In this work we investigated correlations between the internal microstructure and sample size (lateral as well as thickness) of mesoscopic, tens of nanometer thick graphite (multigraphene) samples and the temperature $(T)$ and field $(B)$ dependence of their electrical resistivity $ρ(T,B)$. Low energy transmission electron microscopy reveals that the original highly oriented pyrolytic graphite material -- from which the multigraphene samples were obtained by exfoliation -- is composed of a stack of $\sim 50 $nm thick and micrometer long crystalline regions separated by interfaces running parallel to the graphene planes. We found a qualitative and quantitative change in the behavior of $ρ(T,B)$ upon thickness of the multigraphene samples, indicating that their internal microstructure is important.} {The overall results indicate that the metallic-like behavior of $ρ(T)$ at zero field measured for bulk graphite samples is not intrinsic of ideal graphite. The results suggest that the interfaces between crystalline regions may be responsible for the superconducting-like properties observed in graphite. Our transport measurements also show that reducing the sample lateral size as well as the length between voltage electrodes decreases the magnetoresistance, in agreement with recently published results. The magnetoresistance of the multigraphene samples shows a scaling of the form ($(R(B) - R(0))/R(0))/T^α= f(B/T)$ with a sample dependent exponent $α\sim 1$, which applies in the whole temperature 2 K $\le T \le 270$K and magnetic field range $B \le 8 $T.
We investigate the magnetotransport properties of a thin graphite wire resting on a silicon oxide substrate. The electric field effect is demonstrated with back and side gate electrodes. We study the conductance fluctuations as a function of gate voltage, magnetic field and temperature. The phase coherence length extracted from weak localization is larger than the wire width even at the lowest carrier densities making the system effectively one-dimensional. We find that the phase coherence length increases linearly with the conductivity suggesting that at 1.7 K dephasing originates mainly from…
Excess conductance fluctuations with peculiar temperature-dependence from 1.4 to 250 K were observed in curved nano-graphite sheets with an electrode gap length of 300 and 450 nm, whereas the conductance fluctuation is greatly suppressed above 4.2 K when the electrode gap length increases to 800 and 1000 nm. The former is discussed in the context of the presence of a small energy bandgap in the nano-graphite sheets, while the latter is attributed to the crossover from coherent transport to diffusive transport regime.
The electrical, in-plane resistance as a function of temperature $R(T)$ of bulk and mesoscopic thin graphite flakes obtained from the same batch was investigated. Samples thicker than $\sim 30$ nm show metalliclike contribution in a temperature range that increases with the sample thickness, whereas a semiconductinglike behavior was observed for thinner samples. The temperature dependence of the in-plane resistance of all measured samples and several others from literature can be very well explained between 2 K and 1100 K assuming three contributions in parallel: a metalliclike conducting path…
Isolating the natural edges of bilayer graphene in gate-defined mesoscopic devices
University of Basel（巴塞尔大学）；Advanced Materials Laboratory, National Institute for Materials Science（国家材料科学研究所先进材料实验室）；Solid State Physics Laboratory, ETH Zürich（苏黎世联邦理工学院固体物理实验室）；Swiss Nanoscience Institute（瑞士纳米科学研究所）
Interlayer space in graphite is impermeable to ions and molecules, including protons. Its controlled expansion would find several applications in desalination, gas purification, high-density batteries, etc. In the past, metal intercalation has been used to modify graphitic interlayer spaces; however, resultant intercalation compounds are unstable in water. Here, we successfully expanded graphite interlayer spaces by intercalating aqueous KCl ions electrochemically. The water conductivity shows several orders of enhancement when compared to unintercalated graphite. Water evaporation experiments…
In the hydrodynamic regime, phonons drift with a nonzero collective velocity under a temperature gradient, reminiscent of viscous gas and fluid flow. The study of hydrodynamic phonon transport has spanned over half a century but has been mostly limited to cryogenic temperatures (~1 K) and more recently to low-dimensional materials. Here, we identify graphite as a three-dimensional material that supports phonon hydrodynamics at significantly higher temperatures (~100 K) based on first-principles calculations. In particular, by solving the Boltzmann equation for phonon transport in graphite ribb…
A simple one-stage solution-based method was developed to produce graphene nanoribbons by sonicating graphite powder in organic solutions with polymer surfactant. The graphene nanoribbons were deposited on silicon substrate, and characterized by Raman spectroscopy and atomic force microscopy. Single-layer and few-layer graphene nanoribbons with a width ranging from sub-10 nm to tens of nm and length ranging from hundreds of nm to 1 μm were routinely observed. Electrical transport properties of individual graphene nanoribbons were measured in both the back-gate and polymer-electrolyte top-gate …
We show that the presence of electrically insulating graphite oxide (GO) within a single wall carbon nanotube network strongly enhances electrical conductivity, whereas reduced graphite oxide, even though electrically conductive, suppresses electrical conductivity within a composite network with single wall carbon nanotubes. Measurements of Young modulus and of Raman spectra strongly support our interpretation of the indirect role of the oxide groups, present in graphite oxide within the single wall carbon nanotubes/graphite oxide composite, through electronic doping of metallic single wall ca…
This work deals with the intrinsic and extrinsic properties of the graphene layers inside the graphite structure, in particular the influence of defects and interfaces. We discuss the evidence for ballistic transport found in mesoscopic graphite samples and the possibility to obtain the intrinsic carrier density of graphite, without the need of free parameters or arbitrary assumptions. The influence of internal interfaces on the transport properties of bulk graphite is described in detail. We show that in specially prepared multigraphene samples the transport properties show clear signs for th…
Lattice vacancy effects on electrical conductance of nanographite ribbon are investigated by means of the Landauer approach using a tight binding model. In the low-energy regime ribbons with zigzag boundary provide a single conducting channel whose origin is connected with the presence of edge states. It is found that the chemical potential dependence of conductance strongly depends on the difference ($Δ$) of the number of removed A and B sublattice sites. The large lattice vacancy with $Δ\neq 0$ shows $2Δ$ zero-conductance dips in the single-channel region, however, the large lattice vacancy …
The transport properties of highly oriented pyrolitic graphite (HOPG) and polycrystal graphite have been studied. The electric conductivity of HOPG is several times larger than that of the polycrystal graphite. Along with the large magnetoresistances (MR), the polycrystal graphite show the accordant semiconductor-like character in a wide temperature (roughly range from 20K to 120K) under 0, 4, 8, 12 T applied magnetic field, while the magnetic-field-induced metal-semiconductor-like transition was only found in HOPG. The difference of transport properties originates from the Coulomb interaction…
Electron transport properties of a non-interacting mesoscopic ring sandwiched between two metallic electrodes are investigated by the use of Green's function formalism. We introduce a parametric approach based on the tight-binding model to study the transport properties. The electronic transport characteristics are investigated in three aspects: (a) ring-electrode interface geometry, (b) coupling strength of the ring to the electrodes and (c) magnetic flux threaded by the ring.
We investigate theoretically the spin transport in two-terminal mesoscopic rings in the presence of both the Rashba spin-orbit interaction (RSOI) and the Dresselhaus spin-orbit interaction (DSOI). We find that the interplay between the RSOI and DSOI breaks the original cylindric symmetry of mesoscopic ring and consequently leads to the anisotropic spin transport, i.e., the conductance is sensitive to the positions of the incoming and outgoing leads. The anisotropic spin transport can survive even in the presence of disorder caused by impurity elastic scattering in a realistic system.
Having driven a large part of the decade's progress in physics, nanoelectronics is now passing from today's realm of the extraordinary to tomorrow's commonplace. This carries the problem of turning proofs of concept into practical artefacts. Better and more sharply focussed predictive modelling will be the ultimate guide to optimising mesoscopic technology as it matures. Securing this level of understanding needs a reassessment of the assumptions at the base of the present state of the field. We offer a brief overview of the underlying assumptions of mesoscopic transport.
The scaling of friction with the contact size $A$ and (in)commensurabilty of nanoscopic and mesoscopic crystals on a regular substrate are investigated analytically for triangular nanocrystals on hexagonal substrates. The crystals are assumed to be stiff, but not completely rigid. Commensurate and incommensurate configurations are identified systematically. It is shown that three distinct friction branches coexist, an incommensurate one that does not scale with the contact size ($A^0$) and two commensurate ones which scale differently (with $A^{1/2}$ and $A$) and are associated with various co…
We studied the influence of 30keV Ga$^+$-ions -- commonly used in focused ion beam (FIB) devices -- on the transport properties of thin crystalline graphite flake, La$_{0.7}$Ca$_{0.3}$MnO$_3$ and Co thin films. The changes of the electrical resistance were measured in-situ during irradiation and also the temperature and magnetic field dependence before and after irradiation. Our results show that the transport properties of these materials strongly change at Ga$^+$ fluences much below those used for patterning and ion beam induced deposition (IBID), limiting seriously the use of FIB when the i…
We have made thermal and electrical transport measurements of uncompressed pyrolytic graphite sheet (uPGS), a mass-produced thin graphite sheet with various thicknesses between 10 and 100 μm, at temperatures between 2 and 300 K. Compared to exfoliated graphite sheets like Grafoil, uPGS has much higher conductivities by an order of magnitude because of its high crystallinity confirmed by X-ray diffraction and Raman spectroscopy. This material is advantageous as a thermal link of light weight in a wide temperature range particularly above 60 K where the thermal conductivity is much higher than c…
We consider mesoscopic thermal transport between two bulk dielectrics joined by a narrow wire or weak mechanical link. In the ``tunneling'' regime where the phonon transmission probability through the link is small and the thermal conductance is much less than the value for a single channel, the thermal current is determined by a product of the local vibrational spectral densities of the two bodies. We derive an expression for the thermal current that is a thermal analog of the well-known formula for the electrical current through a tunneling barrier.
Electronic transport through a quantum wire sandwiched between two metallic electrodes and coupled to a quantum ring, threaded by a magnetic flux $ϕ$, is studied. An analytic approach for the electron transport through the bridge system is presented based on the tight-binding model. The transport properties are discussed in three aspects: (a) presence of an external magnetic filed, (b) strength of the wire to electrode coupling, and (c) presence of in-plane electric field.
An interplay between the increase in the number of carriers and the decrease in the scattering time is expected to result in a saturation of the in-plane resistivity, $ρ_{ab}$, in graphite above room temperature. Contrary to this expectation, we observe a pronounced increase in $ρ_{ab}$ in the interval between 300 and 900 K. We provide a theory of this effect based on intervalley scattering of charge carriers by high-frequency, graphene-like optical phonons.
We investigated the influence of thickness reduction on the transport properties of graphite microflakes. Using oxygen plasma etching we decreased the thickness of highly oriented pyrolytic graphite (HOPG) microflakes from $\sim 100$~nm to $\sim 20$~nm systematically. Keeping current and voltage electrodes intact, the electrical resistance $R(T)$, the magnetoresistance (MR) and Raman spectra were measured in every individual sample and after each etching step of a few nm. The results show that $R(T)$ and MR can increase or decrease with the sample thickness in a non-systematic way. The results…
We present a combined experimental and theoretical study of the self-diffusion of ammonia on exfoliated graphite. Using neutron time-of-flight spectroscopy we are able to resolve the ultrafast diffusion process of adsorbed ammonia, NH$_3$, on graphite. Together with van der Waals corrected density functional theory calculations we show that the diffusion of NH$_3$ follows a hopping motion on a weakly corrugated potential energy surface with an activation energy of about 4 meV which is particularly low for this type of diffusive motion. The hopping motion includes further a significant number o…
Graphite is a layered material showing a strong anisotropy. Among the unconventional properties reported by experiments, the electronic transport along the c-axis, which has direct implications in order to build graphitic devices, remains a controversial topic. We study the influence of inelastic scattering on the electron tunnelling between layers. In the presence of electron electron interactions, tunnelling processes are modified by inelastic scattering events.
Long coherence lifetimes of electron spins transported using moving potential dots are shown to result from the mesoscopic confinement of the spin vector. The confinement dimensions required for spin control are governed by the characteristic spin-orbit length of the electron spins, which must be larger than the dimensions of the dot potential. We show that the coherence lifetime of the electron spins is independent of the local carrier densities within each potential dot and that the precession frequency, which is determined by the Dresselhaus contribution to the spin-orbit coupling, can be m…
Thick Li-ion battery electrodes with high ion transport rates could enable batteries that cost less and that have higher gravimetric and volumetric energy density, because they require fewer inactive cell-components. Finding ways to increase ion transport rates in thick electrodes would be especially valuable for electrodes made with graphite platelets, which have been shown to have tortuosities in the thru-plane direction about 3 times higher than in the in-plane direction. Here, we predict that bi-tortuous electrode structures (containing electrolyte-filled macro-pores embedded in micro-poro…
The intrinsic values of the carriers mobility and density of the graphene layers inside graphite, the well known structure built on these layers in the Bernal stacking configuration, are not well known mainly because most of the research was done in rather bulk samples where lattice defects hide their intrinsic values. By measuring the electrical resistance through microfabricated constrictions in micrometer small graphite flakes of a few tens of nanometers thickness we studied the ballistic behavior of the carriers. We found that the carriers' mean free path is micrometer large with a mobilit…
Electron transport properties are investigated in an array of mesoscopic rings, where each ring is threaded by a magnetic flux $ϕ$. The array is attached to two semi-infinite one-dimensional metallic electrodes, namely, source and drain, where the rings are considered either in series or in parallel configuration. A simple tight-binding model is used to describe the system and all the calculations are done based on the Green's function formalism. Here, we present conductance-energy and current-voltage characteristics in terms of ring-to-electrode coupling strength, ring-electrode interface geo…
Recent theories and experiments have suggested hydrodynamic phonon transport features in graphite at unusually high temperatures. Here, we report a pico-second pump-probe thermal reflectance measurement of heat pulse propagation in graphite. The measurement results reveal transient lattice cooling near the adiabatic center of a 15 $μ$m diameter ring-shape pump beam at temperatures between 80 and 120 K. While such lattice cooling has not been reported in recent diffraction measurements of second sound in graphite, the observation here is consistent with both hydrodynamic phonon transport theory…
There is great interest in the development of novel nanomachines that use charge, spin, or energy transport, to enable new sensors with unprecedented measurement capabilities. Electrical and thermal transport in these mesoscopic systems typically involves wave propagation through a nanoscale geometry such as a quantum wire. In this paper we present a general theoretical technique to describe wave propagation through a curved wire of uniform cross-section and lying in a plane, but of otherwise arbitrary shape. The method consists of (i) introducing a local orthogonal coordinate system, the arcl…
The quantum anomalous Hall (QAH) effect has been demonstrated in two-dimensional topological insulator systems incorporated with ferromagnetism. However, a comprehensive understanding of mesoscopic transport in sub-micron QAH devices has yet been established. Here we fabricated miniaturized QAH devices with channel widths down to 600 nm, where the QAH features are still preserved. A back-scattering channel is formed in narrow QAH devices through percolative hopping between 2D compressible puddles. Large resistance fluctuations are observed in narrow devices near the coercive field, which is as…
The 2D Fermi surface of 1st stage PdAl2Cl8 acceptor-type graphite intercalation compounds (GICs) has been investigated using the Shubnikov-de Haas (SdH) effect. One fundamental frequency is observed, the angular variation of which confirms its strongly 2D nature, as previously found through electrical conductivity measurements. The energy spectrum can be described by the 2D band structure model proposed by Blinowski et al. We obtain the following parameter values: intraplane C-C interaction energy gamma_0 = 2.7 eV, Fermi energy E_F = -1.1 eV and carrier density n_SdH= 1.1x10^27 m^-3. Some fewe…
Using a linear array of voltage electrodes with a separation of several micrometers on a $20 $nm thick and 30 $μ$m long multigraphene sample we show that the measured resistance does not follow the usual length dependence according to Ohm's law. The deviations can be quantitatively explained taking into account Sharvin-Knudsen formula for ballistic transport. This allows us to obtain without free parameters the mean free path of the carriers in the sample at different temperatures. In agreement with recently reported values obtained with a different experimental method, we obtain that the carr…
We discuss the mass transport of a degenerate Fermi liquid $^3$He film over a rough surface, and the film momentum relaxation time, in the framework of theoretical predictions. In the mesoscopic régime, the anomalous temperature dependence of the relaxation time is explained in terms of the interference between elastic boundary scattering and inelastic quasiparticle-quasiparticle scattering within the film. We exploit a quasiclassical treatment of quantum size effects in the film in which the surface roughness, whose power spectrum is experimentally determined, is mapped into an effective diso…
In this work we show that for a quasi-2D system of size $Ω$ and thickness $t$ the resistance goes as $(2ρ/πt)\ln(Ω/W)$, diverging logarithmically with the size. Measurements in highly oriented pyrolytic graphite (HOPG) as well as numerical simulations confirm this relation. Furthermore, we present an experimental method that allows us to obtain the carriers mean free path $l(T)$, the Fermi wavelength $λ(T)$ and the mobility $μ(T)$ directly from experiments without adjustable parameters. Measuring the electrical resistance through microfabricated constrictions in HOPG and observing the transiti…
The influence of contacts on linear transport through a molecular wire attached to mesoscopic tubule leads is studied. It is shown that low dimensional leads, such as carbon nanotubes, in contrast to bulky electrodes, strongly affect transport properties. By focusing on the specificity of the lead-wire contact, we show, in a fully analytical treatment, that the geometry of this hybrid system supports a mechanism of channel selection and a sum rule, which is a distinctive hallmark of the mesoscopic nature of the electrodes.
The correlation between the transport properties and structural degrees of freedom of conducting polymers is a central concern in both practical applications and scientific research. In this study, we demonstrated the existence of mesoscopic two-dimensional (2D) coherent charge transport in poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) film by performing structural investigations and high-field magnetoconductance (MC) measurements in magnetic fields of up to 15 T. We succeeded in observing marked positive MCs reflecting 2D electronic states in a conventional drop-cast fil…
The spectacular metal-to-insulator transition of V2O3 can be progressively suppressed in thin film samples. Evidence for phase separation was observed using microbridges as a mesoscopic probe of transport properties where the same film possesses domains that exhibit a metal-to-insulator transition with clear first order features or remain metallic down to low temperatures. A simple model consisting of two parallel resistors can be used to quantify a phase coexistence scenario explaining the measured macroscopic transport properties. The interaction between film and substrate is the most plausi…
