Thin film growth of ferroelectric or multiferroic materials on SrTiO3(111) with a buffer electrode has been hampered by the difficulty of growing flat electrodes on this polar orientation. We report on the growth and characterization of SrRuO3 thin films deposited by pulsed laser deposition on SrTiO3(111). We show that our SrRuO3(111) films are epitaxial and display magnetic bulk-like properties. Films presenting a thickness between 20 and 30nm are found to be very flat (with an RMS of about 0.5 nm) and therefore suitable as bottom electrodes in heterostructures.
Poor electrical conductivity and large volume expansion during repeated charge and discharge is what has characterized many battery electrode materials in current use. This has led to 2D materials, specifically multi-layered 2D systems, being considered as alternatives. Among these 2D multi-layered systems are the graphene-based van der Waals heterostructures with transition metal di-chalcogenides (TMDCs) as one of the layers. Thus in this study, graphene-Hafnium disulphide (Gr-HfS$_2$) system, has been investigated as a prototype Gr-TMDC system for application as battery electrode. Density fu…
Epitaxial orthorhombic Hf0.5Zr0.5O2 (HZO) films on La0.67Sr0.33MnO3 (LSMO) electrodes show robust ferroelectricity, with high polarization, endurance and retention. However, no similar results have been achieved using other perovskite electrodes so far. Here, LSMO and other perovskite electrodes are compared. A small amount of orthorhombic phase and low polarization is found in HZO films grown on La-doped BaSnO3 and Nb-doped SrTiO3, while null amounts of orthorhombic phase and polarization are detected in films on LaNiO3 and SrRuO3. The critical effect of the electrode on the stabilized phases…
The development of scalable techniques to make 2D material heterostructures is a major obstacle that needs to be overcome before these materials can be implemented in device technologies industrially. Electrodeposition is an industrially compatible deposition technique that offers unique advantages in scaling 2D heterostructures. In this work, we demonstrate the electrodeposition of atomic layers of WS$_2$ over graphene electrodes using a single source precursor. Using conventional microfabrication techniques, graphene was patterned to create micro-electrodes where WS$_2$ was site-selectively …
Surface oxidation of the bottom ferromagnetic (FM) electrode, one of the major detrimental factors to the performance of a Magnetic Tunnel Junction (MTJ), is difficult to avoid during the fabrication process of the MTJ's tunnel barrier. Since Co rich alloys are commonly used for the FM electrodes in MTJs, over-oxidation of the tunnel barrier results in the formation of a CoO antiferromagnetic (AF) interface layer which couples with the bottom FM electrode to form a typical AF/FM exchange bias (EB) system. In this work, surface oxidation of the CoFe and CoFeB bottom electrodes was detected via …
The effective barrier height between an electrode and a ferroelectric (FE) depends on both macroscopic electrical properties and microscopic chemical and electronic structure. The behavior of a prototypical electrode/FE/electrode structure, Pt/BaTiO3/Nb-doped SrTiO3, under in-situ bias voltage is investigated using X-Ray Photoelectron Spectroscopy. The full band alignment is measured and is supported by transport measurements. Barrier heights depend on interface chemistry and on the FE polarization. A differential response of the core levels to applied bias as a function of the polarization st…
Effect of Pt bottom electrode texture selection on the tetragonality and physical properties of Ba0.8Sr0.2TiO3 thin films produced by pulsed laser deposition
Two-dimensional transition metal-dichalcogenides are emerging as efficient and cost-effective electrocatalysts for hydrogen evolution reaction (HER). However, only the edge sites of their trigonal prismatic phase show HER-electrocatalytic properties, while the basal plane, which is absent of defective/unsaturated sites, is inactive. Here, we tackle the key challenge that is increasing the number of electrocatalytic sites by designing and engineering heterostructures composed of single-/few-layer MoSe2 flakes and carbon nanomaterials (graphene or single-wall carbon nanotubes (SWNTs)) produced b…
The material and electrical properties of the CNT single vias and array vias grown by microwave plasma-enhanced chemical vapor deposition were investigated. The diameters of multiwall carbon nanotubes (MWNTs) grown on the bottom electrode of Ta decrease with increasing pretreatment power and substrate temperature while the effects of the growth power and methane flow ratio are insignificant The decrease of CNT diameters leads to the decrease of the CNT via diode devices. The increase of growth power enhances the CNT graphitization degree and thue the conductivity of CNT via diode devices. In t…
We study the magnetic and transport properties of all-manganite heterostructures consisting of ferromagnetic metallic electrodes separated by an antiferromagnetic barrier. We find that the magnetic ordering in the barrier is influenced by the relative orientation of the electrodes magnetization producing a large difference in resistance between the parallel and antiparallel orientations of the ferromagnetic layers. The external application of a magnetic field in a parallel configuration also leads to large magnetoresistance.
In thin film ferroelectric capacitor the chemical and electronic structure of the electrode/FE interface can play a crucial role in determining the kinetics of polarization switching. We investigate the electronic structure of a Pt/BaTiO3/SrTiO3:Nb capacitor using time-resolved photoemission spectroscopy. The chemical, electronic and depth sensitivity of core level photoemission is used to probe the transient response of different parts of the upper electrode/ferroelectric interface to voltage pulse induced polarization reversal. The linear response of the electronic structure agrees quantitat…
Stacked van der Waals (vdW) heterostructures where semi-conducting two-dimensional (2D) materials are contacted by overlayed graphene electrodes enable atomically-thin, flexible electronics. We use first-principles quantum transport simulations of graphene-contacted MoS2 devices to show how the transistor effect critically depends on the stacking configuration relative to the gate electrode. We can trace this behavior to the stacking-dependent response of the contact region to the capacitive electric field induced by the gate. The contact resistance is a central parameter and our observation e…
We investigated the electronic and optoelectronic properties of vertical van der Waals heterostructure photodetectors using layered p type GaSe and n type InSe, with graphene as the transparent electrodes. Not only the photocurrent peaks from the layered GaSe and InSe themselves were observed, also the interlayer optical transition peak was observed, which is consistent with the first-principles calculation. The built-in electric field between p-n heterojunction and the advantage of the graphene electrodes can effectively separate the photo-induced electron-hole pairs, and thus lead to the res…
In this study, we proposed and demonstrated a self-rectifying property of silicon nitride (Si3N4)-based resistive random access memory device by employing p-type silicon (p-Si) as bottom electrode. The RRAM devices consisted of Al/Si3N4/p-Si are fabricated by a low presure chemical vapor deposition and exhibited an intrinsic diode property with non-linear current-voltage (I-V) behavior. In addition, compared to conventional metal/insulator/metal (MIM) structure of Al/Si3N4/Ti RRAM cells, operating current in whole bias regions for proposed metal/insulator/semiconductor (MIS) cells has been dra…
Bottom-up realization of a type-II organic-TMD heterointerface: Pentacene on monolayer WS2
TU Dortmund University（多特蒙德工业大学）；Institute of Physics, NAWI Graz, University of Graz（格拉茨大学NAWI格拉茨物理研究所）；Institute of Solid State Physics, Friedrich Schiller University Jena（耶拿弗里德里希·席勒大学固体物理研究所）；Universidad Autónoma de Madrid and IFIMAC（马德里自治大学及IFIMAC）
Pt/Ti metallisation bilayers are used as bottom electrodes for ferroelectric thin films. During deposition of the ferroelectric films, these electrodes are exposed to elevated temperatures causing modifications of the Pt/Ti bottom electrode. Diffusion and oxidation of the Ti adhesion layer have been studied by the application of factor analysis to AES depth profile data and by RBS. Factor analysis was employed to extract the chemical information from the measured AES spectra and to derive semiquantitative depth profiles of the identified material compounds. RBS was used to obtain the quantitat…
An approach is presented to modify the WF of solution-processed sol-gel derived ZnOover an exceptionally wide range of more than 2.3 eV. This approach relies on the formation of dense and homogeneous self-assembled monolayers based on phosphonic acids with different dipole moments. This allows us to apply ZnO as charge selective bottom electrodes in either regular or inverted solar cell structures, using P3HT:PCBM as the active layer. These devices compete with or even exceed the performance of the reference cell on ITO/PEDOT:PSS. Our finding challenges the current view that bottom electrodes …
Independent control of carrier density and out-of-plane displacement field is essential for accessing novel phenomena in two-dimensional material heterostructures. While this is achieved with independent top and bottom metallic gate electrodes in transport experiments, it remains a challenge for near-field optical studies as the top electrode interferes with the optical path. Here, we systematically characterize the requirements for a material to be used as top-gate electrode, and demonstrate experimentally that few-layer WSe_2 can be used as a transparent, ambipolar top gate electrode in infr…
The performance of solution-processed organic light emitting diodes (OLEDs) is often limited by non-uniform contacts. In this work, we introduce Ni-containing solution-processed metal oxide (MO) interfacial layers inserted between indium tin oxide (ITO) and poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate) (PEDOT:PSS) to improve the bottom electrode contact for OLEDs using the poly(p-phenylene vinylene) (PPV) derivative Super-Yellow (SY) as an emission layer. For ITO/Ni-containing MO/PEDOT:PSS bottom electrode structures we show enhanced wetting properties that result in an improved OLE…
Heterostructures consisting of PbZr0.2Ti0.8O3 and PbZr0.4Ti0.6O3 films grown on a SrTiO3 (100) substrate with a SrRuO3 bottom electrode were prepared by pulsed laser deposition. Using the additional interface provided by the ferroelectric bilayer structure and changing the sequence of the layers, the dislocation content and domain patterns were varied. The resulting microstructure was investigated by transmission electron microscopy. Macroscopic ferroelectric measurements have shown a large impact of the formation of dislocations and the a/c domain structure on the ferroelectric polarization a…
A model for Metal-Ferroelectric-Metal structures with Schottky contacts is proposed. The model adapts the general theories of metal-semiconductor rectifying contacts for the particular case of metal-ferroelectric contact by introducing: the ferroelectric polarization as a sheet of surface charge located at a finite distance from the electrode interface; a deep trapping level of high concentration; the static and dynamic values of the dielectric constant. Consequences of the proposed model on relevant quantities of the Schottky contact such as built-in voltage, charge density and depletion widt…
The influence of depolarizing field on the magnitude and stability of a uniform polarization in ferroelectric capacitors and tunnel junctions is studied using a nonlinear thermodynamic theory. It is predicted that, in heterostructures involving strained epitaxial films and metal electrodes, the homogeneous polarization state may remain stable against transformations into the paraelectric phase and into polydomain states down to the nanoscale. This result supports the possibility of depolarizing-field-related resistive switching in ferroelectric tunnel junctions with dissimilar electrodes. The …
The International Roadmap for Ferroelectric Memories requires three-dimensional integration of high-dielectric materials onto metal interconnects or bottom electrodes by 2010. We report the first integration of high-dielectric oxide films onto carbon nanotube electrodes with an aim of ultra-high integration density of FeRAMs (Tb/in2).
Current Induced Resistance Switching (CIS) was recently observed in thin tunnel junctions (TJs) with ferromagnetic (FM) electrodes and attributed to electromigration of metallic atoms in nanoconstrictions in the insulating barrier. The CIS effect is here studied in TJs with two thin (20 Å) non-magnetic (NM) Ta electrodes inserted above and below the insulating barrier. We observe resistance (R) switching for positive applied electrical current (flowing from the bottom to the top lead), characterized by a continuous resistance decrease and associated with current-driven displacement of metallic…
Thin van der Waals (vdW) layered magnetic materials disclose the possibility to realize vdW heterostructures with new functionalities. Here we report on the realization and investigation of tunneling spin valves based on van der Waals heterostructures consisting of an atomically thin hBN layer acting as tunnel barrier and two exfoliated Fe3GeTe2 crystals acting as ferromagnetic electrodes. Low-temperature anomalous Hall effect measurements show that thin Fe3GeTe2 crystals are metallic ferromagnets with an easy axis perpendicular to the layers, and a very sharp magnetization switching at magnet…
The overall quality of multilayer thin films prepared by electrodeposition is strongly influenced by the surface and interface roughness which increases with the layer number. For that very reason the reliable analysis of the first few layers can be necessary. However, in depth profiling methods based on sputtering techniques the first layer is always found at the bottom of the sputtered crater. Since the depth resolution decreases during sputtering, the analysis of the first few layers are difficult. In order to circumvent this problem, we used reverse Secondary Neutral Mass Spectrometry (SNM…
The structural interface properties of layered Pt/Ti/SiO2/Si electrodes have been investigated using high-resolution specular and diffuse x-ray reflectivity under grazing angles. Currently this multilayer system represents a technological standard as bottom electrodes for ferroelectric thin film applications. For the electronic and ferroelectric properties of integrated devices, the film-electrode interface is of crucial importance. We focused on Pt-100nm/Ti-10nm/SiO2/Si electrodes prepared under annealing conditions as employed in industrial processing, prior to the deposition of ferroelectri…
The challenge of parasitic bulk doping in Bi-based 3D topological insulator materials is still omnipresent, especially when preparing samples by molecular beam epitaxy (MBE). Here, we present a heterostructure approach for epitaxial BSTS growth. A thin n-type Bi$_2$Se$_3$ (BS) layer is used as an epitaxial and electrostatic seed which drastically improves the crystalline and electronic quality and reproducibility of the sample properties. In heterostructures of BS with p-type (Bi$_{1-x}$Sb$_x$)$_2$(Te$_{1-y}$Se$_y$)$_3$ (BSTS) we demonstrate intrinsic band bending effects to tune the electroni…
The instability of ferroelectric ordering in ultra-thin films is one of the most important fundamental issues pertaining realization of a number of electronic devices with enhanced functionality, such as ferroelectric and multiferroic tunnel junctions or ferroelectric field effect transistors. In this paper, we investigate the polarization state of archetypal ultrathin (several nanometres) ferroelectric heterostructures: epitaxial single-crystalline BaTiO$_3$ films sandwiched between the most habitual perovskite electrodes, SrRuO$_3$, on top of the most used perovskite substrate, SrTiO$_3$. We…
We report on the exchange bias between antiferromagnetic and ferroelectric hexagonal YMnO3 epitaxial thin films sandwiched between a metallic electrode (Pt) and a soft ferromagnetic layer (Py). Anisotropic magnetoresistance measurements are performed to monitor the presence of an exchange bias field. When the heteroestructure is biased by an electric field, it turns out that the exchange bias field is suppressed. We discuss the dependence of the observed effect on the amplitude and polarity of the electric field. Particular attention is devoted to the role of current leakage across the ferroel…
We propose a tunneling heterostructure by replacing one of the metal electrodes in a metal/ferroelectric/metal ferroelectric tunnel junction with a heavily doped semiconductor. In this metal/ferroelectric/semiconductor tunnel diode, both the height and the width of the tunneling barrier can be electrically modulated due to the ferroelectric field effect, leading to a colossal tunneling electroresistance. This idea is implemented in Pt/BaTiO3/Nb:SrTiO3 heterostructures, in which an ON/OFF conductance ratio above 10$^4$ can be readily achieved at room temperature. The colossal tunneling electror…
We studied metastable $α$-FeGe$_2$, a novel layered tetragonal material, embedded as a spacer layer in spin valve structures with ferromagnetic Fe$_3$Si and Co$_2$FeSi electrodes. For both types of electrodes, spin valve operation is demonstrated with a metallic transport behavior of the $α$-FeGe$_2$ spacer layer. The spin valve signals are found to increase both with temperature and spacer thickness, which is discussed in terms of a decreasing magnetic coupling strength between the ferromagnetic bottom and top electrodes. The temperature-dependent resistances of the spin valve structures exhi…
La$_2$NiO$_4$ is a very promising cathode material for intermediate and low temperature solid oxide cell applications, due to its good electronic and ionic conductivity, together with its high oxygen exchange activity with a low activation energy. Oxygen incorporation and transport in La$_2$NiO$_4$ (L2NO4) thin films is limited by surface reactions. Hence, tailoring the morphology is expected to lead to an overall improvement of the electrode performance. We report on the growth of nano-architectured La$_2$NiO$_4$ thin film electrodes by Pulsed Injection Metal Organic Vapour Deposition (PI-MOC…
Electric conduction in thin graphite film was tuned by two gate electrodes to clarify how the gate electric field induces electric carriers in thin graphite. The graphite was sandwiched between two gate electrodes arranged in a top and bottom gate configuration. A scan of the top gate voltage generates a resistance peak in ambiploar response. The ambipolar peak is shifted by the bottom gate voltage, where the shift rate depends on the graphite thickness. The thickness-dependent peak shift was clarified in terms of the inter-layer screening length to the electric field in the double-gated graph…
We investigate a wafer scale tunnel junction fabrication method, where a plasma etched via through a dielectric layer covering bottom Al electrode defines the tunnel junction area. The ex-situ tunnel barrier is formed by oxidation of the bottom electrode in the junction area. Room temperature resistance mapping over a 150 mm wafer give local deviation values of the tunnel junction resistance that fall below 7.5 % with an average of 1.3 %. The deviation is further investigated by sub-1 K measurements of a device, which has one tunnel junction connected to four arrays consisting of N junctions (…
