Ultrafast Carrier Dynamics and Bandgap Renormalization in Layered PtSe2

Carrier interactions in 2D nanostructures are of central importance not only in condensed‐matter physics but also for a wide range of optoelectronic and photonic applications. Here, new insights into the behavior of photoinduced carriers in layered platinum diselenide (PtSe₂) through ultrafast time‐resolved pump–probe and nonlinear optical measurements are presented. The measurements reveal the temporal evolution of carrier relaxation, chemical potential and bandgap renormalization in PtSe₂. These results imply that few‐layer PtSe₂ has a semiconductor‐like carrier relaxation instead of a metal‐like one. The relaxation follows a triple‐exponential decay process and exhibits thickness‐dependent relaxation times. This occurs along with a band‐filling effect, which can be controlled based on the number of layers and may be applied in saturable absorption for generating ultrafast laser pulses. The findings may provide means to study many‐body physics in 2D materials as well as potentially leading to applications in the field of optoelectronics and ultrafast photonics.     

Phase‐Engineered PtSe2‐Layered Films by a Plasma‐Assisted Selenization Process toward All PtSe2‐Based Field Effect Transistor to Highly Sensitive,Flexible, and Wide‐Spectrum Photoresponse Photodetectors

The formation of PtSe₂‐layered films is reported in a large area by the direct plasma‐assisted selenization of Pt films at a low temperature, where temperatures, as low as 100 °C at the applied plasma power of 400 W can be achieved. As the thickness of the Pt film exceeds 5 nm, the PtSe₂‐layered film (five monolayers) exhibits a metallic behavior. A clear p‐type semiconducting behavior of the PtSe₂‐layered film (≈trilayers) is observed with the average field effective mobility of 0.7 cm² V^?1 s^?1 from back‐gated transistor measurements as the thickness of the Pt film reaches below 2.5 nm. A full PtSe₂ field effect transistor is demonstrated where the thinner PtSe₂, exhibiting a semiconducting behavior, is used as the channel material, and the thicker PtSe₂, exhibiting a metallic behavior, is used as an electrode, yielding an ohmic contact. Furthermore, photodetectors using a few PtSe₂‐layered films as an adsorption layer synthesized at the low temperature on a flexible substrate exhibit a wide range of absorption and photoresponse with the highest photocurrent of 9 µA under the laser wavelength of 408 nm. In addition, the device can maintain a high photoresponse under a large bending stress and 1000 bending cycles.     

Ultrathin Two‐Dimensional Multinary Layered Metal Chalcogenide Nanomaterials

Ultrathin two‐dimensional (2D) layered transition metal dichalcogenides (TMDs), such as MoS₂, WS₂, TiS₂, TaS₂, ReS₂, MoSe₂ and WSe₂, have attracted considerable attention over the past six years owing to their unique properties and great potential in a wide range of applications. Aiming to achieve tunable properties and optimal application performances, great effort is devoted to the exploration of 2D multinary layered metal chalcogenide nanomaterials, which include ternary metal chalcogenides with well‐defined crystal structures, alloyed TMDs, heteroatom‐doped TMDs and 2D metal chalcogenide heteronanostructures. These novel 2D multinary layered metal chalcogenide nanomaterials exhibit some unique properties compared to 2D binary TMD counterparts, thus holding great promise in various potential applications including electronics/optoelectronics, catalysis, sensors, biomedicine, and energy storage and conversion with enhanced performances. This article focuses on the state‐of‐art progress on the preparation, characterization and applications of ultrathin 2D multinary layered metal chalcogenide nanomaterials.     

Graphitic Carbon Nitride Materials: Sensing,Imaging and Therapy

Graphitic carbon nitrides (g‐C₃N₄) are a class of 2D polymeric materials mainly composed of carbon and nitrogen atoms. g‐C₃N₄ are attracting dramatically increasing interest in the areas of sensing, imaging, and therapy, due to their unique optical and electronic properties. Here, the luminescent properties (mainly includes photoluminescence and electrochemiluminescence), and catalytic and photoelectronic properties related to sensing and therapy applications of g‐C₃N₄ materials are reviewed. Furthermore, the fabrication and advantages of sensing, imaging and therapy systems based on g‐C₃N₄ materials are summarized. Finally, the future perspectives for developing the sensing, imaging and therapy applications of the g‐C₃N₄ materials are discussed.     

The Langmuir‐Blodgett Approach to Making Colloidal Photonic Crystals from Silica Spheres

The area of colloidal photonic crystal research has attracted enormous attention in recent years as a result of the potential of such materials to provide the means of fabricating new or improved photonic devices. As an area where chemistry still predominates over engineering the field is still in its infancy in terms of finding real applications being limited by ease of fabrication, reproducibility and ‘quality’‐ for example the extent to which ordered structures may be prepared over large areas. It is our contention that the Langmuir‐Blodgett assembly method when applied to colloidal particles of silica and perhaps other materials, offers a way of overcoming these issues. To this end the assembly of silica and other particles into colloidal photonic crystals using the Langmuir‐Blodgett (LB) method is described and some of the numerous papers on this topic, which have been published, are reviewed. It is shown that the layer‐by‐layer control of photonic crystal growth afforded by the LB method allows for the fabrication of a range of novel, layered photonic crystals that may not be easily assembled using any other approach. Some of the more interesting of these structures, including so‐called heterostructured photonic crystals comprising of layers of spheres having different diameters are presented and their optical properties described. Finally, we offer our comments as to future applications of this interesting technology.     

C3N—A 2D Crystalline,Hole‐Free,Tunable‐Narrow‐Bandgap Semiconductor with Ferromagnetic Properties

Graphene has initiated intensive research efforts on 2D crystalline materials due to its extraordinary set of properties and the resulting host of possible applications. Here the authors report on the controllable large‐scale synthesis of C₃N, a 2D crystalline, hole‐free extension of graphene, its structural characterization, and some of its unique properties. C₃N is fabricated by polymerization of 2,3‐diaminophenazine. It consists of a 2D honeycomb lattice with a homogeneous distribution of nitrogen atoms, where both N and C atoms show a D_6h‐symmetry. C₃N is a semiconductor with an indirect bandgap of 0.39 eV that can be tuned to cover the entire visible range by fabrication of quantum dots with different diameters. Back‐gated field‐effect transistors made of single‐layer C₃N display an on–off current ratio reaching 5.5 × 10¹⁰. Surprisingly, C₃N exhibits a ferromagnetic order at low temperatures (<96 K) when doped with hydrogen. This new member of the graphene family opens the door for both fundamental basic research and possible future applications.     

Highly Confined and Tunable Hyperbolic Phonon Polaritons in Van Der Waals Semiconducting Transition Metal Oxides

2D van der Waals (vdW) layered polar crystals sustaining phonon polaritons (PhPs) have opened up new avenues for fundamental research and optoelectronic applications in the mid‐infrared to terahertz ranges. To date, 2D vdW crystals with PhPs are only experimentally demonstrated in hexagonal boron nitride (hBN) slabs. For optoelectronic and active photonic applications, semiconductors with tunable charges, finite conductivity, and moderate bandgaps are preferred. Here, PhPs are demonstrated with low loss and ultrahigh electromagnetic field confinements in semiconducting vdW α‐MoO₃. The α‐MoO₃ supports strong hyperbolic PhPs in the mid‐infrared range, with a damping rate as low as 0.08. The electromagnetic confinements can reach ≈λ₀/120, which can be tailored by altering the thicknesses of the α‐MoO₃ 2D flakes. Furthermore, spatial control over the PhPs is achieved with a metal‐ion‐intercalation strategy. The results demonstrate α‐MoO₃ as a new platform for studying hyperbolic PhPs with tunability, which enable switchable mid‐infrared nanophotonic devices.     

Flexible and High‐Performance All‐2D Photodetector for Wearable Devices

Emerging novel applications at the forefront of innovation horizon raise new requirements including good flexibility and unprecedented properties for the photoelectronic industry. On account of diversity in transport and photoelectric properties, 2D layered materials have proven as competent building blocks toward next‐generation photodetectors. Herein, an all‐2D Bi₂Te₃‐SnS‐Bi₂Te₃ photodetector is fabricated with pulsed‐laser deposition. It is sensitive to broadband wavelength from ultraviolet (370 nm) to near‐infrared (808 nm). In addition, it exhibits great durability to bend, with intact photoresponse after 100 bend cycles. Upon 370 nm illumination, it achieves a high responsivity of 115 A W^?1, a large external quantum efficiency of 3.9 × 10⁴%, and a superior detectivity of 4.1 × 10¹¹ Jones. They are among the best figures‐of‐merit of state‐of‐the‐art 2D photodetectors. The synergistic effect of SnS's strong light–matter interaction, efficient carrier separation of Bi₂Te₃–SnS interface, expedite carrier injection across Bi₂Te₃–SnS interface, and excellent carrier collection of Bi₂Te₃ topological insulator electrodes accounts for the superior photodetection properties. In summary, this work depicts a facile all‐in‐one fabrication strategy toward a Bi₂Te₃‐SnS‐Bi₂Te₃ photodetector. More importantly, it reveals a novel all‐2D concept for construction of flexible, broadband, and high‐performance photoelectronic devices by integrating 2D layered metallic electrodes and 2D layered semiconducting channels.     

New Generation Beta-Gallium Oxide Nanomaterials: Growth and Performances in Electronic Devices

In the last decade, beta-gallium oxide (β-Ga₂O₃) has been the subject of extensive research and has rapidly developed as a material for ultra-wide bandgap semiconductors. One-dimensional (1D) β-Ga₂O₃ nanostructures have advantages over bulk β-Ga₂O₃, including a high-specific surface area, sensitivity, and the quantum confinement effect. These advantages are favorable to developing various applications such as power electronics with improved heat dissipation effect, high detectivity photodetectors, and high sensitivity gas sensors. These nanostructures can be fabricated through top-down or bottom-up methods and have been utilized in various shapes, such as nanowires, nanobelts, nanorods, nanotubes, or networks, in various electronic devices. This review summarizes the recent developments in 1D β-Ga₂O₃ nanostructures, focusing on growth methodologies and mechanisms. In detail, the growth methodologies of 1D β-Ga₂O₃ are summarized based on four categories: vapor–liquid–solid, vapor–solid, solution–solid, and template mechanisms. Ten growth techniques regarding different fabrication mechanisms are reviewed and the corresponding applications such as gas sensors, UV photodetectors, resistive random access memories, and photocatalysts are summarized. This review provides material design strategies for developing next-generation optoelectronic or electronic products by summarizing the properties and fabrication methods of 1D β-Ga₂O₃.     

层状二硫化钼材料的制备和应用进展

二硫化钼(MoS2)是具有天然可调控带隙的二维层状材料,其独特的性质引起了科研人员的广泛关注,在微电子及光电领域具有重要的应用前景。介绍了MoS2的基本性质和常用制备方法,对层状MoS2材料在电子和光电子器件方面的应用进行了总结和展望。     

Large-Area Black Phosphorus/PtSe2 Schottky Junction for High Operating Temperature Broadband Photodetectors

High operating temperature (HOT) broadband photodetectors are urgently necessary for extreme condition applications in infrared-guided missiles, infrared night vision, fire safety imaging, and space exploration sensing. However, conventional photodetectors show dramatic carrier mobility decreases and carrier losses with low photoresponsivity at HOT due to the increased carrier scattering in channels at high temperatures. Herein, the HOT broadband photodetectors from room temperature to 470 K are developed for the first time by large-area black phosphorus (BP)/PtSe₂ films device arrays via a depletion-enhanced photocarrier dynamics strategy. Attributed to the 2D Schottky junction at BP/PtSe₂ interface and resulting in full depleted working channels, the BP/PtSe₂ photodetector arrays exhibit high tolerance to carrier mobility decrease during the increasing operating temperature in a wide wavelength range from 532 to 2200 nm. Thus, the photodetector shows a state-of-the-art operating temperature at 470 K with the photo-responsivity (R) and specific detectivity (D*) of 25 A W⁻¹ and 6.4 × 10¹¹ Jones under 1850 nm illumination, respectively. Moreover, BP/PtSe₂ photodetector arrays show high-uniformity photo-response in a large area. This work provides new strategies for high-performance broadband photodetector arrays with HOT by Schottky junction of large-area BP/PtSe₂ films.     

SnSe2 Nanosheets for Subpicosecond Harmonic Mode‐Locked Pulse Generation

Tin diselenide (SnSe₂) nanosheets as novel 2D layered materials have excellent optical properties with many promising application prospects, such as photoelectric detectors, nonlinear optics, infrared photoelectric devices, and ultrafast photonics. Among them, ultrafast photonics has attracted much attention due to its enormous advantages; for instance, extremely fast pulse, strong peak power, and narrow bandwidth. In this work, SnSe₂ nanosheets are fabricated by using solvothermal treatment, and the characteristics of SnSe₂ are systemically investigated. In addition, the solution of SnSe₂ nanosheets is successfully prepared as a fiber‐based saturable absorber by utilizing the evanescent field effect, which can bear a high pump power. 31st‐order subpicosecond harmonic mode locking is generated in an Er‐doped fiber laser, corresponding to the maximum repetition rate of 257.3 MHz and pulse duration of 887 fs. The results show that SnSe₂ can be used as an excellent nonlinear photonic device in many fields, such as frequency comb, lasers, photodetectors, etc.     

Highly Efficient Ionic Photocurrent Generation through WS2‐Based 2D Nanofluidic Channels

The unique feature of nacre‐like 2D layered materials provides a facile, yet highly efficient way to modulate the transmembrane ion transport from two orthogonal transport directions, either vertical or horizontal. Recently, light‐driven active transport of ionic species in synthetic nanofluidic systems attracts broad research interest. Herein, taking advantage of the photoelectric semiconducting properties of 2D transition metal dichalcogenides, the generation of a directional and greatly enhanced cationic flow through WS₂‐based 2D nanofluidic membranes upon asymmetric visible light illumination is reported. Compared with graphene‐based materials, the magnitude of the ionic photocurrent can be enhanced by tens of times, and its photo‐responsiveness can be 2–3.5 times faster. This enhancement is explained by the coexistence of semiconducting and metallic WS₂ nanosheets in the hybrid membrane that facilitates the asymmetric diffusion of photoexcited charge carriers on the channel wall, and the high ionic conductance due to the neat membrane structure. To further demonstrate its application, photonic ion switches, photonic ion diodes, and photonic ion transistors as the fundamental elements for light‐controlled nanofluidic circuits are further developed. Exploring new possibilities in the family of liquid processable colloidal 2D materials provides a way toward high‐performance light‐harvesting nanofluidic systems for artificial photosynthesis and sunlight‐driven desalination.     

Inkjet‐Printed Nanocavities on a Photonic Crystal Template

The last decade has witnessed the rapid development of inkjet printing as an attractive bottom‐up microfabrication technology due to its simplicity and potentially low cost. The wealth of printable materials has been key to its widespread adoption in organic optoelectronics and biotechnology. However, its implementation in nanophotonics has so far been limited by the coarse resolution of conventional inkjet‐printing methods. In addition, the low refractive index of organic materials prevents the use of “soft‐photonics” in applications where strong light confinement is required. This study introduces a hybrid approach for creating and fine tuning high‐Q nanocavities, involving the local deposition of an organic ink on the surface of an inorganic 2D photonic crystal template using a commercially available high‐resolution inkjet printer. The controllability of this approach is demonstrated by tuning the resonance of the printed nanocavities by the number of printer passes and by the fabrication of photonic crystal molecules with controllable splitting. The versatility of this method is evidenced by the realization of nanocavities obtained by surface deposition on a blank photonic crystal. A new method for a free‐form, high‐density, material‐independent, and high‐throughput fabrication technique is thus established with a manifold of opportunities in photonic applications.     

Multifunctional Photonic Nanomaterials for Diagnostic,Therapeutic, and Theranostic Applications

The last decade has seen dramatic progress in the principle, design, and fabrication of photonic nanomaterials with various optical properties and functionalities. Light‐emitting and light‐responsive nanomaterials, such as semiconductor quantum dots, plasmonic metal nanoparticles, organic carbon, and polymeric nanomaterials, offer promising approaches to low‐cost and effective diagnostic, therapeutic, and theranostic applications. Reasonable endeavors have begun to translate some of the promising photonic nanomaterials to the clinic. Here, current research on the state‐of‐the‐art and emerging photonic nanomaterials for diverse biomedical applications is reviewed, and the remaining challenges and future perspectives are discussed.     

Stabilizing the MXenes by Carbon Nanoplating for Developing Hierarchical Nanohybrids with Efficient Lithium Storage and Hydrogen Evolution Capability

The MXenes combining hydrophilic surface, metallic conductivity and rich surface chemistries represent a new family of 2D materials with widespread applications. However, their poor oxygen resistance causes a great loss of electronic properties and surface reactivity, which significantly inhibits the fabrication, the understanding of the chemical nature and full exploitation of the potential of MXene‐based materials. Herein we report a facile carbon nanoplating strategy for efficiently stabilizing the MXenes against structural degradation caused by spontaneous oxidation, which provides a material platform for developing MXene‐based materials with attractive structure and properties. Hierarchical MoS₂/Ti₃C₂‐MXene@C nanohybrids with excellent structural stability, electrical properties and strong interfacial coupling are fabricated by assembling carbon coated few‐layered MoS₂ nanoplates on carbon‐stabilized Ti₃C₂ MXene, exhibiting exceptional performance for Li storage and hydrogen evolution reaction (HER). Remarkably, ultra‐long cycle life of 3000 cycles with high capacities but extremely slow capacity loss of 0.0016% per cycle is achieved for Li storage at a very high rate of 20 A g^?1. They are also highly active HER electrocatalyst with very positive onset potential, low overpotential and long‐term stability in acidic solution. Superb properties highlight the great promise of MXene‐based materials in cornerstone applications of energy storage and conversion.     

A Novel Hybrid‐Layered Organic Phototransistor Enables Efficient Intermolecular Charge Transfer and Carrier Transport for Ultrasensitive Photodetection

The interfacial charge effect is crucial for high‐sensitivity organic phototransistors (OPTs), but conventional layered and hybrid OPTs have a trade‐off in balancing the separation, transport, and recombination of photogenerated charges, consequently impacting the device performance. Herein, a novel hybrid‐layered phototransistor (HL‐OPT) is reported with significantly improved photodetection performance, which takes advantages of both the charge‐trapping effect (CTE) and efficient carrier transport. The HL‐OPT consisting of 2,7‐dioctyl[1]benzothieno[3,2‐b][1]benzothiophene (C8‐BTBT) as conduction channel, C8‐BTBT:[6,6]‐phenyl‐C₆₁‐butyric acid methyl ester (PC₆₁BM) bulk heterojunction as photoactive layer, and sandwiched MoO₃ interlayer as a charge‐transport interlayer exhibits outstanding photodetection characteristics such as a photosensitivity (I_light/I_dark) of 2.9 × 10⁶, photoresponsivity (R) of 8.6 × 10³ A W^?1, detectivity (D*) of 3.4 × 10¹⁴ Jones, and external quantum efficiency of 3 × 10⁶% under weak light illumination of 32 µW cm^?2. The mechanism and strategy described here provide new insights into the design and optimization of high‐performance OPTs spanning the ultraviolet and near infrared (NIR) range as well as fundamental issues pertaining to the electronic and photonic properties of the devices.     

Structural and Functional Diversity in Lead‐Free Halide Perovskite Materials

Lead halide perovskites have emerged as promising semiconducting materials for different applications owing to their superior optoelectronic properties. Although the community holds different views toward the toxic lead in these high‐performance perovskites, it is certainly preferred to replace lead with nontoxic, or at least less‐toxic, elements while maintaining the superior properties. Here, the design rules for lead‐free perovskite materials with structural dimensions from 3D to 0D are presented. Recent progress in lead‐free halide perovskites is reviewed, and the relationships between the structures and fundamental properties are summarized, including optical, electric, and magnetic‐related properties. 3D perovskites, especially A₂B⁺B³⁺X₆‐type double perovskites, demonstrate very promising optoelectronic prospects, while low‐dimensional perovskites show rich structural diversity, resulting in abundant properties for optical, electric, magnetic, and multifunctional applications. Furthermore, based on these structure–property relationships, strategies for multifunctional perovskite design are proposed. The challenges and future directions of lead‐free perovskite applications are also highlighted, with emphasis on materials development and device fabrication. The research on lead‐free halide perovskites at Linköping University has benefited from inspirational discussions with Prof. Olle Inganäs.     

Striated 2D Lattice with Sub‐nm 1D Etch Channels by Controlled Thermally Induced Phase Transformations of PdSe2

2D crystals are typically uniform and periodic in‐plane with stacked sheet‐like structure in the out‐of‐plane direction. Breaking the in‐plane 2D symmetry by creating unique lattice structures offers anisotropic electronic and optical responses that have potential in nanoelectronics. However, creating nanoscale‐modulated anisotropic 2D lattices is challenging and is mostly done using top‐down lithographic methods with ≈10 nm resolution. A phase transformation mechanism for creating 2D striated lattice systems is revealed, where controlled thermal annealing induces Se loss in few‐layered PdSe₂ and leads to 1D sub‐nm etched channels in Pd₂Se₃ bilayers. These striated 2D crystals cannot be described by a typical unit cells of 1–2 Å for crystals, but rather long range nanoscale periodicity in each three directions. The 1D channels give rise to localized conduction states, which have no bulk layered counterpart or monolayer form. These results show how the known family of 2D crystals can be extended beyond those that exist as bulk layered van der Waals crystals by exploiting phase transformations by elemental depletion in binary systems.