Incommensurate Antiferromagnetic Order in Weakly Frustrated Two-Dimensional van der Waals Insulator CrPSe3.

Although magnetic order is suppressed by a strong frustration, it appears in complex forms such as a cycloid or spin density wave in weakly frustrated systems. Herein, we report a weakly magnetically frustrated two-dimensional (2D) van der Waals material CrPSe3. Polycrystalline CrPSe3 was synthesized at an optimized temperature of 700 °C to avoid the formation of any secondary phases (e.g., Cr2Se3). The antiferromagnetic transition appeared at TN ≈ 127 K with a large Curie-Weiss temperature θCW ≈ -301 K via magnetic susceptibility measurements, indicating weak frustration in CrPSe3 with a frustration factor of f (|θCW|/TN) ≈ 2.4. Evidently, the formation of a long-range incommensurate antiferromagnetic order was revealed by neutron diffraction measurements at low temperatures (below 120 K). The monoclinic crystal structure of the C2/m symmetry is preserved over the studied temperature range down to 20 K, as confirmed by Raman spectroscopy measurements. Our findings on the incommensurate antiferromagnetic order in 2D magnetic materials, not previously observed in the MPX3 family, are expected to enrich the physics of magnetism at the 2D limit, thereby opening opportunities for their practical applications in spintronics and quantum devices.

Spin-Selective Hole-Exciton Coupling in a V-Doped WSe2 Ferromagnetic Semiconductor at Room Temperature.

While valley polarization with strong Zeeman splitting is the most prominent characteristic of two-dimensional (2D) transition metal dichalcogenide (TMD) semiconductors under magnetic fields, enhancement of the Zeeman splitting has been demonstrated by incorporating magnetic dopants into the host materials. Unlike Fe, Mn, and Co, V is a distinctive dopant for ferromagnetic semiconducting properties at room temperature with large Zeeman shifting of band edges. Nevertheless, little known is the excitons interacting with spin-polarized carriers in V-doped TMDs. Here, we report anomalous circularly polarized photoluminescence (CPL) in a V-doped WSe2 monolayer at room temperature. Excitons couple to V-induced spin-polarized holes to generate spin-selective positive trions, leading to differences in the populations of neutral excitons and trions between left and right CPL. Using transient absorption spectroscopy, we elucidate the origin of excitons and trions that are inherently distinct for defect-mediated and impurity-mediated trions. Ferromagnetic characteristics are further confirmed by the significant Zeeman splitting of nanodiamonds deposited on the V-doped WSe2 monolayer.

Efficient Gate Modulation in a Screening-Engineered MoS2/Single-Walled Carbon Nanotube Network Heterojunction Vertical Field-Effect Transistor.

In this report, a screening-engineered carbon nanotube (CNT) network/MoS2/metal heterojunction vertical field effect transistor (CNT-VFET) is fabricated for an efficient gate modulation independent of the drain voltage. The gate field in the CNT-VFET transports through the empty space of the CNT network without any screening layer and directly modulates the MoS2 semiconductor energy band, while the gate field from the Si back gate is mostly screened by the graphene layer. Consequently, the on/off ratio of CNT-VFET maintained 103 in overall drain voltages, which is 10 times and 1000 times higher than that of the graphene (Gr) VFET at Vsd = 0.1 (ratio = 81.9) and 1 V (ratio = 3), respectively. An energy band diagram simulation shows that the Schottky barrier modulation of CNT/MoS2 contact along the sweeping gate bias is independent of the drain voltage. On the other hand, the gate modulation of Gr/MoS2 is considerably reduced with increased drain voltage because more electrons are drawn into the graphene electrode and screens the gate field by applying a higher drain voltage to the graphene/MoS2/metal capacitor.

Enhanced Light-Matter Interactions in Self-Assembled Plasmonic Nanoparticles on 2D Semiconductors.

Two-dimensional (2D) transition-metal dichalcogenide (TMD) monolayers of versatile material library are spotlighted for numerous unexplored research fields. While monolayer TMDs exhibit an efficient excitonic emission, the weak light absorption arising from their low dimensionality limits potential applications. To enhance the light-matter interactions of TMDs, while various plasmonic hybridization methods have been intensively studied, controlling plasmonic nanostructures via self-assembly processes remains challenging. Herein, strong light-matter interactions are reported in plasmonic Ag nanoparticles (NPs) hybridized on TMDs via an aging-based self-assembly process at room temperature. This hybridization is implemented by transferring MoS2 monolayers grown via chemical vapor deposition onto thin-spacer-covered Ag films. After a few weeks of aging in a vacuum desiccator, the Ag atoms in the heterolayered film diffuse to the MoS2 layers through a SiO2 spacer and self-cluster onto MoS2 point defects, resulting in the formation of Ag-NPs with an estimated diameter of ≈50 nm. The photoluminescence intensities for the Ag-NP/MoS2 hybrids are enhanced up to 35-fold compared with bare MoS2 owing to the local field enhancement near the plasmonic Ag-NPs. The localized surface plasmon resonances modes of this hybrid are systematically investigated via numerical simulations and dark-field scattering microscopy.

Tunneling Photocurrent Assisted by Interlayer Excitons in Staggered van der Waals Hetero-Bilayers.

Vertically stacked van der Waals (vdW) heterostructures have been suggested as a robust platform for studying interfacial phenomena and related electric/optoelectronic devices. While the interlayer Coulomb interaction mediated by the vdW coupling has been extensively studied for carrier recombination processes in a diode transport, its correlation with the interlayer tunneling transport has not been elucidated. Here, a contrast is reported between tunneling and drift photocurrents tailored by the interlayer coupling strength in MoSe2 /MoS2 hetero-bilayers (HBs). The interfacial coupling modulated by thermal annealing is identified by the interlayer phonon coupling in Raman spectra and the emerging interlayer exciton peak in photoluminescence spectra. In strongly coupled HBs, positive photocurrents are observed owing to the inelastic band-to-band tunneling assisted by interlayer excitons that prevail over exciton recombinations. By contrast, weakly coupled HBs exhibit a negative photovoltaic diode behavior, manifested as a drift current without interlayer excitonic emissions. This study sheds light on tailoring the tunneling transport for numerous optoelectronic HB devices.

Reconfigurable exciton-plasmon interconversion for nanophotonic circuits.

The recent challenges for improving the operation speed of nanoelectronics have motivated research on manipulating light in on-chip integrated circuits. Hybrid plasmonic waveguides with low-dimensional semiconductors, including quantum dots and quantum wells, are a promising platform for realizing sub-diffraction limited optical components. Meanwhile, two-dimensional transition metal dichalcogenides (TMDs) have received broad interest in optoelectronics owing to tightly bound excitons at room temperature, strong light-matter and exciton-plasmon interactions, available top-down wafer-scale integration, and band-gap tunability. Here, we demonstrate principal functionalities for on-chip optical communications via reconfigurable exciton-plasmon interconversions in ∼200-nm-diameter Ag-nanowires overlapping onto TMD transistors. By varying device configurations for each operation purpose, three active components for optical communications are realized: field-effect exciton transistors with a channel length of ∼32 µm, field-effect exciton multiplexers transmitting multiple signals through a single NW and electrical detectors of propagating plasmons with a high On/Off ratio of∼190. Our results illustrate the unique merits of two-dimensional semiconductors for constructing reconfigurable device architectures in integrated nanophotonic circuits.

Two-terminal floating-gate memory with van der Waals heterostructures for ultrahigh on/off ratio.

Concepts of non-volatile memory to replace conventional flash memory have suffered from low material reliability and high off-state current, and the use of a thick, rigid blocking oxide layer in flash memory further restricts vertical scale-up. Here, we report a two-terminal floating gate memory, tunnelling random access memory fabricated by a monolayer MoS2/h-BN/monolayer graphene vertical stack. Our device uses a two-terminal electrode for current flow in the MoS2 channel and simultaneously for charging and discharging the graphene floating gate through the h-BN tunnelling barrier. By effective charge tunnelling through crystalline h-BN layer and storing charges in graphene layer, our memory device demonstrates an ultimately low off-state current of 10(-14) A, leading to ultrahigh on/off ratio over 10(9), about ∼10(3) times higher than other two-terminal memories. Furthermore, the absence of thick, rigid blocking oxides enables high stretchability (>19%) which is useful for soft electronics.

Simultaneous Hosting of Positive and Negative Trions and the Enhanced Direct Band Emission in MoSe2/MoS2 Heterostacked Multilayers.

Heterostacking of layered transition-metal dichalcogenide (LTMD) monolayers (1Ls) offers a convenient way of designing two-dimensional exciton systems. Here we demonstrate the simultaneous hosting of positive trions and negative trions in heterobilayers made by vertically stacking 1L MoSe2 and 1L MoS2. The charge transfer occurring between the 1Ls of MoSe2 and MoS2 converted the polarity of trions in 1L MoSe2 from negative to positive, resulting in the presence of positive trions in the 1L MoSe2 and negative trions in the 1L MoS2 of the same heterostacked bilayer. Significantly enhanced MoSe2 photoluminescence (PL) in the heterostacked bilayers compared to the PL of 1L MoSe2 alone suggests that, unlike other previously reported heterostacked bilayers, direct band transition of 1L MoSe2 in heterobilayer was enhanced after the vertical heterostacking. Moreover, by inserting hexagonal BN monolayers between 1L MoSe2 and 1L MoS2, we were able to adjust the charge transfer to maximize the MoSe2 PL of the heteromultilayers and have achieved a 9-fold increase of the PL emission. The enhanced optical properties of our heterostacked LTMDs suggest the exciting possibility of designing LTMD structures that exploit the superior optical properties of 1L LTMDs.

Carbon nanotube-bridged graphene 3D building blocks for ultrafast compact supercapacitors.

The main obstacles to achieving high electrochemical energy density while retaining high power density are the trade-offs of energy versus power and gravimetric versus volumetric density. Optimizing structural parameters is the key to circumvent these trade-offs. We report here the synthesis of carbon nanotube (CNT)-bridged graphene 3D building blocks via the Coulombic interaction between positively charged CNTs grafted by cationic surfactants and negatively charged graphene oxide sheets, followed by KOH activation. The CNTs were intercalated into the nanoporous graphene layers to build pillared 3D structures, which enhance accessible surface area and allow fast ion diffusion. The resulting graphene/CNT films are free-standing and flexible with a high electrical conductivity of 39,400 S m(-1) and a reasonable mass density of 1.06 g cm(-3). The supercapacitors fabricated using these films exhibit an outstanding electrochemical performance in an ionic liquid electrolyte with a maximum energy density of 117.2 Wh L(-1) or 110.6 Wh kg(-1) at a maximum power density of 424 kW L(-1) or 400 kW kg(-1), which is based on thickness or mass of total active material.

Large-area monolayer hexagonal boron nitride on Pt foil.

Hexagonal boron nitride (h-BN) has recently been in the spotlight due to its numerous applications including its being an ideal substrate for two-dimensional electronics, a tunneling material for vertical tunneling devices, and a growth template for heterostructures. However, to obtain a large area of h-BN film while maintaining uniform thickness is still challenging and has not been realized. Here, we report the systematical study of h-BN growth on Pt foil by using low pressure chemical vapor deposition with a borazine source. The monolayer h-BN film was obtained over the whole Pt foil (2 × 5 cm(2)) under <100 mTorr, where the size is limited only by the Pt foil size. A borazine source was catalytically decomposed on the Pt surface, leading to the self-limiting growth of the monolayer without the associating precipitation, which is very similar to the growth of graphene on Cu. The orientation of the h-BN domains was largely confined by the Pt domain, which is confirmed by polarizing optical microscopy (POM) assisted by the nematic liquid crystal (LC) film. The total pressure and orientation of the Pt lattice plane are crucial parameters for thickness control. At high pressure (∼0.5 Torr), thick film was grown on Pt (111), and in contrast, thin film was grown on Pt (001). Our advances in monolayer h-BN growth will play an important role to further develop a high quality h-BN film that can be used for vertical tunneling, optoelectronic devices and growth templates for a variety of heterostructures.