Highly Sensitive and Ultra-Broadband VO2(B) Photodetector Dominated by Bolometric Effect.

In this study, Wadsley B phase vanadium oxide (VO2(B)) with broad-band photoabsorption ability, a large temperature coefficient of resistance (TCR), and low noise was developed for uncooled broad-band detection. By using a freestanding structure and reducing the size of active area, the VO2(B) photodetector shows stable and excellent performances in the visible to the terahertz region (405 nm to 0.88 mm), with a peak TCR of -4.77% K-1 at 40 °C, a peak specific detectivity of 6.02 × 109 Jones, and a photoresponse time of 83 ms. A terahertz imaging ability with 30 × 30 pixels was demonstrated. Scanning photocurrent imaging and real-time temperature-photocurrent measurements confirm that a photothermal-type bolometric effect is the dominating mechanism. The study shows the potential of VO2(B) in applications as a new type of uncooled broad-band photodetection material and the potential to further raise the performance of broad-band photodetectors by structural design.

Defect Etching of Phase-Transition-Assisted CVD-Grown 2H-MoTe2.

2D molybdenum ditelluride (MoTe2 ) with polymorphism is a promising candidate to developing phase-change memory, high-performance transistors and spintronic devices. The phase-transition-assisted chemical vapor deposition (CVD) process has been used to prepare large-scale 2H-MoTe2 with large grain size and low density of grain boundary. However, because of the lack of precise control of the growth condition, some defects including the amorphous regions and grain boundaries in 2H-MoTe2 are hardly avoidable. Here, a facile method of selectively etching defects in large-scale CVD-grown 2H-MoTe2 by triiodide ion (I3 - ) solution is reported. The defect etching is attributed to the reduced lattice symmetry, high chemisorption activity and high conductivity of the defects due to the high density of Te vacancies. The treated 2H-MoTe2 shows the suppressed hysteresis in the electrical transfer curve, enhances hole mobility and the higher effective barrier height on the metal contact, suggesting the decreased density of defects. Further chemical analysis indicates that the 2H-MoTe2 is not damaged or doped by I3 - solution during the etching process. This simple and low-cost post-processing method is effective for etching the defects in large-area 2H-MoTe2 for high-performance device applications.

A Robust Solid Electrolyte Interphase Layer Augments the Ion Storage Capacity of Bimetallic-Sulfide-Containing Potassium-Ion Batteries.

Metal-organic framework-derived NiCo2.5 S4 microrods wrapped in reduced graphene oxide (NCS@RGO) were synthesized for potassium-ion storage. Upon coordination with organic potassium salts, NCS@RGO exhibits an ultrahigh initial reversible specific capacity (602 mAh g-1 at 50 mA g-1 ) and ultralong cycle life (a reversible specific capacity of 495 mAh g-1 at 200 mA g-1 after 1 900 cycles over 314 days). Furthermore, the battery demonstrates a high initial Coulombic efficiency of 78 %, outperforming most sulfides reported previously. Advanced ex situ characterization techniques, including atomic force microscopy, were used for evaluation and the results indicate that the organic potassium salt-containing electrolyte helps to form thin and robust solid electrolyte interphase layers, which reduce the formation of byproducts during the potassiation-depotassiation process and enhance the mechanical stability of electrodes. The excellent conductivity of the RGO in the composites, and the robust interface between the electrodes and electrolytes, imbue the electrode with useful properties; including, ultrafast potassium-ion storage with a reversible specific capacity of 402 mAh g-1 even at 2 A g-1 .

Fast, Multi-Bit, and Vis-Infrared Broadband Nonvolatile Optoelectronic Memory with MoS2 /2D-Perovskite Van der Waals Heterojunction.

Nonvolatile optoelectronic memory (NVOM) integrating the functions of optical sensing and long-term memory can efficiently process and store a large amount of visual scene information, which has become the core requirement of multiple intelligence scenarios. However, realizing NVOM with vis-infrared broadband response is still challenging. Herein, the room temperature vis-infrared broadband NVOM based on few-layer MoS2 /2D Ruddlesden-Popper perovskite (2D-RPP) van der Waals heterojunction is realized. It is found that the 2D-RPP converts the initial n-type MoS2 into p-type and facilitates hole transfer between them. Furthermore, the 2D-RPP rich in interband states serves as an effective electron trapping layer as well as broadband photoresponsive layer. As a result, the dielectric-free MoS2 /2D-RPP heterojunction enables the charge to transfer quickly under external field, which enables a large memory window (104 V), fast write speed of 20 µs, and optical programmable characteristics from visible light (405 nm) to telecommunication wavelengths (i.e., 1550 nm) at room temperature. Trapezoidal optical programming can produce up to 100 recognizable states (>6 bits), with operating energy as low as 5.1 pJ per optical program. These results provide a route to realize fast, low power, multi-bit optoelectronic memory from visible to the infrared wavelength.

Van der Waals MoS2/Two-Dimensional Perovskite Heterostructure for Sensitive and Ultrafast Sub-Band-Gap Photodetection.

Two-dimensional (2D) hybrid perovskites have been extensively studied as the promising light-sensitive materials in the photodetectors owing to their improved structural stability over that of their three-dimensional counterparts. However, the application of the 2D perovskite-based photodetector in the near-infrared (NIR) region is obstructed by the large intrinsic optical band gap. Herein, we develop a novel van der Waals heterostructure composed of few-layer 2D perovskite/MoS2 nanoflakes, which exhibits high-sensitivity detection performance over a broad spectral region, from the visible region to the telecommunication wavelength (i.e., 1550 nm). In particular, the photoresponsivity and specific detectivity under an 860 nm laser reach 121 A W-1 and 4.3 × 1014 Jones, respectively, whereas the individual nanoflakes show no response under the same wavelength. Meanwhile, the response time at the microsecond (µs) level is obtained, shortened by around 3 orders of magnitude compared to that of the constituting layers. The sensitive and ultrafast photoresponse at the NIR wavelength stems from the strong interlayer transition of sub-band-gap photons and the rapid separation of the photogenerated carriers by the built-in field within the heterojunction area. Our results not only provide an effective approach to achieve sub-band-gap photodetection in 2D perovskite-based structures but also suggest a universal strategy to fabricate high-performance optoelectronic devices.

Photoinduced Multi-Bit Nonvolatile Memory Based on a van der Waals Heterostructure with a 2D-Perovskite Floating Gate.

The development of floating-gate nonvolatile memory (FGNVM) is limited by the charge storage, retention and transfer ability of the charge-trapping layer. Here, it is demonstrated that due to the unique alternate inorganic/organic chain structure and superior optical sensitivity, an insulating 2D Ruddlesden-Popper perovskite (2D-RPP) layer can function both as an excellent charge-storage layer and a photosensitive layer. Optoelectronic memory composed of a MoS2 /hBN/2D-RPP (MBR) van der Waals heterostructure is demonstrated. The MBR device exhibits unique light-controlled charge-storage characteristics, with maximum memory window up to 92 V, high on/off ratio of 104 , negligible degeneration over 103  s, >1000 program/erase cycles, and write speed of 500 µs. Dependent on the initial states, the MBR optoelectronic memory can be programmed in both positive photoconductivity (PPC) and negative photoconductivity (NPC) modes, with up to 11 and 22 distinct resistance states, respectively. The optical program power for each bit is as low as 36/10 pJ for PPC/NPC. The results not only reveal the potential of 2D-RPP as a superior charge-storage medium in floating-gate memory, but also provides an effective strategy toward fast, low-power and stable optical multi-bit storage and neuromorphic computing.

High-κ van der Waals Oxide MoO3 as Efficient Gate Dielectric for MoS2 Field-Effect Transistors.

Two-dimensional van der Waals crystals (2D vdW) are recognized as one of the potential materials to solve the physical limits caused by size scaling. Here, vdW metal oxide MoO3 is applied with the gate dielectric in a 2D field-effect transistor (FET). Due to its high dielectric constant and the good response of MoS2 to visible light, we obtained a field effect transistor for photodetection. In general, the device exhibits a threshold voltage near 0 V, Ion/Ioff ratio of 105, electron mobility about 85 cm2 V-1 s-1 and a good response to visible light, the responsivity is near 5 A/W at low laser power, which shows that MoO3 is a potential material as gate dielectric.

Quantitative Determination of the Vertical Segregation and Molecular Ordering of PBDB-T/ITIC Blend Films with Solvent Additives.

The vertical component distribution of bulk heterojunction (BHJ) active film shows a significant impact on determining the device performance in polymer solar cells (PSCs). Processing solvent additives are well known for regulating the BHJ active layer morphology; however, there are few reports regarding the quantitative evaluation of the effect. Herein, a study of the quantitative determination of the vertical segregation in combination of molecular ordering of PBDB-T/ITIC blend films with various 1,8-diiodooctane (DIO) contents is provided. A 0.5% (volume ratio) DIO-added blend film achieves the highest power conversion efficiency of 10.75%. The reduced performance of the PSCs resulted from the excessive vertical component segregation and overcrystallization investigated by various techniques. X-ray photoelectron spectroscopy indicates that DIO aggravates the PBDB-T enrichment region at the air side. Neutron reflectivity further quantitatively figures out the phase separation effect. Although increased crystallinity of ITIC and a higher face-on ratio of PBDB-T in active layer were obtained with increased DIO content approved by grazing-incidence wide-angle X-ray scattering (GIWAXS), the enhanced vertical distribution along with the enhanced crystal size of ITIC leads to the reduced performance of the PSCs due to the reduced carrier transportation paths between donor and acceptor.

A self-driven approach for local ion intercalation in vdW crystals.

Intercalation has proven to be a powerful strategy for physical and chemical property modulation in two dimensional (2D) van der Waals (vdW) materials. Traditional gaseous and chemical intercalation methods offer the ability for mass production, and the electrochemical method provides reversible fine tuning for in situ material investigation. Spatial control, or even direct patterning, of ions is widely required for practical device fabrication and integration; yet it is not realized. Here we demonstrate a self-driven ion (Co2+, Sn4+, and Cu2+) intercalation approach with patterning ability on vdW α-MoO3. It is proved that the self-driven intercalation was enabled by the formation of a local galvanic cell and could be controlled by the metal electrode potential and the solution concentration. The universality of self-intercalation was confirmed in various types of 2D materials (MoS2, WS2, MoSe2, WSe2 and graphene). Furthermore, the feasibility of building heterostructures by multiple species (Sn & Co) intercalation in a single nanosheet was demonstrated for broadband photodetection. The enhancement of conductivity and photoresponse was found to be due to the synergistic effect of lattice distortion from Sn intercalation and the d orbital from the Co atom. This approach offers a feasible way for direct nano-fabrication in 2D vdW material and functional device integration.

Carboxymethyl Cellulose Binder Greatly Stabilizes Porous Hollow Carbon Submicrospheres in Capacitive K-Ion Storage.

On account of the large radius of K-ions, the electrodes can suffer huge deformation during K-ion insertion and extraction processes. In our work, we unveil the impact of using carboxymethyl cellulose (CMC) instead of poly(vinylidene fluoride) (PVDF) as binders for K-ion storage. Our porous hollow carbon submicrosphere anodes using the CMC binder exhibit a reversible capacity of 208 mA h g-1 after 50 cycles at 50 mA g-1, and even at a high current density of 1 A g-1, they achieve a reversible capacity of 111 mA h g-1 over 3000 cycles with almost no decay, demonstrating remarkably improved reversibility and cycling stability than those using PVDF (18 mA h g-1 after 3000 cycles at 1 A g-1). It is showed that the CMC binder can result in higher adhesion force and better mechanical performance than the PVDF binder, which can restrain the crack during a potassiation/depotassiation process. According to the test of adhesion force, the hollow carbon submicrospheres using the CMC binder show above three times of average adhesion force than that using the PVDF binder. Furthermore, based on the rational design, our hollow carbon submicrospheres also exhibit 62.3% specific capacity contribution below 0.5 V vs K/K+ region, which is helpful to design the full cell with high energy density. We believe that our work will highlight the binder effect to improve the K-ion storage performance.

van der Waals Transition-Metal Oxide for Vis-MIR Broadband Photodetection via Intercalation Strategy.

Defects engineering can broaden the absorption band of wide band gap van der Waals (vdW) materials to the visible or near-IR regime at the expense of material stability and photoresponse speed. Herein, we introduce an atomic intercalation method that brings the wide band gap vdW α-MoO3 for vis-MIR broadband optoelectronic conversion. We confirm experimentally that intercalation significantly enhances photoabsorption and electrical conductivity buts effects negligible change to the lattice structure as compared with ion intercalation. Charge transfer from the Sn atom to the lattices induces an optoelectrical change. As a result, the Sn-intercalated α-MoO3 shows room temperature, air stable, broadband photodetection ability from 405 nm to 10 µm, with photoresponsivity better than 9.0 A W-1 in 405-1500 nm, ∼0.4 A W-1 at 3700 nm, and 0.16 A W-1 at 10 µm, response time of ∼0.1 s, and peak D* of 7.3 × 107 cm Hz0.5 W-1 at 520 nm. We further reveal that photothermal effect dominates in our detection range by real-time photothermal-electrical measurement, and the materials show a high temperature coefficient of resistance value of -1.658% K-1 at 300 K. These results provide feasible route for designing broadband absorption materials for photoelectrical, photothermal, or thermal-electrical application.

Impact of Donor-Acceptor Interaction and Solvent Additive on the Vertical Composition Distribution of Bulk Heterojunction Polymer Solar Cells.

The vertical composition distribution of a bulk heterojunction (BHJ) photoactive layer is known to have dramatic effects on photovoltaic performance in polymer solar cells. However, the vertical composition distribution evolution rules of BHJ films are still elusive. In this contribution, three BHJ film systems, composed of polymer donor PBDB-T, and three different classes of acceptor (fullerene acceptor PCBM, small-molecule acceptor ITIC, and polymer acceptor N2200) are systematically investigated using neutron reflectometry to examine how donor-acceptor interaction and solvent additive impact the vertical composition distribution. Our results show that those three BHJ films possess homogeneous vertical composition distributions across the bulk of the film, while very different composition accumulations near the top and bottom surface were observed, which could be attributed to different repulsion, miscibility, and phase separation between the donor and acceptor components as approved by the measurement of the donor-acceptor Flory-Huggins interaction parameter χ. Moreover, the solvent additive 1,8-diiodooctane (DIO) can induce more distinct vertical composition distribution especially in nonfullerene acceptor-based BHJ films. Thus, higher power conversion efficiencies were achieved in inverted solar cells because of facilitated charge transport in the active layer, improved carrier collection at electrodes, and suppressed charge recombination in BHJ solar cells.

A review on sediment bioflocculation: Dynamics, influencing factors and modeling.

Sediment in a water column provides excellent substratum for microorganism colonization, and biological processes would alter the physical and chemical of sediment, resulting in substantial changes in sediment dynamics. The flocculation of sediment with biological processes are defined as sediment bioflocculation, which has been ubiquitously observed across aquatic ecosystems, activated sludge plants and bioflocculant applications, as a result of various processes involving particle aggregation and breakage under the complex effects of microorganisms and their metabolic products (e.g., extracellular polymeric substances EPS). EPS are complex high-molecular-weight mixtures of polymers, which are the primary components that hold microbial aggregates together by acting as a biological glue. Several mechanistic aggregation theories such as the alginate theory, adsorption bridging theory, divalent cation bridging theory, and Derjaguin-Landau-Verwey-Overbeek (DLVO) theory, and a number of influencing factors (e.g., sediment properties, microbial activity, EPS quantities and components, and external environment conditions) have been proposed to elucidate the role of microorganisms and EPS in sediment aggregation, promoting the investigation of the sediment bioflocculation evolution and kinetics models. However, due to the complex interrelationships of multiple physical, chemical, and biological processes and the incomprehensive knowledge of microorganisms and EPS, considerable research should be further conducted to fully understand their precise roles in the sediment bioflocculation process. In this study, a review of dynamic characterizations, mechanism, influencing factors and models of sediment bioflocculation are given to obtain a more comprehensive understanding of sediment bioflocculation dynamics.