Localization of lattice dynamics in low-angle twisted bilayer graphene.

Twisted bilayer graphene is created by slightly rotating the two crystal networks in bilayer graphene with respect to each other. For small twist angles, the material undergoes a self-organized lattice reconstruction, leading to the formation of a periodically repeated domain1-3. The resulting superlattice modulates the vibrational3,4 and electronic5,6 structures within the material, leading to changes in the behaviour of electron-phonon coupling7,8 and to the observation of strong correlations and superconductivity9. However, accessing these modulations and understanding the related effects are challenging, because the modulations are too small for experimental techniques to accurately resolve the relevant energy levels and too large for theoretical models to properly describe the localized effects. Here we report hyperspectral optical images, generated by a nano-Raman spectroscope10, of the crystal superlattice in reconstructed (low-angle) twisted bilayer graphene. Observations of the crystallographic structure with visible light are made possible by the nano-Raman technique, which reveals the localization of lattice dynamics, with the presence of strain solitons and topological points1 causing detectable spectral variations. The results are rationalized by an atomistic model that enables evaluation of the local density of the electronic and vibrational states of the superlattice. This evaluation highlights the relevance of solitons and topological points for the vibrational and electronic properties of the structures, particularly for small twist angles. Our results are an important step towards understanding phonon-related effects at atomic and nanometric scales, such as Jahn-Teller effects11 and electronic Cooper pairing12-14, and may help to improve device characterization15 in the context of the rapidly developing field of twistronics16.

A scalable neuristor built with Mott memristors.

The Hodgkin-Huxley model for action potential generation in biological axons is central for understanding the computational capability of the nervous system and emulating its functionality. Owing to the historical success of silicon complementary metal-oxide-semiconductors, spike-based computing is primarily confined to software simulations and specialized analogue metal-oxide-semiconductor field-effect transistor circuits. However, there is interest in constructing physical systems that emulate biological functionality more directly, with the goal of improving efficiency and scale. The neuristor was proposed as an electronic device with properties similar to the Hodgkin-Huxley axon, but previous implementations were not scalable. Here we demonstrate a neuristor built using two nanoscale Mott memristors, dynamical devices that exhibit transient memory and negative differential resistance arising from an insulating-to-conducting phase transition driven by Joule heating. This neuristor exhibits the important neural functions of all-or-nothing spiking with signal gain and diverse periodic spiking, using materials and structures that are amenable to extremely high-density integration with or without silicon transistors.

Lognormal switching times for titanium dioxide bipolar memristors: origin and resolution.

We measured the switching time statistics for a TiO(2) memristor and found that they followed a lognormal distribution, which is a potentially serious problem for computer memory and data storage applications. We examined the underlying physical phenomena that determine the switching statistics and proposed a simple analytical model for the distribution based on the drift/diffusion equation and previously measured nonlinear drift behavior. We designed a closed-loop switching protocol that dramatically narrows the time distribution, which can significantly improve memory circuit performance and reliability.

Sub-nanosecond switching of a tantalum oxide memristor.

We report sub-nanosecond switching of a metal-oxide-metal memristor utilizing a broadband 20 GHz experimental setup developed to observe fast switching dynamics. Set and reset operations were successfully performed in the tantalum oxide memristor using pulses with durations of 105 and 120 ps, respectively. Reproducibility of the sub-nanosecond switching was also confirmed as the device switched over consecutive cycles.

Measuring the switching dynamics and energy efficiency of tantalum oxide memristors.

We measured the real-time switching of metal-oxide memristors with sub-nanosecond resolution and recorded the evolution of the current and voltage during both ON (set) and OFF (reset) events. From these we determined the dynamical behavior of the conductivity for different applied bias amplitudes. Quantitative analysis of the energy cost and switching dynamics showed 115 fJ for ON-switching and 13 pJ for OFF-switching when resistance change was limited to 200%. Results are presented that show a favorable scaling with speed in terms of energy cost and reducing unnecessary damage to the devices.

Observation of two resistance switching modes in TiO2 memristive devices electroformed at low current.

We report the observation of two resistance switching modes in certain 50 nm × 50 nm crossbar TiO(2) memristive devices that have been electroformed with a low-current process. The two switching modes showed opposite switching polarities. The intermediate state was shared by both modes (the ON state of the high-resistance mode or the OFF state of the low-resistance mode) and exhibited a relaxation to a more resistive state, including an initial transient decay. The activation energies of such a decay and ON-switching to the intermediate state were determined to be 50-210 meV and 1.1 eV, respectively. Although they are attributed to the coexistence of charge trapping and ionic motion, the ionic motion dominates in both switching modes. Our results indicate that the two switching modes in our system correspond to different switching layers adjacent to the interfaces at the top and bottom electrodes.

The switching location of a bipolar memristor: chemical, thermal and structural mapping.

Memristors are memory resistors promising a rapid integration into future memory technologies. However, progress is still critically limited by a lack of understanding of the physical processes occurring at the nanoscale. Here we correlate device electrical characteristics with local atomic structure, chemistry and temperature. We resolved a single conducting channel that is made up of a reduced phase of the as-deposited titanium oxide. Moreover, we observed sufficient Joule heating to induce a crystallization of the oxide surrounding the channel, with a peculiar pattern that finite element simulations correlated with the existence of a hot spot close to the bottom electrode, thus identifying the switching location. This work reports direct observations in all three dimensions of the internal structure of titanium oxide memristors.

Impact of geometry on the performance of memristive nanodevices.

We examined the influence of memristor geometry on switching endurance by comparing ribbed and planar TiO(2)-based cross-point devices with 50 nm × 50 nm lateral dimensions. We observed that planar devices exhibited a factor of over four improvement in median endurance value over ribbed structures for otherwise identical structures. Our simulations indicated that the corners in the upper wires of the ribbed devices experienced higher current density and more heating during device forming and switching, and hence a shorter life time.

The limits of near field immersion microwave microscopy evaluated by imaging bilayer graphene moiré patterns.

Near field scanning Microwave Impedance Microscopy can resolve structures as small as 1 nm using radiation with wavelengths of 0.1 m. Combining liquid immersion microscopy concepts with exquisite force control exerted on nanoscale water menisci, concentration of electromagnetic fields in nanometer-size regions was achieved. As a test material we use twisted bilayer graphene, because it provides a sample where the modulation of the moiré superstructure pattern can be systematically tuned from Ångstroms up to tens of nanometers. Here we demonstrate that a probe-to-pattern resolution of 108 can be obtained by analyzing and adjusting the tip-sample distance influence on the dynamics of water meniscus formation and stability.

A memristor-based nonvolatile latch circuit.

Memristive devices, which exhibit a dynamical conductance state that depends on the excitation history, can be used as nonvolatile memory elements by storing information as different conductance states. We describe the implementation of a nonvolatile synchronous flip-flop circuit that uses a nanoscale memristive device as the nonvolatile memory element. Controlled testing of the circuit demonstrated successful state storage and restoration, with an error rate of 0.1%, during 1000 power loss events. These results indicate that integration of digital logic devices and memristors could open the way for nonvolatile computation with applications in small platforms that rely on intermittent power sources. This demonstrated feasibility of tight integration of memristors with CMOS (complementary metal-oxide-semiconductor) circuitry challenges the traditional memory hierarchy, in which nonvolatile memory is only available as a large, slow, monolithic block at the bottom of the hierarchy. In contrast, the nonvolatile, memristor-based memory cell can be fast, fine-grained and small, and is compatible with conventional CMOS electronics. This threatens to upset the traditional memory hierarchy, and may open up new architectural possibilities beyond it.

Memristor-CMOS hybrid integrated circuits for reconfigurable logic.

Hybrid reconfigurable logic circuits were fabricated by integrating memristor-based crossbars onto a foundry-built CMOS (complementary metal-oxide-semiconductor) platform using nanoimprint lithography, as well as materials and processes that were compatible with the CMOS. Titanium dioxide thin-film memristors served as the configuration bits and switches in a data routing network and were connected to gate-level CMOS components that acted as logic elements, in a manner similar to a field programmable gate array. We analyzed the chips using a purpose-built testing system, and demonstrated the ability to configure individual devices, use them to wire up various logic gates and a flip-flop, and then reconfigure devices.

Structural and chemical characterization of TiO2 memristive devices by spatially-resolved NEXAFS.

We used spatially-resolved NEXAFS (near-edge x-ray absorption fine structure) spectroscopy coupled with microscopy to characterize the electronic, structural and chemical properties of bipolar resistive switching devices. Metal/TiO2/metal devices were electroformed with both bias polarities and then physically opened to study the resulting material changes within the device. Soft x-ray absorption techniques allowed isolated study of the different materials present in the device with 100 nm spatial resolution. The resulting morphology and structural changes reveal a picture of localized polarity-independent heating occurring within these devices initiated by and subsequently accelerating polarity-dependent electrochemical reduction/oxidation processes.

Quantized conductance coincides with state instability and excess noise in tantalum oxide memristors.

Tantalum oxide memristors can switch continuously from a low-conductance semiconducting to a high-conductance metallic state. At the boundary between these two regimes are quantized conductance states, which indicate the formation of a point contact within the oxide characterized by multistable conductance fluctuations and enlarged electronic noise. Here, we observe diverse conductance-dependent noise spectra, including a transition from 1/f(2) (activated transport) to 1/f (flicker noise) as a function of the frequency f, and a large peak in the noise amplitude at the conductance quantum GQ=2e(2)/h, in contrast to suppressed noise at the conductance quantum observed in other systems. We model the stochastic behaviour near the point contact regime using Molecular Dynamics-Langevin simulations and understand the observed frequency-dependent noise behaviour in terms of thermally activated atomic-scale fluctuations that make and break a quantum conductance channel. These results provide insights into switching mechanisms and guidance to device operating ranges for different applications.

Characterization of electroforming-free titanium dioxide memristors.

Metal-insulator-metal (MIM) structures based on titanium dioxide have demonstrated reversible and non-volatile resistance-switching behavior and have been identified with the concept of the memristor. Microphysical studies suggest that the development of sub-oxide phases in the material drives the resistance changes. The creation of these phases, however, has a number of negative effects such as requiring an elevated voltage, increasing the device-to-device variability, damaging the electrodes due to oxygen evolution, and ultimately limiting the device lifetime. In this work we show that the deliberate inclusion of a sub-oxide layer in the MIM structure maintains the favorable switching properties of the device, while eliminating many of the negative effects. Electrical and microphysical characterization of the resulting structures was performed, utilizing X-ray and electron spectroscopy and microscopy. In contrast to structures which are not engineered with a sub-oxide layer, we observed dramatically reduced microphysical changes after electrical operation.

Continuous electrical tuning of the chemical composition of TaO(x)-based memristors.

TaO(x)-based memristors have recently demonstrated both subnanosecond resistance switching speeds and very high write/erase switching endurance. Here we show that the physical state variable that enables these properties is the oxygen concentration in a conduction channel, based on the measurement of the thermal coefficient of resistance of different TaO(x) memristor states and a set of reference Ta-O films of known composition. The continuous electrical tunability of the oxygen concentration in the channel, with a resolution of a few percent, was demonstrated by controlling the write currents with a one transistor-one memristor (1T1M) circuit. This study demonstrates that solid-state chemical kinetics is important for the determination of the electrical characteristics of this relatively new class of device.

Anatomy of a nanoscale conduction channel reveals the mechanism of a high-performance memristor.

By employing a precise method for locating and directly imaging the active switching region in a resistive random access memory (RRAM) device, a nanoscale conducting channel consisting of an amorphous Ta(O) solid solution surrounded by nearly stoichiometric Ta(2) O(5) is observed. Structural and chemical analysis of the channel combined with temperature-dependent transport measurements indicate a unique resistance switching mechanism.

Sketched oxide single-electron transistor.

Devices that confine and process single electrons represent an important scaling limit of electronics. Such devices have been realized in a variety of materials and exhibit remarkable electronic, optical and spintronic properties. Here, we use an atomic force microscope tip to reversibly 'sketch' single-electron transistors by controlling a metal-insulator transition at the interface of two oxides. In these devices, single electrons tunnel resonantly between source and drain electrodes through a conducting oxide island with a diameter of ∼1.5 nm. We demonstrate control over the number of electrons on the island using bottom- and side-gate electrodes, and observe hysteresis in electron occupation that is attributed to ferroelectricity within the oxide heterostructure. These single-electron devices may find use as ultradense non-volatile memories, nanoscale hybrid piezoelectric and charge sensors, as well as building blocks in quantum information processing and simulation platforms.

Scanning tunneling microscopy of template-stripped Au surfaces and highly ordered self-assembled monolayers.

Template stripping of Au films in ultrahigh vacuum (UHV) produces atomically flat and pristine surfaces that serve as substrates for highly ordered self-assembled monolayer (SAM) formation. Atomic resolution scanning tunneling microscopy of template-stripped (TS) Au stripped in UHV confirms that the stripping process produces a flat, predominantly 111 textured, atomically clean surface. Octanethiol SAMs vapor deposited in situ onto UHV TS Au show a c(4 x 2) superlattice with (square root 3 x square root 3) R30 degrees basic molecular structure having an ordered domain size up to 100 nm wide. These UHV results validate the TS Au surface as a simple, clean and high-quality surface preparation method for SAMs deposited from both vapor phase and solution phase.

Thermodynamics of coherently-strained GexSi1-x nanocrystals on Si(001): alloy composition and island formation.

We determined the enthalpic and entropic contributions to the thermodynamics of coherently strained nanocrystals grown via deposition of pure Ge on Si(001) surfaces at 600 and 700 degrees C by analyzing their composition profile and local strain. We found that the free energy associated with the entropy of mixing, which drives GexSi1-x alloy formation, was significantly larger than the relaxation enthalpy that produces the islands. Thus, entropy plays a significant role in the evolution of the size and shape of the islands during growth through the strong thermodynamic drive to form an alloy.