Revealing Strong Flexoelectricity and Optoelectronic Coupling in 2D Ferroelectric CuInP2S6 Via Large Strain Gradient.

The interplay between flexoelectric and optoelectronic characteristics provides a paradigm for studying emerging phenomena in various 2D materials. However, an effective way to induce a large and tunable strain gradient in 2D devices remains to be exploited. Herein, we propose a strategy to induce large flexoelectric effect in 2D ferroelectric CuInP2S6 by constructing a 1D-2D mixed-dimensional heterostructure. The strong flexoelectric effect is induced by enormous strain gradient up to 4.2 × 106 m-1 resulting from the underlying ZnO nanowires, which is further confirmed by the asymmetric coercive field and the red-shift in the absorption edge. The induced flexoelectric polarization efficiently boosts the self-powered photodetection performance. In addition, the improved photoresponse has a good correlation with the induced strain gradient, showing a consistent size-dependent flexoelectric effect. The mechanism of flexoelectric and optoelectronic coupling is proposed based on the Landau-Ginzburg-Devonshire double-well model, supported by density functional theory (DFT) calculations. This work provides a brand-new method to induce a strong flexoelectric effect in 2D materials, which is not restricted to crystal symmetry and thus offers unprecedented opportunities for state-of-the-art 2D devices.

Exceptional Magnetocaloric Responses in a Gadolinium Silicate with Strongly Correlated Spin Disorder for Sub-Kelvin Magnetic Cooling.

The development of magnetocaloric materials with a significantly enhanced volumetric cooling capability is highly desirable for the application of adiabatic demagnetization refrigerators in confined spatial environments. Here, the thermodynamic characteristics of a magnetically frustrated spin-7/2 Gd9.33[SiO4]6O2 is presented, which exhibits strongly correlated spin disorder below ≈1.5 K. A quantitative model is proposed to describe the magnetization results by incorporating nearest-neighbor Heisenberg antiferromagnetic and dipolar interactions. Remarkably, the recorded magnetocaloric responses are unprecedentedly large and applicable below 1.0 K. It is proposed that the S = 7/2 spin liquids serve as versatile platforms for investigating high-performance magnetocaloric materials in the sub-kelvin regime, particularly those exhibiting a superior cooling power per unit volume.

Electron Transport Layer Engineering Induced Carrier Dynamics Optimization for Efficient Cd-Free Sb2 Se3 Thin-Film Solar Cells.

Antimony selenide (Sb2 Se3 ) is a highly promising photovoltaic material thanks to its outstanding optoelectronic properties, as well as its cost-effective and eco-friendly merits. However, toxic CdS is widely used as an electron transport layer (ETL) in efficient Sb2 Se3 solar cells, which largely limit their development toward market commercialization. Herein, an effective green Cd-free ETL of SnOx is introduced and deposited by atomic layer deposition method. Additionally, an important post-annealing treatment is designed to further optimize the functional layers and the heterojunction interface properties. Such engineering strategy can optimize SnOx ETL with higher nano-crystallinity, higher carrier density, and less defect groups, modify Sb2 Se3 /SnOx heterojunction with better interface performance and much desirable "spike-like" band alignment, and also improve the Sb2 Se3 light absorber layer quality with passivated bulk defects and prolonged carrier lifetime, and therefore to enhance carrier separation and transport while suppressing non-radiative recombination. Finally, the as-fabricated Cd-free Mo/Sb2 Se3 /SnOx /ITO/Ag thin-film solar cell exhibits a stimulating efficiency of 7.39%, contributing a record value for Cd-free substrate structured Sb2 Se3 solar cells reported to date. This work provides a viable strategy for developing and broadening practical applications of environmental-friendly Sb2 Se3 photovoltaic devices.

Design and Fabrication of Biomass Derived Black Carbon Modified g-C3 N4 /FeIn2 S4 Heterojunction as Highly Efficient Photocatalyst for Wastewater Treatment.

The environmental deterioration caused by dye wastewater discharge has received considerable attention in recent decades. One of the most promising approaches to addressing the aforementioned environmental issue is the development of photocatalysts with high solar energy consumption efficiency for the treatment of dye-contaminated water. In this study, a novel low-cost π-π biomass-derived black carbon modified g-C3 N4 coupled FeIn2 S4 composite (i.e., FeInS/BC-CN) photocatalyst is successfully designed and fabricated that reveals significantly improved photocatalytic performance for the degradation of Eosin Yellow (EY) dye in aqueous solution. Under dark and subsequent visible light irradiation, the amount optimized composite reveals 99% removal performance for EY dye, almost three-fold compared to that of the pristine FeInS and BC-CN counterparts. Further, it is confirmed by means of the electron spin resonance spectrometry, quenching experiments, and density functional theory (DFT) calculations, that the hydroxyl radicals (• OH) and superoxide radicals (• O2 - ) are the dominant oxidation species involved in the degradation process of EY dye. In addition, a systematic photocatalytic degradation route is proposed based on the resultant degradation intermediates detectedduring liquid chromatography tandem mass spectrometry (LC-MS/MS) analysis. This work provides an innovative idea for the development of advanced photocatalysts to mitigate water pollution.

Polarization enhanced photoresponse of InSe via 2D ferroelectric CuCrP2S6.

Two-dimensional CuCrP2S6 possesses significant potential for low-power non-volatile devices owing to its multiferroic properties. Nonetheless, comprehensive investigations regarding the modulation of CuCrP2S6 polarization for enhancing semiconductor photodetection capabilities and its potential applications in ferroelectric non-volatile devices are still relatively scarce. In this study, we present a novel, non-volatile, tunable photodetector engineered through the integration of a ferroelectric heterostructure comprising CuCrP2S6 and InSe. Our findings reveal that distinct ferroelectric polarization states of CuCrP2S6 exert varying modulation effects on the InSe photodetection performance. Notably, optimized results give a responsivity of 1839 A W-1 and a detectivity of 1.9 × 1012 Jones at a 300 nm wavelength, featuring a substantial 20.7-fold difference in responsivity between the two polarization states. This investigation underscores the immense potential of CuCrP2S6 in the development of non-volatile, multi-state optoelectronic devices.

Dynamical Behavior of Pure Spin Current in Organic Materials.

Growing concentration on the novel information processing technology and low-cost, flexible materials make the spintronics and organic materials appealing for the future interdisciplinary investigations. Organic spintronics, in this context, has arisen and witnessed great advances during the past two decades owing to the continuous innovative exploitation of the charge-contained spin polarized current. Albeit with such inspiring facts, charge-absent spin angular momentum flow, namely pure spin currents (PSCs) are less probed in organic functional solids. In this review, the past exploring journey of PSC phenomenon in organic materials are retrospected, including non-magnetic semiconductors and molecular magnets. Starting with the basic concepts and the generation mechanism for PSC, the representative experimental observations of PSC in the organic-based networks are subsequently demonstrated and summarized, by accompanying explicit discussion over the propagating mechanism of net spin itself in the organic media. Finally, future perspectives on PSC in organic materials are illustrated mainly from the material point of view, including single molecule magnets, complexes for the organic ligands framework as well as the lanthanide metal complexes, organic radicals, and the emerging 2D organic magnets.

Strong Magnetocaloric Coupling in Oxyorthosilicate with Dense Gd3+ Spins.

Searching for working refrigerant materials is the key element in the design of magnetic cooling devices. Herein, we report on the thermodynamic and magnetocaloric parameters of an X1 phase oxyorthosilicate, Gd2SiO5, by field-dependent static magnetization and specific heat measurements. An overall correlation strength of |J|S2 ≈ 3.4 K is derived via the mean-field estimate, with antiferromagnetic correlations between the ferromagnetically coupled Gd-Gd layers. The magnetic entropy change -ΔSm is quite impressive, reaches 0.40 J K-1 cm-3 (58.5 J K-1 kg-1) at T = 2.7 K, with the largest adiabatic temperature change Tad = 23.2 K for a field change of 8.9 T. At T = 20 K, the lattice entropy SL is small enough compared to the magnetic entropy Sm, Sm/SL = 21.3, which warrants its potential in 2 -20 K cryocoolers with both the Stirling and Carnot cycles. Though with relatively large exchange interactions, the layered A-type spin arrangement ultimately enhances the magnetocaloric coupling, raising the possibilities of designing magnetic refrigerants with a high ratio of cooling capacity to volume.

Nano-phononic metamaterials enable an anomalous enhancement in the interfacial thermal conductance of the GaN/AlN heterojunction.

Improving the interfacial thermal conductance (ITC) is very important for heat dissipation in microelectronic and optoelectronic devices. In this work, taking GaN-AlN contact as an example, we demonstrated a new mechanism to enhance the interfacial thermal conductance using nano-phononic metamaterials. First, how a superlattice affects the ITC is investigated, and it is found that with decreasing superlattice periodic length, the ITC first decreases and then increases, because of the coherent phonon interference effect. However, although constructing a superlattice is effective for tuning the ITC, it cannot enhance the ITC. We suggest that the ITC can be enhanced by 9% through constructing an interfacial nano phononic metamaterial, which is contributed by the additional phonon transport channels for high-frequency phonons with a wide incidence-angle range. These results not only establish a deep understanding of the fundamental physics of the interfacial thermal conductance, but also provide a robust and scalable mechanism, which provides a degree of freedom for efficient thermal management.

Electrical and magnetic anisotropies in van der Waals multiferroic CuCrP2S6.

Multiferroic materials have great potential in non-volatile devices for low-power and ultra-high density information storage, owing to their unique characteristic of coexisting ferroelectric and ferromagnetic orders. The effective manipulation of their intrinsic anisotropy makes it promising to control multiple degrees of the storage "medium". Here, we have discovered intriguing in-plane electrical and magnetic anisotropies in van der Waals (vdW) multiferroic CuCrP2S6. The uniaxial anisotropies of current rectifications, magnetic properties and magnon modes are demonstrated and manipulated by electric direction/polarity, temperature variation and magnetic field. More important, we have discovered the spin-flop transition corresponding to specific resonance modes, and determined the anisotropy parameters by consistent model fittings and theoretical calculations. Our work provides in-depth investigation and quantitative analysis of electrical and magnetic anisotropies with the same easy axis in vdW multiferroics, which will stimulate potential device applications of artificial bionic synapses, multi-terminal spintronic chips and magnetoelectric devices.

Recent Advances in Ferroelectric-Enhanced Low-Dimensional Optoelectronic Devices.

Ferroelectric (FE) materials, including BiFeO3 , P(VDF-TrFE), and CuInP2 S6 , are a type of dielectric material with a unique, spontaneous electric polarization that can be reversed by applying an external electric field. The combination of FE and low-dimensional materials produces synergies, sparking significant research interest in solar cells, photodetectors (PDs), nonvolatile memory, and so on. The fundamental aspects of FE materials, including the origin of FE polarization, extrinsic FE materials, and FE polarization quantification are first discussed. Next, the state-of-the-art of FE-based optoelectronic devices is focused. How FE materials affect the energy band of channel materials and how device structures influence PD performance are also summarized. Finally, the future directions of this rapidly growing field are discussed.

Recent progress of two-dimensional heterostructures for thermoelectric applications.

The rapid development of synthesis and fabrication techniques has opened up a research upsurge in two-dimensional (2D) material heterostructures, which have received extensive attention due to their superior physical and chemical properties. Currently, thermoelectric energy conversion is an effective means to deal with the energy crisis and increasingly serious environmental pollution. Therefore, an in-depth understanding of thermoelectric transport properties in 2D heterostructures is crucial for the development of micro-nano energy devices. In this review, the recent progress of 2D heterostructures for thermoelectric applications is summarized in detail. Firstly, we systematically introduce diverse theoretical simulations and experimental measurements of the thermoelectric properties of 2D heterostructures. Then, the thermoelectric applications and performance regulation of several common 2D materials, as well as in-plane heterostructures and van der Waals heterostructures, are also discussed. Finally, the challenges of improving the thermoelectric performance of 2D heterostructures materials are summarized, and related prospects are described.

Ferroelectric Tuning of ZnO Ultraviolet Photodetectors.

The ferroelectric field effect transistor (Fe-FET) is considered to be one of the most important low-power and high-performance devices. It is promising to combine a ferroelectric field effect with a photodetector to improve the photodetection performance. This study proposes a strategy for ZnO ultraviolet (UV) photodetectors regulated by a ferroelectric gate. The ZnO nanowire (NW) UV photodetector was tuned by a 2D CuInP2S6 (CIPS) ferroelectric gate, which decreased the dark current and enhanced the responsivity and detectivity to 2.40 × 104 A/W and 7.17 × 1011 Jones, respectively. This strategy was also applied to a ZnO film UV photodetector that was tuned by a P(VDF-TrFE) ferroelectric gate. Lower power consumption and higher performance can be enabled by ferroelectric tuning of ZnO ultraviolet photodetectors, providing new inspiration for the fabrication of high-performance photodetectors.

Light-Induced Selective Hydrogenation over PdAg Nanocages in Hollow MOF Microenvironment.

Selective hydrogenation with high efficiency under ambient conditions remains a long-standing challenge. Here, a yolk-shell nanostructured catalyst, PdAg@ZIF-8, featuring plasmonic PdAg nanocages encompassed by a metal-organic framework (MOF, namely, ZIF-8) shell, has been rationally fabricated. PdAg@ZIF-8 achieves selective (97.5%) hydrogenation of nitrostyrene to vinylaniline with complete conversion at ambient temperature under visible light irradiation. The photothermal effect of Ag, together with the substrate enrichment effect of the catalyst, improves the Pd activity. The near-field enhancement effect from plasmonic Ag and optimized Pd electronic state by Ag alloying promote selective adsorption of the -NO2 group and therefore catalytic selectivity. Remarkably, the unique yolk-shell nanostructure not only facilitates access to PdAg cores and protects them from aggregation but also benefits substrate enrichment and preferential -NO2 adsorption under light irradiation, the latter two of which surpass the core-shell counterpart, giving rise to enhanced activity, selectivity, and recyclability.

Cu3 (HHTP)2 c-MOF/ZnO Ultrafast Ultraviolet Photodetector for Wearable Optoelectronics.

Two-dimensional conductive metal-organic frameworks (2D c-MOFs) are a family of highly tunable and electrically conducting materials that can be utilized in optoelectronics. A major issue of 2D c-MOFs for photodetection is their poor charge separation and recombination dynamics upon illumination. This study demonstrates a Cu3 (HHTP)2 /ZnO type-II heterojunction ultraviolet (UV) photodetector fabricated by layer-by-layer (LbL) deposition, in which the charge separation of photogenerated carriers is enhanced. At optimized MOF layer cycles, the device achieves a responsivity of 78.2 A/W and detectivity of 3.8×109 Jones at 1 V. Particularly, the device can be operated in the self-powered mode with an ultrafast response time of 70 µs, which is the record value for MOF-based photodetectors. In addition, even after 1000-time bending of 180°, the flexible device maintains stable performance. This flexible MOF-based UV photodetector with anti-fatigue and anti-bending properties provides strong implication to wearable optoelectronics.

Progress on two-dimensional binary oxide materials.

Two-dimensional van der Waals (2D vdW) materials have attracted much attention because of their unique electronic and optical properties. Since the successful isolation of graphene in 2004, many interesting 2D materials have emerged, including elemental olefins (silicene, germanene, etc.), transition metal chalcogenides, transition metal carbides (nitrides), hexagonal boron, etc. On the other hand, 2D binary oxide materials are an important group in the 2D family owing to their high structural diversity, low cost, high stability, and strong adjustability. This review systematically summarizes the research progress on 2D binary oxide materials. We discuss their composition and structure in terms of vdW and non-vdW categories in detail, followed by a discussion of their synthesis methods. In particular, we focus on strategies to tailor the properties of 2D oxides and their emerging applications in different fields. Finally, the challenges and future developments of 2D binary oxides are provided.

High-performance polarization-sensitive photodetectors on two-dimensional ß-InSe.

Two-dimensional (2D) indium selenide (InSe) has been widely studied for application in transistors and photodetectors, which benefit from its excellent optoelectronic properties. Among the three specific polytypes (γ-, ϵ- and ß-phase) of InSe, only the crystal lattice of InSe in ß-phase (ß-InSe) belongs to a non-symmetry point group of [Formula: see text], which indicates stronger anisotropic transport behavior and potential in the polarized photodetection of ß-InSe-based optoelectronic devices. Therefore, we prepare the stable p-type 2D-layered ß-InSe via temperature gradient method. The anisotropic Raman, transport and photoresponse properties of ß-InSe have been experimentally and theoretically proven, showing that the ß-InSe-based device has a ratio of 3.76 for the maximum to minimum dark current at two orthogonal orientations and a high photocurrent anisotropic ratio of 0.70 at 1 V bias voltage, respectively. The appealing anisotropic properties demonstrated in this work clearly identify ß-InSe as a competitive candidate for filter-free polarization-sensitive photodetectors.

Correlated States in Strained Twisted Bilayer Graphenes Away from the Magic Angle.

Graphene moiré superlattice formed by rotating two graphene sheets can host strongly correlated and topological states when flat bands form at so-called magic angles. Here, we report that, for a twisting angle far away from the magic angle, the heterostrain induced during stacking heterostructures can also create flat bands. Combining a direct visualization of strain effect in twisted bilayer graphene moiré superlattices and transport measurements, features of correlated states appear at "non-magic" angles in twisted bilayer graphene under the heterostrain. Observing correlated states in these "non-standard" conditions can enrich the understanding of the possible origins of the correlated states and widen the freedom in tuning the moiré heterostructures and the scope of exploring the correlated physics in moiré superlattices.

The field-free Josephson diode in a van der Waals heterostructure.

The superconducting analogue to the semiconducting diode, the Josephson diode, has long been sought with multiple avenues to realization being proposed by theorists1-3. Showing magnetic-field-free, single-directional superconductivity with Josephson coupling, it would serve as the building block for next-generation superconducting circuit technology. Here we realized the Josephson diode by fabricating an inversion symmetry breaking van der Waals heterostructure of NbSe2/Nb3Br8/NbSe2. We demonstrate that even without a magnetic field, the junction can be superconducting with a positive current while being resistive with a negative current. The ΔIc behaviour (the difference between positive and negative critical currents) with magnetic field is symmetric and Josephson coupling is proved through the Fraunhofer pattern. Also, stable half-wave rectification of a square-wave excitation was achieved with a very low switching current density, high rectification ratio and high robustness. This non-reciprocal behaviour strongly violates the known Josephson relations and opens the door to discover new mechanisms and physical phenomena through integration of quantum materials with Josephson junctions, and provides new avenues for superconducting quantum devices.

Nonequilibrium Green's function method for phonon heat transport in quantum system.

Phonon heat transport property in quantum devices is of great interesting since it presents significant quantum behaviors. In the past few decades, great efforts have been devoted to establish the theoretical method for phonon heat transport simulation in nanostructures. However, modeling phonon heat transport from wavelike coherent regime to particlelike incoherent regime remains a challenging task. The widely adopted theoretical approach, such as molecular dynamics, semiclassical Boltzmann transport equation, captures quantum mechanical effects within different degrees of approximation. Among them, Non-equilibrium Green's function (NEGF) method has attracted wide attention, as its ability to perform full quantum simulation including many-body interactions. In this review, we summarized recent theoretical advances of phonon NEGF method and the applications on the numerical simulation for phonon heat transport in nanostructures. At last, the challenges of numerical simulation are discussed.

Stability and passivation of 2D group VA elemental materials: black phosphorus and beyond.

Since the successful isolation of graphene in 2004, two-dimensional (2D) materials have become one of the focuses in material science owing to their extraordinary physical and chemical properties. In particular, 2D group VA elemental materials exhibit fascinating thickness-dependent band structures. Unfortunately, the well-known instability issue hinders their fundamental researches and practical applications. In this review, we first discuss the degradation mechanism of black phosphorus (BP), a most studied group VA material. Next, we summarize the methods to enhance BP stability with the focus of multifunctional passivation. Finally, we briefly discuss the protection strategies of other emerging group VA materials in recent years. This review provides insight for the degradation mechanism and protecting strategy for 2D group VA elements materials, which will promote their potential applications in electronics, optoelectronics, and biomedicine.