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The stability of two-dimensional (2D) layers and membranes is subject of a long standing theoretical debate. According to the so called Mermin-Wagner theorem, long wavelength fluctuations destroy the long-range order for 2D crystals. Similarly, 2D membranes embedded in a 3D space have a tendency to be crumpled. These dangerous fluctuations can, however, be suppressed by anharmonic coupling between bending and stretching modes making that a two-dimensional membrane can exist but should present strong height fluctuations. The discovery of graphene, the first truly 2D crystal and the recent experimental observation of ripples in freely hanging graphene makes these issues especially important. Beside the academic interest, understanding the mechanisms of stability of graphene is crucial for understanding electronic transport in this material that is attracting so much interest for its unusual Dirac spectrum and electronic properties. Here we address the nature of these height fluctuations by means of straightforward atomistic Monte Carlo simulations based on a very accurate many-body interatomic potential for carbon. We find that ripples spontaneously appear due to thermal fluctuations with a size distribution peaked around 70 AA which is compatible with experimental findings (50-100 AA) but not with the current understanding of stability of flexible membranes. This unexpected result seems to be due to the multiplicity of chemical bonding in carbon.
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Thermal ripples of graphene are well understood at room temperature, but their quantum counterparts at low temperatures are still in need of a realistic quantitative description. Here we present atomistic path-integral Monte Carlo simulations of freestanding graphene, which show upon cooling a striking classical-quantum evolution of height and angular fluctuations. The crossover takes place at ever-decreasing temperatures for ever-increasing wavelengths so that a completely quantum regime is never attained. Zero-temperature quantum graphene is flatter and smoother than classical at large scales, yet rougher at short scales. The angular fluctuation distribution of the normals can be quantitatively described by coexistence of two Gaussians, one classical strongly T-dependent and one quantum about $2^{circ}$ wide, of zero-point character. The quantum evolution of ripple-induced height and angular spread should be observable in electron diffraction in graphene and other two-dimensional materials like MoS$_2$, bilayer graphene, boron nitride, etc.
Intrinsic ripples with various configurations and sizes were reported to affect the physical and chemical properties of 2D materials. By performing molecular dynamics simulations and theoretical analysis, we use two geometric models of the ripple shape to explore numerically the distribution of ripples in graphene membrane. We focus on the ratio of ripple height to its diameter (t/D) which was recently shown to be the most relevant for chemical activity of graphene membranes. Our result demonstrates that the ripple density decreases as the coefficient t/D increases, in a qualitative agreement with the Boltzmann distribution derived analytically from the bending energy of the membrane. Our theoretical study provides also specific quantitative information on the ripple distribution in graphene and gives new insights applicable to other 2D materials.
We measure the temperature-dependent carrier density and resistivity of the topological surface state of thin exfoliated Bi2Se3 in the absence of bulk conduction. When the gate-tuned chemical potential is near or below the Dirac point the carrier density is strongly temperature dependent reflecting thermal activation from the nearby bulk valence band, while above the Dirac point, unipolar n-type surface conduction is observed with negligible thermal activation of bulk carriers. In this regime linear resistivity vs. temperature reflects intrinsic electron-acoustic phonon scattering. Quantitative comparison with a theoretical transport calculation including both phonon and disorder effects gives the ratio of deformation potential to Fermi velocity D/hbarvF = 4.7 {AA}-1. This strong phonon scattering in the Bi2Se3 surface state gives intrinsic limits for the conductivity and charge carrier mobility at room temperature of ~550 {mu}S per surface and ~10,000 cm2/Vs.
We examine magnetic relaxation in polycrystalline Fe films with strong and weak crystallographic texture. Out-of-plane ferromagnetic resonance (FMR) measurements reveal Gilbert damping parameters of $approx$ 0.0024 for Fe films with thicknesses of 4-25 nm, regardless of their microstructural properties. The remarkable invariance with film microstructure strongly suggests that intrinsic Gilbert damping in polycrystalline Fe is a local property of nanoscale crystal grains, with limited impact from grain boundaries and film roughness. By contrast, the in-plane FMR linewidths of the Fe films exhibit distinct nonlinear frequency dependences, indicating the presence of strong extrinsic damping. To fit our experimental data, we have used a grain-to-grain two-magnon scattering model with two types of correlation functions aimed at describing the spatial distribution of inhomogeneities in the film. However, neither of the two correlation functions is able to reproduce the experimental data quantitatively with physically reasonable parameters. Our finding points to the need to further examine the fundamental impact of film microstructure on extrinsic damping.
Grain boundaries (GBs) are structural imperfections that typically degrade the performance of materials. Here we show that dislocations and GBs in two-dimensional (2D) metal dichalcogenides MX2 (M = Mo, W; X = S, Se) can actually improve the material by giving it a qualitatively new physical property: magnetism. The dislocations studied all have a substantial magnetic moment of ~1 Bohr magneton. In contrast, dislocations in other well-studied 2D materials are typically non-magnetic. GBs composed of pentagon-heptagon pairs interact ferromagnetically and transition from semiconductor to half-metal or metal as a function of tilt angle and/or doping level. When the tilt angle exceeds 47{deg} the structural energetics favor square-octagon pairs and the GB becomes an antiferromagnetic semiconductor. These exceptional magnetic properties arise from an interplay of dislocation-induced localized states, doping, and locally unbalanced stoichiometry. Purposeful engineering of topological GBs may be able to convert MX2 into a promising 2D magnetic semiconductor.
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