Negative Differential Resistance in Carbon-Based Nanostructures
S. A. Evlashin, M. A. Tarkhov, D. A. Chernodubov, A. V. Inyushkin, A. A. Pilevsky, P. V. Dyakonov, A. A. Pavlov, N. V. Suetin, I. S. Akhatov, V. Perebeinos
Nonlinear electrical properties, such as negative differential resistance (NDR), are essential in numerous electrical circuits, including memristors. Several physical origins have been proposed to lead to the NDR phenomena in semiconductor devices in the last more than half a century. Here, we report NDR behavior formation in randomly oriented graphene-like nanostructures up to 37 K and high on-current density up to 10^5 A/cm^2. Our modeling of the current-voltage characteristics, including the self-heating effects, suggests that strong temperature dependence of the low-bias resistance is responsible for the nonlinear electrical behavior. Our findings open opportunities for the practical realization of the on-demand NDR behavior in nanostructures of 2D and 3D material-based devices via heat management in the conducting films and the underlying substrates.
Hyperfine interactions, magnetic interactions between the spins of electrons and nuclei, in graphene and related carbon nanostructures are studied. By using a combination of accurate first principles calculations on graphene fragments and statistical analysis, I show that both isotropic and dipolar hyperfine interactions can be accurately described in terms of the local electron spin distribution and atomic structure. A complete set of parameters describing the hyperfine interactions of C-13 and other nuclear spins at substitution impurities and edge terminations is determined.
Grain boundaries are commonly observed in carbon nanostructures, but their influence on thermal and electric properties are still not completely understood. Using a combined approach of density functional tight-binding theory and non-equilibrium Green functions we investigate electron and phonon transport in carbon based systems. In this work, quantum transport and thermoelectric properties are summarized for graphene sheets, graphene nanoribbons and carbon nanotubes with a variety of grain boundary types in a wide temperature range. Motivated by previous findings that disorder scatters phonon…
Graphdiyne, atomically-thin 2D carbon nanostructure based on sp-sp2 hybridization, is an appealing system potentially showing outstanding mechanical and optoelectronic properties. Surface-catalyzed coupling of halogenated sp-carbon-based molecular precursors represents a promising bottom-up strategy to fabricate extended 2D carbon systems with engineered structure on metallic substrates. Here, we investigate the atomic-scale structure and electronic and vibrational properties of an extended graphdiyne-like sp-sp2 carbon nanonetwork grown on Au(111) by means of on-surface synthesis. The formati…
Using the Büttiker-Landauer formulation of transport theory in the linear response regime, the valley currents and non-local resistances of bilayer graphene nanostructures with broken inversion symmetry are calculated. It is shown that broken inversion symmetry in bilayer graphene nanostructures leads to striking enhancement of the non-local 4-terminal resistance and to valley currents several times stronger than the conventional electric current when the Fermi energy is in the spectral gap close to the energy of Dirac point. The scaling relation between local and non-local resistances is inve…
The impact of the edges and presence of dopants to the work function (WF) of graphene nanoribbons (GNR) and nanoflakes was studied by an ab initio approach. The strong dependence of the WF upon the GNR structure was found and a promising character for the field emission by the donor type impurities was observed. Basing on the predominant impact of the nanostructure edges to the emission properties, the small graphene flakes were investigated as a possible source for the electron emission. The obtained weak dependence of the low WF values of the graphene flakes on their size and shape allows to…
High-dose irradiation of nanostructures consisting of multiple graphene shells, such as spherical 'carbon onions' (CO) or cylindrical multi-walled carbon nanotubes (MWNT), induces shell shrinkage by bond reconstruction around irradiation-induced defects. This leads to build-up of internal stresses and to extreme pressures acting on encapsulated materials or on the carbon cores of the nanostructures. We formulate a model which relates the build-up of internal stresses to the point defect dynamics in graphene shells. Calculations are performed for the special case of irradiated CO. The results a…
Emergence of $π$-magnetism in open-shell nanographenes has been theoretically predicted decades ago but their experimental characterization was elusive due to the strong chemical reactivity that makes their synthesis and stabilization difficult. In recent years, on-surface synthesis under vacuum conditions has provided unprecedented opportunities for atomically precise engineering of nanographenes, which in combination with scanning probe techniques have led to a substantial progress in our capabilities to realize localized electron spin states and to control electron spin interactions at the …
Based on the analysis of the data on the behavior of electric conductivity at the detonation of condensed high explosives (HEs) with the composition CHNO and the carbon mass fraction higher than 0.1, the conclusion was made of the presence of long carbon nanostructures. These structures penetrate all the space of reacting HE. The structures are formed already in the chemical peak region, and they evolve along the detonation wave.
The resistance of the electron gas at the interface between the two band insulators LaAlO3 (LAO) and SrTiO3 (STO) typically drops monotonically with temperature and R/T curves during cooling and warm-up look identical for large area structures. Here we show that if the LAO/STO is laterally restricted by nanopatterning the resistance exhibits a temperature anomaly. Warming up nanostructures from low temperatures leads to one or two pronounced resistance peaks between 50 and 100 K not observed for larger dimensions. During cool-down current filaments emerge at the domain walls that form during t…
The carbon nanostructures are perspective materials for the future applications. This has two reasons: first, the hexagonal atomic structure which enables a high molecular variability by placing different kinds of the defects and second, good electronic properties which can be modified for the purpose of the concrete applications with the help of the defects and of the chemical ingredients. A lot of kinds of the nanostructures was investigated. Here, the properties of less common forms will be examined - the graphitic nanocone and graphitic wormhole.
We report on the observation of non-metallic electrical conduction, resistive switching, and a negative temperature coefficient of resistance in cluster-assembled nanostructured gold films above the electrical percolation and in strong-coupling regime, from room to cryogenic temperatures (24K). The structure of the films is characterized by an extremely high density of randomly oriented crystalline nanodomains, separated by grain boundaries. The observed behavior can be explained by considering space charge limited conduction and Coulomb blockade phenomena highlighting the influence of the hig…
An oscillatory dependence of the drain current on the drain voltage is found in a nanostructure consisting of two crossing semiconductor carbon nanotubes that are suspended over a dielectric trench, which is backed by a doped silicon substrate that acts as a gate. Alternating positive and negative differential resistance regions are generated as a function of the drain source values and can be slightly shifted by the gate voltage. Moreover, the negative differential resistance is retrieved in a large bandwidth, of up to 100 MHz, when the structure is excited with ac signals.
The construction of atomically-precise carbon nanostructures holds promise for developing novel materials for scientific study and nanotechnology applications. Here we show that graphene origami is an efficient way to convert graphene into atomically-precise, complex, and novel nanostructures. By scanning-tunneling-microscope manipulation at low temperature, we repeatedly fold and unfold graphene nanoislands (GNIs) along arbitrarily chosen direction. A bilayer graphene stack featuring a tunable twist angle and a tubular edge connection between the layers are formed. Folding single-crystal GNIs…
We present an experimental investigation on the scaling of resistance in individual single walled carbon nanotube devices with channel lengths that vary four orders of magnitude on the same sample. The electron mean free path is obtained from the linear scaling of resistance with length at various temperatures. The low temperature mean free path is determined by impurity scattering, while at high temperature the mean free path decreases with increasing temperature, indicating that it is limited by electron-phonon scattering. An unusually long mean free path at room temperature has been experim…
In this paper we investigate from first principles the effect of the electron-phonon interaction in two paradigmatic nanostructures: trans-polyacetylene and polyethylene. We found that the strong electron-phonon interaction leads to the appearance of complex structures in the frequency dependent electronic self-energy. Those structures rule out any quasi-particle picture, and make the adiabatic and static approximations commonly used in the well-established Heine Allen Cardona (HAC) approach inadequate. We propose, instead, a fully ab-initio dynamical formulation of the problem within the Many…
In this work we report new silicon and germanium tubular nanostructures with no corresponding stable carbon analogues. The electronic and mechanical properties of these new tubes were investigated through ab initio methods. Our results show that the structures have lower energy than their corresponding nanoribbon structures and are stable up to high temperatures (500 and 1000 K, for silicon and germanium tubes, respectively). Both tubes are semiconducting with small indirect band gaps, which can be significantly altered by both compressive and tensile strains. Large bandgap variations of almos…
Valley currents and non-local resistances of graphene nanostructures with broken inversion symmetry are considered theoretically in the linear response regime. Scattering state wave functions of electrons entering the nanostructure from the contacts represented by groups of ideal leads are calculated by solving the Lippmann- Schwinger equation and are projected onto the valley state subspaces to obtain the valley velocity fields and total valley currents in the nanostructures. In the tunneling regime when the Fermi energy is in the spectral gap around the Dirac point energy, inversion symmetry…
We report an experimental investigation of the edge effect on the room-temperature transport in graphene nanoribbon and graphene sheet (both single-layer and bilayer). By measuring the resistance scaling behaviors at both low and high carrier densities, we show that the transport of single-layer nanoribbons lies in a strong localization regime, which can be attributed to an edge effect. We find that this edge effect can be weakened by enlarging the width, decreasing the carrier densities or adding an extra layer. From graphene nanoribbon to graphene sheet, the data show a dimensional crossover…
We present a simple way to describe the lowest unoccupied diffuse states in carbon nanostructures in density functional theory (DFT) calculations using a minimal LCAO (linear combination of atomic orbitals) basis set. By comparing plane wave basis calculations, we show how these states can be captured by adding long-range orbitals to the standard LCAO basis sets for the extreme cases of planar <it>sp2</it> (graphene) and curved carbon (C60). In particular, using Bessel functions with a long range as additional basis functions retain a minimal basis size. This provides a smaller and simpler ato…
Several data sets of electrical breakdown in air of single-wall carbon nanotubes (SWNTs) on insulating substrates are collected and analyzed. A universal scaling of the Joule breakdown power with nanotube length is found, which appears independent of the insulating substrates used or their thickness. This suggests the thermal resistances at the interface between SWNT and insulator, and between SWNT and electrodes, govern heat sinking from the nanotube. Analytical models for the breakdown power scaling are presented, providing an intuitive, physical understanding of the breakdown process. The e…
Based on Monte Carlo (MC) simulations of the interaction of energetic noble gas ions with carbon nanostructures, we have derived the ion-deposited energy formulas and their applications for the above interaction. We also have studied the nuclear point mass effects i.e. the well-known mass ratio effects, and the nuclear point charge effects on the ion-deposited energy then the damage regularities. In particular, we, for first time, find a straight line of the penetrating point threshold energies for energetic noble gas ions. Near this straight line, the nuclear point charge effects dominate the…
We report the observation of Peierls-type metal-insulator transition in carbon nanostructures formed by chemical vapor deposition inside the pore network of the ZSM-5 zeolite. The Raman spectrum of this nanocarbon@ZSM-5 indicates a clear signature of the radial breathing mode (RBM) for (3,0) carbon nanotubes that can constitute the carbon network segments. Electrical transport measurements on multiple few-micron-sized nanocarbon@ZSM-5 crystals showed metallic temperature of resistance dependence down to 30 K, at which point the resistance exhibited a sharp upturn that is accompanied by the ope…
Understanding the magnetic properties of graphenic nanostructures is instrumental in future spintronics applications. These magnetic properties are known to depend crucially on the presence of defects. Here we review our recent theoretical studies using density functional calculations on two types of defects in carbon nanostructures: Substitutional doping with transition metals, and sp$^3$-type defects created by covalent functionalization with organic and inorganic molecules. We focus on such defects because they can be used to create and control magnetism in graphene-based materials. Our mai…
In the majority of cases nanostructures prepared by focused electron beam induced deposition (FEBID) employing an organometallic precursor contain predominantly carbon-based ligand dissociation products. This is unfortunate with regard to using this high-resolution direct-write approach for the preparation of nanostructures for various fields, such as mesoscopic physics, micromagnetism, electronic correlations, spin-dependent transport and numerous applications. Here we present an in-situ cleaning approach to obtain pure Co-FEBID nanostructures. The purification procedure lies in the exposure …
The study of thermal transport in low-dimensional materials has attracted a lot of attention recently after discovery of high thermal conductivity of graphene. Here we study numerically phonon transport in low-dimensional carbon structures being interested in the hydrodynamic regime revealed through the observation of second sound. We demonstrate that correct numerical modeling of such two-dimensional systems requires semi-classical molecular dynamics simulations of temperature waves that take into account quantum statistics of thermalized phonons. We reveal that second sound can be attributed…
We have studied the resistance of single-wall carbon nanotubes measured in a four-point configuration with noninvasive voltage electrodes. The voltage drop is detected using multiwalled carbon nanotubes while the current is injected through nanofabricated Au electrodes. The resistance at room temperature is shown to be linear with the length as expected for a classical resistor. This changes at cryogenic temperature; the four-point resistance then depends on the resistance at the Au-tube interfaces and can even become negative due to quantum-interference effects.
The absence of backscattering in metallic nanotubes as well as perfect Klein tunneling in potential barriers in graphene are the prominent electronic characteristics of carbon nanostructures. We show that the phenomena can be explained by a peculiar supersymmetry generated by a first order Hamiltonian and zero order supercharge operators. Like the supersymmetry associated with second order reflectionless finite-gap systems, it relates here the low-energy behavior of the charge carriers with the free particle dynamics.
We report on electrical spin injection measurements on MWNTs . We use a ferromagnetic alloy Pd$_{1-x}$Ni$_{x}$ with x $\approx$ 0.7 which allows to obtain devices with resistances as low as 5.6 $kΩ$ at 300 $K$. The yield of device resistances below 100 $kΩ$, at 300 $K$, is around 50%. We measure at 2 $K$ a hysteretic magneto-resistance due to the magnetization reversal of the ferromagnetic leads. The relative difference between the resistance in the antiparallel (AP) orientation and the parallel (P) orientation is about 2%.
A new multiscale modeling approach to unravel the influence of interlayer sp3 bonds on the nonlinear large-deformation and fracture behaviors of 2D carbon nanostructures under tension
Quantum transport properties of intermolecular nanotube contacts are investigated. We find that atomic structure in the contact region plays important roles and resistance of contacts varies strongly with geometry and nanotube chirality. Nanotube end-end contacts have low resistance and show negative differential resistance (NDR) behavior. Contact resistance can be dramatically decreased by exerting small pressure/force between the tubes if the contact is commensurate. Significant variation and nonlinearity of contact resistance may lead to new device applications.
Tomonaga-Luttinger (T-L) theory predicts collective plasmon resonances in 1-D nanostructure conductors of finite length, that vary roughly in inverse proportion to the length of the structure. In-depth quantitative understanding of such resonances which have not been clearly identified in experiments so far, would be invaluable for future generations of nano-photonic and nano-electronic devices that employ 1-D conductors. Here we provide evidence of the plasmon resonances in a number of representative 1-D finite carbon-based nanostructures using first-principle computational electronic spectro…
The ability to tune the thermal resistance of carbon nanotube mechanical supports from insulating to conducting could permit the next generation of thermal management devices. Here, we demonstrate fabrication techniques for carbon nanotube supports that realize either weak or strong thermal coupling, selectively. Direct imaging by in-situ electron thermal microscopy shows that the thermal contact resistance of a nanotube weakly-coupled to its support is greater than 250 K*m/W and that this value can be reduced to 4.2(+5.6/-2.1) K*m/W by imbedding the nanotube in metal contacts.
We have calculated the effects of structural distortions of armchair carbon nanotubes on their electrical transport properties. We found that the bending of the nanotubes decreases their transmission function in certain energy ranges and leads to an increased electrical resistance. Electronic structure calculations show that these energy ranges contain localized states with significant $σ$-$π$ hybridization resulting from the increased curvature produced by bending. Our calculations of the contact resistance show that the large contact resistances observed for SWNTs are likely due to the weak …
We report our recent numerical study on the effects of dephasing on a perfectly conducting channel (PCC), its presence believed to be dominant in the transport characteristics of a zigzag graphene nanoribbons (GNR) and of a metallic carbon nanotubes (CNT). Our data confirms an earlier prediction that a PCC in GNR exhibits a peculiar robustness against dephasing, in contrast to that of the CNT. By studying the behavior of the conductance as a function of the system's length we show that dephasing destroys the PCC in CNT, whereas it stabilizes the PCC in GNR. Such opposing responses of the PCC a…
Nonreciprocal plasmons in one-dimensional carbon nanostructures
Max-Born-Institut（马克斯·玻恩研究所）；Center for Nanophotonics, NWO Institute AMOLF（纳米光子学中心，NWO AMOLF研究所）；ICFO-Institut de Ciencies Fotoniques, The Barcelona Institute of Science and Technology（ICFO-光子科学研究所，巴塞罗那科学技术研究所）；ICREA-Institució Catalana de Recerca i Estudis Avançats（ICREA-加泰罗尼亚研究高级学院）；POLIMA—Center for Polariton-driven Light–Matter Interactions, University of Southern Denmark（POLIMA-极化激元驱动光物质相互作用中心，南丹麦大学）；Danish Institute for Advanced Study, University of Southern Denmark（丹麦高等研究院，南丹麦大学）
We investigate the response of multi-walled carbon nanotubes to mechanical strain applied with an Atomic Force Microscope (AFM) probe. We find that in some samples, changes in the contact resistance dominate the measured resistance change. In others, strain large enough to fracture the tube can be applied without a significant change in the contact resistance. In this case we observe that enough force is applied to break the tube without any change in resistance until the tube fails. We have also manipulated the ends of the broken tube back in contact with each other, re-establishing a finite …
It was aimed to determine whether plasma processing could contribute to enhanced capacitance and energy density of activated carbon electrode based electrochemical capacitors, through the formation of additional surface charges. While an increase of up to 35% of the gravimetric capacitance, along with ~ 20% decrease in resistance, was obtained through optimal plasma processing, increased plasma exposure yielded a drastic reduction (/increase) in the capacitance (/resistance). It was also found that the capacitance and resistance modulation was a sensitive function of sample processing as well …
We introduce a new simplified method for computing the electron field emission current in short carbon nanotubes using ab-initio computation in periodic simulation cells. We computed the evolution of the wave functions using Time-Dependent Density Functional Theory, where we have utilized the Crank-Nicholson propagator. We found that in pristine carbon nanotubes, the emitted charge tends to emerge mostly from electrons that are concentrated at the nanotube tip region. The charge beam concentrates into specific channel structures, showing the utility of carbon nanotubes in precision emission ap…
We show that the energy differences between the lowest optical singlet exciton and the lowest triplet exciton in semiconducting single-walled carbon nanotubes with diameter $\sim 1$ nm and graphene nanoribbons with widths $\sim 2$ nm are an order of magnitude smaller than in the $π$-conjugated polymer poly(para-phenylenevinylene). Our calculated energy gaps between the singlet and triplet excitons are in excellent agreement with the measured values in three different nanotubes with diameters close to 1 nm. The spatial extent of the triplet exciton is nearly the same as that of the singlet exci…
We theoretically investigate the electro-mechanics of a Suspended Carbon Nanotube with a Deflection Sensitive Resistance subjected to a homogeneous Magnetic Field and a constant Voltage Bias. We show that, (with the exception of a singular case), for a sufficiently high magnetic field the time-independent state of charge transport through the nanotube becomes unstable to selfexcitations of the mechanical vibration accompanied by oscialltions in the voltage drop and current across the nanotube.
Exploring the mechanism of interfacial thermal transport and reducing the interfacial thermal resistance is of great importance for thermal management and modulation. Herein, the interfacial thermal resistance between overlapped graphene nanoribbons is largely reduced by adding bonded carbon chains by performing molecular dynamics simulations. And the analytical model (cross-interface model, CIM) is utilized to analyze and explain the two-dimensional thermal transport mechanism at cross-interface. An order of magnitude reduction in interfacial thermal resistance is found as the graphene nanori…
Nanoscrolls (papyrus-like nanostructures) are very attractive structures for a variety of applications, due to their tunable diameter values and large accessible surface area. They have been successfully synthesized from different materials. In this work we have investigated, through fully atomistic molecular dynamics simulations, the dynamics of scroll formation for a series of graphenelike carbon nitride (CN) twodimensional systems: gCN, triazinebased gC3N4, and heptazinebased gC3N4. Our results show that stable nanoscrolls can be formed for all of these structures. Possible synthetic routes…
The features of the $IV$ characteristics of metallic carbon nanotubes (m-NTs) in different experimental setups are studied using semi-classical Boltzmann transport equation together with the heat dissipation equation to account for significant thermal effects at high electric bias. Our model predicts that the shape of the m-NT characteristics is basically controlled by heat removal mechanisms. In particular we show that the onset of negative differential resistance in free standing nanotubes finds its origins in strong transport nonlinearities associated with poor heat removal unlike in substr…
Carbon fiber and graphene-based nanostructures such as carbon nanotubes (CNTs) and defective structures have extraordinary potential as strong and lightweight materials. A longstanding bottleneck has been lack of understanding and implementation of atomic-scale engineering to harness the theoretical limits of modulus and tensile strength, of which only a fraction is routinely reached today. Here we demonstrate accurate and fast predictions of mechanical properties for CNTs and arbitrary 3D graphitic assemblies based on a training set of over 1000 stress-strain curves from cutting-edge reactive…
In the last three decades or so, we have witnessed an extraordinary progress in the research and technology of carbon-based nanomaterials. Among the peculiar highlights are the discoveries of fullerene, the carbon nanotubes and the magnificent simple scotch tape exfoliated graphene. The unique photophysical properties of these different allotropic forms of the nanocarbon have opened up vast application possibilities in many fields of science and technology, with particular emphasis on optoelectronics and photonics. A prerequisite for many of these applications is a thorough understanding of th…
Transitions to immeasurably small electrical resistance in thin films of Ag/Au nanostructure-based films have generated significant interest because such transitions can occur even at ambient temperature and pressure. While the zero-bias resistance and magnetic transition in these films have been reported recently, the non-equilibrium current-voltage ($I-V$) transport characteristics at the transition remains unexplored. Here we report the $I-V$ characteristics at zero magnetic field of a prototypical Ag/Au nanocluster film close to its resistivity transition at the critical temperature $T_{C}…
Capillary and van der Waals forces cause nanotubes to deform or even collapse under metal contacts. Using ab-initio bandstructure calculations, we find that these deformations reduce the bandgap by as much as 30\%, while fully collapsed nanotubes become metallic. Moreover degeneracy lifting, due to the broken axial symmetry and wavefunctions mismatch between the fully collapsed and the round portions of a CNT, leads to a three times higher contact resistance. The latter we demonstrate by contact resistance calculations within the tight-binding approach.
We report on the temperature dependence of the intrinsic resistance of long individual disordered single-wall carbon nanotubes. The resistance grows dramatically as the temperature is reduced, and the functional form is consistent with an activated behavior. These results are described by Coulomb blockade along a series of quantum dots. We occasionally observe a kink in the activated behavior that reflects the change of the activation energy as the temperature range is changed. This is attributed to charge hopping events between non-adjacent quantum dots, which is possible through cotunneling …
The comment to article "Coexistence of Diamagnetism and Vanishingly Small Electrical Resistance at Ambient Temperature and Pressure in Nanostructures" shows the role of local electron pairing and Bose-Einstein-Condensation of pairs for superconductivity at Tc = 286 K in nanostructures.
We present first-principles calculations of quantum transport which show that the resistance of metallic carbon nanotubes can be changed dramatically with homogeneous transverse electric fields if the nanotubes have impurities or defects. The change of the resistance is predicted to range over more than two orders of magnitude with experimentally attainable electric fields. This novel property has its origin that backscattering of conduction electrons by impurities or defects in the nanotubes is strongly dependent on the strength and/or direction of the applied electric fields. We expect this …
Experimental results from irradiated-carbon nanostructures can be partially explained by selective applications of classical damage theories and ad-hoc thermal models by treating the binary atomic collision cascades and multi-atomic thermal spikes as energy-dissipating mechanisms. An information-theoretic model is developed by treating the irradiated single-walled carbon nanotubes and C60 as entropy-generating dissipative structures. The model is based on evaluating the experimental probability distribution functions of the sputtered constituents and components from the irradiated carbon nanos…
Percolation phenomena are investigated and discussed in three kinds of nanostructures: first two are nanocrystalline silicon-based systems, Si nanodots embedded in amorphous SiO2 matrix and porous silicon formed by an oxidized nanowire network, and the third consisting of a multi-walled carbon nanotube network embedded in amorphous SiN. The current-voltage characteristics measured on first two systems present voltage percolation thresholds with the same shape - a saturation plateau region of the current, followed by an abrupt increase. The current-voltage and conductance-voltage curves measure…
