Electric Switching of the Charge-Density-Wave and Normal Metallic Phases in Tantalum Disulfide Thin-Film Devices

We report on switching among three charge-density-wave phases - commensurate, nearly commensurate, incommensurate - and the high-temperature normal metallic phase in thin-film 1T-TaS2 devices induced by application of an in-plane electric field. The electric switching among all phases has been achieved over a wide temperature range, from 77 K to 400 K. The low-frequency electronic noise spectroscopy has been used as an effective tool for monitoring the transitions, particularly the switching from the incommensurate charge-density-wave phase to the normal metal phase. The noise spectral density exhibits sharp increases at the phase transition points, which correspond to the step-like changes in resistivity. Assignment of the phases is consistent with low-field resistivity measurements over the temperature range from 77 K to 600 K. Analysis of the experimental data and calculations of heat dissipation suggest that Joule heating plays a dominant role in the electric-field induced transitions in the tested 1T-TaS2 devices on Si/SiO2 substrates. The possibility of electrical switching among four different phases of 1T-TaS2 is a promising step toward nanoscale device applications. The results also demonstrate the potential of noise spectroscopy for investigating and identifying phase transitions in materials.Comment: 32 pages, 7 figure

Spin - Phonon Coupling in Nickel Oxide Determined from Ultraviolet Raman Spectroscopy

Nickel oxide (NiO) has been studied extensively for various applications ranging from electrochemistry to solar cells [1,2]. In recent years, NiO attracted much attention as an antiferromagnetic (AF) insulator material for spintronic devices [3-10]. Understanding the spin - phonon coupling in NiO is a key to its functionalization, and enabling AF spintronics' promise of ultra-high-speed and low-power dissipation [11,12]. However, despite its status as an exemplary AF insulator and a benchmark material for the study of correlated electron systems, little is known about the spin - phonon interaction, and the associated energy dissipation channel, in NiO. In addition, there is a long-standing controversy over the large discrepancies between the experimental and theoretical values for the electron, phonon, and magnon energies in NiO [13-23]. This gap in knowledge is explained by NiO optical selection rules, high Neel temperature and dominance of the magnon band in the visible Raman spectrum, which precludes a conventional approach for investigating such interaction. Here we show that by using ultraviolet (UV) Raman spectroscopy one can extract the spin - phonon coupling coefficients in NiO. We established that unlike in other materials, the spins of Ni atoms interact more strongly with the longitudinal optical (LO) phonons than with the transverse optical (TO) phonons, and produce opposite effects on the phonon energies. The peculiarities of the spin - phonon coupling are consistent with the trends given by density functional theory calculations. The obtained results shed light on the nature of the spin - phonon coupling in AF insulators and may help in developing innovative spintronic devices.Comment: 16 pages; 2 figure

Thermal Conductivity and Thermal Rectification in Graphene Nanoribbons: a Molecular Dynamics Study

We have used molecular dynamics to calculate the thermal conductivity of symmetric and asymmetric graphene nanoribbons (GNRs) of several nanometers in size (up to ~4 nm wide and ~10 nm long). For symmetric nanoribbons, the calculated thermal conductivity (e.g. ~2000 W/m-K @400K for a 1.5 nm {\times} 5.7 nm zigzag GNR) is on the similar order of magnitude of the experimentally measured value for graphene. We have investigated the effects of edge chirality and found that nanoribbons with zigzag edges have appreciably larger thermal conductivity than nanoribbons with armchair edges. For asymmetric nanoribbons, we have found significant thermal rectification. Among various triangularly-shaped GNRs we investigated, the GNR with armchair bottom edge and a vertex angle of 30{\deg} gives the maximal thermal rectification. We also studied the effect of defects and found that vacancies and edge roughness in the nanoribbons can significantly decrease the thermal conductivity. However, substantial thermal rectification is observed even in the presence of edge roughness.Comment: 13 pages, 5 figures, slightly expanded from the published version on Nano Lett. with some additional note

Direct Observation of Martensitic Phase-Transformation Dynamics in Iron by 4D Single-Pulse Electron Microscopy

The in situ martensitic phase transformation of iron, a complex solid-state transition involving collective atomic displacement and interface movement, is studied in real time by means of four-dimensional (4D) electron microscopy. The iron nanofilm specimen is heated at a maximum rate of ∼10^(11) K/s by a single heating pulse, and the evolution of the phase transformation from body-centered cubic to face-centered cubic crystal structure is followed by means of single-pulse, selected-area diffraction and real-space imaging. Two distinct components are revealed in the evolution of the crystal structure. The first, on the nanosecond time scale, is a direct martensitic transformation, which proceeds in regions heated into the temperature range of stability of the fcc phase, 1185−1667 K. The second, on the microsecond time scale, represents an indirect process for the hottest central zone of laser heating, where the temperature is initially above 1667 K and cooling is the rate-determining step. The mechanism of the direct transformation involves two steps, that of (barrier-crossing) nucleation on the reported nanosecond time scale, followed by a rapid grain growth typically in ∼100 ps for 10 nm crystallites

Ultrathin Oxide Films by Atomic Layer Deposition on Graphene

In this paper, a method is presented to create and characterize mechanically robust, free standing, ultrathin, oxide films with controlled, nanometer-scale thickness using Atomic Layer Deposition (ALD) on graphene. Aluminum oxide films were deposited onto suspended graphene membranes using ALD. Subsequent etching of the graphene left pure aluminum oxide films only a few atoms in thickness. A pressurized blister test was used to determine that these ultrathin films have a Young's modulus of 154 \pm 13 GPa. This Young's modulus is comparable to much thicker alumina ALD films. This behavior indicates that these ultrathin two-dimensional films have excellent mechanical integrity. The films are also impermeable to standard gases suggesting they are pinhole-free. These continuous ultrathin films are expected to enable new applications in fields such as thin film coatings, membranes and flexible electronics.Comment: Nano Letters (just accepted

Simulation of dimensionality effects in thermal transport

The discovery of nanostructures and the development of growth and fabrication techniques of one- and two-dimensional materials provide the possibility to probe experimentally heat transport in low-dimensional systems. Nevertheless measuring the thermal conductivity of these systems is extremely challenging and subject to large uncertainties, thus hindering the chance for a direct comparison between experiments and statistical physics models. Atomistic simulations of realistic nanostructures provide the ideal bridge between abstract models and experiments. After briefly introducing the state of the art of heat transport measurement in nanostructures, and numerical techniques to simulate realistic systems at atomistic level, we review the contribution of lattice dynamics and molecular dynamics simulation to understanding nanoscale thermal transport in systems with reduced dimensionality. We focus on the effect of dimensionality in determining the phononic properties of carbon and semiconducting nanostructures, specifically considering the cases of carbon nanotubes, graphene and of silicon nanowires and ultra-thin membranes, underlying analogies and differences with abstract lattice models.Comment: 30 pages, 21 figures. Review paper, to appear in the Springer Lecture Notes in Physics volume "Thermal transport in low dimensions: from statistical physics to nanoscale heat transfer" (S. Lepri ed.

Effect of Layer-Stacking on the Electronic Structure of Graphene Nanoribbons

The evolution of electronic structure of graphene nanoribbons (GNRs) as a function of the number of layers stacked together is investigated using \textit{ab initio} density functional theory (DFT) including interlayer van der Waals interactions. Multilayer armchair GNRs (AGNRs), similar to single-layer AGNRs, exhibit three classes of band gaps depending on their width. In zigzag GNRs (ZGNRs), the geometry relaxation resulting from interlayer interactions plays a crucial role in determining the magnetic polarization and the band structure. The antiferromagnetic (AF) interlayer coupling is more stable compared to the ferromagnetic (FM) interlayer coupling. ZGNRs with the AF in-layer and AF interlayer coupling have a finite band gap while ZGNRs with the FM in-layer and AF interlayer coupling do not have a band gap. The ground state of the bi-layer ZGNR is non-magnetic with a small but finite band gap. The magnetic ordering is less stable in multilayer ZGNRs compared to single-layer ZGNRs. The quasipartcle GW corrections are smaller for bilayer GNRs compared to single-layer GNRs because of the reduced Coulomb effects in bilayer GNRs compared to single-layer GNRs.Comment: 10 pages, 5 figure

A Self Assembled Nanoelectronic Quantum Computer Based on the Rashba Effect in Quantum Dots

Quantum computers promise vastly enhanced computational power and an uncanny ability to solve classically intractable problems. However, few proposals exist for robust, solid state implementation of such computers where the quantum gates are sufficiently miniaturized to have nanometer-scale dimensions. Here I present a new approach whereby a complete computer with nanoscale gates might be self-assembled using chemical synthesis. Specifically, I demonstrate how to self-assemble the fundamental unit of this quantum computer - a 2-qubit universal quantum controlled-NOT gate - based on two exchange coupled multilayered quantum dots. Then I show how these gates can be wired using thiolated conjugated molecules as electrical connectors. A qubit is encoded in the ground state of a quantum dot spin-split by the Rashba interaction. Arbitrary qubit rotations are effected by bringing the spin splitting energy in a target quantum dot in resonance with a global ac magnetic field by applying a potential pulse of appropriate amplitude and duration to the dot. The controlled dynamics of the 2-qubit controlled-NOT operation (XOR) can be realized by exploiting the exchange coupling with the nearest neighboring dot. A complete prescription for initialization of the computer and data input/output operations is presented.Comment: 22 pages, 4 figure