Melting of Unidirectional Charge Density Waves across Twin Domain Boundaries in GdTe3.

Solids undergoing a transition from order to disorder experience a proliferation of topological defects. The melting process generates transient quantum states. However, their dynamic nature with a femtosecond lifetime hinders exploration with atomic precision. Here, we suggest an alternative approach to the dynamic melting process by focusing on the interface created by competing degenerate quantum states. We use a scanning tunneling microscope (STM) to visualize the unidirectional charge density wave (CDW) and its spatial progression ("static melting") across a twin domain boundary (TDB) in the layered material GdTe3. Combining the STM with a spatial lock-in technique, we reveal that the order parameter amplitude attenuates with the formation of dislocations and thus two different unidirectional CDWs coexist near the TDB, reducing the CDW anisotropy. Notably, we discovered a correlation between this anisotropy and the CDW gap. Our study provides valuable insight into the behavior of topological defects and transient quantum states.

Luminance enhancement of top-emitting blue organic light emitting diodes encapsulated with silicon nitride thin films by a double-layer nano-structure.

Even though it is in high demand to introduce a nano-structure (NS) light extraction technology on a silicon nitride to be used as a thin film encapsulation material for an organic light-emitting diode (OLED), only an industry-incompatible wet method has been reported. This work demonstrates a double-layer NS fabrication on the silicon nitride using a two-step organic vapor phase deposition (OVPD) of an industry-compatible dry process. The NS showed a wrinkle-like shape caused by coalescence of the nano-lenses. The NS integrated top-emitting OLED revealed 40 percent enhancement of current efficiency and improvement of the luminance distribution and color change according to viewing angle.

Origin of the Insulating Phase and First-Order Metal-Insulator Transition in 1T-TaS_{2}.

Using density functional theory calculations, we investigate the origin of the insulating phase and metal-insulator transition (MIT) in octahedral tantalum disulfide (1T-TaS_{2}), a layered van der Waals material with a prominent two-dimensional (2D) charge density wave (CDW) order. We show that the MIT is driven not by the 2D order itself, but by the vertical ordering of the 2D CDWs or the 3D CDW order. We identify two exceptionally stable 3D CDW configurations; one is insulating and the other is metallic. The competition and mixing of the two CDW configurations account for many mysterious features of the MIT in 1T-TaS_{2}, including the pressure- and doping-induced transitions and the hysteresis behavior. The present results emphasize that interlayer electronic ordering can play an important role in electronic phase transitions in layered materials.

Nanofabricated tips for device-based scanning tunneling microscopy.

We report on the fabrication and performance of a new kind of tip for scanning tunneling microscopy. By fully incorporating a metallic tip on a silicon chip using modern micromachining and nanofabrication techniques, we realize so-called smart tips and show the possibility of device-based STM tips. Contrary to conventional etched metal wire tips, these can be integrated into lithographically defined electrical circuits. We describe a new fabrication method to create a defined apex on a silicon chip and experimentally demonstrate the high performance of the smart tips, both in stability and resolution. In situ tip preparation methods are possible and we verify that they can resolve the herringbone reconstruction and Friedel oscillations on Au(111) surfaces. We further present an overview of possible applications.

Overcoming the efficiency limit of organic light-emitting diodes using ultra-thin and transparent graphene electrodes.

We propose an effective way to enhance the out-coupling efficiencies of organic light-emitting diodes (OLEDs) using graphene as a transparent electrode. In this study, we investigated the detrimental adsorption and internal optics occurring in OLEDs with graphene anodes. The optical out-coupling efficiencies of previous OLEDs with transparent graphene electrodes barely exceeded those of OLEDs with conventional transparent electrodes because of the weak microcavity effect. To overcome this issue, we introduced an internal random scattering layer for light extraction and reduced the optical absorption of the graphene by reducing the number of layers in the multilayered graphene film. The efficiencies of the graphene-OLEDs increased significantly with decreasing the number of graphene layers, strongly indicating absorption reduction. The maximum light extraction efficiency was obtained by using a single-layer graphene electrode together with a scattering layer. As a result, a widened angular luminance distribution with a remarkable external quantum efficiency and a luminous efficacy enhancement of 52.8% and 48.5%, respectively, was achieved. Our approach provides a demonstration of graphene-OLED having a performance comparable to that of conventional OLEDs.

Simultaneously enhanced device efficiency, stabilized chromaticity of organic light emitting diodes with lambertian emission characteristic by random convex lenses.

An optical functional film applicable to various lighting devices is demonstrated in this study. The phase separation of two immiscible polymers in a common solvent was used to fabricate the film. In this paper, a self-organized lens-like structure is realized in this manner with optical OLED functional film. For an OLED, there are a few optical drawbacks, including light confinement or viewing angle distortion. By applying the optical film to an OLED, the angular spectra distortion resulting from the designed organic stack which produced the highest efficiency was successfully stabilized, simultaneously enhancing the efficiency of the OLED. We prove the effect of the film on the efficiency of OLEDs through an optical simulation. With the capability to overcome the main drawbacks of OLEDs, we contend that the proposed film can be applied to various lighting devices.

FDTD analysis of the light extraction efficiency of OLEDs with a random scattering layer.

The light extraction efficiency of OLEDs with a nano-sized random scattering layer (RSL-OLEDs) was analyzed using the Finite Difference Time Domain (FDTD) method. In contrast to periodic diffraction patterns, the presence of an RSL suppresses the spectral shift with respect to the viewing angle. For FDTD simulation of RSL-OLEDs, a planar light source with a certain spatial and temporal coherence was incorporated, and the light extraction efficiency with respect to the fill factor of the RSL and the absorption coefficient of the material was investigated. The design results were compared to the experimental results of the RSL-OLEDs in order to confirm the usefulness of FDTD in predicting experimental results. According to our FDTD simulations, the light confined within the ITO-organic waveguide was quickly absorbed, and the absorption coefficients of ITO and RSL materials should be reduced in order to obtain significant improvement in the external quantum efficiency (EQE). When the extinction coefficient of ITO was 0.01, the EQE in the RSL-OLED was simulated to be enhanced by a factor of 1.8.

Light diffusing effects of nano and micro-structures on OLED with microcavity.

We examined the light diffusing effects of nano and micro-structures on microcavity designed OLEDs. The results of FDTD simulations and experiments showed that the pillar shaped nano-structure was more effective than the concave micro-structure for light diffusing of microcavity OLEDs. The sharp luminance distribution of the microcavity OLED was changed to near Lambertian luminance distribution by the nano-structure, and light diffusing effects increased with the height of the nano-structure. Furthermore, the nano-structure has advantages including light extraction of the substrate mode, reproducibility of manufacturing process, and minimizing pixel blur problems in an OLED display panel. The nano-structure is a promising candidate for a light diffuser, resolving the viewing angle problems in microcavity OLEDs.

Random nanostructure scattering layer for suppression of microcavity effect and light extraction in OLEDs.

In this study, we investigated the effect of a random nanostructure scattering layer (RSL) on the microcavity and light extraction in organic light emitting diodes (OLEDs). In the case of the conventional OLED, the optical properties change with the thickness of the hole transporting layer (HTL) because of the presence of a microcavity. However, OLEDs equipped with the an RSL showed similar values of external quantum efficiency and luminous efficacy regardless of the HTL thickness. These phenomena can be understood by the scattering effect because of the RSL, which suppresses the microcavity effect and extracts the light confined in the device. Moreover, OLEDs with the RSL led to reduced spectrum and color changes with the viewing angle.

Time-resolved energy transduction in a quantum capacitor.

The capability to deposit charge and energy quantum-by-quantum into a specific atomic site could lead to many previously unidentified applications. Here we report on the quantum capacitor formed by a strongly localized field possessing such capability. We investigated the charging dynamics of such a capacitor by using the unique scanning tunneling microscopy that combines nanosecond temporal and subangstrom spatial resolutions, and by using Si(001) as the electrode as well as the detector for excitations produced by the charging transitions. We show that sudden switching of a localized field induces a transiently empty quantum dot at the surface and that the dot acts as a tunable excitation source with subangstrom site selectivity. The timescale in the deexcitation of the dot suggests the formation of long-lived, excited states. Our study illustrates that a quantum capacitor has serious implications not only for the bottom-up nanotechnology but also for future switching devices.

Origin of Distinct Insulating Domains in the Layered Charge Density Wave Material 1T-TaS2.

Vertical charge order shapes the electronic properties in layered charge density wave (CDW) materials. Various stacking orders inevitably create nanoscale domains with distinct electronic structures inaccessible to bulk probes. Here, the stacking characteristics of bulk 1T-TaS2 are analyzed using scanning tunneling spectroscopy (STS) and density functional theory (DFT) calculations. It is observed that Mott-insulating domains undergo a transition to band-insulating domains restoring vertical dimerization of the CDWs. Furthermore, STS measurements covering a wide terrace reveal two distinct band insulating domains differentiated by band edge broadening. These DFT calculations reveal that the Mott insulating layers preferably reside on the subsurface, forming broader band edges in the neighboring band insulating layers. Ultimately, buried Mott insulating layers believed to harbor the quantum spin liquid phase are identified. These results resolve persistent issues regarding vertical charge order in 1T-TaS2, providing a new perspective for investigating emergent quantum phenomena in layered CDW materials.

Wafer-Scale Synthesis of Highly Oriented 2D Topological Semimetal PtTe2 via Tellurization.

Platinum ditelluride (1T-PtTe2) is a two-dimensional (2D) topological semimetal with a distinctive band structure and flexibility of van der Waals integration as a promising candidate for future electronics and spintronics. Although the synthesis of large-scale, uniform, and highly crystalline films of 2D semimetals system is a prerequisite for device application, the synthetic methods meeting these criteria are still lacking. Here, we introduce an approach to synthesize highly oriented 2D topological semimetal PtTe2 using a thermally assisted conversion called tellurization, which is a cost-efficient method compared to the other epitaxial deposition methods. We demonstrate that achieving highly crystalline 1T-PtTe2 using tellurization is not dependent on epitaxy but rather relies on two critical factors: (i) the crystallinity of the predeposited platinum (Pt) film and (ii) the surface coverage ratio of the Pt film considering lateral lattice expansion during transformation. By optimizing the surface coverage ratio of the epitaxial Pt film, we successfully obtained 2 in. wafer-scale uniformity without in-plane misalignment between antiparallelly oriented domains. The electronic band structure of 2D topological PtTe2 is clearly resolved in momentum space, and we observed an interesting 6-fold gapped Dirac cone at the Fermi surface. Furthermore, ultrahigh electrical conductivity down to ∼3.8 nm, which is consistent with that of single crystal PtTe2, was observed, proving its ultralow defect density.

Charge density wave surface reconstruction in a van der Waals layered material.

Surface reconstruction plays a vital role in determining the surface electronic structure and chemistry of semiconductors and metal oxides. However, it has been commonly believed that surface reconstruction does not occur in van der Waals layered materials, as they do not undergo significant bond breaking during surface formation. In this study, we present evidence that charge density wave (CDW) order in these materials can, in fact, cause CDW surface reconstruction through interlayer coupling. Using density functional theory calculations on the 1T-TaS2 surface, we reveal that CDW reconstruction, involving concerted small atomic displacements in the subsurface layer, results in a significant modification of the surface electronic structure, transforming it from a Mott insulator to a band insulator. This new form of surface reconstruction explains several previously unexplained observations on the 1T-TaS2 surface and has important implications for interpreting surface phenomena in CDW-ordered layered materials.

Single-electron charge transfer into putative Majorana and trivial modes in individual vortices.

Majorana bound states are putative collective excitations in solids that exhibit the self-conjugate property of Majorana fermions-they are their own antiparticles. In iron-based superconductors, zero-energy states in vortices have been reported as potential Majorana bound states, but the evidence remains controversial. Here, we use scanning tunneling noise spectroscopy to study the tunneling process into vortex bound states in the conventional superconductor NbSe2, and in the putative Majorana platform FeTe0.55Se0.45. We find that tunneling into vortex bound states in both cases exhibits charge transfer of a single electron charge. Our data for the zero-energy bound states in FeTe0.55Se0.45 exclude the possibility of Yu-Shiba-Rusinov states and are consistent with both Majorana bound states and trivial vortex bound states. Our results open an avenue for investigating the exotic states in vortex cores and for future Majorana devices, although further theoretical investigations involving charge dynamics and superconducting tips are necessary.

Light extraction from organic light emitting diodes using chemically etched glass substrates.

We have manufactured highly efficient OLED devices fabricated on chemically etched glass substrates. The external quantum efficiency of the OLED devices with the etched glass substrates was increased by 5-27% in comparison with the reference flat glass substrate. Surface morphology, such as indented patterns, significantly affected the external luminance efficiency. A clean surface and the presence of smooth bent edges of indented patterns were found to be important for improving the external luminous efficacy.

Spatially dispersing Yu-Shiba-Rusinov states in the unconventional superconductor FeTe0.55Se0.45.

By using scanning tunneling microscopy (STM) we find and characterize dispersive, energy-symmetric in-gap states in the iron-based superconductor FeTe0.55Se0.45, a material that exhibits signatures of topological superconductivity, and Majorana bound states at vortex cores or at impurity locations. We use a superconducting STM tip for enhanced energy resolution, which enables us to show that impurity states can be tuned through the Fermi level with varying tip-sample distance. We find that the impurity state is of the Yu-Shiba-Rusinov (YSR) type, and argue that the energy shift is caused by the low superfluid density in FeTe0.55Se0.45, which allows the electric field of the tip to slightly penetrate the sample. We model the newly introduced tip-gating scenario within the single-impurity Anderson model and find good agreement to the experimental data.

Direct evidence for Cooper pairing without a spectral gap in a disordered superconductor above Tc.

The idea that preformed Cooper pairs could exist in a superconductor at temperatures higher than its zero-resistance critical temperature (Tc) has been explored for unconventional, interfacial, and disordered superconductors, but direct experimental evidence is lacking. We used scanning tunneling noise spectroscopy to show that preformed Cooper pairs exist up to temperatures much higher than Tc in the disordered superconductor titanium nitride by observing an enhancement in the shot noise that is equivalent to a change of the effective charge from one to two electron charges. We further show that the spectroscopic gap fills up rather than closes with increasing temperature. Our results demonstrate the existence of a state above Tc that, much like an ordinary metal, has no (pseudo)gap but carries charge through paired electrons.

Optical Analysis of Power Distribution in Top-Emitting Organic Light Emitting Diodes Integrated with Nanolens Array Using Finite Difference Time Domain.

Recently, we have addressed that a formation mechanism of a nanolens array (NLA) fabricated by using a maskless vacuum deposition is explained as the increase in surface tension of organic molecules induced by their crystallization. Here, as another research using finite difference time domain simulations, not electric field intensities but transmitted energies of electromagnetic waves inside and outside top-emitting blue organic light-emitting diodes (TOLEDs), without and with NLAs, are obtained, to easily grasp the effect of NLA formation on the light extraction of TOLEDs. Interestingly, the calculations show that NLA acts as an efficient light extraction structure. With NLA, larger transmitted energies in the direction from emitting layer to air are observed, indicating that NLAs send more light to air otherwise trapped in the devices by reducing the losses by waveguide and absorption. This is more significant for higher refractive index of NLA. Simulation and measurement results are consistent. A successful increase in both light extraction efficiency and color stability of blue TOLEDs, rarely reported before, is accomplished by introducing the highly process-compatible NLA technology using the one-step dry process. Blue TOLEDs integrated with a N, N'-di(1-naphthyl)- N, N'-diphenyl-(1,1'-biphenyl)-4,4'-diamine NLA with a refractive index of 1.8 show a 1.55-times-higher light extraction efficiency, compared to those without it. In addition, viewing angle characteristics are enhanced and image blurring is reduced, indicating that the manufacturer-adaptable technology satisfies the requirements of highly efficient and color-stable top-emission displays.

Correlated electronic states at domain walls of a Mott-charge-density-wave insulator 1T-TaS2.

Domain walls in interacting electronic systems can have distinct localized states, which often govern physical properties and may lead to unprecedented functionalities and novel devices. However, electronic states within domain walls themselves have not been clearly identified and understood for strongly correlated electron systems. Here, we resolve the electronic states localized on domain walls in a Mott-charge-density-wave insulator 1T-TaS2 using scanning tunneling spectroscopy. We establish that the domain wall state decomposes into two nonconducting states located at the center of domain walls and edges of domains. Theoretical calculations reveal their atomistic origin as the local reconstruction of domain walls under the strong influence of electron correlation. Our results introduce a concept for the domain wall electronic property, the walls own internal degrees of freedom, which is potentially related to the controllability of domain wall electronic properties.The electronic states within domain walls in an interacting electronic system remain elusive. Here, Cho et al. report that the domain wall state in a charge-density-wave insulator 1T-TaS2 decomposes into two localized but nonconducting states at the center or edges of domain walls.

Crystallization-assisted nano-lens array fabrication for highly efficient and color stable organic light emitting diodes.

To date, all deposition equipment has been developed to produce planar films. Thus lens arrays with a lens diameter of <1 mm have been manufactured by combining deposition with other technologies, such as masks, surface treatment, molding etc. Furthermore, a nano-lens array (NLA) with a sufficiently small lens diameter (<1 µm) is necessary to avoid image quality degradation in high resolution displays. In this study, an organic NLA made using a conventional deposition technique - without combining with other techniques - is reported. Very interestingly, grazing-incidence small-angle X-ray scattering (GI-SAXS) experiments indicate that the NLA is formed by the crystallization of organic molecules and the resulting increase in surface tension. The lens diameter can be tuned for use with any kind of light by controlling the process parameters. As an example of their potential applications, we use NLAs as a light extraction film for organic light emitting diodes (OLEDs). The NLA is integrated by directly depositing it on the top electrode of a collection of OLEDs. This is a dry process, meaning that it is fully compatible with the current OLED production process. Devices with NLAs exhibited a light extraction efficiency 1.5 times higher than devices without, which corresponds well with simulation results. The simulations show that this high efficiency is due to the reduction of the guided modes by scattering at the NLA. The NLAs also reduce image blurring, indicating that they increase color stability.