a BNNSs loading of 60 wt%, the resulting coaxial fibers showed exceptional properties, including an ultrahigh Herman orientation parameter of 0.81, thermal conductivity of 17.2 W m-1 K-1, and tensile strength of 192.5 MPa. These results surpassed those of uniaxial fibers and previously reported BNNSs composite fibers, making them highly suitable for applications such as wearable thermal management textiles. Our findings present a promising strategy for fabricating high-performance composite fibers based on BNNSs.

Deep ultraviolet hydrogel based on 2D cobalt-doped titanate.

Birefringent optical elements that work in deep ultraviolet (DUV) region become increasingly important these years. However, most of the DUV optical elements have fixed birefringence which is hard to be tuned. Here, we invent a birefringence-tunable optical hydrogel with mechano-birefringence effect in the DUV region, based on two-dimensional (2D) low-cobalt-doped titanate. This 2D oxide material has an optical anisotropy factor of 1.5 × 10-11 C2 J-1 m-1, larger than maximum value obtained previously, leading to an extremely large specific magneto-optical Cotton-Mouton coefficient of 3.9 × 106 T-2 m-1. The extremely large coefficient enables the fabrication of birefringent hydrogel in a small magnetic field with an ultra-low concentration of 2D oxide material. The hydrogel can stably and continuously modulate 303 nm DUV light with large phase tunability by varying the strain (compression or stretching) from 0 to 50%. Our work opens the door to design and fabricate new proof-of-concept DUV birefringence-tunable element, as demonstrated by optical hydrogels capable of DUV modulation by mechanical stimuli.

A Malleable Composite Dough with Well-Dispersed and High-Content Boron Nitride Nanosheets.

Aggregation of two-dimensional (2D) nanosheet fillers in a polymer matrix is a prevalent problem when the filler loading is high, leading to degradation of physical and mechanical properties of the composite. To avoid aggregation, a low-weight fraction of the 2D material (<5 wt %) is usually used to fabricate the composite, limiting performance improvement. Here, we develop a mechanical interlocking strategy where well-dispersed high filling content (up to 20 wt %) of boron nitride nanosheets (BNNSs) can be incorporated into a polytetrafluoroethylene (PTFE) matrix, resulting in a malleable, easy-to-process and reusable BNNS/PTFE composite dough. Importantly, the well-dispersed BNNS fillers can be rearranged into a highly oriented direction due to the malleable nature of the dough. The resultant composite film has a high thermal conductivity (4408% increase), low dielectric constant/loss, and excellent mechanical properties (334%, 69%, 266%, and 302% increases for tensile modulus, strength, toughness, and elongation, respectively), making it suitable for thermal management applications in the high-frequency areas. The technique is useful for the large-scale production of other 2D material/polymer composites with a high filler content for different applications.

A multifunctional optoelectronic device based on 2D material with wide bandgap.

Low-dimensional materials exhibit unique quantum confinement effects and morphologies as a result of their nanoscale size in one or more dimensions, making them exhibit distinctive physical properties compared to bulk counterparts. Among all low-dimensional materials, due to their atomic level thickness, two-dimensional materials possess extremely large shape anisotropy and consequently are speculated to have large optically anisotropic absorption. In this work, we demonstrate an optoelectronic device based on the combination of two-dimensional material and carbon dot with wide bandgap. High-efficient luminescence of carbon dot and extremely large shape anisotropy (>1500) of two-dimensional material with the wide bandgap of >4 eV cooperatively endow the optoelectronic device with multi-functions of optically anisotropic blue-light emission, visible light modulation, wavelength-dependent ultraviolet-light detection as well as blue fluorescent film assemble. This research opens new avenues for constructing multi-function-integrated optoelectronic devices via the combination of nanomaterials with different dimensions.

Charge dynamics in solar cells with a blend of π-conjugated polymer-fullerene studied by transient photo-generated voltage.

The biphasic feature of transient photo-generated voltage (TPV) is investigated in organic solar cells (OSCs) with a blend active layer of poly(3-hexylthiophene) (P3HT) and phenyl C61 butyric acid methyl ester (PCBM). The positive and negative components in biphasic TPV are explained through PCBM only and P3HT only devices. The negative and positive components are ascribed to the dipole formation at the buried interface of P3HT/indium tin oxide (ITO) and PCBM/ITO respectively. Based on these findings, two fundamental phenomena are revealed as follows: (1) interfacial modification on the buried interface inverts the negative component in biphasic TPV to a positive component, which prevents the leakage current channel in the conventional OSC structure; and (2) the solvent chosen transforms the positive component in biphasic TPV into a negative signal, which blocks the leakage current channel in the inverted OSC structure. Consequently, the study of TPV polarity provides the justification of the interaction at the buried interface. Besides, the decay of TPV is found to be bi-exponential, which can be used as a tool to estimate the degree of charge balance in OSCs.

Magnetically tunable and stable deep-ultraviolet birefringent optics using two-dimensional hexagonal boron nitride.

Birefringence is a fundamental optical property that can induce phase retardation of polarized light. Tuning the birefringence of liquid crystals is a core technology for light manipulation in current applications in the visible and infrared spectral regions. Due to the strong absorption or instability of conventional liquid crystals in deep-ultraviolet light, tunable birefringence remains elusive in this region, notwithstanding its significance in diverse applications. Here we show a stable and birefringence-tunable deep-ultraviolet modulator based on two-dimensional hexagonal boron nitride. It has an extremely large optical anisotropy factor of 6.5 × 10-12 C2 J-1 m-1 that gives rise to a specific magneto-optical Cotton-Mouton coefficient of 8.0 × 106 T-2 m-1, which is about five orders of magnitude higher than other potential deep-ultraviolet-transparent media. The large coefficient, high stability (retention rate of 99.7% after 270 cycles) and wide bandgap of boron nitride collectively enable the fabrication of stable deep-ultraviolet modulators with magnetically tunable birefringence.

Angstrom-confined catalytic water purification within Co-TiOx laminar membrane nanochannels.

The freshwater scarcity and inadequate access to clean water globally have rallied tremendous efforts in developing robust technologies for water purification and decontamination, and heterogeneous catalysis is a highly-promising solution. Sub-nanometer-confined reaction is the ultimate frontier of catalytic chemistry, yet it is challenging to form the angstrom channels with distributed atomic catalytic centers within, and to match the internal mass transfer and the reactive species' lifetimes. Here, we resolve these issues by applying the concept of the angstrom-confined catalytic water contaminant degradation to achieve unprecedented reaction rates within 4.6 Å channels of two-dimensional laminate membrane assembled from monolayer cobalt-doped titanium oxide nanosheets. The demonstrated degradation rate constant of the target pollutant ranitidine (1.06 ms-1) is 5-7 orders of magnitude faster compared with the state-of-the-art, achieving the 100% degradation over 100 h continuous operation. This approach is also ~100% effective against diverse water contaminates with a retention time of <30 ms, and the strategy developed can be also extended to other two-dimensional material-assembled membranes. This work paves the way towards the generic angstrom-confined catalysis and unravels the importance of utilizing angstrom-confinement strategy in the design of efficient catalysts for water purification.

A 2D material-based transparent hydrogel with engineerable interference colours.

Transparent hydrogels are key materials for many applications, such as contact lens, imperceptible soft robotics and invisible wearable devices. Introducing large and engineerable optical anisotropy offers great prospect for endowing them with extra birefringence-based functions and exploiting their applications in see-through flexible polarization optics. However, existing transparent hydrogels suffer from limitation of low and/or non-fine engineerable birefringence. Here, we invent a transparent magneto-birefringence hydrogel with large and finely engineerable optical anisotropy. The large optical anisotropy factor of the embedded magnetic two-dimensional material gives rise to the large magneto-birefringence of the hydrogel in the transparent condition of ultra-low concentration, which is several orders of magnitude larger than usual transparent magnetic hydrogels. High transparency, large and tunable optical anisotropy cooperatively permit the magnetic patterning of interference colours in the hydrogel. The hydrogel also shows mechanochromic and thermochromic property. Our finding provides an entry point for applying hydrogel in optical anisotropy and colour centred fields, with several proof-of-concept applications been demonstrated.

2D Functional Minerals as Sustainable Materials for Magneto-Optics.

Liquid crystal devices using organic molecules are nowadays widely used to modulate transmitted light, but this technology still suffers from relatively weak response, high cost, toxicity and environmental concerns, and cannot fully meet the demand of future sustainable society. Here, an alternative approach to color-tunable optical devices, which is based on sustainable inorganic liquid crystals derived from 2D mineral materials abundant in nature, is described. The prototypical 2D mineral of vermiculite is massively produced by a green method, possessing size-to-thickness aspect ratios of >103 , in-plane magnetization of >10 emu g-1 , and an optical bandgap of >3 eV. These characteristics endow 2D vermiculite with sensitive magneto-birefringence response, been several orders of magnitude larger than organic counterparts, as well as capability of broad-spectrum modulation. The finding consequently permits the fabrication of various magnetochromic or mechanochromic devices with low or even zero-energy consumption during operation. This work creates opportunities for the application of sustainable materials in advanced optics.

Viscous Solvent-Assisted Planetary Ball Milling for the Scalable Production of Large Ultrathin Two-Dimensional Materials.

Ball milling is a widely used method to produce graphene and other two-dimensional (2D) materials for both industry and research. Conventional ball milling generates strong impact forces, producing small and thick nanosheets that limit their applications. In this study, a viscous solvent-assisted planetary ball milling method has been developed to produce large thin 2D nanosheets. The viscous solvent simultaneously increases the exfoliation energy (Ee) and lowers the impact energy (Ei). Simulations show a giant ratio of η = Ee/Ei, for the viscous solvent, 2 orders of magnitude larger than that of water. The method provides both a high exfoliation yield of 74%, a high aspect ratio of the generated nanosheets of 571, and a high quality for a representative 2D material of boron nitride nanosheets (BNNSs). The large thin BNNSs can be assembled into high-performance functional films, such as separation membranes and thermally conductive flexible films with some performance parameters better than those 2D nanosheets produced by chemical exfoliation methods.

Largely Tunable Magneto-Coloration of Monolayer 2D Materials via Size Tailoring.

Magnetically influenced light-matter interaction provides a contactless, noninvasive and power-free way for material characterization and light modulation. Shape anisotropy of active materials mainly determines the sensitivity of magneto-optic response, thereby making magnetic two-dimensional (2D) materials suitable in achieving the giant magneto-birefringence effect as discovered recently. Consequently, relationship between magneto-birefringence response and shape anisotropy of 2D materials is critical but has remained elusive, restricting its widespread applications. Here, we report the highly sensitive and largely tunable magneto-coloration via manipulating the shape-anisotropy of magnetic 2D materials. We reveal a quadratic increasing relationship between the magneto-optic Cotton-Mouton coefficient and the lateral size of 2D materials and achieve a more than one order of magnitude tunable response. This feature enables the engineerable transmissive magneto-coloration of 2D materials by tailoring their shape anisotropy. Our work deepens the understanding of the tunability of magneto-optic response by size effect of active materials, offering various opportunities for their applications in vast areas where color is concerned.

A Scalable Artificial Neuron Based on Ultrathin Two-Dimensional Titanium Oxide.

A spiking neural network consists of artificial synapses and neurons and may realize human-level intelligence. Unlike the widely reported artificial synapses, the fabrication of large-scale artificial neurons with good performance is still challenging due to the lack of a suitable material system and integration method. Here, we report an ultrathin (less than10 nm) and inch-size two-dimensional (2D) oxide-based artificial neuron system produced by a controllable assembly of solution-processed 2D monolayer TiOx nanosheets. Artificial neuron devices based on such 2D TiOx films show a high on/off ratio of 109 and a volatile resistance switching phenomenon. The devices can not only emulate the leaky integrate-and-fire activity but also self-recover without additional circuits for sensing and reset. Moreover, the artificial neuron arrays are fabricated and exhibited good uniformity, indicating their large-area integration potential. Our results offer a strategy for fabricating large-scale and ultrathin 2D material-based artificial neurons and 2D spiking neural networks.