We calculate the long-wavelength static screening properties of both neutral and doped graphene in the framework of density-functional theory. We use a plane-wave approach with periodic images in the third dimension and truncate the Coulomb interactions to eliminate spurious interlayer screening. We carefully address the issue of extracting two dimensional dielectric properties from simulated three-dimensional potentials. We compare this method with analytical expressions derived for two dimensional massless Dirac fermions in the random phase approximation. We evaluate the contributions of the deviation from conical bands, exchange-correlation and local-fields. For momenta smaller than twice the Fermi wavevector, the static screening of graphene within the density-functional perturbative approach agrees with the results for conical bands within random phase approximation and neglecting local fields. For larger momenta, we find that the analytical model underestimates the static dielectric function by $\approx 10%$, mainly due to the conical band approximation.
The development of new high dielectric materials is essential for advancement in modern electronics. Oxides are generally regarded as the most promising class of high dielectric materials for industrial applications as they possess both high dielectric constants and large band gaps. Most previous researches on high dielectrics were limited to already known materials. In this study, we conducted an extensive search for high dielectrics over a set of ternary oxides by combining crystal structure prediction and density functional perturbation theory calculations. From this search, we adopted mult…
We investigate the structural damage of graphene underlying dielectrics (HfO2 and Al2O3) by remote plasma-enhanced atomic layer deposition (PE-ALD). Dielectric film is grown on bilayer graphene without inducing significant damage to the bottom graphene layer. Based on Raman spectra, we demonstrate that the bottom graphene layer has the salient features of single layer graphene. During the initial half-cycle PE-ALD, the upper graphene layer reacts with the metal precursor, forming uniform nucleation islands or an active metallic carbide layer. After monolayer dielectric coverage, the bottom gra…
Two-dimensional (2D) hexagonal boron nitride (BN) nanosheets are excellent dielectric substrate for graphene, molybdenum disulfide and many other 2D nanomaterials based electronic and photonic devices. To optimize the performance of these 2D devices, it is essential to understand the dielectric screening properties of BN nanosheets as a function of the thickness. Here, electric force microscopy along with theoretical calculations based on both state-of-the-art first-principles calculations with van der Waals interactions under consideration and non-linear Thomas-Fermi theory models are used to…
The exciton Wannier equation for graphene is solved for different background dielectric constants. It is shown that freestanding graphene features strong Coulomb effects with a very large exciton binding energy exceeding $3\,$eV. A second-order transition to a weak Coulomb regime is found if the effective background dielectric constant exceeds a critical value. All bound-state solutions vanish for epitaxial graphene on a substrate with large background permittivity, such as SiC.
The effect of various dielectrics on charge mobility in single layer graphene is investigated. By calculating the remote optical phonon scattering arising from the polar substrates, and combining it with their effect on Coulombic impurity scattering, a comprehensive picture of the effect of dielectrics on charge transport in graphene emerges. It is found that though high-$κ$ dielectrics can strongly reduce Coulombic scattering by dielectric screening, scattering from surface phonon modes arising from them wash out this advantage. By comparing the room-temperature transport properties with narr…
A simple effective screening parameter for screened range-separated hybrid is constructed from the compressibility sum rule in the context of linear-response time-dependent Density Functional Theory. When applied to the dielectric-dependent hybrid (DDH), it becomes remarkably accurate for bulk solids compared to those obtained from fitting with the model dielectric function or depending on the valence electron density of materials. The present construction of the screening parameter is simple and realistic. The screening parameter developed in this way is physically appealing and practically u…
The phonon dispersion of graphene on Ir(111) has been determined by means of angle-resolved inelastic electron scattering and density functional calculations. Kohn anomalies of the highest optical-phonon branches are observed at the $Γ$ and K point of the surface Brillouin zone. At K the Kohn anomaly is weaker than observed from pristine graphene and graphite. This observation is rationalized in terms of a decrease of the electron-phonon coupling due to screening of graphene electron correlations by the metal substrate.
We develop a first-principles computational method for investigating the dielectric screening in extended systems using the self-consistent Sternheimer equation and localized non-orthogonal basis sets. Our approach does not require the explicit calculation of unoccupied electronic states, only uses two-center integrals, and has a theoretical scaling of order O(N^3). We demonstrate this method by comparing our calculations for silicon, germanium, diamond, and LiCl with reference planewaves calculations. We show that accuracy comparable to planewaves calculations can be achieved via a systematic…
We reduce the dimensionless interaction strength in graphene by adding a water overlayer in ultra-high vacuum, thereby increasing dielectric screening. The mobility limited by long-range impurity scattering is increased over 30 percent, due to the background dielectric constant enhancement leading to reduced interaction of electrons with charged impurities. However, the carrier-density-independent conductivity due to short range impurities is decreased by almost 40 percent, due to reduced screening of the impurity potential by conduction electrons. The minimum conductivity is nearly unchanged,…
The unusual transport properties of graphene are the direct consequence of a peculiar bandstructure near the Dirac point. We determine the shape of the pi bands and their characteristic splitting, and the transition from a pure 2D to quasi-2D behavior for 1 to 4 layers of graphene by angle-resolved photoemission. By exploiting the sensitivity of the pi bands to the electronic potential, we derive the layer-dependent carrier concentration, screening length and strength of interlayer interaction by comparison with tight binding calculations, yielding a comprehensive description of multilayer gra…
Using physical insights and advanced first-principles calculations, we suggest that corundum is an ideal gate dielectric material for graphene transistors. Clean interface exists between graphene and Al-terminated (or hydroxylated) Al2O3 and the valence band offsets for these systems are large enough to create injection barrier. Remarkably, a band gap of » 180 meV can be induced in graphene layer adsorbed on Al-terminated surface, which could realize large ON/OFF ratio and high carrier mobility in graphene transistors without additional band gap engineering and significant reduction of transpo…
Graphene field-effect transistors are integrated with solution-processed multilayer hybrid organic-inorganic self-assembled nanodielectrics (SANDs). The resulting devices exhibit low-operating voltage (2 V), negligible hysteresis, current saturation with intrinsic gain > 1.0 in vacuum (pressure < 2 x 10-5 Torr), and overall improved performance compared to control devices on conventional SiO2 gate dielectrics. Statistical analysis of the field-effect mobility and residual carrier concentration demonstrate high spatial uniformity of the dielectric interfacial properties and graphene transistor …
In this paper we report: the use of GO in aqueous solution as a gate dielectric material, its application to a MOS transistor based on organic semiconductor and the use of paper as substrate material.
We report on a large improvement in the wetting of Al2O3 thin films grown by un-seeded atomic layer deposition on monolayer graphene, without creating point defects. This enhanced wetting is achieved by greatly increasing the nucleation density through the use of polar traps induced on the graphene surface by an underlying metallic substrate. The resulting Al2O3/graphene stack is then transferred to SiO2 by standard methods.
The full potential of graphene in integrated circuits can only be realized with a reliable ultra-thin high-κ top-gate dielectric. Here, we report the first statistical analysis of the breakdown characteristics of dielectrics on graphene, which allows the simultaneous optimization of gate capacitance and the key parameters that describe large-area uniformity and dielectric strength. In particular, vertically heterogeneous and laterally homogenous Al2O3 and HfO2 stacks grown via atomic-layer deposition and seeded by a molecularly thin perylene-3,4,9,10-tetracarboxylic dianhydride organic monolay…
Enhanced Screening in Epitaxial Graphene via Nearly Free-Electron Metal Intercalation
Universität Würzburg（维尔茨堡大学）；Würzburg-Dresden Cluster of Excellence ctd.qmat, Universität Würzburg（维尔茨堡大学维尔茨堡-德累斯顿卓越集群ctd.qmat）；Institut für Theoretische Physik und Astrophysik, Universität Würzburg（维尔茨堡大学理论与天体物理研究所）；Diamond Light Source（钻石光源）
High quality epitaxial graphene films can be applied as templates for tailoring graphene-substrate interfaces that allow for precise control of the charge carrier behavior in graphene through doping and many-body effects. By combining scanning tunneling microscopy, angle-resolved photoemission spectroscopy and density functional theory we demonstrate that oxygen intercalated epitaxial graphene on Ir(111) has high structural quality, is quasi free-standing, and shows signatures of many-body interactions. Using this system as a template, we show that tunable pn-junctions can be patterned by adso…
We study the effects of insulating oxides in their crystalline forms on the energy band structure of monolayer and bilayer graphene using a \textit{first principles} density functional theory based electronic structure method and a local density approximation. We consider the dielectric oxides, SiO$_{2}$ ($α$-quartz) and Al$_{2}$O$_{3}$ (alumina or $α$-sapphire) each with two surface terminations. Our study suggests that atomic relaxations and resulting equilibrium separations play a critical role in perturbing the linear band structure of graphene in contrast to the less critical role played …
Various many-body perturbation theory techniques for calculating electron behavior rely on {\it W}, the screened Coulomb interaction. Computing {\it W} requires complete knowledge of the dielectric response of the electronic system, and the fidelity of the calculated dielectric response limits the reliability of predicted electronic and structural properties. As a simplification, calculations often begin with the random-phase approximation (RPA). However, even RPA calculations are costly and scale poorly, typically as $N^4$ ($N$ representing the system size). A local approach has been shown to…
Monolayers of transition-metal dichalcogenides (TMDs) hold great promise as future nanoelectronic and optoelectronic devices. An essential feature for achieving high device performance is the use of suitable supporting substrates, which can affect the electronic and optical properties of these two-dimensional (2D) materials. Here, we perform many-body GW calculations using the SternheimerGW method to investigate the quasiparticle band structure of monolayer MoS2 subject to an effective dielectric screening model, which is meant to approximately describe substrate polarization in real device ap…
We derive a gap equation for bilayer excitonic systems based on density functional theory and benchmark our results against quantum Monte-Carlo simulations and recent experiments on double bilayer graphene. The gap equation has a mean-field form but includes a consistent treatment of dynamical screening. We show that the gap survives at much higher densities than previously thought from mean-field estimates which gives strong indications that the double-bilayer graphene systems at zero magnetic field can be used as model systems to investigate the BCS-BEC crossover. Furthermore, we show that J…
We demonstrate the growth of graphene nanocrystals by molecular beam methods that employ a solid carbon source, and that can be used on a diverse class of large area dielectric substrates. Characterization by Raman and Near Edge X-ray Absorption Fine Structure spectroscopies reveal a sp2 hybridized hexagonal carbon lattice in the nanocrystals. Lower growth rates favor the formation of higher quality, larger size multi-layer graphene crystallites on all investigated substrates. The surface morphology is determined by the roughness of the underlying substrate and graphitic monolayer steps are ob…
Graphene layers grown by chemical vapour deposition (CVD) method and transferred from Cu-foils to the oxidized Si-substrates were investigated by spectroscopic ellipsometry (SE), Raman and X-Ray Photoelectron Spectroscopy (XPS) methods. The optical properties of transferred CVD graphene layers do not always correspond to the ones of the exfoliated graphene due to the contamination from the chemicals used in the transfer process. However, the real thickness and the mean properties of the transferred CVD graphene layers can be found using ellipsometry if a real thickness of the SiO2 layer is tak…
We report the 1/f noise characteristics at low-frequency in graphene field-effect transistors that utilized a high-k dielectric tantalum oxide encapsulated layer (a few nanometers thick) placed by atomic layer deposition on Si3N4. A low-noise level of ~ 2.2 x 10^(-10) Hz-1 has been obtained at f = 10 Hz. The origin and physical mechanism of the noise can be interpreted by the McWhorter context, where fluctuations in the carrier number contribute dominantly to the low-frequency noise. Optimizing fabrication processes reduced the number of charged impurities in the graphene field-effect transist…
Engineering of the dielectric environment represents a powerful strategy to control the electronic and optical properties of two-dimensional (2D) materials without compromising their structural integrity. Here we show that the recent development of high-$κ$ 2D materials present new opportunities for dielectric engineering. By solving a 2D Mott-Wannier exciton model for WSe$_2$ on different substrates using a screened electron-hole interaction obtained from first principles, we demonstrate that the exciton Rydberg series changes qualitatively when the dielectric screening within the 2D semicond…
Relaxing the assumption of "infinite and homogenous background" the dielectric response function of one-dimensional (1D) semiconducting nanowires embedded in a dielectric environment is calculated. It is shown that high-k (higher than semiconductor dielectric constant) dielectric environment reduces the screening by the free carriers inside the nanostructure whereas, low dielectric environment increases the Coulombic interaction between free carriers and enhances the strength of screening function. In long wavelength limit, dielectric screening and collective excitation of electron gas are fou…
The electronic properties of doped bilayer graphene in presence of bottom and top gates have been studied and characterized by means of Density Functional Theory calculations. Varying independently the bottom and top gates it is possible to control separately the total doping charge on the sample, and the average external electric field acting on the bilayer. We show that, at fixed doping level, the band gap at the K point in the Brillouin zone depends linearly on the average electric field, whereas the corresponding proportionality coefficient has a non-monotonic dependence on doping. We find…
We calculate the static polarizability of multilayer graphene and study the effect of stacking arrangement, carrier density, and onsite energy difference on graphene screening properties. At low densities, the energy spectrum of multilayer graphene is described by a set of chiral two-dimensional electron systems and the associated chiral nature determines the screening properties of multilayer graphene showing very different behavior depending on whether the chirality index is even or odd. As density increases, the energy spectrum follows that of the monolayer graphene and thus the polarizabil…
We investigate the carrier mobility in mono- and bi-layer graphene with a top HfO2 dielectric, as a function of the HfO2 film thickness and temperature. The results show that the carrier mobility decreases during the deposition of the first 2-4 nm of top dielectric and remains constant for thicker layers. The carrier mobility shows a relatively weak dependence on temperature indicating that phonon scattering does not play a dominant role in controlling the carrier mobility. The data strongly suggest that fixed charged impurities located in close proximity to the graphene are responsible for th…
It is shown that a ``vacuum polarization'' induced by Coulomb potential in graphene leads to a strong suppression of electric charges even for undoped case (no charge carriers). A standard linear response theory is therefore not applicable to describe the screening of charge impurities in graphene. In particular, it overestimates essentially the contributions of charge impurities into the resistivity of graphene.
We utilize an organic polymer buffer layer between graphene and conventional gate dielectrics in top-gated graphene transistors. Unlike other insulators, this dielectric stack does not significantly degrade carrier mobility, allowing for high field-effect mobilities to be retained in top-gate operation. This is demonstrated in both two-point and four-point analysis, and in the high-frequency operation of a graphene transistor. Temperature dependence of the carrier mobility suggests that phonons are the dominant scatterers in these devices.
We have theoretically studied the dielectric environment effect on the charged-impurity-limited carrier mobility of graphene double-layer structure (GDLS) on the basis of the Boltzmann transport theory. In this system, two graphene layers are separated by a dielectric barrier layer. It is pointed out that the carrier mobility strongly depends on the dielectric constant of the barrier layer when the interlayer distance becomes larger than the inverse of the Fermi wave vector. Moreover, the conditions to improve the charged-impurity-limited carrier mobility of the GDLS are evaluated.
A fully selfconsistent treatment for gap generation and Coulomb screening in excitonic insulators is presented. The method is based on the equations of motion for the relevant dynamical variables combined with a variational approach. Applying the theory for a model system of bilayer graphene, an excitonic groundstate with a gap exceeding 10 meV is predicted.
Screening of a large external charge in graphene is studied. The charge is assumed to be displaced away or smeared over a finite region of the graphene plane. The initial decay of the screened potential with distance is shown to follow the 3/2 power. It gradually changes to the Coulomb law outside of a hypercritical core whose radius is proportional to the external charge.
We consider the effect of periodic scalar and vector potentials generated by periodic deformations of the graphene crystal lattice, on the energy spectrum of electrons. The dependence of electron velocity near the Dirac point on the periodic perturbations of different types is discussed. We also investigated the effect of screening of the scalar potential by calculating the dielectric function as a function of the wave length of the periodic potential. This calculation shows that the periodic scalar field is strongly suppressed by the screening. Using the dependence of electron velocity on the…
Moiré superlattices of two-dimensional van der Waals materials have emerged as a powerful platform for designing electronic band structures and discovering emergent physical phenomena. A key concept involves the creation of long-wavelength periodic potential and moiré bands in a crystal through interlayer hybridization when two materials are overlaid. Here we demonstrate a new approach based on spatially periodic dielectric screening to create moiré bands in a monolayer semiconductor. It relies on reduced dielectric screening of the Coulomb interactions in monolayer semiconductors and their en…
Electromagnetic fields bound tightly to charge carriers in a two-dimensional sheet, namely surface plasmons, are shielded by metallic plates that are a part of a device. It is shown that for epitaxial graphenes, the propagation velocity of surface plasmons is suppressed significantly through a partial screening of the electron charge by the interface states. On the basis of analytical calculations of the electron lifetime determined by the screened Coulomb interaction, we show that the screening effect gives results in agreement with those of a recent experiment.
We investigate the conductivity of doped graphene in the semiclassical Boltzmann limit, as well as the conductivity minimum within the self-consistent transport theory. Using the hard-disk model for a two-dimensional distribution of impurities gives rise to both strong increase in the slope of conductivity at low charge carrier densities in graphene and a strongly sub-linear behavior of the conductivity at high charge carrier densities when the correlation distance between the impurities is large. On the other hand, we find that a super-linear dependence of the conductivity on charge carrier d…
We study the charge density distribution, the electric field profile, and the resistance of an electrostatically created lateral p-n junction in graphene. We show that the electric field at the interface of the electron and hole regions is strongly enhanced due to limited screening capacity of Dirac quasiparticles. Accordingly, the junction resistance is lower than estimated in previous literature.
Environmental dielectric screening effects on exciton transition energies in single-walled carbon nanotubes (SWNTs) have been studied quantitatively in the range of dielectric constants from 1.0 to 37 by immersing SWNTs bridged over trenches in various organic solvents by means of photoluminescence and the excitation spectroscopies. With increasing environmental dielectric constant ($ε_{\rm env}$), both $E_{11}$ and $E_{22}$ exhibited a redshift by several tens meV and a tendency to saturate at a $ε_{\rm env} \sim 5$ without an indication of significant ($n$,$m$) dependence. The redshifts can …
We calculate the screening function in bilayer graphene (BLG) both in the intrinsic (undoped) and the extrinsic (doped) regime within random phase approximation, comparing our results with the corresponding single layer graphene (SLG) and the regular two dimensional electron gas (2DEG). We find that the Kohn anomaly is strongly enhanced in BLG. We also discuss the Friedel oscillation and the RKKY interaction, which are associated with the non-analytic behavior of the screening function at $q=2k_F$. We find that the Kohn anomaly, the Friedel oscillation, and the RKKY interaction are all qualita…
With the motivation of improving the performance and reliability of aggressively scaled nano-patterned graphene field-effect transistors, we present the first systematic experimental study on charge and current distribution in multilayer graphene field-effect transistors. We find a very particular thickness dependence for Ion, Ioff, and the Ion/Ioff ratio, and propose a resistor network model including screening and interlayer coupling to explain the experimental findings. In particular, our model does not invoke modification of the linear energy-band structure of graphene for the multilayer c…
We describe scanning tunneling spectroscopy (STS) measurements performed on individual cobalt (Co) atoms deposited onto backgated graphene devices. We find that Co adatoms on graphene can be ionized by either the application of a global backgate voltage or by the application of a local electric field from a scanning tunneling microscope (STM) tip. Large screening clouds are observed to form around Co adatoms ionized in this way, and we observe that some intrinsic graphene defects display a similar behavior. Our results provide new insight into charged impurity scattering in graphene, as well a…
Raman intensity of Rhodamine B (RhB) is enhanced by inserting a thin high \k{appa} dielectric layer which reduces the surface plasmon damping at the gold-graphene interface. The results indicate that the Raman intensity increases sharply by plasmonic resonance enhancement while maintaining efficient fluorescence quenching with optimized dielectric layer thickness.
The conductivity of the system magnetic dielectric (EuO) - graphene channel - ferroelectric substrate was considered. The magnetic dielectric locally transforms the band spectrum of graphene by inducing an energy gap in it and making it spin-asymmetric with respect to the free electrons. The range of spontaneous polarization (2- 5)mC/m2 that can be easily realized in thin films of proper and incipient ferroelectrics, was under examination. It was demonstrated, that if the Fermi level in the graphene channel belongs to energy intervals where the graphene band spectrum, modified by EuO, becomes …
We analyze the response of bilayer graphene to an external transverse electric field using a variational method. A previous attempt to do so in a recent paper by Falkovsky [Phys. Rev. B 80, 113413 (2009)] is shown to be flawed. Our calculation reaffirms the original results obtained by one of us [E. McCann, Phys. Rev. B 74, 161403(R) (2006)] by a different method. Finally, we generalize these original results to describe a dual-gated bilayer graphene device.
The screening properties and collective excitations (plasmons) in AA-stacked bilayer graphene are studied within the random phase approximation (RPA). Whereas long lived plasmons in single layer graphene and in AB-stacked bilayer graphene can exist only in doped samples, we find that coherent plasmons can disperse in AA-stacked bilayer graphene {\it even in the absence of doping}. Moreover, we show that the characteristic low energy dispersion relation is unaffected by changes in the number of carriers, unless the chemical potential of the doped sample exceeds the inter-layer hopping energy. W…
Screening of charge impurities in graphene is analyzed using the exact solution for vacuum polarization obtained from the massless Dirac-Kepler problem. For the impurity charge below certain critical value no density perturbation is found away from the impurity, in agreement with the linear response theory result. For supercritical charge, however, the polarization distribution is shown to have a power law profile, leading to screening of the excess charge at large distances. The Dirac-Kepler scattering states give rise to standing wave oscillations in the local density of states which appear …
The growth of single and multilayer graphene nano-flakes on MgO and ZrO2 at low temperatures is shown through transmission electron microscopy. The graphene nano-flakes are ubiquitously anchored at step edges on MgO (100) surfaces. Density functional theory investigations on MgO (100) indicate C2H2 decomposition and carbon adsorption at step-edges. Hence, both the experimental and theoretical data highlight the importance of step sites for graphene growth on MgO.
Terahertz (THz) lasers on optically pumped multiple-graphene-layer (MGL) structures as their active region are proposed and evaluated. The developed device model accounts for the interband and intraband transitions in the degenerate electron-hole plasma generated by optical radiation in the MGL structure and the losses in the slot or dielectric waveguide. The THz laser gain and the conditions of THz lasing are found. It is shown that the lasers under consideration can operate at frequencies > 1 THz at room temperatures.
We show that by combining high-k dielectric substrate and high density of charge carriers, Coulomb impurity can be effectively screened, leading to an unprecedented room-temperature mobility of ~150cm2/Vs in monolayer MoS2. The high sample quality enables us to quantitatively extract the mobility components limited by Coulomb impurities, intrinsic and surface optical phonons, and study their scaling with temperature, carrier density and dielectric constant. The excellent agreement between our theoretical analysis and experimental data demonstrates unambiguously that room-temperature phonon-lim…
Graphene oxide relative dielectric permittivity, both its real and imaginary parts, have been measured under various humidity conditions at GHz. It is demonstrated that the relative dielectric permittivity increases with increasing humidity due to water uptake. This electrical property of graphene oxide was used to create a battery-free wireless radio-frequency identification (RFID) humidity sensor by coating printed graphene antenna with the graphene oxide layer. The resonance frequency as well as the backscattering phase of such graphene oxide/graphene antenna become sensitive to the surroun…
