Promotion of Processability in a p-Type Thin-Film Transistor Using a Se-Te Alloying Channel Layer.

p-type thin-film transistors (pTFTs) have proven to be a significant impediment to advancing electronics beyond traditional Si-based technology. A recent study suggests that a thin and highly crystalline Te layer shows promise as a channel for high-performance pTFTs. However, achieving this still requires specific conditions, such as a cryogenic growth temperature and an extremely thin channel thickness on the order of a few nanometers. These conditions critically limit the practical feasibility of the fabrication process. Here, we report a high-performance pTFT incorporating a 60-nm-thick highly crystalline Se-Te alloyed channel layer, produced using pulsed laser ablation at room temperature. The Se0.5Te0.5 alloy system enhances crystalline temperature and widens the band gap compared to a pure Te channel. Consequently, this approach results in a field-effect mobility of 3 cm2/V·s, with an on/off current ratio of 3 × 105, a subthreshold slope of 2.1 V/decade, and a turn-on voltage of 6.5 V, achieved through conventional annealing at 250 °C. To demonstrate its applicability in complementary circuit applications, we integrate a complementary-type inverter using a p-type Se0.5Te0.5 TFT and an n-type Al-doped InZnSnO, demonstrating a high voltage gain of 12 and a low static power consumption of 17 nW. This suggests that the Se-Te alloyed channel approach paves the way to a more straightforward and cost-effective process for Te-based pTFT devices and their applications.

Acceleration of NO2 gas sensitivity in two-dimensional SnSe2 by Br doping.

The authors report a Br doping effect on the NO2 gas sensing properties of a two-dimensional (2D) SnSe2 semiconductor. Single crystalline 2D SnSe2 samples with different Br contents are grown by a simple melt-solidification method. By analyzing the structural, vibrational as well as electrical properties, it can be confirmed that the Br impurity substitutes on the Se-site in SnSe2 serving as an efficient electron donor. When we measure the change of resistance under a 20 ppm NO2 gas flow condition at room temperature, both responsivity and response time are drastically improved by Br doping from 1.02% and 23 s to 3.38% and 15 s, respectively. From these results, it can be concluded that Br doping plays a key role for encouraging the charge transfer efficiency from the SnSe2 surface to the NO2 molecule by elaborating Fermi level in 2D SnSe2.

Study on the decisive factor for metal-insulator transitions in a LaVO3 Mott-Hubbard insulator.

The decisive physical parameters on electrical conduction in a LaVO3 Mott-Hubbard system are systematically investigated by analyzing pure, Ca-, and Sr-doped samples. The Rietveld refinement of the X-ray diffraction data indicates that a drastic change occurs along the c-axis to reduce the octahedral tilt thereby relaxing the distortion for the doped compounds, in contrast to an insignificant change in the in-plane distortion. From electrical, optical, and photoemission measurements, both Ca and Sr-doping in LaVO3 induce insulator to metal transitions under a similar hole carrier concentration as suppressing the Mott-gap excitation. Fitting results on temperature-dependent resistivity based on various conduction models indicate that the most localized conduction behavior takes place for the highly distorted pure LaVO3, while disordered Fermi liquid behavior starts to appear for moderately distorted Ca-doped LaVO3. The least distorted Sr-doped LaVO3 exhibits fully delocalized conduction governed by a non-Fermi-liquid-like behavior in the whole temperature range. Our analysis indicates that the difference in the transport mechanism arises from the differing degree of hybridization of the V 3d and O 2p states in the pure and doped systems, strongly associated with the structural distortion.

Graphene Bridge Heterostructure Devices for Negative Differential Transconductance Circuit Applications.

Two-dimensional van der Waals (2D vdW) material-based heterostructure devices have been widely studied for high-end electronic applications owing to their heterojunction properties. In this study, we demonstrate graphene (Gr)-bridge heterostructure devices consisting of laterally series-connected ambipolar semiconductor/Gr-bridge/n-type molybdenum disulfide as a channel material for field-effect transistors (FET). Unlike conventional FET operation, our Gr-bridge devices exhibit non-classical transfer characteristics (humped transfer curve), thus possessing a negative differential transconductance. These phenomena are interpreted as the operating behavior in two series-connected FETs, and they result from the gate-tunable contact capacity of the Gr-bridge layer. Multi-value logic inverters and frequency tripler circuits are successfully demonstrated using ambipolar semiconductors with narrow- and wide-bandgap materials as more advanced circuit applications based on non-classical transfer characteristics. Thus, we believe that our innovative and straightforward device structure engineering will be a promising technique for future multi-functional circuit applications of 2D nanoelectronics.

Fermi-Level Pinning-Free WSe2 Transistors via 2D Van der Waals Metal Contacts and Their Circuits.

Precise control over the polarity of transistors is a key necessity for the construction of complementary metal-oxide-semiconductor circuits. However, the polarity control of 2D transistors remains a challenge because of the lack of a high-work-function electrode that completely eliminates Fermi-level pinning at metal-semiconductor interfaces. Here, a creation of clean van der Waals contacts is demonstrated, wherein a metallic 2D material, chlorine-doped SnSe2 (Cl-SnSe2 ), is used as the high-work-function contact, providing an interface that is free of defects and Fermi-level pinning. Such clean contacts made from Cl-SnSe2 can pose nearly ideal Schottky barrier heights, following the Schottky-Mott limit and thus permitting polarity-controllable transistors. With the integration of Cl-SnSe2 as contacts, WSe2 transistors exhibit pronounced p-type characteristics, which are distinctly different from those of the devices with evaporated metal contacts, where n-type transport is observed. Finally, this ability to control the polarity enables the fabrication of functional logic gates and circuits, including inverter, NAND, and NOR.

Direct Observation of Orbital Driven Strong Interlayer Coupling in Puckered Two-Dimensional PdSe2.

Interlayer coupling between individual unit layers is known to be critical in manipulating the layer-dependent properties of two-dimensional (2D) materials. While recent studies have revealed that several 2D materials with significant degrees of interlayer interaction (such as black phosphorus) show strongly layer-dependent properties, the origin based on the electronic structure is drawing intensive attention along with 2D materials exploration. Here, the direct observation of a highly dispersive single electronic band along the interlayer direction in puckered 2D PdSe2 as an experimental hallmark of strong interlayer couplings is reported. Remarkably large band dispersion along the kz -direction near Fermi level, which is even wider than the in-plane one, is observed by the angle-resolved photoemission spectroscopy measurement. Employing X-ray absorption spectroscopy and density functional theory calculations, it is revealed that the strong interlayer coupling in 2D PdSe2 originates from the unique directional bonding of Pd d orbitals associated with unexpected Pd 4d9 configuration, which consequently plays a decisive role for the strong layer-dependency of the band gap.

Antiperovskite Gd3 SnC: Unusual Coexistence of Ferromagnetism and Heavy Fermions in Gd Lattice.

Inverted structures of common crystal lattices, referred to as antistructures, are rare in nature due to their thermodynamic constraints imposed by the switched cation and anion positions in reference to the original structure. However, a stable antistructure formed with mixed bonding characters of constituent elements in unusual valence states can provide unexpected material properties. Here, a heavy-fermion behavior of ferromagnetic gadolinium lattice in Gd3 SnC antiperovskite is reported, contradicting the common belief that ferromagnetic gadolinium cannot be a heavy-fermion system due to the deep energy level of localized 4f-electrons. The specific heat shows an unusually large Sommerfeld coefficient of ≈1114 mJ mol-1 K-2 with a logarithmic behavior of non-Fermi-liquid state. It is demonstrated that the heavy-fermion behavior in the non-Fermi-liquid state appears to arise from the hybridized electronic states of gadolinium 5d-electrons participating in metallic GdGd and covalent GdC bonds. These results accentuate the unusual chemical bonds in CGd6 octahedra with the dual characters of gadolinium 5d-electrons for the emergence of heavy fermions.

Stoner enhancement from interstitial electrons in Y2C toward a spontaneous ferromagnetic electride.

The evolutionary magnetism associated with the interlayer spacing in two-dimensional (2D) Y2C electrides has been investigated by first-principles total-energy calculations based on density functional theory. Several structures with different c-axis parameters around the optimized value were taken into our consideration. Mapping of the electron localization function shows that the interstitial electron is strongly localized at the body center position (denoted as the X-site) in the primitive rhombohedral unit cell, serving as an anion which is ionically bonded with the cationic framework of the Y2C layer. As the c-axis parameter decreases, the volume of the X-site is systematically reduced while both the charge and magnetization density for X are increased. It indicates that the compressed inter-layer space effectively increases the degree of localization of interstitial anionic electrons (IAEs) correlated with their enhanced local magnetic moments. We have found that the exchange splitting of the density of states for Y2C becomes more prominent with a decrease in the c-axis parameter as predicted from a pressurized alkali metal system. Accompanied by the calculated magnetization values, it can be concluded that the increased degree of localization for IAEs between cationic framework layers has greatly influenced the Stoner parameter leading to the increased magnetic moment based on the Stoner enhancement mechanism; hence, it plays a key role in the emergence of a spontaneous ferromagnetic electride.

Water- and acid-stable self-passivated dihafnium sulfide electride and its persistent electrocatalytic reaction.

Electrides have emerged as promising materials with exotic properties, such as extraordinary electron-donating ability. However, the inevitable instability of electrides, which is caused by inherent excess electrons, has hampered their widespread applications. We report that a self-passivated dihafnium sulfide electride ([Hf2S]2+∙2e-) by double amorphous layers exhibits a strong oxidation resistance in water and acid solutions, enabling a persistent electrocatalytic hydrogen evolution reaction. The naturally formed amorphous Hf2S layer on the cleaved [Hf2S]2+∙2e- surface reacts with oxygen to form an outermost amorphous HfO2 layer with ~10-nm thickness, passivating the [Hf2S]2+∙2e- electride. The excess electrons in the [Hf2S]2+∙2e- electride are transferred through the thin HfO2 passivation layer to water molecules under applied electric fields, demonstrating the first electrocatalytic reaction with excellent long-term sustainability and no degradation in performance. This self-passivation mechanism in reactive conditions can advance the development of stable electrides for energy-efficient applications.

Author Correction: Ferromagnetic quasi-atomic electrons in two-dimensional electride.

An amendment to this paper has been published and can be accessed via a link at the top of the paper.

Effects of Intense Pulsed Light (IPL) Rapid Annealing and Back-Channel Passivation on Solution-Processed In-Ga-Zn-O Thin Film Transistors Array.

We report on the effects of the intense pulsed light (IPL) rapid annealing process and back-channel passivation on the solution-processed In-Ga-Zn-O (IGZO) thin film transistors (TFTs) array. To improve the electrical properties, stability and uniformity of IGZO TFTs, the oxide channel layers were treated by IPL at atmospheric ambient and passivated by photo-sensitive polyimide (PSPI). When we treated the IGZO channel layer by the IPL rapid annealing process, saturation field effect mobility and subthreshold swing (S.S.) were improved. And, to protect the back-channel of oxide channel layers from oxygen and water molecules, we passivated TFT devices with photo-sensitive polyimide. The IGZO TFTs on glass substrate treated by IPL rapid annealing without PSPI passivation showed the field effect mobility (µFE) of 1.54 cm2/Vs and subthreshold swing (S.S.) of 0.708 V/decade. The PSPI-passivated IGZO TFTs showed higher µFE of 2.17 cm2/Vs than that of device without passivation process and improved S.S. of 0.225 V/decade. By using a simple and fast intense pulsed light treatment with an appropriate back-channel passivation layer, we could improve the electrical characteristics and hysteresis of IGZO-TFTs. We also showed the improved uniformity of electrical characteristics for IGZO TFT devices in the area of 10 × 40 mm2. Since this IPL rapid annealing process could be performed at a low temperature, it can be applied to flexible electronics on plastic substrates in the near future.

Ferromagnetic quasi-atomic electrons in two-dimensional electride.

An electride, a generalized form of cavity-trapped interstitial anionic electrons (IAEs) in a positively charged lattice framework, shows exotic properties according to the size and geometry of the cavities. Here, we report that the IAEs in layer structured [Gd2C]2+·2e- electride behave as ferromagnetic elements in two-dimensional interlayer space and possess their own magnetic moments of ~0.52 µB per quasi-atomic IAE, which facilitate the exchange interactions between interlayer gadolinium atoms across IAEs, inducing the ferromagnetism in [Gd2C]2+·2e- electride. The substitution of paramagnetic chlorine atoms for IAEs proves the magnetic nature of quasi-atomic IAEs through a transition from ferromagnetic [Gd2C]2+·2e- to antiferromagnetic Gd2CCl caused by attenuating interatomic exchange interactions, consistent with theoretical calculations. These results confirm that quasi-atomic IAEs act as ferromagnetic elements and trigger ferromagnetic spin alignments within the antiferromagnetic [Gd2C]2+ lattice framework. These results present a broad opportunity to tailor intriguing ferromagnetism originating from quasi-atomic interstitial electrons in low-dimensional materials.

Influence of Pd Doping on Electrical and Thermal Properties of n-Type Cu0.008Bi2Te2.7Se0.3 Alloys.

Doping is known as an effective way to modify both electrical and thermal transport properties of thermoelectric alloys to enhance their energy conversion efficiency. In this project, we report the effect of Pd doping on the electrical and thermal properties of n-type Cu0.008Bi2Te2.7Se0.3 alloys. Pd doping was found to increase the electrical conductivity along with the electron carrier concentration. As a result, the effective mass and power factors also increased upon the Pd doping. While the bipolar thermal conductivity was reduced with the Pd doping due to the increased carrier concentration, the contribution of Pd to point defect phonon scattering on the lattice thermal conductivity was found to be very small. Consequently, Pd doping resulted in an enhanced thermoelectric figure of merit, zT, at a high temperature, due to the enhanced power factor and the reduced bipolar thermal conductivity.

Abnormal Optoelectric Properties of Two-Dimensional Protonic Ruthenium Oxide with a Hexagonal Structure.

Two-dimensional structures can potentially lead to not only modulation of electron transport but also the variations of optical property. Protonic ruthenium oxide, a two-dimensional atomic sheet material, has been synthesized, and its optoelectric properties have been investigated. The results indicate that protonic ruthenium oxide is an excellent candidate for use as a flexible, transparent conducting material. A hydrated-ruthenium-oxide sheet has been first prepared via the chemical exfoliation of sodium intercalated ruthenium oxide (NaRuO2) and, subsequently, converted into a protonic ruthenium oxide sheet using thermal treatment. A thermally activated transport mechanism is dominant in hydrated ruthenium oxide but diminishes in protonic ruthenium oxide; this resulted in a high electrical conductivity of ∼200 S/cm of the protonic sheet. Because of the unique interband and intraband structure, protonic ruthenium oxide has a small optical absorption coefficient of ∼1.62%/L. Consequently, such high conductivity and low absorption coefficient of protonic ruthenium oxide results in excellent transparent conducting properties.

Interband Transitions in Monolayer and Few-Layer WSe2 Probed Using Photoexcited Charge Collection Spectroscopy.

Transition-metal dichalcogenides are currently under rigorous investigation because of their distinct layer-dependent physical properties originating from the corresponding evolution of the band structure. Here, we report the highly resolved probing of layer-dependent band structure evolution for WSe2 using photoexcited charge collection spectroscopy (PECCS). Monolayer, few-layer, and multilayer WSe2 can be probed in top-gate field-effect transistor platforms, and their interband transitions are efficiently observed. Our theoretical calculations show a great coincidence with the PECCS results, proving that the indirect Γ-K and Γ-Λ transitions as well as the direct K-K transition are clearly resolved in multilayer WSe2 by PECCS.

Role of fluorine in two-dimensional dichalcogenide of SnSe 2.

Authors report an effect of F substitution on layered SnSe2 through the successful synthesis of polycrystalline SnSe2-δF x (0.000 ≤ x ≤ 0.010) by solid-state reaction. Accompanied with density functional theory calculations, the blue shift of A1g peak in Raman spectra reveal that F- ions are substituted at Se vacancy sites as decreasing the reduced mass of vibrational mode associated with Sn-Se bonding. From the measurements of electrical parameters, conductivity as well as carrier concentration are governed by thermally activated behavior, while such behavior is suppressed in Hall mobility, which occurs as F ratio increases. Based on Arrhenius relation, it is found that the potential barrier height at the grain boundary is suppressed with increasing F amount, suggesting that the F- ion is a promising candidate for the grain boundary passivation in the two-dimensional dichalcogenide system.

Tuning the Spin-Alignment of Interstitial Electrons in Two-Dimensional Y2C Electride via Chemical Pressure.

We report that the spin-alignment of interstitial anionic electrons (IAEs) in two-dimensional (2D) interlayer spacing can be tuned by chemical pressure that controls the magnetic properties of 2D electrides. It was clarified from the isovalent Sc substitution on the Y site in the 2D Y2C electride that the localization degree of IAEs at the interlayer becomes stronger as the unit cell volume and c-axis lattice parameter were systematically reduced by increasing the Sc contents, thus eventually enhancing superparamagnetic behavior originated from the increase in ferromagnetic particle concentration. It was also found that the spin-aligned localized IAEs dominated the electrical conduction of heavily Sc-substituted Y2C electride. These results indicate that the physcial properties of 2D electrides can be tailored by adjusting the localization of IAEs at interlayer spacing via structural modification that controls the spin instability as found in three-dimensional elemental electrides of pressurized potassium metals.

Strong Localization of Anionic Electrons at Interlayer for Electrical and Magnetic Anisotropy in Two-Dimensional Y2C Electride.

We have synthesized a single crystalline Y2C electride of centimeter-scale by floating-zone method and successfully characterized its anisotropic electrical and magnetic properties. In-plane resistivity upturn at low temperature together with anisotropic behavior of negative magnetoresistance is ascribed to the stronger suppression of spin fluctuation along in-plane than that along the c-axis, verifying the existence of magnetic moments preferred for the c-axis. A superior magnetic moment along the c-axis to that along the in-plane direction strongly demonstrates the anisotropic magnetism of Y2C electride containing a magnetically easy axis. It is clarified from the theoretical calculations that the anisotropic nature of the Y2C electride originates from strongly localized anionic electrons with an inherent magnetic anisotropy in the interlayer spaces.

First-Principles Prediction of Thermodynamically Stable Two-Dimensional Electrides.

Two-dimensional (2D) electrides, emerging as a new type of layered material whose electrons are confined in interlayer spaces instead of at atomic proximities, are receiving interest for their high performance in various (opto)electronics and catalytic applications. Experimentally, however, 2D electrides have been only found in a couple of layered nitrides and carbides. Here, we report new thermodynamically stable alkaline-earth based 2D electrides by using a first-principles global structure optimization method, phonon spectrum analysis, and molecular dynamics simulation. The method was applied to binary compounds consisting of alkaline-earth elements as cations and group VA, VIA, or VIIA nonmetal elements as anions. We revealed that the stability of a layered 2D electride structure is closely related to the cation/anion size ratio; stable 2D electrides possess a sufficiently large cation/anion size ratio to minimize electrostatic energy among cations, anions, and anionic electrons. Our work demonstrates a new avenue to the discovery of thermodynamically stable 2D electrides beyond experimental material databases and provides new insight into the principles of electride design.

Metallic conduction induced by direct anion site doping in layered SnSe2.

The emergence of metallic conduction in layered dichalcogenide semiconductor materials by chemical doping is one of key issues for two-dimensional (2D) materials engineering. At present, doping methods for layered dichalcogenide materials have been limited to an ion intercalation between layer units or electrostatic carrier doping by electrical bias owing to the absence of appropriate substitutional dopant for increasing the carrier concentration. Here, we report the occurrence of metallic conduction in the layered dichalcogenide of SnSe2 by the direct Se-site doping with Cl as a shallow electron donor. The total carrier concentration up to ~10(20) cm(-3) is achieved by Cl substitutional doping, resulting in the improved conductivity value of ~170 S · cm(-1) from ~1.7 S · cm(-1) for non-doped SnSe2. When the carrier concentration exceeds ~10(19) cm(-3), the conduction mechanism is changed from hopping to degenerate conduction, exhibiting metal-insulator transition behavior. Detailed band structure calculation reveals that the hybridized s-p orbital from Sn 5s and Se 4p states is responsible for the degenerate metallic conduction in electron-doped SnSe2.