Improving infra-red polarized imaging efficiency in a bilayer wire-grid polarizer.

The optical, plasmonic, and imaging performance of an infra-red polarized system exceeds that of a conventional infra-red detector due to its high resolution and precision. The wire-grid polarizer has large potential for use in an infra-red polarized imaging device owing to its large polarization efficiency. In this study, we theoretically and experimentally investigate a method to improve the polarization efficiency of a wire-grid polarizer. Here, we demonstrated a high-performance wire grid polarizer with a maximum extinction ratio (ER) of 355 using a bilayer structure and dielectric material in the mid-wavelength infra-red (MWIR) region (3000 nm-5000 nm), which is a 4 times higher ER value than that of the monolayer structure. More interestingly, we were able to improve the performance of the bilayer wire-grid polarizer by devising a method to improve the surface roughness using Ar ion milling. The ER for the after-milled sample was 1255, which was markedly larger than that of the before-milled sample. The results of transmittance measurement confirmed that the improvement in the ER was due to the Fabry-Perot (F-P) phenomenon caused by constructive or destructive interference in the bilayer wire-grid structure and the enhancement of the surface smoothness. These results will help design a polarizer structure that will maximize the polarization efficiency and realize a high-performance infrared polarized imaging system.

Graphene nano-electromechanical mass sensor with high resolution at room temperature.

The inherent properties of 2D materials-light mass, high out-of-plane flexibility, and large surface area-promise great potential for precise and accurate nanomechanical mass sensing, but their application is often hampered by surface contamination. Here we demonstrate a tri-layer graphene nanomechanical resonant mass sensor with sub-attogram resolution at room temperature, fabricated by a bottom-up process. We found that Joule-heating is effective in cleaning the graphene membrane surface, which results in a large improvement in the stability of the resonance frequency. We characterized the sensor by depositing Cr metal using a stencil mask and found a mass-resolution that is sufficient to weigh very small particles, like large proteins and protein complexes, with potential applications in the fields of nanobiology and medicine.

Direct probing of phonon mode specific electron-phonon scatterings in two-dimensional semiconductor transition metal dichalcogenides.

Electron-phonon scatterings in solid-state systems are pivotal processes in determining many key physical quantities such as charge carrier mobilities and thermal conductivities. Here, we report direct probing of phonon mode specific electron-phonon scatterings in layered semiconducting transition metal dichalcogenides WSe2, MoSe2, WS2, and MoS2 through inelastic electron tunneling spectroscopy measurements, quantum transport simulations, and density functional calculation. We experimentally and theoretically characterize momentum-conserving single- and two-phonon electron-phonon scatterings involving up to as many as eight individual phonon modes in mono- and bilayer films, among which transverse, longitudinal acoustic and optical, and flexural optical phonons play significant roles in quantum charge flows. Moreover, the layer-number sensitive higher-order inelastic electron-phonon scatterings, which are confirmed to be generic in all four semiconducting layers, can be attributed to differing electronic structures, symmetry, and quantum interference effects during the scattering processes in the ultrathin semiconducting films.

Superconducting Nanoelectromechanical Transducer Resilient to Magnetic Fields.

Nanoscale electromechanical coupling provides a unique route toward control of mechanical motions and microwave fields in superconducting cavity electromechanical devices. However, conventional devices composed of aluminum have presented severe constraints on their operating conditions due to the low superconducting critical temperature (1.2 K) and magnetic field (0.01 T) of aluminum. To enhance their potential in device applications, we fabricate a superconducting electromechanical device employing niobium and demonstrate a set of cavity electromechanical dynamics, including back-action cooling and amplification, and electromechanically induced reflection at 4.2 K and in strong magnetic fields up to 0.8 T. Niobium-based electromechanical transducers operating at this temperature could potentially be employed to realize compact, nonreciprocal microwave devices in place of conventional isolators and cryogenic amplifiers. Moreover, with their resilience to magnetic fields, niobium devices utilizing the electromechanical back-action effects could be used to study spin-phonon interactions for nanomechanical spin-sensing.

Doping effect in graphene-graphene oxide interlayer.

Interlayer coupling in graphene-based van der Waals (vdW) heterostructures plays a key role in determining and modulating their physical properties. Hence, its influence on the optical and electronic properties cannot be overlooked in order to promote various next-generation applications in electronic and opto-electronic devices based on the low-dimensional materials. Herein, the optical and electrical properties of the vertically stacked large area heterostructure of the monolayer graphene transferred onto a monolayer graphene oxide film are investigated. An effective and stable p-doping property of this structure is shown by comparison to that of the graphene device fabricated on a silicon oxide substrate. Through Raman spectroscopy and density functional theory calculations of the charge transport characteristics, it is found that graphene is affected by sustainable p-doping effects induced from underneath graphene oxide even though they have weak interlayer interactions. This finding can facilitate the development of various fascinating graphene-based heterostructures and extend their practical applications in integrated devices with advanced functionalities.

Spectroscopic studies of atomic defects and bandgap renormalization in semiconducting monolayer transition metal dichalcogenides.

Assessing atomic defect states and their ramifications on the electronic properties of two-dimensional van der Waals semiconducting transition metal dichalcogenides (SC-TMDs) is the primary task to expedite multi-disciplinary efforts in the promotion of next-generation electrical and optical device applications utilizing these low-dimensional materials. Here, with electron tunneling and optical spectroscopy measurements with density functional theory, we spectroscopically locate the mid-gap states from chalcogen-atom vacancies in four representative monolayer SC-TMDs-WS2, MoS2, WSe2, and MoSe2-, and carefully analyze the similarities and dissimilarities of the atomic defects in four distinctive materials regarding the physical origins of the missing chalcogen atoms and the implications to SC-mTMD properties. In addition, we address both quasiparticle and optical energy gaps of the SC-mTMD films and find out many-body interactions significantly enlarge the quasiparticle energy gaps and excitonic binding energies, when the semiconducting monolayers are encapsulated by non-interacting hexagonal boron nitride layers.

Nanoelectromechanical graphene switches for the multi-valued logic systems.

Graphene based multi-valued nanoelectromechanical switches are suggested and demonstrated. The device structure having multiple contact sites with different heights under the doubly clamped suspended beam provides multiple contacts to be formed sequentially from the taller electrode to the shorter electrode, which results in multiple logic states. Based on the finite element method simulation, we found that our device characteristics, such as turn-on and threshold voltages, are highly governed by the device design. The proof-of-concept device realized by using a newly developed 3D fabrication method based on the e-beam lithography expresses quaternary logic states successfully with a high stability in repetitive operations.

Ultimate limit in size and performance of WSe2 vertical diodes.

Precise doping-profile engineering in van der Waals heterostructures is a key element to promote optimal device performance in various electrical and optical applications with two-dimensional layered materials. Here, we report tungsten diselenide- (WSe2) based pure vertical diodes with atomically defined p-, i- and n-channel regions. Externally modulated p- and n-doped layers are respectively formed on the bottom and the top facets of WSe2 single crystals by direct evaporations of high and low work-function metals platinum and gadolinium, thus forming atomically sharp p-i-n heterojunctions in the homogeneous WSe2 layers. As the number of layers increases, charge transport through the vertical WSe2 p-i-n heterojunctions is characterized by a series of quantum tunneling events; direct tunneling, Fowler-Nordheim tunneling, and Schottky emission tunneling. With optimally selected WSe2 thickness, our vertical heterojunctions show superb diode characteristics of an unprecedentedly high current density and low turn-on voltages while maintaining good current rectification.

Accurate Gap Determination in Monolayer and Bilayer Graphene/ h-BN Moiré Superlattices.

High mobility single and few-layer graphene sheets are in many ways attractive as nanoelectronic circuit hosts but lack energy gaps, which are essential to the operation of field-effect transistors. One of the methods used to create gaps in the spectrum of graphene systems is to form long period moiré patterns by aligning the graphene and hexagonal boron nitride ( h-BN) substrate lattices. Here, we use planar tunneling devices with thin h-BN barriers to obtain direct and accurate tunneling spectroscopy measurements of the energy gaps in single-layer and bilayer graphene- h-BN superlattice structures at charge neutrality (first Dirac point) and at integer moiré band occupancies (second Dirac point, SDP) as a function of external electric and magnetic fields and the interface twist angle. In single-layer graphene, we find, in agreement with previous work, that gaps are formed at neutrality and at the hole-doped SDP, but not at the electron-doped SDP. Both primary and secondary gaps can be determined accurately by extrapolating Landau fan patterns to a zero magnetic field and are as large as ≈17 meV for devices in near-perfect alignment. For bilayer graphene, we find that gaps occur only at charge neutrality where they can be modified by an external electric field.

Layer dependent magnetoresistance of vertical MoS2 magnetic tunnel junctions.

Spin polarization of electrons through transition metal dichalcogenides (TMDs) from ferromagnetic metals (FMs) is a fascinating phenomenon in condensed matter physics. The spin polarized current makes high- and low-resistance states in FM/TMDs/FM junctions depending on magnetization alignment of FM electrodes. We have manifested vertical spin valve junctions by incorporating MoS2 layers of different thicknesses by an ultraclean fabrication method. The current-voltage (I-V) characteristics show the ohmic contact behavior, indicating that mono-, bi-, and tri-layer MoS2 work as conducting thin film. In contrast, FM/multilayer MoS2/FM junction shows non-linear I-V characteristics and the junction resistance increases as the temperature is lowered, indicating that multilayer MoS2 provides a tunneling barrier between FM electrodes. We have found that the magnetoresistance (MR) ratio increases gradually as the thickness of the MoS2 layer is increased. Our investigation will provide a guide to make an optimal choice in the development of magnetic tunnel junctions with two-dimensional layered TMDs.

Layer number identification of CVD-grown multilayer graphene using Si peak analysis.

Since the successful exfoliation of graphene, various methodologies have been developed to identify the number of layers of exfoliated graphene. The optical contrast, Raman G-peak intensity, and 2D-peak line-shape are currently widely used as the first level of inspection for graphene samples. Although the combination analysis of G- and 2D-peaks is powerful for exfoliated graphene samples, its use is limited in chemical vapor deposition (CVD)-grown graphene because CVD-grown graphene consists of various domains with randomly rotated crystallographic axes between layers, which makes the G- and 2D-peaks analysis difficult for use in number identification. We report herein that the Raman Si-peak intensity can be a universal measure for the number identification of multilayered graphene. We synthesized a few-layered graphene via the CVD method and performed Raman spectroscopy. Moreover, we measured the Si-peak intensities from various individual graphene domains and correlated them with the corresponding layer numbers. We then compared the normalized Si-peak intensity of the CVD-grown multilayer graphene with the exfoliated multilayer graphene as a reference and successfully identified the layer number of the CVD-grown graphene. We believe that this Si-peak analysis can be further applied to various 2-dimensional (2D) materials prepared by both exfoliation and chemical growth.

Nanoscale Structural Switching of Plasmonic Nanograin Layers on Hydrogel Colloidal Monolayers for Highly Sensitive and Dynamic SERS in Water with Areal Signal Reproducibility.

Developing substrates that enable both reproducible and highly sensitive Raman detection of trace amounts of molecules in aqueous systems remains a challenge, although these substrates are crucial in biomedicine and environmental sciences. To address this issue, we report spatially uniform plasmonic nanowrinkles formed by intimate contact between plasmonic nanograins on the surface of colloidal crystal monolayers. The Au or Ag nanograin layers coated on hydrogel colloidal crystal monolayers can reversibly wrinkle and unwrinkle according to changes in the water temperature. The reversible switches are directed by surface structural changes in the colloidal crystal monolayers, while the colloids repeat the hydration-dehydration process. The Au and Ag nanowrinkles are obtained upon hydration, thus enabling the highly reproducible detection of Raman probes in water at the nano- and picomolar levels, respectively, throughout the entire substrate area. Additionally, the reversible switching of the nanostructures in the plasmonic nanograin layers causes reversible dynamic changes in the corresponding Raman signals upon varying the water temperature.

Graphene bubbles and their role in graphene quantum transport.

Graphene bubbles are often formed when graphene and other layered two-dimensional materials are vertically stacked as van der Waals heterostructures. Here, we investigate how graphene bubbles and their related disorder impact the quantum transport behavior of graphene in the absence and presence of external magnetic fields. By combining experimental observations and numerical simulations, we find that the disorder induced by the graphene bubbles is mainly from p-type dopants and the charge transport in pristine graphene can be severely influenced by the presence of bubbles via long- and short-range scattering even with a small bubble-coverage of 2% and below. Upon bubble density increase, we observe an overall decrease in carrier mobility, and the appearance of a second Dirac point on the electron carrier side. At high magnetic fields, the disorder from graphene bubbles primarily impacts the quantization of the lowest Landau level, resulting in quantum Hall features associated with a new Dirac cone at high charge carrier density.

Accurate and Precise Determination of Mechanical Properties of Silicon Nitride Beam Nanoelectromechanical Devices.

Accurate and precise determination of mechanical properties of nanoscale materials is mandatory since device performances of nanoelectromechanical systems (NEMS) are closely related to the flexural properties of the materials. In this study, the intrinsic mechanical properties of highly stressed silicon nitride (SiN) beams of varying lengths are investigated using two different techniques: Dynamic flexural measurement using optical interferometry and quasi-static flexural measurement using atomic force microscopy. The resonance frequencies of the doubly clamped, highly stressed beams are found to be inversely proportional to their length, which is not usually observed from a beam but is expected from a string-like structure. The mass density of the SiN beams can be precisely determined from the dynamic flexural measurements by using the values for internal stress and Young's modulus determined from the quasi-static measurements. As a result, the mass resolution of the SiN beam resonators was predicted to be a few attograms, which was found to be in excellent agreement with the experimental results. This work suggests that accurate and precise determination of mechanical properties can be achieved through combined flexural measurement techniques, which is a crucial key for designing practical NEMS applications such as biomolecular sensors and gas detectors.

Direct Probing of the Electronic Structures of Single-Layer and Bilayer Graphene with a Hexagonal Boron Nitride Tunneling Barrier.

The chemical and mechanical stability of hexagonal boron nitride (h-BN) thin films and their compatibility with other free-standing two-dimensional (2D) crystals to form van der Waals heterostructures make the h-BN-2D tunnel junction an intriguing experimental platform not only for the engineering of specific device functionalities but also for the promotion of quantum measurement capabilities. Here, we exploit the h-BN-graphene tunnel junction to directly probe the electronic structures of single-layer and bilayer graphene in the presence and the absence of external magnetic fields with unprecedented high signal-to-noise ratios. At a zero magnetic field, we identify the tunneling spectra related to the charge neutrality point and the opening of the electric-field-induced bilayer energy gap. In the quantum Hall regime, the quantization of 2D electron gas into Landau levels (LL) is seen as early as 0.2 T, and as many as 30 well-separated LL tunneling conductance oscillations are observed for both electron- and hole-doped regions. Our device simulations successfully reproduce the experimental observations. Additionally, we extract the relative permittivity of three-to-five layer h-BN and find that the screening capability of thin h-BN films is as much as 60% weaker than bulk h-BN.

Engineering Optical and Electronic Properties of WS2 by Varying the Number of Layers.

The optical constants, bandgaps, and band alignments of mono-, bi-, and trilayer WS2 were experimentally measured, and an extraordinarily high dependency on the number of layers was revealed. The refractive indices and extinction coefficients were extracted from the optical-contrast oscillation for various thicknesses of SiO2 on a Si substrate. The bandgaps of the few-layer WS2 were both optically and electrically measured, indicating high exciton-binding energies. The Schottky-barrier heights (SBHs) with Au/Cr contact were also extracted, depending on the number of layers (1-28). From an engineering viewpoint, the bandgap can be modulated from 3.49 to 2.71 eV with additional layers. The SBH can also be reduced from 0.37 eV for a monolayer to 0.17 eV for 28 layers. The technique of engineering materials' properties by modulating the number of layers opens pathways uniquely adaptable to transition-metal dichalcogenides.

Enhancement of resistive switching under confined current path distribution enabled by insertion of atomically thin defective monolayer graphene.

Resistive random access memory (ReRAM) devices have been extensively investigated resulting in significant enhancement of switching properties. However fluctuations in switching parameters are still critical weak points which cause serious failures during 'reading' and 'writing' operations of ReRAM devices. It is believed that such fluctuations may be originated by random creation and rupture of conducting filaments inside ReRAM oxides. Here, we introduce defective monolayer graphene between an oxide film and an electrode to induce confined current path distribution inside the oxide film, and thus control the creation and rupture of conducting filaments. The ReRAM device with an atomically thin interlayer of defective monolayer graphene reveals much reduced fluctuations in switching parameters compared to a conventional one. Our results demonstrate that defective monolayer graphene paves the way to reliable ReRAM devices operating under confined current path distribution.

Bright visible light emission from graphene.

Graphene and related two-dimensional materials are promising candidates for atomically thin, flexible and transparent optoelectronics. In particular, the strong light-matter interaction in graphene has allowed for the development of state-of-the-art photodetectors, optical modulators and plasmonic devices. In addition, electrically biased graphene on SiO2 substrates can be used as a low-efficiency emitter in the mid-infrared range. However, emission in the visible range has remained elusive. Here, we report the observation of bright visible light emission from electrically biased suspended graphene devices. In these devices, heat transport is greatly reduced. Hot electrons (∼2,800 K) therefore become spatially localized at the centre of the graphene layer, resulting in a 1,000-fold enhancement in thermal radiation efficiency. Moreover, strong optical interference between the suspended graphene and substrate can be used to tune the emission spectrum. We also demonstrate the scalability of this technique by realizing arrays of chemical-vapour-deposited graphene light emitters. These results pave the way towards the realization of commercially viable large-scale, atomically thin, flexible and transparent light emitters and displays with low operation voltage and graphene-based on-chip ultrafast optical communications.

Stencil nano lithography based on a nanoscale polymer shadow mask: towards organic nanoelectronics.

A stencil lithography technique has been developed to fabricate organic-material-based electronic devices with sub-micron resolution. Suspended polymethylmethacrylate (PMMA) membranes were used as shadow masks for defining organic channels and top electrodes. Arrays of pentacene field effect transistors (FETs) with various channel lengths from 50 µm down to 500 nm were successfully produced from the same batch using this technique. Electrical transport measurements showed that the electrical contacts of all devices were stable and the normalized contact resistances were much lower than previously studied organic FETs. Scaling effects, originating from the bulk space charge current, were investigated by analyzing the channel-length-dependent mobility and hysteresis behaviors. This novel lithography method provides a reliable means for studying the fundamental transport properties of organic materials at the nanoscale as well as enabling potential applications requiring the fabrication of integrated organic nanoelectronic devices.

Focused-laser-enabled p-n junctions in graphene field-effect transistors.

With its electrical carrier type as well as carrier densities highly sensitive to light, graphene is potentially an ideal candidate for many optoelectronic applications. Beyond the direct light-graphene interactions, indirect effects arising from induced charge traps underneath the photoactive graphene arising from light-substrate interactions must be better understood and harnessed. Here, we study the local doping effect in graphene using focused-laser irradiation, which governs the trapping and ejecting behavior of the charge trap sites in the gate oxide. The local doping effect in graphene is manifested by large Dirac voltage shifts and/or double Dirac peaks from the electrical measurements and a strong photocurrent response due to the formation of a p-n-p junction in gate-dependent scanning photocurrent microscopy. The technique of focused-laser irradiation on a graphene device suggests a new method to control the charge-carrier type and carrier concentration in graphene in a nonintrusive manner as well as elucidate strong light-substrate interactions in the ultimate performance of graphene devices.