Photoluminescence Induced by Substitutional Nitrogen in Single-Layer Tungsten Disulfide.

The electronic and optical properties of two-dimensional materials can be strongly influenced by defects, some of which can find significant implementations, such as controllable doping, prolonged valley lifetime, and single-photon emissions. In this work, we demonstrate that defects created by remote N2 plasma exposure in single-layer WS2 can induce a distinct low-energy photoluminescence (PL) peak at 1.59 eV, which is in sharp contrast to that caused by remote Ar plasma. This PL peak has a critical requirement on the N2 plasma exposure dose, which is strongest for WS2 with about 2.0% sulfur deficiencies (including substitutions and vacancies) and vanishes at 5.6% or higher sulfur deficiencies. Both experiments and first-principles calculations suggest that this 1.59 eV PL peak is caused by defects related to the sulfur substitutions by nitrogen, even though low-temperature PL measurements also reveal that not all the sulfur vacancies are remedied by the substitutional nitrogen. The distinct low-energy PL peak suggests that the substitutional nitrogen defect in single-layer WS2 can potentially serve as an isolated artificial atom for creating single-photon emitters, and its intensity can also be used to monitor the doping concentrations of substitutional nitrogen.

A Library of Atomically Thin 2D Materials Featuring the Conductive-Point Resistive Switching Phenomenon.

Non-volatile resistive switching (NVRS) is a widely available effect in transitional metal oxides, colloquially known as memristors, and of broad interest for memory technology and neuromorphic computing. Until recently, NVRS was not known in other transitional metal dichalcogenides (TMDs), an important material class owing to their atomic thinness enabling the ultimate dimensional scaling. Here, various monolayer or few-layer 2D materials are presented in the conventional vertical structure that exhibit NVRS, including TMDs (MX2 , M = transitional metal, e.g., Mo, W, Re, Sn, or Pt; X = chalcogen, e.g., S, Se, or Te), TMD heterostructure (WS2 /MoS2 ), and an atomically thin insulator (h-BN). These results indicate the universality of the phenomenon in 2D non-conductive materials, and feature low switching voltage, large ON/OFF ratio, and forming-free characteristic. A dissociation-diffusion-adsorption model is proposed, attributing the enhanced conductance to metal atoms/ions adsorption into intrinsic vacancies, a conductive-point mechanism supported by first-principle calculations and scanning tunneling microscopy characterizations. The results motivate further research in the understanding and applications of defects in 2D materials.

Observation of single-defect memristor in an MoS2 atomic sheet.

Non-volatile resistive switching, also known as memristor1 effect, where an electric field switches the resistance states of a two-terminal device, has emerged as an important concept in the development of high-density information storage, computing and reconfigurable systems2-9. The past decade has witnessed substantial advances in non-volatile resistive switching materials such as metal oxides and solid electrolytes. It was long believed that leakage currents would prevent the observation of this phenomenon for nanometre-thin insulating layers. However, the recent discovery of non-volatile resistive switching in two-dimensional monolayers of transition metal dichalcogenide10,11 and hexagonal boron nitride12 sandwich structures (also known as atomristors) has refuted this belief and added a new materials dimension owing to the benefits of size scaling10,13. Here we elucidate the origin of the switching mechanism in atomic sheets using monolayer MoS2 as a model system. Atomistic imaging and spectroscopy reveal that metal substitution into a sulfur vacancy results in a non-volatile change in the resistance, which is corroborated by computational studies of defect structures and electronic states. These findings provide an atomistic understanding of non-volatile switching and open a new direction in precision defect engineering, down to a single defect, towards achieving the smallest memristor for applications in ultra-dense memory, neuromorphic computing and radio-frequency communication systems2,3,11.

Detection of the Spin-Chemical Potential in Topological Insulators Using Spin-Polarized Four-Probe STM.

We demonstrate a new method for the detection of the spin-chemical potential in topological insulators using spin-polarized four-probe scanning tunneling microscopy on in situ cleaved Bi_{2}Te_{2}Se surfaces. Two-dimensional (2D) surface and 3D bulk conductions are separated quantitatively via variable probe-spacing measurements, enabling the isolation of the nonvanishing spin-dependent electrochemical potential from the Ohmic contribution. This component is identified as the spin-chemical potential arising from the 2D charge current through the spin momentum locked topological surface states (TSS). This method provides a direct measurement of spin current generation efficiency and opens a new avenue to access the intrinsic spin transport associated with pristine TSS.

Isoelectronic Tungsten Doping in Monolayer MoSe2 for Carrier Type Modulation.

Carrier-type modulation is demonstrated in 2D transition metal dichalcogenides as n-type monolayer MoSe2 is converted to nondegenerate p-type monolayer Mo1-x Wx Se2 through isoelectronic doping. Although the alloys are mesoscopically uniform, the p-type conduction in monolayer Mo1-x Wx Se2 appears to originate from the upshift of the valenceband maximum toward the Fermi level at highly localized "W-rich" regions in the lattice.

High-throughput electrical measurement and microfluidic sorting of semiconductor nanowires.

Existing nanowire electrical characterization tools not only are expensive and require sophisticated facilities, but are far too slow to enable statistical characterization of highly variable samples. They are also generally not compatible with further sorting and processing of nanowires. Here, we demonstrate a high-throughput, solution-based electro-orientation-spectroscopy (EOS) method, which is capable of automated electrical characterization of individual nanowires by direct optical visualization of their alignment behavior under spatially uniform electric fields of different frequencies. We demonstrate that EOS can quantitatively characterize the electrical conductivities of nanowires over a 6-order-of-magnitude range (10(-5) to 10 S m(-1), corresponding to typical carrier densities of 10(10)-10(16) cm(-3)), with different fluids used to suspend the nanowires. By implementing EOS in a simple microfluidic device, continuous electrical characterization is achieved, and the sorting of nanowires is demonstrated as a proof-of-concept. With measurement speeds two orders of magnitude faster than direct-contact methods, the automated EOS instrument enables for the first time the statistical characterization of highly variable 1D nanomaterials.

Differentiation of Surface and Bulk Conductivities in Topological Insulators via Four-Probe Spectroscopy.

We show a new method to differentiate conductivities from the surface states and the coexisting bulk states in topological insulators using a four-probe transport spectroscopy in a multiprobe scanning tunneling microscopy system. We derive a scaling relation of measured resistance with respect to varying interprobe spacing for two interconnected conduction channels to allow quantitative determination of conductivities from both channels. Using this method, we demonstrate the separation of 2D and 3D conduction in topological insulators by comparing the conductance scaling of Bi2Se3, Bi2Te2Se, and Sb-doped Bi2Se3 against a pure 2D conductance of graphene on SiC substrate. We also quantitatively show the effect of surface doping carriers on the 2D conductance enhancement in topological insulators. The method offers a means to understanding not just the topological insulators but also the 2D to 3D crossover of conductance in other complex systems.

Contactless Determination of Electrical Conductivity of One-Dimensional Nanomaterials by Solution-Based Electro-orientation Spectroscopy.

Nanowires of the same composition, and even fabricated within the same batch, often exhibit electrical conductivities that can vary by orders of magnitude. Unfortunately, existing electrical characterization methods are time-consuming, making the statistical survey of highly variable samples essentially impractical. Here, we demonstrate a contactless, solution-based method to efficiently measure the electrical conductivity of 1D nanomaterials based on their transient alignment behavior in ac electric fields of different frequencies. Comparison with direct transport measurements by probe-based scanning tunneling microscopy shows that electro-orientation spectroscopy can quantitatively measure nanowire conductivity over a 5-order-of-magnitude range, 10(-5)-1 Ω(-1) m(-1) (corresponding to resistivities in the range 10(2)-10(7) Ω·cm). With this method, we statistically characterize the conductivity of a variety of nanowires and find significant variability in silicon nanowires grown by metal-assisted chemical etching from the same wafer. We also find that the active carrier concentration of n-type silicon nanowires is greatly reduced by surface traps and that surface passivation increases the effective conductivity by an order of magnitude. This simple method makes electrical characterization of insulating and semiconducting 1D nanomaterials far more efficient and accessible to more researchers than current approaches. Electro-orientation spectroscopy also has the potential to be integrated with other solution-based methods for the high-throughput sorting and manipulation of 1D nanomaterials for postgrowth device assembly.