Ultrafast relaxation of hot optical phonons in monolayer and multilayer graphene on different substrates

Hot carrier cooling in few-layer and multilayer epitaxial graphene on SiC, and chemical vapor deposition (CVD) grown graphene transferred onto a glass substrate was investigated by transient absorption spectroscopy and imaging. Coupling to the substrate was found to play a critical role in charge carrier cooling. For both multilayer epitaxial graphene and monolayer CVD graphene, charge carriers transfer heat predominantly to intrinsic in-plane optical phonons of graphene. At high pump intensity, a significant number of optical phonons are accumulated, and the optical phonon lifetime presents a bottleneck for charge carrier cooling. This hot phonon effect did not occur in few-layer epitaxial graphene because of strong coupling to the substrate, which provided additional cooling channels. The limiting charge carrier lifetimes at high excitation densities were 1.8 ± 0.1 ps and 1.4 ± 0.1 ps for multilayer epitaxial graphene and monolayer CVD graphene, respectively. These values represent lower limits on the optical phonon lifetime for the graphene samples.     

Thermal properties of graphene and multilayer graphene: Applications in thermal interface materials

We review the thermal properties of graphene and multilayer graphene, and discuss graphene’s applications in thermal management of advanced electronics and optoelectronics. A special attention is paid to the use of the liquid-phase-exfoliated graphene and multilayer graphene as the fillers in the thermal interface materials. It has been demonstrated that addition of an optimized mixture of graphene and multilayer graphene to the composites with different matrix materials produces the record-high enhancement of the effective thermal conductivity at the small filler loading fraction (f≤10 vol%). The thermal conductivity enhancement due to the presence of graphene in the composites has been observed for a range of matrix materials used by industry. The hybrid composites where graphene is utilized together with metallic micro- and nanoparticles allow one to tune both the thermal and electrical conductivity of these materials. Theoretical considerations indicate that the graphene-based thermal interface materials can outperform those with carbon nanotubes, metal nanoparticles and other fillers owing to graphene’s geometry, mechanical flexibility and lower Kapitza resistance at the graphene–base material interface.     

Charge-transfer-induced cesium superlattices on graphene

We investigate cesium (Cs) adsorption on graphene formed on a 6H-SiC(0001) substrate by a combined scanning tunneling microscopy and density functional theory study. Individual Cs atoms adsorb preferentially at the rim region of the well-defined 6×6 substrate superstructure and on multilayer graphene. By finely controlling the graphene thickness and Cs coverages (1/3 ML and 1?ML), we here demonstrate two intriguing and well-ordered Cs superlattices on bilayer and multilayer graphene (<6 layers). Statistical analysis of the Cs-Cs interatomic distance reveals a hitherto unobserved Cs-Cs long-range electrostatic potential caused by charge transfer from Cs to graphene, which couples with the inhomogeneous substrate potential to stabilize the observed Cs superlattices. The present study provides a new avenue to fabricate atomic and molecular superlattices for applications in high-density recording and data storage.     

On the transistor effect in a vertical structure with a nonconjugated polymer as a transport layer

The charge carrier transport in a multilayer film structure based on a nonconjugated polymer has been studied. The conditions under which the charge carrier transport can be controlled by an electric field due to variations in the potential at the control electrode have been established. The results obtained are discussed within the model of passage of charge particles through a multibarrier system.     

Reversal of Klein reflection by magnetic barriers in bilayer graphene

Massless Dirac fermions in monolayer graphene exhibit total transmission when normally incident on a scalar potential barrier, a consequence of the Klein paradox originally predicted by O Klein for relativistic electrons obeying the 3 + 1 dimensional Dirac equation. For bilayer graphene, charge carriers are massive Dirac fermions and, due to different chiralities, electron and hole states are not coupled to each other. Therefore, the wavefunction of an incident particle decays inside a barrier as for the non-relativistic Schr?dinger equation. This leads to exponentially small transmission upon normal incidence. We show that, in the presence of magnetic barriers, such massive Dirac fermions can have transmission even at normal incidence. The general consequences of this behavior for multilayer graphene consisting of massless and massive modes are mentioned. We also briefly discuss the effect of a bias voltage on such magnetotransport.     

第一性原理研究气体小分子吸附的石墨烯负载金属原子体系

石墨烯负载的单个金属原子体系(M-gra)具有高的结构稳定性,显正电性的金属原子可作为活性位用在气敏器件和催化材料.本文采用基于密度泛函理论的第一性原理方法研究单个有毒气体小分子(NO和CO)在M-gra表面的吸附特性.研究结果表明:单个NO分子吸附的稳定性高于CO分子,由于其能够从反应衬底获得更多的转移电荷,因此,M-gra衬底对NO分子表现出高的灵敏度.此外,不同小分子吸附能够改变M-gra体系的电荷密度和自旋电荷分布,进而使得气体分子吸附体系表现出不同大小的磁矩.通过对比气体分子吸附前后M-gra体系的磁矩变化,能够有效判断吸附分子和反应衬底的类型.     

Phonons of graphene and graphitic materials derived from the empirical potential LCBOPII

We present the interatomic force constants and phonon dispersions of graphite and graphene from the LCBOPII empirical bond order potential. We find a good agreement with experimental results, particularly in comparison to other bond order potentials. From the flexural mode we determine the bending rigidity of graphene to be 0.69 eV at zero temperature. We discuss the large increase of this constant with temperature and argue that derivation of force constants from experimental values should take this feature into account. We examine also other graphitic systems, including multilayer graphene for which we show that the splitting of the flexural mode can provide a tool for characterization.     

Graphene based single molecule nanojunction

We introduce the ab-initio framework for zigzag-edged graphene fragment based single-electron transistor (SET) operating in the Coulomb blockade regime. Graphene is modeled using the density-functional theory and the environment is described by a continuum model. The interaction between graphene and the SET environment is treated self-consistently through the Poisson equation. We calculate the charging energy as a function of an external gate potential, and from this we obtain the charge stability diagram. Specifically, the importance of including re-normalization of the charge states due to the polarization of the environment has been demonstrated.     

First–principles study of potassium adsorption and diffusion on graphene

Potassium–ion batteries (KIBs) are a new–type of energy storage devices that have attracted increasing attention due to their low cost and the abundant resource of K in the Earth’s crust. Monolayer and multilayer graphene are promising electrode materials for KIBs. Herein, the adsorption and diffusion of potassium atoms on the surface of graphene were studied using the first–principles calculations including the van der Waals interaction. It was determined that K atoms can stably adsorb on the surface of graphene. The climbing image nudged elastic band method was employed to calculate the diffusion barriers of a single K atom and two K atoms on the surface of graphene. The results demonstrated that the diffusion barrier of a single K atom on graphene was low. The interaction between K atoms was considered and it facilitates the K atom diffusion to the second and third nearest–neighbour site of the K adatom, but prevents the K atom diffusion to the far nearest–neighbour site of the K adatom. Moreover, the difference in charge density demonstrates that there was a significant charge transfer from two K adatoms to its nearest–neighbour carbon atoms.     

Metal to insulator transition in epitaxial graphene induced by molecular doping

The capability to control the type and amount of charge carriers in a material and, in the extreme case, the transition from metal to insulator, is one of the key challenges of modern electronics. By employing angle-resolved photoemission spectroscopy we find that a reversible metal to insulator transition and a fine-tuning of the charge carriers from electrons to holes can be achieved in epitaxial bilayer and single layer graphene by molecular doping. The effects of electron screening and disorder are also discussed. These results demonstrate that epitaxial graphene is suitable for electronics applications, as well as provide new opportunities for studying the hole doping regime of the Dirac cone in graphene.     

基于石墨烯用于微弱能量获取的柔性微结构研究

本文首次提出了一种基于石墨烯用于微弱能量获取的柔性基板/石墨烯/ZnO纳米线/石墨烯的柔性微结构.首先,从理论上进行了该新结构的设计及其工作原理分析;其次,研究了该结构制备过程中的关键工艺,并设计了该结构的制备流程;最后,成功制备了该结构,并进行了相关测试.最终测试结果表明该结构能够成功输出数百毫伏的电压.这些理论和实验上的研究为自驱动微纳系统提供了研究基础,同时也对集成微纳系统的实用化发展具有一定的研究意义.     

Manifestations of topological effects in graphene

Graphene is a monoatomic layer of graphite with carbon atoms arranged in a two-dimensional honeycomb lattice configuration. It has been known for more than 60 years that the electronic structure of graphene can be modelled by two-dimensional massless relativistic fermions. This property gives rise to numerous applications, both in applied sciences and in theoretical physics. Electronic circuits made out of graphene could take advantage of its high electron mobility that is witnessed even at room temperature. In the theoretical domain the Dirac-like behaviour of graphene can simulate high energy effects, such as the relativistic Klein paradox. Even more surprisingly, topological effects can be encoded in graphene such as the generation of vortices, charge fractionalisation and the emergence of anyons. The impact of the topological effects on graphene's electronic properties can be elegantly described by the Atiyah–Singer index theorem. Here we present a pedagogical encounter of this theorem and review its various applications to graphene. A direct consequence of the index theorem is charge fractionalisation that is usually known from the fractional quantum Hall effect. The charge fractionalisation gives rise to the exciting possibility of realising graphene based anyons that unlike bosons or fermions exhibit fractional statistics. Besides being of theoretical interest, anyons are a strong candidate for performing error free quantum information processing.     

One-step synthesis of TiC/multilayer graphene composite by thermal plasma

Graphene hybrid materials have been attracting a great deal of attention due to their superior properties. Nevertheless, problems such as expensive and complicated production processes have limited their application to industrial fields. Here, we introduce a one-step synthesis of titanium carbide (TiC) nanoparticles on multilayer graphene nanosheet (TiC/multilayer graphene) composites using thermal plasma. Although there are three types of titanium alkoxides (titanium ethoxide, titanium isopropoxide and titanium n-butoxide), the TiC/multilayer graphene was synthesized from only titanium isopropoxide. The injection temperature of the precursor was varied to investigate the effects of the precursor concentration in the plasma region. A TiC/multilayer graphene hybrid material with crystalline TiC nanoparticles below 50 nm on graphene nanosheets was observed. The number of graphene nanosheet layers varied from one to over 10 according to the injection temperature. When titanium ethoxide and titanium butoxide were injected, TiC with amorphous carbon and graphite were synthesized. The formation of graphene is considered to be affected by the structure of the carbon chain in the precursors and the concentration in the plasma region.     

Interfacial thermal resistance in multilayer graphene structures

The cross-plane thermal conductivities of multilayer graphene are investigated using nonequilibrium molecular dynamics simulation. It is found that the interfacial thermal resistance in multilayer graphene structures is strongly layer number dependent. It decreases with increasing layer number and reaches a limit as layer number is large enough. The interfacial thermal resistance for graphite and multilayer graphene has an anomalous relationship with temperature compared with that in superlattice structures. It increases with the temperatures above room temperature, which is attributed to phonon tunneling effects. Phonon tunneling probability is reduced due to the decreased phonon wavelength while temperature rises, which in turn causes the increased interfacial thermal resistance.     

多层石墨烯的表面起伏的分子动力学模拟

运用经典分子动力学方法,研究了呈现不同堆积方式的多层石墨烯在不同温度下的表面起伏,并且和单层、双层石墨烯做对比,计算发现:室温下,多层石墨烯中存在着横向特征尺寸约为100 A的起伏,该尺寸会随着温度的升高而增大;同时,起伏的高度也随着温度的升高而增大,这些石墨烯的层内起伏高度关联函数都遵从幂指数标度行为G_h(q)αq~(-α),对于同一种石墨烯,温度越高幂指数越小;而在同一温度下,不同堆积方式的石墨烯的幂指数也不同,所有这些特征都来源于温度以及层间耦合作用引起的非谐效应。     

Correlated states in alternating twisted bilayer-monolayer-monolayer graphene heterostructure

Highly controlled electronic correlation in twisted graphene heterostructures has gained enormous research interests recently, encouraging exploration in a wide range of moiré superlattices beyond the celebrated twisted bilayer graphene. Here we characterize correlated states in an alternating twisted Bernal bilayer-monolayer-monolayer graphene of ～ 1.74°, and find that both van Hove singularities and multiple correlated states are asymmetrically tuned by displacement fields. In particular, when one electron per moiré unit cell is occupied in the electron-side flat band, or the hole-side flat band (i.e., three holes per moiré unit cell), the correlated peaks are found to counterintuitively grow with heating and maximize around 20 K - a signature of Pomeranchuk effect. Our multilayer heterostructure opens more opportunities to engineer complicated systems for investigating correlated phenomena.     

光抽运多层石墨烯太赫兹表面等离子体增益特性的研究

本文建立了光抽运多层石墨烯表面等离子体模型,计算了光抽运多层石墨烯等离子体传播系数的实部和吸收系数,讨论了动量弛豫时间、温度、层数、准费米能级对表面等离子体传播系数的实部和吸收系数的影响.研究结果表明,光抽运多层石墨烯使其动态电导率的实部在太赫兹频段内出现负值时,石墨烯表面等离子体实现增益.通过光抽运剥离层石墨烯和含有底层石墨烯结构表面等离子体传播系数和吸收系数比较,表明光抽运剥离层石墨烯能更有效地实现表面等离子体的增益.同时,在低温下,光抽运具有合适层数的石墨烯比光抽运单层石墨烯能获得更大的表面等离子体增益.     

石墨烯超快动态光学性质

通过建立石墨烯的光学布洛赫方程, 研究了弱光场下的单层石墨烯超快动态光学性质. 理论研究表明在太赫兹辐射光场下由于泡利不相容和能量守恒原理使得石墨烯系统建立动态非平衡载流子并达到饱和的时间是20–200 fs, 能够在1 ps之内迅速产生光电流. 研究发现√2ev_F E₀ t<0 和ω 分别对应入射光的强度和频率, t为时间, v_F是石墨烯狄拉克点附近电子的费米速度. 研究发现光子能量?ω越大, 电极化强度以及光电流越强. 我们的理论研究结果与已有的众多实验结果一致, 表明石墨烯在超快动态光学领域尤其是太赫兹领域拥有重要的研究和应用价值.     

Symmetric scrolled packings of multilayered carbon nanoribbons

Scrolled packings of single-layer and multilayer graphene can be used for the creation of supercapacitors, nanopumps, nanofilters, and other nanodevices. The full atomistic simulation of graphene scrolls is restricted to consideration of relatively small systems in small time intervals. To overcome this difficulty, a two-dimensional chain model making possible an efficient calculation of static and dynamic characteristics of nanoribbon scrolls with allowance for the longitudinal and bending stiffness of nanoribbons is proposed. The model is extended to the case of scrolls of multilayer graphene. Possible equilibrium states of symmetric scrolls of multilayer carbon nanotribbons rolled up so that all nanoribbons in the scroll are equivalent are found. Dependences of the number of coils, the inner and outer radii, lowest vibrational eigenfrequencies of rolled packages on the length L of nanoribbons are obtained. It is shown that the lowest vibrational eigenfrequency of a symmetric scroll decreases with a nanoribbon length proportionally to L^–1. It is energetically unfavorable for too short nanoribbons to roll up, and their ground state is a stack of plane nanoribbons. With an increasing number k of layers, the nanoribbon length L necessary for creation of symmetric scrolls increases. For a sufficiently small number of layers k and a sufficiently large nanoribbon length L, the scrolled packing has the lowest energy as compared to that of stack of plane nanoribbons and folded structures. The results can be used for development of nanomaterials and nanodevices on the basis of graphene scrolled packings.