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Atomically thin two-dimensional (2D) materials have emerged as promising candidates for flexible and transparent electronic applications. Here, we introduce non-volatile charge trapping memory devices, based on the 2D heterostructure field-effect transistor consisting of a few-layer MoS2 channel and CrPS4 charge-trapping gate stack. Clockwise hysteresis behaviors in transfer curves measured at room temperature show strong dependence on the thickness of CrPS4, which are attributed to charge trapping at trap sites in the CrPS4 layers. Our heterostructure memory device with 75 nm-thick CrPS4 layer exhibits both large memory windows up to 100 V and a high on/off current ratio (3 $$\times$$ 105) with good endurance during 625 cycles because of excellent trapping ability of trap sites in the CrPS4. Especially, the memory window size can be effectively tuned from 7.6 to 100 V by changing the sweep range of gate voltage. Such high performances of the charge-trapping memory device with a simple heterostructure provide a promising route towards next-generation memory devices utilizing 2D materials.

Semiconductors have long been perceived as a prerequisite for solid-state transistors. Although switching principles for nanometer-scale devices have emerged based on the deployment of two-dimensional (2D) van der Waals heterostructures, tunneling and ballistic currents through short channels are difficult to control, and semiconducting channel materials remain indispensable for practical switching. In this study, we report a semiconductor-less solid-state electronic device that exhibits an industry-applicable switching of the ballistic current. This device modulates the field emission barrier height across the graphene-hexagonal boron nitride interface with ION/IOFF of 106 obtained from the transfer curves and adjustable intrinsic gain up to 4, and exhibits unprecedented current stability in temperature range of 15–400 K. The vertical device operation can be optimized with the capacitive coupling in the device geometry. The semiconductor-less switching resolves the long-standing issue of temperature-dependent device performance, thereby extending the potential of 2D van der Waals devices to applications in extreme environments. In field-effect transistors, a semiconducting channel is indispensable for device switching. Here, the authors demonstrate semiconductor-less switching via modulation of the field emission barrier height across a graphene-hBN interface with ON/OFF ratio of 106.

Separation of two-dimensional thin-film-materials into single layers had been considered very challenging both theoretically and experimentally until the mechanical exfoliation method was discovered. After the successful separation of single- and/or few-layer graphene, the possibility of wrinkle formation has been one of the main open topics because they were not readily observed in experiments. Here, we report experimental observations of different kinds of repetitive nanoscale deformations (ripples, wrinkles, and crumples) in folded single-layer graphene (SLG) on an SiO2 substrate. Using high-vacuum atomic force microscopy, we observed that SLG that was pre-transferred onto an SiO2 substrate was accidentally folded multiple times during the tip-scanning, resulting in the formation of bilayer and trilayer graphene (TLG). Through high-resolution tapping-mode scanning, we could observe the wrinkles, ripples, and crumples in TLG. Additionally, we observed a herringbone pattern that was attributed to an intermediate stage between the wrinkles and ripples; this intermediate state was labeled as wrinklon structure. In our analysis, to characterize the ripples, wrinkles, and crumples, we measured the spatial repetition and amplitude of each pattern using their average line profile and compared them.

We report the enhanced electrical performance of a MoS2 field-effect transistor (FET) by using a contact with a layered CrPS4. Our transport measurements revealed that MoS2 channel with CrPS4 junction showed higher mobility of 33.9 cm2/Vs than that without CrPS4 junction on SiO2/Si substrate. We also fabricated a MoS2 FET with a top gate insulator, CrPS4, which showed low leakage current of 10−11 A and high on/off ratio of 105. In a dual-gated FET with SiO2 bottom gate insulator and CrPS4 top gate insulator, much decreased sub-threshold swing of 0.70 V/dec was obtained.

Next-generation electronic and optoelectronic devices require a high-quality channel layer. Graphene is a good candidate because of its high carrier mobility and unique ambipolar transport characteristics. However, the on/off ratio and photoresponsivity of graphene are typically low. Transition metal dichalcogenides (e.g., MoSe2) are semiconductors with high photoresponsivity but lower mobility than that of graphene. Here, we propose a graphene/MoSe2 barristor with a high-k ion-gel gate dielectric. It shows a high on/off ratio (3.3 × 104) and ambipolar behavior that is controlled by an external bias. The barristor exhibits very high external quantum efficiency (EQE, 66.3%) and photoresponsivity (285.0 mA/W). We demonstrate that an electric field applied to the gate electrode substantially modulates the photocurrent of the barristor, resulting in a high gate tuning ratio (1.50 μA/V). Therefore, this barristor shows potential for use as an ambipolar transistor with a high on/off ratio and a gate-tunable photodetector with a high EQE and responsivity. An approach that enhances control over charge carrier movement in graphene-based transistors may be useful in applications such as bendable circuits and light sensors. The difference in current flow when a transistor turns from on to off plays a critical role in determining device performance. Bae Ho Park from Konkuk University in Seoul, South Korea, and colleagues report that stacking graphene on top of another two-dimensional (2D) film of molybdenum selenide can lead to larger on/off current ratios than conventional graphene transistors. Optical and electrical characterizations revealed that the interface between the 2D films created a potential barrier that blocked current flow in the device’s off state without compromising graphene’s mechanical flexibility. Using an external voltage to modulate current flow through the barrier region also allowed the stacked device to serve as a high-efficiency photodetector. we report a field-effect device with a graphene/MoSe2 channel layer and high-k ion-gel gate dielectric. The device shows a high carrier mobility (~247 cm2/V ∙ s), a high on/off ratio (3.3 × 104), and ambipolar behavior that are controlled by an applied gate voltage. The strong gating effect of the device results in higher external quantum efficiency (EQE) (66.3%), photoresponsivity (285.0 mA/W), and gate-tuning ratio (1.50 μA/V) compared to pristine devices. Therefore, our graphene/MoSe2 barristor device can be a suitable candidate for use in ambipolar transistors and gate-tunable broad-area photodetectors.

Memristive electrochemical metallization (ECM) devices based on cation migration and electrochemical metallization in solid electrolytes are considered promising for neuromorphic computing systems. Two-dimensional (2D) layered materials are emerging as potential candidates for electrolytes in reliable ECM devices due to their two-dimensionally confined material properties. However, electrochemical metallization within a single-crystalline 2D layered material has not yet been verified. Here, we use transmission electron microscopy and energy-dispersive X-ray spectroscopy to investigate the resistive switching mechanism of an ECM device containing a single-crystalline 2D layered CrPS4 electrolyte. We observe the various conductive filament (CF) configurations induced by an applied voltage in an Ag/CrPS4/Au device in the initial/low-resistance/high-resistance/breakdown states. These observations provide concrete experimental evidence that CFs consisting of Ag metal can be formed inside single-crystalline 2D layered CrPS4 and that their configuration can be changed by an applied voltage. Density functional theory calculations confirm that the sulfur vacancies in single-crystalline CrPS4 can facilitate Ag ion migration from the active electrode layer. The electrically induced changes in Ag CFs inside single-crystalline 2D layered CrPS4 raise the possibility of a reliable ECM device that exploits the properties of two-dimensionally confined materials. A 2D layered material has provided critical insights toward improving the stability of devices that can emulate biological synapses. Researchers in Seoul, South Korea, led by Jae-Pyoung Ahn at the Korea Institute of Science and Technology and Bae Ho Park from Konkuk University have used high-resolution microscopy to investigate electrochemical metallization cells, a new type of non-volatile computer memory. These cells, made by infusing insulators with tiny metallic filaments, can mimic the low and high conductivity states of synapses. When the team looked at the structure of a chromium thiophosphate insulator composed of numerous 2D crystal layers, they found that the pathways the filaments follow are guided by specific crystal defects. These findings may help manufacturers produce more reliable electrochemical metallization cells by reducing the likelihood of random, non-uniform filament formation. We report on the formation and rupture of CFs through Ag ion migration inside a single-crystalline 2D van der Waals (vdW) solid electrolyte material within an ECM device structure. This study provides clear experimental evidence that CFs consisting of Ag can be formed inside single-crystalline 2D layered chromium thiophosphate (CrPS4) and their configuration can be changed by an applied voltage. Density functional theory calculations confirm that the Ag ion migration is an energetically favorable process. The electrically induced changes in Ag CFs inside single-crystalline CrPS4 raise the possibility of a reliable ECM device that exploits the properties of two-dimensionally confined materials.

Two-dimensional (2D)-layered semiconducting materials with considerable band gaps are emerging as a new class of materials applicable to next-generation devices. Particularly, black phosphorus (BP) is considered to be very promising for next-generation 2D electrical and optical devices because of its high carrier mobility of 200–1000 cm2 V–1 s–1 and large on/off ratio of 104 to 105 in field-effect transistors (FETs). However, its environmental instability in air requires fabrication processes in a glovebox filled with nitrogen or argon gas followed by encapsulation, passivation, and chemical functionalization of BP. Here, we report a new method for reduction of BP-channel devices fabricated without the use of a glovebox by galvanic corrosion of an Al overlayer. The reduction of BP induced by an anodic oxidation of Al overlayer is demonstrated through surface characterization of BP using atomic force microscopy, Raman spectroscopy, and X-ray photoemission spectroscopy along with electrical measurement of a...

Two-dimensional (2D) van der Waals (vdW) materials have recently attracted considerable attention due to their excellent electrical and mechanical properties. TmPSx (where Tm = a transition metal), which is a new class of 2D vdW materials, is expected to show various physical phenomena depending on the Tm used. In this paper, the unprecedented synaptic behavior of a vertical Ag/CrPS4/Au capacitor structure, where CrPS4 is a single-crystalline 2D vdW layer, is reported. Multi-stable resistive states were obtained using an external voltage of less than 0.3 V. Both short-term plasticity and long-term potentiation were observed by controlling the interval of the external voltage pulse. Simple mechanical exfoliation was used to develop a synaptic device based on a very thin CrPS4 layer with a thickness of ~17 nm. Therefore, it was demonstrated that vertical Ag/CrPS4/Au capacitors could be promising inorganic synaptic devices compatible with next-generation, flexible neuromorphic technologies. A capacitor made of a chromium thiophosphate (CrPS4) layer sandwiched between a silver electrode and a gold electrode behaves like a synapse. A Korea-based team led by Bae Ho Park from Konkuk University, Seoul, peeled very thin, crystalline CrPS4 layers of different thicknesses from the bulk material and fabricated top and bottom electrodes to prepare a series of Ag/CrPS4/Au capacitors. Under electrical pulses of different amplitudes, durations and intervals, these structures mimicked short-term and long-term variations in synaptic strength—neural behaviors involved in learning and memory. The devices’ behavior is attributed to the electrochemically induced migration of silver ions across the CrPS4 layer, leading to the formation and rupture of a conducting filament between the electrodes. The Ag/CrPS4/Au structure is promising for computing technologies that imitate neural pathways in the nervous system. We suggest synaptic devices using cation migration along thickness direction in a new class of 2D layered materials. An electrochemically active metal, such as Ag and Cu, is used for the operation of the synaptic device and chromium thiophosphate (CrPS4) single crystal is used as an electrolyte material. Multi-stable resistive states, short-term plasticity, and long-term potentiation are observed by controlling external voltage pulse with height smaller than 0.3 V. Given that simple mechanical exfoliation can generate very thin CrPS4 layers, the vertical Ag/CrPS4/Au capacitor offers a promising inorganic synaptic device compatible with next-generation flexible neuromorphic technology.

We report the effect of the oxygen content of the LaAlO3 layer on the synaptic behavior in the Pt/LaAlO3/Nb-doped SrTiO3 memristor for neuromorphic applications. As the oxygen-content decreases, the current becomes larger and the spike time-dependent plasticity (STDP) becomes less sensitive to the time difference between pre- and post-synaptic spike voltage. In addition, the conduction mechanism, which was found to be a combination of thermionic and Poole-Frenkel emissions, and the effect of oxygen content are explained in association with the oxygen vacancy in the LaAlO3 layer. The trade-off between large current and efficient STDP can be controlled by the oxygen content. Furthermore, the results of extracting the synaptic strength-based model parameters indicate that the Pt/LaAlO3/Nb-doped SrTiO3 shows the efficient STDP characteristics in comparison to previously reported memristor materials.

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

Lead-free (100 − x)BiFeO3–xBaTiO3 (BFBTx, x = 0, 30, 33, 40 and 50) piezoelectric thin films were deposited on platinized silicon substrates by using a pulsed laser deposition method. The BFBTx thin films has a single-phase perovskite structure with (111) preferred orientations. Atomic force microscopy images showed the dense morphology, and large piezoresponses were observed in the piezoelectric force microscope measurements. The best local piezoelectric coefficient, value of 259 pm V−1, was observed in the BFBT40 thin film. This result is one of the best values in lead-free piezoelectric thin films with a simple geometry. The BFBT40 piezoelectric thin film can be considered as a strong candidate to replace lead-based piezoelectric thin films for piezoelectric-based microelectromechanical systems.

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

An oxide-based resistance memory is a leading candidate to replace Si-based flash memory as it meets the emerging specifications for future memory devices. The non-uniformity in the key switching parameters and low endurance in conventional resistance memory devices are preventing its practical application. Here, a novel strategy to overcome the aforementioned challenges has been unveiled by tuning the growth direction of epitaxial brownmillerite SrFeO2.5 thin films along the SrTiO3 [111] direction so that the oxygen vacancy channels can connect both the top and bottom electrodes rather directly. The controlled oxygen vacancy channels help reduce the randomness of the conducting filament (CF). The resulting device displayed high endurance over 106 cycles, and a short switching time of ∼10 ns. In addition, the device showed very high uniformity in the key switching parameters for device-to-device and within a device. This work demonstrates a feasible example for improving the nanoscale device performance by controlling the atomic structure of a functional oxide layer.

We studied the optical, electrical and magnetic properties of ZnO films prepared by using a pulsed laser deposition method. Low-temperature photoluminescence (PL) measurements revealed a strong emission line at 3.333 eV. A dependence of this emission intensity on oxygen adsorbed on the surface was observed, indicating a near-surface origin for the emission. The transition at 3.333 eV was attributed to bound exciton, and the observed anomalously small thermal activation energy in comparison with the localization energy could be explained by a modification of the surface state. The observed resistance switching effect and ferromagnetism in the ZnO films were related to the existence of defects responsible for the PL emission at 3.333 eV.

12CaO x 7Al2O3, insulator (C12A7) doped indium tin oxide (ITO) (ITO:C12A7) films were fabricated using a radio frequency magnetron co-sputtering system with ITO and C12A7 targets. The qualitative and quantitative properties of ITO:C12A7 films, as a function of C12A7 concentration, were examined via X-ray photoemission spectroscopy and synchrotron X-ray scattering as well as by conducting atomic force microscopy. The work function of ITO:C12A7 (1.3%) films of approximately 2.8 eV obtained by high resolution photoemission spectroscopy measurements make them a reasonable cathode for top-emission organic light-emitting diodes.

Dye-sensitized solar cells (DSSCs) based on titanium dioxide () have been extensively studied because of their promising low-cost alternatives to conventional semiconductor based solar cells. DSSCs consist of molecular dye at the interface between a liquid electrolyte and a mesoporous wide-bandgap semiconductor oxide. Most efforts for high conversion efficiencies have focused on dye and liquid electrolytes. However, interface engineering between dye and electrode is also important to reduce recombination and improve efficiency. In this work, for interface engineering, we deposited semiconducting ferroelectric with bandgap of 2.8 eV on nanoparticles and nanotubes. Photovoltaic properties of DSSCs were characterized as a function of thickness of . We showed that ferroelectric -coated electrodes enable to increase overall efficiency of DSSCs, which was associated with efficient electron transport due to internal electric field originating from electric polarization. It was suggested that engineering the dye- interface using ferroelectric materials as inorganic modifiers can be key parameter for enhanced photovoltaic performance of the cell.

Selectively activated inorganic synaptic devices, showing a high on/off ratio, ultrasmall dimensions, low power consumption, and short programming time, are required to emulate the functions of high-capacity and energy-efficient reconfigurable human neural systems combining information storage and processing (Li et al. Sci. Rep. 2014, 4, 4096). Here, we demonstrate that such a synaptic device is realized using a Ag/PbZr0.52Ti0.48O3 (PZT)/La0.8Sr0.2MnO3 (LSMO) ferroelectric tunnel junction (FTJ) with ultrathin PZT (thickness of ∼4 nm). Ag ion migration through the very thin FTJ enables a large on/off ratio (107) and low energy consumption (potentiation energy consumption = ∼22 aJ and depression energy consumption = ∼2.5 pJ). In addition, the simple alignment of the downward polarization in PZT selectively activates the synaptic plasticity of the FTJ and the transition from short-term plasticity to long-term potentiation.

The room-temperature resistive switching characteristics of ferroelectric, ferroelastic, and multiferroic materials are promising for application in nonvolatile memory devices. These resistive switching characteristics can be accompanied by a change in the ferroic order parameters via applied external electric and magnetic excitations. However, the dynamic evolution of the order parameters between two electrodes, which is synchronized with resistive switching, has rarely been investigated. In this study, for the first time, we directly monitor the ferroelectric/ferroelastic domain switching dynamics between two electrodes in multiferroic BiFeO3 (BFO) planar devices, which cause resistive switching, using piezoresponse force microscopy. It is demonstrated that the geometrical relationship between the ferroelectric domain and electrode in BFO planar capacitors with only 71° domain walls significantly affects both the ferroelectric domain dynamics and the resistive switching. The direct observation of domain...

ReRAM is a compelling candidate for next-generation non-volatile memory owing to its various advantages. However, fluctuation of operation parameters are critical weakness occurring failures in ‘reading’ and ‘writing’ operations. To enhance the stability, it is important to understand the mechanism of the devices. Although numerous studies have been conducted using AFM or TEM, the understanding of the device operation is still limited due to the destructive nature and/or limited imaging range of the previous methods. Here, we propose a new hybrid device composed of ReRAM and LED enabling us to monitor the conducting filament (CF) configuration on the device scale during resistive switching. We directly observe the change in CF configuration across the whole device area through light emission from our hybrid device. In contrast to former studies, we found that minor CFs were formed earlier than major CF contributing to the resistive switching. Moreover, we investigated the substitution of a stressed major CF with a fresh minor CF when large fluctuation of operation voltage appeared after more than 50 times of resistive switching in atmospheric condition. Our results present an advancement in the understanding of ReRAM operation mechanism, and a step toward stabilizing the fluctuations in ReRAM switching parameters.

Resistive switching memory, which is mostly based on polycrystalline thin films, suffers from wide distributions in switching parameters-including set voltage, reset voltage, and resistance-in their low- and high-resistance states. One of the most commonly used methods to overcome this limitation is to introduce inhomogeneity. By contrast, in this paper, we obtained uniform resistive switching parameters and sufficiently low forming voltage by maximizing the uniformity of an epitaxial thin film. To achieve this result, we deposited an SrFeOx/SrRuO3 heteroepitaxial structure onto an SrTiO3 (001) substrate by pulsed laser deposition, and then we deposited an Au top electrode by electron-beam evaporation. This device exhibited excellent bipolar resistance switching characteristics, including a high on/off ratio, narrow distribution of key switching parameters, and long data retention time. We interpret these phenomena in terms of a local, reversible phase transformation in the SrFeOx film between brownmillerite and perovskite structures. Using the brownmillerite structure and atomically uniform thickness of the heteroepitaxial SrFeOx thin film, we overcame two major hurdles in the development of resistive random-access memory devices: high forming voltage and broad distributions of switching parameters.

The graphene/SiO2 system is a promising building block for next-generation electronic devices, integrating the high electromagnetic performance of graphene with the mature technology of Si-based electronic devices. It is well known that the electromagnetic performance of graphene/SiO2 is dramatically reduced by structural defects, such as wrinkles and folding, which are suspected to result from water droplets. Therefore, understanding water diffusion between graphene and SiO2 is required for controlling structural defects and thus improving the electromagnetic performance of this system. Although the behavior of water between graphene and atomically flat mica has been investigated, the characteristics and effects of diffused water between graphene and SiO2 remain unidentified. We have investigated water diffusion between monolayer graphene and SiO2 under high humidity conditions using atomic force microscopy. For a relative humidity of over 90%, water diffuses into graphene/SiO2 and forms an ice-like structure up to two layers thick. Liquid-like water can further diffuse in, stacking over the ice-like layer and evaporating relatively easily in the air causing graphene to wrinkle and fold. By similarly investigating water diffusion between graphene and mica, we argue that water-induced wrinkle formation depends on the hydrophilicity and roughness of the substrate. Open image in new window

Resistive switching (RS) memory effect in metal-oxide-metal junctions is a fascinating phenomenon toward next-generation universal nonvolatile memories. However the lack of understanding the electrical nature of RS has held back the applications. Here we demonstrate the electrical nature of bipolar RS in cobalt oxides, such as the conduction mechanism and the switching location, by utilizing a planar single oxide nanowire device. Experiments utilizing field effect devices and multiprobe measurements have shown that the nanoscale RS in cobalt oxides originates from redox events near the cathode with p-type conduction paths, which is in contrast with the prevailing oxygen vacancy based model.

As the physical limitation of scaling NAND flash memory is expected in the near future, many types of memory devices and methods to increase the memory density, such as multilayer stacking and multilevel cells, have been proposed. The cross-point structure, an effective and promising structure for multilayer stacking, is composed of alternating bit lines and word lines perpendicular to each other, with memory elements lying between them. To realize a multistack memory where bit/ word lines are designed to work as top electrodes of the lower cells and bottom electrodes of the upper cells at the same time, proper switch elements thatmeet the requisites in respect of both electronics and integration are essential. In this work, we demonstrate a room-temperature-grown oxide-based p–n heterojunction thin-film diode with high forward current density (ca. 3.5 10 A cm ) that can be used as switch elements for 3D stackable cross-point resistive memory devices. The cross-point structure, shown in Figure 1, can be combined with any type of memory cell that utilizes bistable resistance states as logic states that can be programmed and read electrically through the bit line and the word line in contact. However, when a cross-point memory is constructed in an array structure, misreading of cell resistance via lowresistance paths through unselected neighboring cells can occur. A cell in a high-resistance state is misread as being in a low-resistance state when three neighboring cells in the low-resistance state form a conducting detour. The black dotted line in Figure 1 represents one of the possible

Highly nonlinear bistable current-voltage (I–V) characteristics are necessary in order to realize high density resistive random access memory (ReRAM) devices that are compatible with cross-point stack structures. Up to now, such I–V characteristics have been achieved by introducing complex device structures consisting of selection elements (selectors) and memory elements which are connected in series. In this study, we report bipolar resistive switching (RS) behaviours of nano-crystalline BiFeO3 (BFO) nano-islands grown on Nb-doped SrTiO3 substrates, with large ON/OFF ratio of 4,420. In addition, the BFO nano-islands exhibit asymmetric I–V characteristics with high nonlinearity factor of 1,100 in a low resistance state. Such selector-free RS behaviours are enabled by the mosaic structures and pinned downward ferroelectric polarization in the BFO nano-islands. The high resistance ratio and nonlinearity factor suggest that our BFO nano-islands can be extended to an N × N array of N = 3,740 corresponding to ~107 bits. Therefore, our BFO nano-island showing both high resistance ratio and nonlinearity factor offers a simple and promising building block of high density ReRAM.

A one-bit cell of a general nonvolatile memory consists of a memory element and a switch element. Several memory elements have been tried given that any bistable states, that is, two charging states, two spin states, or two resistance states, can be used for a memory element. On the other hand, silicon-based transistors have been the most popularly used switch element. However, silicon-based transistors do not conform to high-density, nonvolatile memories with three-dimensional (3D) stack structures due to their high processing temperatures and the difficulty of growing high-quality epitaxial silicon over metals. Here, we show a low-temperaturegrown oxide diode, Pt/p-NiOx/n-TiOx/Pt, applied as a switch element for high-density, nonvolatile memories. The diode exhibits good rectifying characteristics at room temperature: a rectifying ratio of 10 at ± 3 V, a forward current density of up to ∼ 5×10 A cm, an ideality factor of 4.3, and a turn-on voltage of 2 V. Furthermore, we verify its ability to allow and deny access to the Pt/NiO/Pt memory element with two stable resistance states. Under the forward-bias condition, we could access the memory element and change the resistance state, although access was denied under the reverse bias condition. This one-diode/one-resistor (1D/1R) structure could be a promising building block for high-density, nonvolatile random-access memories with 3D stack structures. A p–n diode, like a transistor, is a fundamental circuit element for thin-film electronics. Until now, epitaxial silicon was most frequently used to fabricate p–n diodes in electronic devices with planar structures. However, to increase device density further, we require p–n diodes that are applicable to devices with 3D stack structures. Epitaxial silicon-based p–n diodes cannot be fabricated with stack structures as it is difficult to grow on a metal layer and high processing temperatures are required. On the other hand, although amorphous silicon allows for lower processing temperatures, it does not provide the required semiconducting performance. Therefore, to realize high-density electronic devices with 3D stack structures, we need new p–n diodes composed of semiconducting materials with low processing temperatures and high performance. In particular, new p–n diodes with low processing temperatures and high performance are indispensable to high-density, nonvolatile random-access memory devices. By replacing a transistor with a simpler diode as a switch element, there exists the possibility of producing memory cells with cross-point structures composed of bit lines and word lines perpendicular to each other, with a memory element lying between them. Theoretically, by utilizing this cross-point structure, the cell size can be scaled down to 4F (F: feature size used for patterning the cell), which is the smallest cell size attainable in nonvolatile memories with planar structures. Furthermore, by fabricating 3D stacks of the cross-point structure, the effective cell size can be scaled down to 2F, 1F, and so on. A common issue in realizing a cross-point structure is the availability of a thin-film diode with the high rectifying ratio and current density required for the switch element to access the memory element. Oxide based p–n diodes are good candidates to provide solutions to the issues associated with Si-based diodes. Most oxides, such as TiO2, [4] ZrO2, [5] ZnO, and indium tin oxide (ITO), are well-known n-type semiconductors that are characterized by the electron-transport properties of oxygen vacancies. As NiOx is a well-known p-type semiconductor beC O M M U N IC A IO N

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

High-quality channel layer is required for next-generation flexible electronic devices. Graphene is a good candidate due to its high carrier mobility and unique ambipolar transport characteristics but typically shows a low on/off ratio caused by gapless band structure. Popularly investigated organic semiconductors, such as pentacene, suffer from poor carrier mobility. Here, we propose a graphene/pentacene channel layer with high-k ion-gel gate dielectric. The graphene/pentacene device shows both high on/off ratio and carrier mobility as well as excellent mechanical flexibility. Most importantly, it reveals ambipolar behaviors and related negative differential resistance, which are controlled by external bias. Therefore, our graphene/pentacene barristor with ion-gel gate dielectric can offer various flexible device applications with high performances.

We have studied ferroelectricity in ultrathin (down to 5 nm) PbZrO3/PbTiO3 artificial superlattice by scanning probe microscopy (SPM). Synchrotron x-ray diffraction patterns showed only (00l) reflections. The average c-axis lattice parameters decreased with decreasing film thickness from 20 nm down to 5 nm along with the decrease in piezoresponse signal. By means of piezoresponse images and d33 hysteresis measurement using piezoresponse force microscope (PFM), we demonstrated that the atomically smooth superlattices showed the uniform polarized domain patterns and ferroelectric polarization switching. The results reveal that the superlattice retains a stable ferroelectricity down to 5 nm thickness, although with a reduced piezoresponse signal.

Pb0.65Ba0.35ZrO3 (PBZ) thin films have been grown on MgO (001) substrates by pulsed-laser deposition (PLD). We have compared the structural and dielectric properties of PBZ films grown at various temperatures. A highly c-axis orientation has appeared at PBZ film grown at the deposition temperature of 550oC. The c-axis oriented PBZ film has also shown the largest tunability among all the PBZ films in capacitance-voltage measurements. The tunability and dielectric loss of the PBZ film was 20% and 0.00959, respectively. In addition, we have compared the temperature coefficient of capacitance (TCC) of a PBZ film with that of a Ba0.5Sr0.5TiO3 (BST) film which is a well-known material applicable to tunable microwave devices. We have confirmed that TCC value of a PBZ thin film was three-times smaller than that of a BST thin film.

PbZrO3 (PZO)/PbTiO3 (PTO) artificial superlattices have been grown on La0.5Sr0.5CoO3 (LSCO) (100)/MgO (100) substrate by pulsed laser deposition (PLD) with various stacking periods from 1 to 100 unit-cells. The ferroelectric properties of the superlattices were investigated by scanning probe microscopy (SPM). We have compared the superlattices to Pb(Zr0.5Ti0.5)O3 (PZT) thin films with respect to topographic features (roughness and grain size) and local polarization behavior. The polarization of PZT and superlattices was evaluated by measuring the surface potential using Kelvin force microscopy (KFM). The roughness and grain size of the superlattices were smaller than that of PZT thin films. The surface potential of superlattice with a 2 unit cell-stacking period (PZO2/PTO2) was as large as 1009 mV compared to PZT thin films with same thickness (i.e., 50 nm). As the total thickness of PZO2/PTO2 decreased, the corresponding surface potential decreased. The polarized domain size of the superlattice was depen...

With a simply modified circuit design connecting a Pt/NiO/Pt capacitor to a serial load resistor (RL), resistive switching (RS) characteristics are significantly improved. Distributions of current at low-resistance state and switching voltages during reset and set processes are much reduced, and RS endurance is much enhanced. Using percolation theory, we find that a multiply connected conducting filament (CF) is preferentially formed in a Pt/NiO/Pt capacitor serially connected to an RL of 1 kΩ. The multiply connected CF may provide uniform heat distribution to a Pt/NiO/Pt capacitor, resulting in reduced randomness during heat-assisted reset process and improved RS characteristics.

We have heteroepitaxially deposited pure and TiO2-doped Ba0.6Sr0.4TiO3(BST-0.4) films on (001)-oriented MgO substrates using pulsed-laser deposition. By optimizing microstructures, we have successfully increased the dielectric nonlinearity and decreased the dielectric loss of BST films. By inserting a very thin Ba1-xSrxTiO3 (x=0.1–0.7) interlayer between the MgO substrate and the main layer of BST-0.4, we are able to manipulate strain states and dielectric properties of BST-0.4 films. In addition, we have systematically compared the dielectric properties of pure and TiO2-doped BST-0.4 films.

High-performance ultra-thin oxide layers are required for various next-generation electronic and optical devices. In particular, ultra-thin resistive switching (RS) oxide layers are expected to become fundamental building blocks of three-dimensional high-density non-volatile memory devices. Until now, special deposition techniques have been introduced for realization of high-quality ultra-thin oxide layers. Here, we report that ultra-thin oxide layers with reliable RS behavior can be self-assembled by field-induced oxygen migration (FIOM) at the interface of an oxide-conductor/oxide-insulator or oxide-conductor/metal. The formation via FIOM of an ultra-thin oxide layer with a thickness of approximately 2-5 nm and 2.5% excess oxygen content is demonstrated using cross-sectional transmission electron microscopy and secondary ion mass spectroscopy depth profile. The observed RS behavior, such as the polarity dependent forming process, can be attributed to the formation of an ultra-thin oxide layer. In general, as oxygen ions are mobile in many oxide-conductors, FIOM can be used for the formation of ultra-thin oxide layers with desired properties at the interfaces or surfaces of oxide-conductors in high-performance oxide-based devices.

Our work on tunable rf and microwave devices based on 90° off-axis magnetron sputtered Ba0.6Sr0.4TiO3 epitaxial thin films is reviewed. In particular, we have studied the effects of energetic bombardment during deposition on the structural and electrical properties of these films. The fundamental result of changing the energetic bombardment conditions during deposition is to affect the stress/strain state of the films. We show that high bombardment conditions result in films with significantly extended out-of-plane lattice constants and depressed dielectric constants and tunabilities.

A floating gate (FG) memory structure employing Zr nanocrystals (NCs) embedded in a ZrO2 dielectric layer was fabricated for the first time through a one-step process using dc-magnetron sputtering deposition. The unique FG memory stacked only with an NC-capping ZrO2 control oxide layer, without a tunneling oxide layer, was obtained under oxygen-deficient conditions during the sputtering process. Transmission electron microscopy (TEM) revealed that crystalline Zr-NCs with sizes ranging from 3 to 8 nm were embedded in the ZrO2 layer with densities of Zr-NC up to 1.22 ×1012 cm-2. Capacitance versus voltage (C–V) curves of a Zr-NC-based metal–oxide–semiconductor (MOS) capacitor were also obtained. The clockwise C–V hysteresis loops on the basis of the Zr-NC-based MOS structure fabricated in this work were understood by the electron trapping of Zr–O dangling bonds at the interface between Zr-NCs and the ZrO2 capping layer.

Epitaxial Bi4Ti3O12 (BTO) thin films were deposited on MgO(001) substrates using Pt layers as top and bottom electrodes. In spite of the apparently symmetric capacitor structure, polarization–voltage measurements revealed strong imprint failures and current–voltage measurements showed rectifying behaviors. Imprint pulse tests with a 5 V dc bias and post-annealing treatments suggested that the asymmetric behaviors should be due to interfacial states induced by thermal processes. To probe the interfacial states, capacitance–voltage (C–V) measurements were performed. By fitting the C–V data with a model which describes the Pt/BTO/Pt structure as a series circuit composed of three capacitors, built-in voltages at the top and the bottom interfaces could be determined. Difference in the built-in voltages could explain the imprint failures and the rectifying behaviors. The interfacial states in the BTO capacitors were controlled by varying electrode materials.

Negative resistance behavior and reproducible resistance switching were found in polycrystalline NiO films deposited by dc magnetron reactive sputtering methods. Oxygen to argon gas ratio during deposition was critical in deciding the detailed switching characteristics of either bi-stable memory switching or mono-stable threshold switching. Both metallic nickel defects and nickel vacancies influenced the negative resistance and the switching characteristics. We obtained a distribution of low resistance values which were dependent on the compliance current of high-to-low resistance switching. At 200°C, the low-resistance state kept its initial resistance value while the high-resistance state reached 85% of its initial resistance value after 5×105s. We suggested that the negative resistance and the switching mechanism could be described by electron conduction related to metallic nickel defect states existing in deep levels and by small-polaron hole hopping conduction.

We report the impact of intrinsic defects in epitaxial BiFeO3 films on charge conduction and resistive switching of Pt/BiFeO3/SrRuO3 capacitors, although the BiFeO3 films show very similar ferroelectric domain types probed by piezoresponse force microscopy. Capacitors with p-type Bi-deficient and n-type Bi-rich BiFeO3 films exhibit switchable diode and conventional bipolar resistive switching behaviors, respectively. Both the capacitors show good retention properties with a high ON/OFF ratio of >100 in Bi-deficient films and that of >1000 in Bi-rich films. The present investigation advances considerably understanding of interface control through defect engineering of BiFeO3 thin films for non-volatile memory application.

We have presented a study of the bipolar resistance switching characteristics in the Ag/ZnO/Pt cell. This switching is accompanied by a change in intensity of the photoluminescence emission at 3.33 eV which is attributed to zinc vacancy related transitions in ZnO film. Besides voltage-driven resistance switching phenomena, a transition from a high-resistance state to a lower one is observed under laser illumination at low temperature. These results demonstrate that the bipolar resistance switching can originate due to an electron trapping/de-trapping process at zinc-vacancy defects localized in the interface layer. The Mott metal-insulator transition is proposed as a possible mechanism of the memory effect.

Electrically driven resistance change phenomenon in metal/NiO/metal junctions, so-called resistive switching (RS), is a candidate for next-generation universal nonvolatile memories. However, the knowledge as to RS mechanisms is unfortunately far from comprehensive, especially the spatial switching location, which is crucial information to design reliable devices. In this communication, we demonstrate the identification of the spatial switching location of bipolar RS by introducing asymmetrically passivated planar NiO nanowire junctions. We have successfully identified that the bipolar RS in NiO occurs near the cathode rather than the anode. This trend can be interpreted in terms of an electrochemical redox model based on ion migration and p-type conduction.

We have investigated structural, electrical, and electro-mechanical properties of lead-free piezoelectric BaTiO3 doped Na0.5K0.5NbO3 (BTO-NKN) thin films deposited by pulsed laser deposition (PLD) methods. BTO-NKN thin films have been deposited on La0.5Sr0.5CoO3 (LSCO) bottom electrodes with LaAlO3 (LAO) substrates. X-ray diffraction data have shown that all the BTO-NKN and bottom electrodes are highly oriented with their c-axes normal to the substrates. In order to improve the morphology of BTO-NKN thin films, we have located an eclipse shutter between a target and a substrate. Root-mean-square roughness was changed from 91 nm to 21 nm with eclipse shutter enhanced PLD (E-PLD) method. Furthermore, the enhanced surface morphology leads to the improvement in electrical or electro-mechanical properties mainly due to increased density. Typical capacitance and d33 values of a BTO-NKN film deposited by E-PLD method are 1000 pF and 30 pmN, respectively.

Non-volatile memory devices are so named because they retain information when power is interrupted; thus they are important computer components. In this context, there has been considerable recent interest1,2 in developing non-volatile memories that use ferroelectric thin films—‘ferroelectric random access memories’, or FRAMs—in which information is stored in the polarization state of the ferroelectric material. To realize a practical FRAM, the thin films should satisfy the following criteria: compatibility with existing dynamic random access memory technologies, large remnant polarization (Pr) and reliable polarization-cycling characteristics. Early work focused on lead zirconate titanate (PZT) but, when films of this material were grown on metal electrodes, they generally suffered from a reduction of Pr (‘fatigue’) with polarity switching. Strontium bismuth tantalate (SBT) and related oxides have been proposed to overcome the fatigue problem3, but such materials have other shortcomings, such as a high deposition temperature. Here we show that lanthanum-substituted bismuth titanate thin films provide a promising alternative for FRAM applications. The films are fatigue-free on metal electrodes, they can be deposited at temperatures of ∼650 °C and their values of Pr are larger than those of the SBT films.

We observed bipolar switching behavior from an epitaxial strontium cobaltite film grown on a SrTiO3 (001) substrate. The crystal structure of strontium cobaltite has been known to undergo topotactic phase transformation between two distinct phases: insulating brownmillerite (SrCoO2.5) and conducting perovskite (SrCoO3−δ) depending on the oxygen content. The current–voltage characteristics of the strontium cobaltite film showed that it could have a reversible insulator-to-metal transition triggered by electrical bias voltage. We propose that the resistance switching in the SrCoOx thin film could be related to the topotactic phase transformation and the peculiar structure of SrCoO2.5.

We report a carrier type dependence on the spatial asymmetry of unipolar resistive switching for various metal oxides, including NiOx, CoOx, TiO2−x, YSZ, and SnO2−x. n-type oxides show a unipolar resistive switching at the anode side whereas p-type oxides switch at the cathode side. During the forming process, the electrical conduction path of p-type oxides extends from the anode to cathode while that of n-type oxides forms from the cathode to anode. The carrier type of switching oxide layer critically determines the spatial inhomogeneity of unipolar resistive switching during the forming process possibly triggered via the oxygen ion drift.