Printed electronics has emerged as a pathway for large scale, flexible, and wearable devices enabled by graphene and two-dimensional (2D) materials. Solution processing of graphite and layered materials demonstrated mass production of inks allowing techniques such as inkjet printing to be used for device fabrication. However, the complexity of the ink formulations and the polycrystalline nature of the thin films, together with the metal, semimetal, and semiconducting behaviour of different 2D materials, have impeded the investigation of charge transport in inkjet printed 2D material devices. Here we unveil the charge transport mechanisms of surfactant-and solvent-free inkjet-printed thin-film devices of representative few-layer graphene (semi-metal), molybdenum disulfide (MoS2, semiconductor) and titanium carbide MXene (Ti3C2, metal) by investigating the temperature (T ), gate and magnetic field dependencies of their electrical conductivity. We find that charge transport in printed few-layer MXene and MoS2 devices is dominated by the intrinsic transport mechanism of the constituent flakes: MXene devices exhibit a weakly-localized 2D metallic behavior at any T , whereas MoS2 devices behave as insulators with a crossover from 3D-Mott variable-range hopping at low T to nearest-neighbor hopping around at ∼ 200 K. The charge transport in printed few-layer graphene devices is dominated by the transport mechanism between different flakes, which exhibit 3D-Mott variable range hopping conduction at any T . These findings reveal and finally establish the fundamental mechanisms responsible for charge transport in inkjet-printed devices with 2D materials, paving the way for a reliable design of high performance printed electronics.

Abstract2D material hydrogels have recently sparked tremendous interest owing to their potential in diverse applications. However, research on the emerging 2D MXene hydrogels is still in its infancy. Herein, we show a universal 4D printing technology for manufacturing MXene hydrogels with customizable geometries, which suits a family of MXenes such as Nb2CTx, Ti3C2Tx, and Mo2Ti2C3Tx. The obtained MXene hydrogels offer 3D porous architectures, large specific surface areas, high electrical conductivities, and satisfying mechanical properties. Consequently, ultrahigh capacitance (3.32 F cm−2 (10 mV s−1) and 233 F g−1 (10 V s−1)) and mass loading/thickness-independent rate capabilities are achieved. The further 4D-printed Ti3C2Tx hydrogel micro-supercapacitors showcase great low-temperature tolerance (down to –20 °C) and deliver high energy and power densities up to 93 μWh cm−2 and 7 mW cm−2, respectively, surpassing most state-of-the-art devices. This work brings new insights into MXene hydrogel manufacturing and expands the range of their potential applications.

The rapidly expanding fields of bioelectronics, and biological interfaces with sensors and stimulators, are placing an increasing demand on candidate materials to serve as robust surfaces that are both biocompatible, stable and electroconductive.

The properties and performance of two-dimensional (2D) materials can be greatly affected by point defects. PtTe2, a 2D material that belongs to the group 10 transition metal dichalcogenides, is a type-II Dirac semimetal, which has gained a lot of attention recently due to its potential for applications in catalysis, photonics, and spintronics. Here, we provide an experimental and theoretical investigation of point defects on and near the surface of PtTe2. Using scanning tunneling microscopy and scanning tunneling spectroscopy (STS) measurements, in combination with first-principle calculations, we identify and characterize five common surface and subsurface point defects. The influence of these defects on the electronic structure of PtTe2 is explored in detail through grid STS measurements and complementary density functional theory calculations. We believe these findings will be of significance to future efforts to engineer point defects in PtTe2, which is an interesting and enticing approach to tune the charge-carrier mobility and electron–hole recombination rates, as well as the site reactivity for catalysis.

Titanium (Ti)-doped hematite (α-Fe2O3) films were grown in oxygen-depleted condition by using the spray pyrolysis technique. The impact of post-deposition annealing in oxygen-rich condition on both the conductivity and water splitting efficiency was investigated. The X-ray diffraction pattern revealed that the films are of rhombohedral α-Fe2O3 structure and dominantly directed along (012). The as-grown films were found to be highly conductive with electrons as the majority charge carriers (n-type), a carrier concentration of 1.09×1020 cm−3, and a resistivity of 5.9×10−2 Ω-cm. The conductivity of the films were reduced upon post-deposition annealing. The origin of the conductivity was attributed firstly to Ti4+ substituting Fe3+ and secondly to the ionized oxygen vacancies (VO) in the crystal lattice of hematite. Upon annealing the samples in oxygen-rich condition, VO slowly depleted and the conductivity reduced. The photocurrent of the as-grown samples was found to be 3.4 mA/cm−2 at 1.23 V vs. RHE. The solar-to-hydrogen efficiency for the as-grown sample was calculated to be 4.18% at 1.23 V vs. RHE. The photocurrents were found to be significantly stable in aqueous environment. A linear relationship between conductivity and water-splitting efficiency was established.

In this report, reactive and nonreactive sputtering of amorphous ZnSnO y (a-ZnSnO y ) was investigated, and extensive composition maps have been measured by X-ray photoelectron spectroscopy. The comprehensive analysis of the ((ZnO) x (SnO 2 ) 1−x ) composition reveals that the best Zn/Sn ratio for high conductivity of the material can vary depending on the deposition technique utilized. Best conductivities of 225 S/cm were found to occur at x = 0.32 for reactive sputtering of a Sn target and x = 0.27 for nonreactive sputtering of a SnO 2 target. These values correspond to unstable polymorphs of a-ZnSnO y , ZnSn 2 O 5 , and ZnSn 3 O 7 . Distinct local bonding arrangements have been confirmed by Raman spectroscopy.

The current best performing p-type transparent conducting oxides are typically highly crystalline materials, deposited at high temperatures, and hence incompatible with the drive to low cost flexible electronics. We investigated a nanocrystalline, copper deficient CuxCrO2, deposited at low temperatures upon a flexible polyimide substrate. The as-deposited film without post annealing has an electrical conductivity of 6Scm−1. We demonstrate that this p-type transparent oxide retains its excellent electrical conductivity under tensile strain, withstanding more than one thousand bending cycles without visible cracks or degradation in electrical properties. In contrast, compressive strain is shown to lead to an immediate reduction in conductivity which we attribute to a de-lamination of the thin film from the substrate.

NbO terminated Nb(110) and its oxidation are examined by scanning tunneling microscopy and spectroscopy (STS). The oxide structures are strongly influenced by the structural and electronic properties of the underlying NbO substrate. The NbO is terminated by one-dimensional few-nanometer nanocrystals, which form an ordered pattern. High-resolution STS measurements reveal that the nanocrystals and the regions between the nanocrystals exhibit different electronic characters. Lowdosage oxidation, sufficient for sub-monolayer coverage of the NbO, with subsequent UHV annealing results in the formation of resolved sub-nanometer clusters, positioned in-between the nanocrystals. Higher dosage oxidation results in the formation of a closed Nb 2 o 5−y layer, which is confirmed by X-ray photoelectron spectroscopy measurements. The pentoxide is amorphous at the atomic-scale. However, large scale (tens of nanometers) structures are observed with their symmetry matching that of the underlying nanocrystals.