Topography and probability diagram of cervical and intra-parotid lymph node metastasis in parotid gland cancer.

In parotid gland cancer (PGC), cervical lymph node metastasis (LNM) and intra-parotid LNM are known as significant indicators of poor prognosis. However, the topography of LNM in the affected parotid gland and the lymphatic progression of PGC has never been explored in detail. This was a retrospective analysis of data from 423 patients with previously untreated primary PGC (2005 to 2020), excluding patients with squamous cell carcinoma, lymphoma or metastatic disease in the parotid gland. The pattern of LNM was analyzed by neck sub-level and parotid sub-site. Using the conditional probability of neck level involvement, a probability diagram was plotted on several thresholds to visualize the sequential progression of LNM in PGC. The pattern of LNM progression was found to be similar between low- and high-grade pathology, but the incidence differed significantly (8.0% vs. 45.4%). Intra-parotid LNs and level IIa LNs were the most common sites (57.3% and 61.0%) of LNM in PGC, followed by level III (31.7%), Ib (25.6%), IV (22.0%), IIb (20.7%) and Va (20.7%) LNM. In intra-parotid LNs, the incidence of LNM in the deep parotid LNs was relatively low (9.4%); most intra-parotid LNMs were observed in the superficial parotid (90.6%) and peri-tumoral (in contact with the tumor) (31.3%) LNs. LNM to levels Ia, Vb and contra-lateral LNM occurred only in the very late stage. Our results provide detailed information about LNM progression in PGC at the sub-level and can help clinicians decide the treatment extent, including surgery or radiation.

Correction to: Cellular and biomolecular detection based on suspended microchannel resonators.

[This corrects the article DOI: 10.1007/s13534-021-00207-7.].

PCA-based sub-surface structure and defect analysis for germanium-on-nothing using nanoscale surface topography.

Empty space in germanium (ESG) or germanium-on-nothing (GON) are unique self-assembled germanium structures with multiscale cavities of various morphologies. Due to their simple fabrication process and high-quality crystallinity after self-assembly, they can be applied in various fields including micro-/nanoelectronics, optoelectronics, and precision sensors, to name a few. In contrast to their simple fabrication, inspection is intrinsically difficult due to buried structures. Today, ultrasonic atomic force microscopy and interferometry are some prevalent non-destructive 3-D imaging methods that are used to inspect the underlying ESG structures. However, these non-destructive characterization methods suffer from low throughput due to slow measurement speed and limited measurable thickness. To overcome these limitations, this work proposes a new methodology to construct a principal-component-analysis based database that correlates surface images with empirically determined sub-surface structures. Then, from this database, the morphology of buried sub-surface structure is determined only using surface topography. Since the acquisition rate of a single nanoscale surface micrograph is up to a few orders faster than a thorough 3-D sub-surface analysis, the proposed methodology benefits from improved throughput compared to current inspection methods. Also, an empirical destructive test essentially resolves the measurable thickness limitation. We also demonstrate the practicality of the proposed methodology by applying it to GON devices to selectively detect and quantitatively analyze surface defects. Compared to state-of-the-art deep learning-based defect detection schemes, our method is much effortlessly finetunable for specific applications. In terms of sub-surface analysis, this work proposes a fast, robust, and high-resolution methodology which could potentially replace the conventional exhaustive sub-surface inspection schemes.

Heusler-based synthetic antiferrimagnets.

Antiferromagnet spintronic devices eliminate or mitigate long-range dipolar fields, thereby promising ultrafast operation. For spin transport electronics, one of the most successful strategies is the creation of metallic synthetic antiferromagnets, which, to date, have largely been formed from transition metals and their alloys. Here, we show that synthetic antiferrimagnetic sandwiches can be formed using exchange coupling spacer layers composed of atomically ordered RuAl layers and ultrathin, perpendicularly magnetized, tetragonal ferrimagnetic Heusler layers. Chemically ordered RuAl layers can both be grown on top of a Heusler layer and allow for the growth of ordered Heusler layers deposited on top of it that are as thin as one unit cell. The RuAl spacer layer gives rise to a thickness-dependent oscillatory interlayer coupling with an oscillation period of ~1.1 nm. The observation of ultrathin ordered synthetic antiferrimagnets substantially expands the family of synthetic antiferromagnets and magnetic compounds for spintronic technologies.

Cellular and biomolecular detection based on suspended microchannel resonators.

Suspended microchannel resonators (SMRs) have been developed to measure the buoyant mass of single micro-/nanoparticles and cells suspended in a liquid. They have significantly improved the mass resolution with the aid of vacuum packaging and also increased measurement throughput by fast resonance frequency tracking while target objects travel through the microchannel without stopping or even slowing down. Since their invention, various biological applications have been enabled, including simultaneous measurements of cell growth and cell cycle progression, and measurements of disease associated physicochemical change, to name a few. Extension and advancement towards other promising applications with SMRs are continuously ongoing by adding multiple functionalities or incorporating other complementary analytical metrologies. In this paper, we will thoroughly review the development history, basic and advanced operations, and key applications of SMRs to introduce them to researchers working in biological and biomedical sciences who mostly rely on classical and conventional methodologies. We will also provide future perspectives and projections for SMR technologies.

Pyropia yezoensis Extract Suppresses IFN-Gamma- and TNF-Alpha-Induced Proinflammatory Chemokine Production in HaCaT Cells via the Down-Regulation of NF-κB.

Pyropia yezoensis, a red alga, is popular and harvested a lot in East Asia and is famous for its medicinal properties attributable to its bioactive compounds including amino acids (porphyra-334 and shinorine, etc.), polysaccharides, phytosterols, and pigments, but its anti-inflammatory effect and mechanism of anti-atopic dermatitis (AD) have not been elucidated. In this study, we investigate the anti-AD effect of P. yezoensis extract (PYE) on mRNA and protein levels of the pro-inflammatory chemokines, thymus, and activation-regulated chemokine (TARC/CCL17) and macrophage-derived chemokine (MDC/CCL22), in human HaCaT keratinocyte cells treated to interferon (IFN)-γ or tumor necrosis factor (TNF)-α (10 ng/mL each). The effect of the PYE on extracellular signal-regulated kinase (ERK) and other mitogen-activated protein kinases (MAPKs) was related to its suppression of TARC and MDC production by blocking NF-κB activation in HaCaT cells. Furthermore, astaxanthin and xanthophyll from P. yezoensis were identified as anti-AD candidate compounds. These results suggest that the PYE may improve AD and contained two carotenoids by regulating pro-inflammatory chemokines.

Fast Spiking of a Mott VO2-Carbon Nanotube Composite Device.

The recent surge of interest in brain-inspired computing and power-efficient electronics has dramatically bolstered development of computation and communication using neuron-like spiking signals. Devices that can produce rapid and energy-efficient spiking could significantly advance these applications. Here we demonstrate direct current or voltage-driven periodic spiking with sub-20 ns pulse widths from a single device composed of a thin VO2 film with a metallic carbon nanotube as a nanoscale heater, without using an external capacitor. Compared with VO2-only devices, adding the nanotube heater dramatically decreases the transient duration and pulse energy, and increases the spiking frequency, by up to 3 orders of magnitude. This is caused by heating and cooling of the VO2 across its insulator-metal transition being localized to a nanoscale conduction channel in an otherwise bulk medium. This result provides an important component of energy-efficient neuromorphic computing systems and a lithography-free technique for energy-scaling of electronic devices that operate via bulk mechanisms.

Localized Triggering of the Insulator-Metal Transition in VO2 Using a Single Carbon Nanotube.

Vanadium dioxide (VO2) has been widely studied for its rich physics and potential applications, undergoing a prominent insulator-metal transition (IMT) near room temperature. The transition mechanism remains highly debated, and little is known about the IMT at nanoscale dimensions. To shed light on this problem, here we use ∼1 nm-wide carbon nanotube (CNT) heaters to trigger the IMT in VO2. Single metallic CNTs switch the adjacent VO2 at less than half the voltage and power required by control devices without a CNT, with switching power as low as ∼85 µW at 300 nm device lengths. We also obtain potential and temperature maps of devices during operation using Kelvin probe microscopy and scanning thermal microscopy. Comparing these with three-dimensional electrothermal simulations, we find that the local heating of the VO2 by the CNT plays a key role in the IMT. These results demonstrate the ability to trigger IMT in VO2 using nanoscale heaters and highlight the significance of thermal engineering to improve device behavior.

Chiral domain wall motion in unit-cell thick perpendicularly magnetized Heusler films prepared by chemical templating.

Heusler alloys are a large family of compounds with complex and tunable magnetic properties, intimately connected to the atomic scale ordering of their constituent elements. We show that using a chemical templating technique of atomically ordered X'Z' (X' = Co; Z' = Al, Ga, Ge, Sn) underlayers, we can achieve near bulk-like magnetic properties in tetragonally distorted Heusler films, even at room temperature. Excellent perpendicular magnetic anisotropy is found in ferrimagnetic X3Z (X = Mn; Z = Ge, Sn, Sb) films, just 1 or 2 unit-cells thick. Racetracks formed from these films sustain current-induced domain wall motion with velocities of more than 120 m s-1, at current densities up to six times lower than conventional ferromagnetic materials. We find evidence for a significant bulk chiral Dzyaloshinskii-Moriya exchange interaction, whose field strength can be systematically tuned by an order of magnitude. Our work is an important step towards practical applications of Heusler compounds for spintronic technologies.

3D Printed Polymer Photodetectors.

Extrusion-based 3D printing, an emerging technology, has been previously used in the comprehensive fabrication of light-emitting diodes using various functional inks, without cleanrooms or conventional microfabrication techniques. Here, polymer-based photodetectors exhibiting high performance are fully 3D printed and thoroughly characterized. A semiconducting polymer ink is printed and optimized for the active layer of the photodetector, achieving an external quantum efficiency of 25.3%, which is comparable to that of microfabricated counterparts and yet created solely via a one-pot custom built 3D-printing tool housed under ambient conditions. The devices are integrated into image sensing arrays with high sensitivity and wide field of view, by 3D printing interconnected photodetectors directly on flexible substrates and hemispherical surfaces. This approach is further extended to create integrated multifunctional devices consisting of optically coupled photodetectors and light-emitting diodes, demonstrating for the first time the multifunctional integration of multiple semiconducting device types which are fully 3D printed on a single platform. The 3D-printed optoelectronic devices are made without conventional microfabrication facilities, allowing for flexibility in the design and manufacturing of next-generation wearable and 3D-structured optoelectronics, and validating the potential of 3D printing to achieve high-performance integrated active electronic materials and devices.

Evidence for Ionic Liquid Gate-Induced Metallization of Vanadium Dioxide Bars over Micron Length Scales.

It has recently been shown that the metal-insulator transition in vanadium dioxide epitaxial films can be suppressed and the material made metallic to low temperatures by ionic liquid gating due to migration of oxygen. The gating is only possible on certain crystal facets where volume channels along the VO2's rutile c-axis intersect the surface. Here, we fabricate bars with the c-axis in plane and oriented parallel to or perpendicular to the length of the bars. We show that only bars with the c-axis perpendicular to the bars, for which the volume channels are accessible from the sides of the bar, can be metallized by ionic liquid gating. Moreover, we find that bars up to at least 0.5 µm wide can be fully gated, demonstrating the possibility of the electric field induced migration of oxygen over very long distances, ∼5 times longer than previously observed.

Reversible Formation of 2D Electron Gas at the LaFeO3 /SrTiO3 Interface via Control of Oxygen Vacancies.

A conducting 2D electron gas (2DEG) is formed at the interface between epitaxial LaFeO3 layers >3 unit cells thick and the surface of SrTiO3 single crystals. The 2DEG is exquisitely sensitive to cation intermixing and oxygen nonstoichiometry. It is shown that the latter thus allows the controllable formation of the 2DEG via ionic liquid gating, thereby forming a nonvolatile switch.

Metallization of Epitaxial VO2 Films by Ionic Liquid Gating through Initially Insulating TiO2 Layers.

Ionic liquid gating has been shown to metallize initially insulating layers formed from several different oxide materials. Of these vanadium dioxide (VO2) is of especial interest because it itself is metallic at temperatures above its metal-insulator transition. Recent studies have shown that the mechanism of ionic liquid gated induced metallization is entirely distinct from that of the thermally driven metal-insulator transition and is derived from oxygen migration through volume channels along the (001) direction of the rutile structure of VO2. Here we show that it is possible to metallize the entire volume of 10 nm thick layers of VO2 buried under layers of rutile titanium dioxide (TiO2) up to 10 nm thick. Key to this process is the alignment of volume channels in the respective oxide layers, which have the same rutile structure with clamped in-plane lattice constants. The metallization of the VO2 layers is accompanied by large structural expansions of up to ∼6.5% in the out-of-plane direction, but the structure of the TiO2 layer is hardly affected by gating. The TiO2 layers become weakly conducting during the gating process, but in contrast to the VO2 layers, the conductivity disappears on exposure to air. Indeed, even after air exposure, X-ray photoelectron spectroscopy studies show that the VO2 films have a reduced oxygen content after metallization. Ionic liquid gating of the VO2 films through initially insulating TiO2 layers is not consistent with conventional models that have assumed the gate induced carriers are of electrostatic origin.

Facet-Independent Electric-Field-Induced Volume Metallization of Tungsten Trioxide Films.

Reversible metallization of band and Mott insulators by ionic-liquid gating is accompanied by significant structural changes. A change in conductivity of seven orders of magnitude at room temperature is found in epitaxial films of WO3 with an associated monoclinic-to-cubic structural reorganization. The migration of oxygen ions along open volume channels is the underlying mechanism.

Mesoscopic structural phase progression in photo-excited VO2 revealed by time-resolved x-ray diffraction microscopy.

Dynamical phase separation during a solid-solid phase transition poses a challenge for understanding the fundamental processes in correlated materials. Critical information underlying a phase transition, such as localized phase competition, is difficult to reveal by measurements that are spatially averaged over many phase separated regions. The ability to simultaneously track the spatial and temporal evolution of such systems is essential to understanding mesoscopic processes during a phase transition. Using state-of-the-art time-resolved hard x-ray diffraction microscopy, we directly visualize the structural phase progression in a VO2 film upon photoexcitation. Following a homogenous in-plane optical excitation, the phase transformation is initiated at discrete sites and completed by the growth of one lattice structure into the other, instead of a simultaneous isotropic lattice symmetry change. The time-dependent x-ray diffraction spatial maps show that the in-plane phase progression in laser-superheated VO2 is via a displacive lattice transformation as a result of relaxation from an excited monoclinic phase into a rutile phase. The speed of the phase front progression is quantitatively measured, and is faster than the process driven by in-plane thermal diffusion but slower than the sound speed in VO2. The direct visualization of localized structural changes in the time domain opens a new avenue to study mesoscopic processes in driven systems.

Termination layer compensated tunnelling magnetoresistance in ferrimagnetic Heusler compounds with high perpendicular magnetic anisotropy.

Although high-tunnelling spin polarization has been observed in soft, ferromagnetic, and predicted for hard, ferrimagnetic Heusler materials, there has been no experimental observation to date of high-tunnelling magnetoresistance in the latter. Here we report the preparation of highly textured, polycrystalline Mn3Ge films on amorphous substrates, with very high magnetic anisotropy fields exceeding 7 T, making them technologically relevant. However, the small and negative tunnelling magnetoresistance that we find is attributed to predominant tunnelling from the lower moment Mn-Ge termination layers that are oppositely magnetized to the higher moment Mn-Mn layers. The net spin polarization of the current reflects the different proportions of the two distinct termination layers and their associated tunnelling matrix elements that result from inevitable atomic scale roughness. We show that by engineering the spin polarization of the two termination layers to be of the same sign, even though these layers are oppositely magnetized, high-tunnelling magnetoresistance is possible.

Broadband extreme ultraviolet probing of transient gratings in vanadium dioxide.

Nonlinear spectroscopy in the extreme ultraviolet (EUV) and soft x-ray spectral range offers the opportunity for element selective probing of ultrafast dynamics using core-valence transitions (Mukamel et al., Acc. Chem. Res. 42, 553 (2009)). We demonstrate a step on this path showing core-valence sensitivity in transient grating spectroscopy with EUV probing. We study the optically induced insulator-to-metal transition (IMT) of a VO(2) film with EUV diffraction from the optically excited sample. The VO(2) exhibits a change in the 3p-3d resonance of V accompanied by an acoustic response. Due to the broadband probing we are able to separate the two features.

Giant reversible, facet-dependent, structural changes in a correlated-electron insulator induced by ionic liquid gating.

The use of electric fields to alter the conductivity of correlated electron oxides is a powerful tool to probe their fundamental nature as well as for the possibility of developing novel electronic devices. Vanadium dioxide (VO2) is an archetypical correlated electron system that displays a temperature-controlled insulating to metal phase transition near room temperature. Recently, ionic liquid gating, which allows for very high electric fields, has been shown to induce a metallic state to low temperatures in the insulating phase of epitaxially grown thin films of VO2. Surprisingly, the entire film becomes electrically conducting. Here, we show, from in situ synchrotron X-ray diffraction and absorption experiments, that the whole film undergoes giant, structural changes on gating in which the lattice expands by up to ∼3% near room temperature, in contrast to the 10 times smaller (∼0.3%) contraction when the system is thermally metallized. Remarkably, these structural changes are fully reversible on reverse gating. Moreover, we find these structural changes and the concomitant metallization are highly dependent on the VO2 crystal facet, which we relate to the ease of electric-field-induced motion of oxygen ions along chains of edge-sharing VO6 octahedra that exist along the (rutile) c axis.

Distinct electronic structure of the electrolyte gate-induced conducting phase in vanadium dioxide revealed by high-energy photoelectron spectroscopy.

The development of new phases of matter at oxide interfaces and surfaces by extrinsic electric fields is of considerable significance both scientifically and technologically. Vanadium dioxide (VO2), a strongly correlated material, exhibits a temperature-driven metal-to-insulator transition, which is accompanied by a structural transformation from rutile (high-temperature metallic phase) to monoclinic (low-temperature insulator phase). Recently, it was discovered that a low-temperature conducting state emerges in VO2 thin films upon gating with a liquid electrolyte. Using photoemission spectroscopy measurements of the core and valence band states of electrolyte-gated VO2 thin films, we show that electronic features in the gate-induced conducting phase are distinct from those of the temperature-induced rutile metallic phase. Moreover, polarization-dependent measurements reveal that the V 3d orbital ordering, which is characteristic of the monoclinic insulating phase, is partially preserved in the gate-induced metallic phase, whereas the thermally induced metallic phase displays no such orbital ordering. Angle-dependent measurements show that the electronic structure of the gate-induced metallic phase persists to a depth of at least ∼40 Å, the escape depth of the high-energy photoexcited electrons used here. The distinct electronic structures of the gate-induced and thermally induced metallic phases in VO2 thin films reflect the distinct mechanisms by which these states originate. The electronic characteristics of the gate-induced metallic state are consistent with the formation of oxygen vacancies from electrolyte gating.

Suppression of ionic liquid gate-induced metallization of SrTiO3(001) by oxygen.

Ionic liquid gating of three terminal field effect transistor devices with channels formed from SrTiO3(001) single crystals induces a metallic state in the channel. We show that the metallization is strongly affected by the presence of oxygen gas introduced external to the device whereas argon and nitrogen have no effect. The suppression of the gating effect is consistent with electric field induced migration of oxygen that we model by oxygen-induced carrier annihilation.