Abnormal Seebeck Effect in Vertically Stacked 2D/2D PtSe2 /PtSe2 Homostructure.

When a thermoelectric (TE) material is deposited with a secondary TE material, the total Seebeck coefficient of the stacked layer is generally represented by a parallel conductor model. Accordingly, when TE material layers of the same thickness are stacked vertically, the total Seebeck coefficient in the transverse direction may change in a single layer. Here, an abnormal Seebeck effect in a stacked two-dimensional (2D) PtSe2 /PtSe2 homostructure film, i.e., an extra in-plane Seebeck voltage is produced by wet-transfer stacking at the interface between the PtSe2 layers under a transverse temperature gradient is reported. This abnormal Seebeck effect is referred to as the interfacial Seebeck effect in stacked PtSe2 /PtSe2 homostructures. This effect is attributed to the carrier-interface interaction, and has independent characteristics in relation to carrier concentration. It is confirmed that the in-plane Seebeck coefficient increases as the number of stacked PtSe2 layers increase and observed a high Seebeck coefficient exceeding ≈188 µV K-1 at 300 K in a four-layer-stacked PtSe2 /PtSe2 homostructure.

Enhanced Transverse Seebeck Coefficients in 2D/2D PtSe2/MoS2 Heterostructures Using Wet-Transfer Stacking.

It is very challenging to estimate thermoelectric (TE) properties when applying millimeter-scale two-dimensional (2D) transition metal dichalcogenide (TMDC) materials to TE device applications, particularly their Seebeck coefficient due to their high intrinsic electrical resistance. This paper proposes an innovative approach to measure large transverse (i.e., in-plane) Seebeck coefficients for 2D TMDC materials by placing a low resistance (LR) semimetallic PtSe2 film on high-resistance (HR) semiconducting MoS2 (>10 MΩ), whose internal resistance is too high to measure the Seebeck coefficient, forming a heterojunction structure using wet-transfer stacking. The vertically stacked LR-PtSe2 (3 nm)/HR-MoS2 (12 nm) heterostructure film exhibits a high Seebeck coefficient > 190 µV/K up to 5 K temperature difference. This unusual behavior can be explained by an additional Seebeck effect induced at the interface between the LR-2D/HR-2D heterostructure. The proposed stacked LR-PtSe2/HR-MoS2 heterostructure film offers promising phenomena 2D/2D materials that enable innovative TE device applications.

Interface-Induced Seebeck Effect in PtSe2/PtSe2 van der Waals Homostructures.

The Seebeck effect refers to the production of an electric voltage when different temperatures are applied on a conductor, and the corresponding voltage-production efficiency is represented by the Seebeck coefficient. We report a Seebeck effect: thermal generation of driving voltage from the heat flowing in a thin PtSe2/PtSe2 van der Waals homostructure at the interface. We refer to the effect as the interface-induced Seebeck effect. By exploiting this effect by directly attaching multilayered PtSe2 over high-resistance PtSe2 thin films as a hybridized single structure, we obtained the highly challenging in-plane Seebeck coefficient of the PtSe2 films that exhibit extremely high resistances. This direct attachment further enhanced the in-plane thermal Seebeck coefficients of the PtSe2/PtSe2 van der Waals homostructure on sapphire substrates. Consequently, we successfully enhanced the in-plane Seebeck coefficients for the PtSe2 (10 nm)/PtSe2 (2 nm) homostructure approximately 42% compared to that of a pure PtSe2 (10 nm) layer at 300 K. These findings represent a significant achievement in understanding the interface-induced Seebeck effect and provide an effective strategy for promising large-area thermoelectric energy harvesting devices using two-dimensional transition metal dichalcogenide materials, which are ideal thermoelectric platforms with high figures of merit.

Extrinsic Surface Magnetic Anisotropy Contribution in Pt/Y3Fe5O12 Interface in Longitudinal Spin Seebeck Effect by Graphene Interlayer.

A recent study found that magnetization curves for Y3Fe5O12 (YIG) slab and thick films (>20 µm thick) differed from bulk system curves by their longitudinal spin Seebeck effect in a Pt/YIG bilayer system. The deviation was due to intrinsic YIG surface magnetic anisotropy, which is difficult to adopt extrinsic surface magnetic anisotropy even when in contact with other materials on the YIG surface. This study experimentally demonstrates evidence for extrinsic YIG surface magnetic anisotropy when in contact with a diamagnetic graphene interlayer by observing the spin Seebeck effect, directly proving intrinsic YIG surface magnetic anisotropy interruption. We show the Pt/YIG bilayer system graphene interlayer role using large area single and multilayered graphenes using the longitudinal spin Seebeck effect at room temperature, and address the presence of surface magnetic anisotropy due to magnetic proximity between graphene and YIG layer. These findings suggest a promising route to understand new physics of spin Seebeck effect in spin transport.

Giant Thermoelectric Seebeck Coefficients in Tellurium Quantum Wires Formed Vertically in an Aluminum Oxide Layer by Electrical Breakdown.

High efficiency thermoelectric (TE) materials still require high thermopower for energy harvesting applications. A simple elemental metallic semiconductor, tellurium (Te), has been considered critical to realize highly efficient TE conversion due to having a large effective band valley degeneracy. This paper demonstrates a novel approach to directly probe the out-of-plane Seebeck coefficient for one-dimensional Te quantum wires (QWs) formed locally in the aluminum oxide layer by well-controlled electrical breakdown at 300 K. Surprisingly, the out-of-plane Seebeck coefficient for these Te QWs ≈ 0.8 mV/K at 300 K. This thermopower enhancement for Te QWs is due to Te intrinsic nested band structure and enhanced energy filtering at Te/AO interfaces. Theoretical calculations support the enhanced high Seebeck coefficient for elemental Te QWs in the oxide layer. The local-probed observation and detecting methodology used here offers a novel route to designing enhanced thermoelectric materials and devices in the future.

Role of Ferromagnetic Monolayer WSe2 Flakes in the Pt/Y3Fe5O12 Bilayer Structure in the Longitudinal Spin Seebeck Effect.

The spin Seebeck effect (SSE) has attracted renewed interest as a promising phenomenon for energy harvesting systems. A noteworthy effort has been devoted to improving the SSE voltage by inserting ultrathin magnetic layers including Fe70Cu30 interlayers in Pt/Y3Fe5O12 (Pt/YIG) systems with increased spin-mixing conductance at the interfaces. Nevertheless, the responsible underlying physics associated with the role of the interlayer in Pt/YIG systems in the SSE is still unknown. In this paper, we demonstrate that with a monolayer tungsten diselenide (ML WSe2) interlayer in the Pt/YIG bilayer system, the longitudinal SSE (LSSE) voltage is significantly increased by the increased spin accumulation in the Pt layer; the spin fluctuation in ML WSe2 amplifies the spin current transmission because the in-plane-aligned WSe2 spins are coupled to thermally pumped spins under nonequilibrium magnetization conditions in the LSSE configuration at room temperature. The thermopower (VLSSE/ΔT) improves by 323% with respect to the value of the reference Pt/YIG bilayer sample in the LSSE at room temperature. In addition, the induced ferromagnetic properties of the ML WSe2 flakes on YIG increase the LSSE voltage (VLSSE) of the sample; the ferromagnetic properties are a result of the improved magnetic moment density in the ML WSe2 flakes and their two-dimensional (2D) ML nature in the LSSE under nonequilibrium magnetization conditions. The results can extend the application range of the materials in energy harvesting and provide important information on the physics of the LSSE with a transition metal dichalcogenide intermediate layer in spin transport.

Enhanced Spin Seebeck Thermopower in Pt/Holey MoS2/Y3Fe5O12 Hybrid Structure.

We first observed the spin-to-charge conversion due to both the inverse Rashba-Edelstein effect (IREE) and inverse spin-Hall effect in a holey multilayer molybdenum disulfide (MoS2) intermediate layer in a Pt/YIG structure via LSSE measurements under nonequilibrium magnetization. We found an enhancement of approximately 238%, 307%, and 290% in the longitudinal spin Seebeck effect (LSSE) voltage, spin-to-charge current, and thermoelectric (TE) power factor, respectively, compared with the monolayer MoS2 interlayer in a Pt/YIG structure. Such an enhancement in the LSSE performance of Pt/holey MoS2/YIG can be explained by the improvement of spin accumulation in the Pt layer by induced spin fluctuation as well as increased additional spin-to-charge conversion due to in-plane IREE. Our findings represent a significant achievement in the understanding of spin transport in atomically thin MoS2 interlayers and pave the way toward large-area TE energy-harvesting devices in two-dimensional transition metal dichalcogenide materials.

Surface Coverage Dependence of Spin-to-Charge Current across Pt/MoS2/Y3Fe5O12 Layers via Longitudinal Spin Seebeck Effect.

The voltage induced by the inverse spin Hall effect (ISHE) is affected by several factors, including the spin Hall angle of the normal metal (NM), the quality and magnetic properties of the ferromagnetic material (FM), and the interface conditions between the NM and FM bilayers in longitudinal spin Seebeck effect (LSSE) measurement. Specifically, the interface conditions in NM/FM systems via LSSE devices play a crucial role in determining the efficiency of spin current injection into the NM layer. In this letter, we report a new approach to controlling the efficiency of spin current injection into a Pt layer across a Pt/Y3Fe5O12 (YIG) interface by surface coverage of the intermediate layer. A continuous, large-area multilayer molybdenum dichalcogenide (MoS2) thin film grown by chemical vapor deposition is inserted between the Pt and YIG layers in the LSSE configuration. We found that, when the large-area multilayer MoS2 film was present, the measured ISHE-induced voltage and theoretically calculated spin current in the Pt/MoS2/YIG trilayer increased by ∼510% and 470%, respectively, compared to those of a Pt/YIG bilayer. The induced voltage and spin current were very sensitive to the surface conductance, which was affected by the surface coverage of the multilayer MoS2 films in the LSSE measurement. Furthermore, the theoretically calculated spin current and spin mixing conductance in the trilayer geometry are in qualitatively good agreement with the experimental observations. These measurements enable us to explain the effect of the interface conditions on the spin Seebeck effect in spin transport.

Achieving Out-of-Plane Thermoelectric Figure of Merit ZT = 1.44 in a p-Type Bi2Te3/Bi0.5Sb1.5Te3 Superlattice Film with Low Interfacial Resistance.

Recently, low-dimensional superlattice films have attracted significant attention because of their low dimensionality and anisotropic thermoelectric (TE) properties such as the Seebeck coefficient, electrical conductivity, and thermal conductivity. For these superlattice structures, both electrons and phonons show highly anisotropic behavior and exhibit much stronger interface scattering in the out-of-plane direction of the films compared to the in-plane direction. However, no detailed information is available in the literature for the out-of-plane TE properties of the superlattice-based films. In this report, we present the out-of-plane Seebeck coefficient, thermal conductivity, and electrical properties of p-type Bi2Te3/Bi0.5Sb1.5Te3 (bismuth telluride/bismuth antimony telluride, BT/BST) superlattice films in the temperature range of 77-500 K. Because of the synergistic combination of the energy filtering effect and low interfacial resistance of the superlattice structure, an impressively high ZT of 1.44 was achieved at 400 K for the 200 nm-thick p-type BT/BST superlattice film, corresponding to a 43% ZT enhancement compared to the pristine p-BST films with the same thickness.

Controllable Seebeck Coefficients of a Metal-Diffused Aluminum Oxide Layer via Conducting Filament Density and Energy Filtering.

We investigate the intrinsic thermoelectric (TE) properties of the metal-diffused aluminum oxide (AO) layer in metal/AO/metal structures, where the metallic conducting filaments (CFs) were locally formed in the structures via an electrical breakdown (EBD) process as shown by resistive switching memory devices, by directly measuring cross-plane Seebeck coefficients on the CF-containing insulating AO layers. The results showed that the Seebeck coefficients of the CF-containing AO layer in metal/AO/metal structures were influenced by the generation of the metallic CFs, which is due to the diffusion of the metal into the insulating AO layers when exposed to a temperature gradient in the direction of the cross plane of the sample. In addition, the increase in the Seebeck coefficients of the CF-containing AO layer when the number of EBD-processed patterns was increased is satisfactorily explained by the low-energy carrier (i.e., minority carriers) filtering through the metal-oxide interfacial barriers in the metal/AO/metal structures.

Direct Probing of Cross-Plane Thermal Properties of Atomic Layer Deposition Al2O3/ZnO Superlattice Films with an Improved Figure of Merit and Their Cross-Plane Thermoelectric Generating Performance.

There is a recent interest in semiconducting superlattice films because their low dimensionality can increase the thermal power and phonon scattering at the interface in superlattice films. However, experimental studies in all cross-plane thermoelectric (TE) properties, including thermal conductivity, Seebeck coefficient, and electrical conductivity, have not been performed from these semiconducting superlattice films because of substantial difficulties in the direct measurement of the Seebeck coefficient and electrical conductivity. Unlike the conventional measurement method, we present a technique using a structure of sandwiched superlattice films between two embedded heaters as the heating source, and electrodes with two Cu plates, which directly enables the investigation of the Seebeck coefficient and electrical conductivity across the Al2O3/ZnO superlattice films, prepared by the atomic layer deposition method. Used in combination with the promising cross-plane four-point probe 3-ω method, our measurements and analysis demonstrate all cross-plane TE properties of Al2O3/ZnO superlattice films in the temperature range of 80 to 500 K. Our experimental methodology and the obtained results represent a significant advancement in the understanding of phonons and electrical transports in nanostructured materials, especially in semiconducting superlattice films in various temperature ranges.

Functionalized vertical GaN micro pillar arrays with high signal-to-background ratio for detection and analysis of proteins secreted from breast tumor cells.

The detection of cancer biomarkers has recently attracted significant attention as a means of determining the correct course of treatment with targeted therapeutics. However, because the concentration of these biomarkers in blood is usually relatively low, highly sensitive biosensors for fluorescence imaging and precise detection are needed. In this study, we have successfully developed vertical GaN micropillar (MP) based biosensors for fluorescence sensing and quantitative measurement of CA15-3 antigens. The highly ordered vertical GaN MP arrays result in the successful immobilization of CA15-3 antigens on each feature of the arrays, thereby allowing the detection of an individual fluorescence signal from the top surface of the arrays owing to the high regularity of fluorophore-tagged MP spots and relatively low background signal. Therefore, our fluorescence-labeled and CA15-3 functionalized vertical GaN-MP-based biosensor is suitable for the selective quantitative analysis of secreted CA15-3 antigens from MCF-7 cell lines, and helps in the early diagnosis and prognosis of serious diseases as well as the monitoring of the therapeutic response of breast cancer patients.

Microfluidic channel-coupled 3D quartz nanohole arrays for high capture and release efficiency of BT20 cancer cells.

Nanostructured materials, such as silicon nanowires, quartz nanostructures, and polymer-modified nanostructures, are a promising new class of materials for the capture and enumeration of very rare tumor cells, including circulating tumor cells (CTCs), to examine their biological characteristics in whole blood of cancer patients. These cells can then be used for transplantation, anti-tumor cell therapy, and cell-secreted protein studies. It is believed that 3-dimensional (3D) nanostructured substrates efficiently enhance cell capture yields due to the increased local contacts between the 3D nanostructures and extracellular extensions of the tumor cells. Recent studies have been performed with enhanced cell capture yields thanks to various nanostructured platforms; however, there remains an urgent need both to capture and release viable rare tumor cells for further molecular (i.e., protein) analysis and to develop patient-specific drugs. Here, we first demonstrate that our 3D quartz nanohole array (QNHA) tumor cell capture and release system allows us not only to selectively capture rare tumor cells, but also to release the cells with high capture and release rates. This system was developed using streptavidin (STR)-functionalized QNHA (STR-QNHA) with a microfluidic channel. Our system has ideal cell-separation yields of as high as 85-91% and high release rates of >90% for the BT20 cell line. We suggest that the use of a microfluidic channel technique coupled with a STR-QNHA cell capture and release chip (STR-QNHA cell chip) would be a powerful and simple process to evaluate the capture, enumeration, and release of CTCs from patient whole blood for studying further cell therapy and tumor-cell-secreted molecules.

Anisotropic temperature-dependent thermal conductivity by an Al2O3 interlayer in Al2O3/ZnO superlattice films.

The thermal conductivity of superlattice films is generally anisotropic and should be studied separately in the in-plane and cross-plane directions of the films. However, previous works have mostly focused on the cross-plane thermal conductivity because the electrons and phonons in the cross-plane direction of superlattice films may result in much stronger interface scattering than that in the in-plane direction. Nevertheless, it is highly desirable to perform systematic studies on the effect of interface formation in semiconducting superlattice films on both in-plane and cross-plane thermal conductivities. In this study, we determine both the in-plane and cross-plane thermal conductivities of Al2O3 (AO)/ZnO superlattice films grown by atomic layer deposition (ALD) on SiO2/Si substrates in the temperature range of 50-300 K by the four-point-probe 3-ω method. Our experimental results indicate that the formation of an atomic AO layer (0.82 nm) significantly contributes to the decrease of the cross-plane thermal conductivity of the AO/ZnO superlattice films compared with that of AO/ZnO thin films. The cross-plane thermal conductivity (0.26-0.63 W m-1 K-1 of the AO/ZnO superlattice films (with an AO layer of ∼0.82 nm thickness) is approximately ∼150%-370% less than the in-plane thermal conductivity (0.96-1.19 W m-1 K-1) of the corresponding film, implying significant anisotropy. This indicates that the suppression of the cross-plane thermal conductivity is mainly attributed to the superlattice, rather than the nanograin columnar structure in the films. In addition, we theoretically analyzed strong anisotropic behavior of the in-plane and cross-plane thermal conductivities of the AO/ZnO superlattice films in terms of temperature dependence.

Effect of graphene oxide ratio on the cell adhesion and growth behavior on a graphene oxide-coated silicon substrate.

Control of living cells on biocompatible materials or on modified substrates is important for the development of bio-applications, including biosensors and implant biomaterials. The topography and hydrophobicity of substrates highly affect cell adhesion, growth, and cell growth kinetics, which is of great importance in bio-applications. Herein, we investigate the adhesion, growth, and morphology of cultured breast cancer cells on a silicon substrate, on which graphene oxides (GO) was partially formed. By minimizing the size and amount of the GO-containing solution and the further annealing process, GO-coated Si samples were prepared which partially covered the Si substrates. The coverage of GO on Si samples decreases upon annealing. The behaviors of cells cultured on two samples have been observed, i.e. partially GO-coated Si (P-GO) and annealed partially GO-coated Si (Annealed p-GO), with a different coverage of GO. Indeed, the spreading area covered by the cells and the number of cells for a given culture period in the incubator were highly dependent on the hydrophobicity and the presence of oxygenated groups on GO and Si substrates, suggesting hydrophobicity-driven cell growth. Thus, the presented method can be used to control the cell growth via an appropriate surface modification.

Lateral heat flow distribution and defect-dependent thermal resistance in an individual silicon nanowire.

Studies aiming to significantly improve thermal properties, such as figure-of-merit, of silicon nanowires (SiNW) have focused on diameter reduction and surface or interface roughness control. However, the mechanism underlying thermal conductivity enhancement of roughness controlled NWs remains unclear. Here, we report a significant influence of stacking faults (SFs) on the lateral thermal conductivity of a single SiNW, using a combination of newly developed in situ spatially-resolved thermal resistance experiments and high-resolution transmission electron microscopy measurements. We used as-grown SiNWs tapered along the growth direction with progressively lower roughness and SFs density. The results clearly confirmed that both surface roughness and twins or SFs densities suppress the thermal conductivity of an individual SiNW. The results and measurement techniques presented here hold great potential for inspecting minute changes in thermal resistance along an individual SiNW, caused by induced SFs on the nanostructure, and for improving one-dimensional nanowire-based thermoelectric device performance.

Drug response of captured BT20 cells and evaluation of circulating tumor cells on a silicon nanowire platform.

Research on specific drug responses of circulating tumor cells (CTCs) provides very important information for treatment of cancer patients at a patient-specific level. For this reason, platforms for high capture efficiency of CTCs are essential for clinical evaluation of patient-specific drug responses of CTCs. Recently, nanostructure based platforms have been developed with a high capture efficiency of more than 93% due to high-affinity binding and the 3D nanotopographic features of the nanostructure substrate. In this study, the breast carcinoma cell-line (BT20) cells with an ultra-low abundance range were captured by streptavidin (STR)-functionalized silicon nanowire (SiNW) platforms for evaluation of capture efficiency. A capture efficiency of more than 90% was achieved. Specific drug responses of BT20 cells captured on STR-SiNW platforms were analyzed using tamoxifen or docetaxel as a function of incubation time and dose, and compared with a 96-well plate platform. The drug responses of CTCs on STR-SiNW platforms were more sensitive than a 96-well plate platform. In addition, CTCs were successfully captured and evaluated their size distribution from the blood of breast cancer patients using fluorescence imaging. In conclusion, we suggest that the SiNW platform is adaptable for clinical use in evaluation of CTCs and drug response tests.

Filopodial morphology correlates to the capture efficiency of primary T-cells on nanohole arrays.

Nanostructured surfaces emerge as a new class of material for capture and separation of cell populations including primary immune cells and disseminating rare tumor cells, but the underlying mechanism remains elusive. Although it has been speculated that nanoscale topological structures on cell surface are involved in the cell capture process, there are no studies that systematically analyze the relation between cell surface structures and the capture efficiency. Here we report on the first mechanistic study by quantifying the morphological parameters of cell surface nanoprotrusions, including filopodia, lamellipodia, and microvilli in the early stage of cell capture (< 20 min) in correlation to the efficiency of separating primary T lymphocytes. This was conducted by using a set of nanohole arrays (NHAs) with varying hole and pitch sizes. Our results showed that the formation of filopodia (e.g., width of filopodia and the average number of the filopodial filaments per cell) depends on the feature size of the nanostructures and the cell separation efficiency is strongly correlated to the number of filopodial fibers, suggesting a possible role of early stage mechanosensing and cell spreading in determining the efficiency of cell capture. In contrast, the length of filopodial filaments was less significantly correlated to the cell capture efficiency and the nanostructure dimensions of the NHAs. This is the first mechanistic study on nanostructure-based immune cell capture and provides new insights to not only the biology of cell-nanomaterial interaction but also the design of new rare cell capture technologies with improved efficiency and specificity.

Dependence of filopodia morphology and the separation efficiency of primary CD4⁺ T-lymphocytes on nanopillars.

Despite significant improvement in separation efficiency using nanostructure-based platforms, the mechanism underlying the high efficiency of rare cell capture remains elusive. Here we report on the first mechanistic study by developing highly controlled nanostructures to investigate cell surface nanomorphology to better understand the cellular response of CD4(+) T-lymphocytes in contact with nanostructured surfaces and to elucidate key mechanisms for enhancing separation efficiency. Our results showed that actin-rich filopodia protruded from T-cells in the early stage of cell capture (<20 min), demonstrate the different morphologies in response to various quartz nanopillar (QNP) arrays functionalized with streptavidin and the generation of sufficient adhesion sites for rendering more stable binding through three-dimensional local nanotopographic interactions between filopodia-QNPs and cell-substrate, leading to synergistic effects for enhancing cell-capture efficiency. This responsive mechanism of T-cells on nanotopographic templates provides new insights to understand the enhanced cell-capture efficiency and specificity from the primary cell suspension on nanostructured substrates.

Electrical transport characterization of PEDOT:PSS/n-Si Schottky diodes and their applications in solar cells.

We demonstrate locally contacted PEDOT:PSS Schottky diodes with excellent rectifying behavior, fabricated on n-type Si substrates using a spin-coating process and a reactive-ion etching process. Electrical transport characterizations of these Schottky diodes were investigated by both current-voltage (I-V) and capacitance-voltage (C-V) measurements. We found that these devices exhibit excellent modulation in the current with an on/off ratio of - 10(6). Schottky junction solar cells composed of PEDOT:PSS and n-Si structures were also examined. From the current density-voltage (J-V) measurement of a solar cell under illumination, the short circuit current (I(sc)), open circuit voltage (V(oc)), and conversion efficiency (eta) were - 19.7 mA/cm2, - 578.5 mV, and - 6.5%, respectively. The simple and low-cost fabrication process of the PEDOT:PSS/n-Si Schottky junctions makes them a promising candidate for further high performance solar cell applications.