Although two-dimensional (2D) materials have attracted considerable research interest for use in the development of innovative wearable optoelectronic systems, the integrated optoelectronic performance of 2D materials photodetectors, including flexibility, transparency, broadband response and stability in air, remains quite low to date. Here, we demonstrate a flexible, transparent, high-stability and ultra-broadband photodetector made using large-area and highly-crystalline WSe2 films that were prepared by pulsed-laser deposition (PLD). Benefiting from the 2D physics of WSe2 films, this device exhibits excellent average transparency of 72% in the visible range and superior photoresponse characteristics, including an ultra-broadband detection spectral range from 370 to 1064 nm, reversible photoresponsivity approaching 0.92 A W(-1), external quantum efficiency of up to 180% and a relatively fast response time of 0.9 s. The fabricated photodetector also demonstrates outstanding mechanical flexibility and durability in air. Also, because of the wide compatibility of the PLD-grown WSe2 film, we can fabricate various photodetectors on multiple flexible or rigid substrates, and all these devices will exhibit distinctive switching behavior and superior responsivity. These indicate a possible new strategy for the design and integration of flexible, transparent and broadband photodetectors based on large-area WSe2 films, with great potential for practical applications in the wearable optoelectronic devices.

The progress in the field of graphene has aroused a renaissance of keen research interest in layered transition metal dichalcogenides (TMDs). Tungsten disulfide (WS2), a typical TMD with favorable semiconducting band gap and strong light-matter interaction, exhibits great potential for highly-responsive photodetection. However, WS2-based photodetection is currently unsatisfactory due to the low optical absorption (2%-10%) and poor carrier mobility (0.01-0.91 cm(2) V(-1) s(-1)) of the thin WS2 layers grown by chemical vapor deposition (CVD). Here, we introduce pulsed-laser deposition (PLD) to prepare multilayered WS2 films. Large-area WS2 films of the magnitude of cm(2) are achieved. Comparative measurements of a WS2-based photoresistor demonstrate its stable broadband photoresponse from 370 to 1064 nm, the broadest range demonstrated in WS2 photodetectors. Benefiting from the large optical absorbance (40%-85%) and high carrier mobility (31 cm(2) V(-1) s(-1)), the responsivity of the device approaches a high value of 0.51 A W(-1) in an ambient environment. Such a performance far surpasses the CVD-grown WS2-based photodetectors (μA W(-1)). In a vacuum environment, the responsivity is further enhanced to 0.70 A W(-1) along with an external quantum efficiency of 137% and a photodetectivity of 2.7 × 10(9) cm Hz(1/2) W(-1). These findings stress that the PLD-grown WS2 film may constitute a new paradigm for the next-generation stable, broadband and highly-responsive photodetectors.

A facile pathway of the electrocatalytic nitrogen oxidation reaction (NOR) to nitrate is proposed, and Ru‐doped TiO2/RuO2 (abbreviated as Ru/TiO2) as a proof‐of‐concept catalyst is employed accordingly. Density functional theory (DFT) calculations suggest that Ruδ+ can function as the main active center for the NOR process. Remarkably doping Ru into the TiO2 lattice can induce an upshift of the d‐band center of the Ru site, resulting in enhanced activity for accelerating electrochemical conversion of inert N2 to active NO*. Overdoping of Ru ions will lead to the formation of additional RuO2 on the TiO2 surface, which provides oxygen evolution reaction (OER) active sites for promoting the redox transformation of the NO* intermediate to nitrate. However, too much RuO2 in the catalyst is detrimental to both the selectivity of the NOR and the Faradaic efficiency due to the dominant OER process. Experimentally, a considerable nitrate yield rate of 161.9 µmol h−1 gcat−1 (besides, a total nitrate yield of 47.9 µg during 50 h) and a highest nitrate Faradaic efficiency of 26.1% are achieved by the Ru/TiO2 catalyst (with the hybrid composition of RuxTiyO2 and extra RuO2 by 2.79 wt% Ru addition amount) in 0.1 m Na2SO4 electrolyte.

The oxygen evolution reaction (OER) is a key process involved in energy and environment‐related technologies. An ideal OER electrocatalyst should show high exposure of active sites and optimal adsorption energies of oxygenated species. However, earth‐abundant transition‐metal‐based OER electrocatalysts still operate with sluggish OER kinetics. Here, a cation‐exchange route is reported to fabricate cobalt‐vanadium‐iron (oxy)hydroxide (CoV‐Fe0.28) nanosheets with tunable binding energies for the oxygenated intermediates. The formation of an amorphous/crystalline heterostructure in the CoV‐Fe0.28 catalyst boosts the exposure of active sites compared to their crystalline and amorphous counterparts. Furthermore, the synergetic interaction of Co, V, and Fe cations in the CoV‐Fe0.28 catalyst subtly regulates the local coordination environment and electronic structure, resulting in the optimal thermodynamic barrier for this elementary reaction step. As a result, the CoV‐Fe0.28 catalyst exhibits superior electrocatalytic activity toward the OER. A low overpotential of 215 mV is required to afford a current density of 10 mA cm−2 with a small Tafel slope of 39.1 mV dec−1, which outperforms commercial RuO2 (321 mV and 86.2 mV dec−1, respectively).

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The successful peeling of graphene heralded the era of van der Waals material (vdWM) electronics. However, photodetectors based on semiconducting transition metal dichalcogenides (TMDs), formulated as MX2 (M = Mo, W; X = S, Se), often suffer either poor responsivity or long response time because of their high density of deep-level defect states (DLDSs). Alloy engineering, which can shift the DLDSs to shallow-level defect states, is proposed to be an efficient strategy to solve this problem. However, proof-of-concept is still lacking, which is probably because of the absence of a facile technology to grow high-quality alloyed TMDs. Here, we report the growth of large-scale and high-quality Mo0.5W0.5S2 alloy films via pulsed laser deposition (PLD). We demonstrate that the resulting Mo0.5W0.5S2 photodetector possesses a stable photoresponse from 370 to 1064 nm. The photocurrent exhibits positive dependence on both the source-drain voltage and incident power density, providing good tunability for multifunctional photoelectrical applications. We also establish that, because of the suppression of DLDSs with alloy engineering, the Mo0.5W0.5S2 photodetector achieves a good responsivity of 5.8 A/W and a response time shorter than 150 ms. The working mechanism for the suppression of DLDSs in Mo0.5W0.5S2 is unveiled by qualitatively analyzing the alloying-dressed band structure. In conclusion, the excellent performance of the PLD-grown Mo0.5W0.5S2 photodetector may pave the way for next-generation photodetection. The approach shown here represents a fundamental and universal scenario for the development of alloyed TMDs.

Nanoelectronics is in urgent demand of exceptional device architecture with ultrathin thickness below 10 nm and dangling‐bond‐free surface to break through current physical bottleneck and achieve new record of integration level. The advance in 2D van der Waals materials endows scientists with new accessibility. This study reports an all‐layered 2D Bi2Te3‐SnSe‐Bi2Te3 photodetector, and the broadband photoresponse of the device from ultraviolet (370 nm) to near‐infrared (808 nm) is demonstrated. In addition, the optimized responsivity reaches 5.5 A W−1, with the corresponding eternal quantum efficiency of 1833% and detectivity of 6 × 1010 cm Hz1/2 W−1. These figures‐of‐merits are among the best values of the reported all‐layered 2D photodetectors, which are several orders of magnitude higher than those of the previous SnSe photodetectors. The superior device performance is attributed to the synergy of highly conductive surface state of Bi2Te3 topological insulator, perfect band alignment between Bi2Te3 and SnSe as well as small interface potential fluctuation. Meanwhile, the all‐layered 2D device is further constructed onto flexible mica substrate and its photoresponse is maintained roughly unchanged upon 60 bending cycles. The findings represent a fundamental scenario for advancement of the next generation high performance and high integration level flexible optoelectronics.

Broadband photodetection is central to various technological applications including imaging, sensing and optical communications. On account of their Dirac-like surface state, Topological insulators (TIs) are theoretically predicted to be promising candidate materials for broadband photodetection from the infrared to the terahertz. Here, we report a vertically-constructed ultra-broadband photodetector based on a TI Bi2Te3-Si heterostructure. The device demonstrated room-temperature photodetection from the ultraviolet (370.6 nm) to terahertz (118 μm) with good reproducibility. Under bias conditions, the visible responsivity reaches ca. 1 A W(-1) and the response time is better than 100 ms. As a self-powered photodetector, it exhibits extremely high photosensitivity approaching 7.5 × 10(5) cm(2) W(-1), and decent detectivity as high as 2.5 × 10(11) cm Hz(1/2) W(-1). In addition, such a prototype device without any encapsulation suffers no obvious degradation after long-time exposure to air, high-energy UV illumination and acidic treatment. In summary, we demonstrate that TI-based heterostructures hold great promise for addressing the long lasting predicament of stable room-temperature high-performance broadband photodetectors.