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J. H. Los

Publications and source records attributed to J. H. Los.

11 recordsLinked to original sources

Stress-controlled Poisson ratio of a crystalline membrane: Application to graphene

We demonstrate that a key elastic parameter of a suspended crystalline membrane---the Poisson ratio (PR) $ν$---is a non-trivial function of the applied stress $σ$ and of the system size $L$, i.e., $ν=ν_L(σ)$. We consider a generic 2D membrane embedded into space of dimensionality $2+d_c$. (The physical situation corresponds to $d_c=1$.) A particularly important application of our results is free-standing graphene. We find that at very low stress, where the membrane exhibits a linear response, the PR $ν_L(0)$ decreases with increasing $L$ and saturates for $ L\to \infty$ at a value which depends on the boundary conditions and is essentially different from the value $ν=-1/3$ previously predicted by the membrane theory within a self-consisted scaling analysis. By increasing $σ$, one drives a membrane into a non-linear regime characterized by a universal value of PR that depends solely on $d_c.$ This universal non-linear PR acquires its minimum value $ν_{\rm min}=-1$ in the limit $d_c\to \infty.$ With the further increase of $σ$, the PR changes sign and finally saturates at a positive non-universal value prescribed by the conventional elasticity theory. We also show that one should distinguish between the absolute and differential PR ($ν$ and $ν^{\rm diff}$, respectively). While coinciding in the limits of very low and very high stresses, they differ in general, $ν\neq ν^{\rm diff}$. In particular, in the non-linear universal regime, $ν^{\rm diff}$ takes a universal value which, similarly to absolute PR, is a function solely of $d_c$ but is different from the universal value of $ν$. In the limit $d_c\to \infty$, the universal value of $ν^{\rm diff}$ tends to $-1/3$, at variance with the limiting value $-1$ of $ν$. Finally, we briefly discuss generalization of these results to a disordered membrane.

cond-mat.mes-hall

Mechanics of thermally fluctuating membranes

Besides having unique electronic properties, graphene is claimed to be the strongest material in nature. In the press release of the Nobel committee it is claimed that a hammock made of a squared meter of one-atom thick graphene could sustain the wight of a 4 kg cat. More practically important are applications of graphene like scaffolds and sensors which are crucially dependent on the mechanical strength. Meter-sized graphene is even being considered for the lightsails in the starshot project to reach the star alpha centaury. The predicted strength of graphene is based on its very large Young modulus which is, per atomic layer, much larger than that of steel. This reasoning however would apply to conventional thin plates but does not take into account the peculiar properties of graphene as a thermally fluctuating crystalline membrane. It was shown recently both experimentally and theoretically that thermal fluctuations lead to a dramatic reduction of the Young modulus and increase of the bending rigidity for micron-sized graphene samples in comparison with atomic scale values. This makes the use of the standard Föppl-von Karman elasticity (FvK) theory for thin plates not directly applicable to graphene and other single atomic layer membranes. This fact is important because the current interpretation of experimental results is based on the FvK theory. In particular, we show that the FvK-derived Schwerin equation, routinely used to derive the Young modulus from indentation experiments has to be essentially modified for graphene at room temperature and for micron sized samples. Based on scaling analysis and atomistic simulation we investigate the mechanics of graphene under transverse load up to breaking. We determine the limits of applicability of the FvK theory and provide quantitative estimates for the different regimes.

cond-mat.mes-hall

Scaling behavior and strain dependence of in-plane elastic properties of graphene

We show by atomistic simulations that, in the thermodynamic limit, the in-plane elastic moduli of graphene at finite temperature vanish with system size $ L $ as a power law $ ~ L^{-η_u} $ with $ η_u \simeq 0.325 $, in agreement with the membrane theory. Our simulations clearly reveal the size and strain dependence of graphene's elastic moduli, allowing comparison to experimental data. Although the recently measured difference of a factor 2 between the asymptotic value of the Young modulus for tensilely strained systems and the value from {\it ab initio} calculations remains unsolved, our results do explain the experimentally observed increase of more than a factor 2 for a tensile strain of only a few permille. We also discuss the scaling of the Poisson ratio, for which our simulations disagree with the predictions of the self-consistent screening approximation.

cond-mat.mes-hall

Melting temperature of graphene

We present an approach to the melting of graphene based on nucleation theory for a first order phase transition from the 2D solid to the 3D liquid via an intermediate quasi-2D liquid. The applicability of nucleation theory, supported by the results of systematic atomistic Monte Carlo simulations, provides an intrinsic definition of the melting temperature of graphene, $ T_m $, and allows us to determine it. We find $T_m \simeq 4510$ K, about 250 K higher than that of graphite using the same interatomic interaction model. The found melting temperature is shown to be in good agreement with the asymptotic results of melting simulations for finite disks and ribbons of graphene. Our results strongly suggest that graphene is the most refractory of all known materials.

cond-mat.mes-hall

Spiral graphone and one sided fluorographene nano-ribbons

The instability of a free-standing one sided hydrogenated/fluorinated graphene nano-ribbon, i.e. graphone/fluorographene, is studied using ab-initio, semiempirical and large scale molecular dynamics simulations. Free standing semi-infinite arm-chair like hydrogenated/fluorinated graphene (AC-GO/AC-GF) and boat like hydrogenated/fluorinated graphene (B-GO/B-GF) (nano-ribbons which are periodic along the zig-zag direction) are unstable and spontaneously transform into spiral structures. We find that rolled, spiral B-GO and B-GF are energetically more favorable than spiral AC-GO and AC-GF which is opposite to the double sided flat hydrogenated/fluorinated graphene, i.e. graphane/fluorographene. We found that the packed, spiral structures exhibit unexpected localized HOMO-LUMO at the edges with increasing energy gap during rolling. These rolled hydrocarbon structures are stable beyond room temperature up to at least $T$=1000\,K.

cond-mat.mes-hall

Thermal rippling behavior of graphane

Thermal fluctuations of single layer hydrogenated graphene (graphane) are investigated using large scale atomistic simulations. By analyzing the mean square value of the height fluctuations $ $ and the height-height correlation function $H(q)$ for different system sizes and temperatures we show that hydrogenated graphene is an un-rippled system in contrast to graphene. The height fluctuations are bounded, which is confirmed by a $ H(q) $ tending to a constant in the long wavelength limit instead of showing the characteristic scaling law $ q^{4-η} (η\simeq 0.85)$ predicted by membrane theory. This unexpected behaviour persists up to temperatures of at least 900 K and is a consequence of the fact that in graphane the thermal energy can be accommodated by in-plane bending modes, i.e. modes involving C-C-C bond angles in the buckled carbon layer, instead of leading to significant out-of-plane fluctuations that occur in graphene.

cond-mat.mtrl-sci

Melting of graphene: from two to one dimension

The high temperature behaviour of graphene is studied by atomistic simulations based on an accurate interatomic potential for carbon. We find that clustering of Stone-Wales defects and formation of octagons are the first steps in the process of melting which proceeds via the formation of carbon chains. The molten state forms a three-dimensional network of entangled chains rather than a simple liquid. The melting temperature estimated from the two-dimensional Lindemann criterion and from extrapolation of our simulation for different heating rates is about 4900 K.

cond-mat.mtrl-sci

Atomistic simulations of structural and thermodynamic properties of bilayer graphene

We study the structural and thermodynamic properties of bilayer graphene, a prototype two-layer membrane, by means of Monte Carlo simulations based on the empirical bond order potential LCBOPII. We present the temperature dependence of lattice parameter, bending rigidity and high temperature heat capacity as well as the correlation function of out-of-plane atomic displacements. The thermal expansion coefficient changes sign from negative to positive above $\approx 400$ K, which is lower than previously found for single layer graphene and close to the experimental value of bulk graphite. The bending rigidity is twice as large than for single layer graphene, making the out-of-plane fluctuations smaller. The crossover from correlated to uncorrelated out-of-plane fluctuations of the two carbon planes occurs for wavevectors shorter than $\approx 3$ nm$^{-1}$

cond-mat.mtrl-sci

State-of-the-art models for the phase diagram of carbon and diamond nucleation

We review recent developments in the modelling of the phase diagram and the kinetics of crystallization of carbon. In particular, we show that a particular class of bond-order potentials (the so-called LCBOP models) account well for many of the known structural and thermodynamic properties of carbon at high pressures and temperatures. We discuss the LCBOP models in some detail. In addition, we briefly review the ``history'' of experimental and theoretical studies of the phase behaviour of carbon. Using a well-tested version of the LCBOP model (viz. LCBOPI+) we address some of the more controversial hypotheses concerning the phase behaviour of carbon, in particular: the suggestion that liquid carbon can exist in two phases separated by a first-order phase transition and the conjecture that diamonds could have formed by homogeneous nucleation in Uranus and Neptune.

cond-mat.mtrl-sci

Scaling Properties of Flexible Membranes from Atomistic Simulations: Application to Graphene

Structure and thermodynamics of crystalline membranes are characterized by the long wavelength behavior of the normal-normal correlation function G(q). We calculate G(q) by Monte Carlo and Molecular Dynamics simulations for a quasi-harmonic model potential and for a realistic potential for graphene. To access the long wavelength limit for finite-size systems (up to 40000 atoms) we introduce a Monte Carlo sampling based on collective atomic moves (wave moves). We find a power-law behaviour $G(q)\propto q^{-2+η}$ with the same exponent $η\approx 0.85$ for both potentials. This finding supports, from the microscopic side, the adequacy of the scaling theory of membranes in the continuum medium approach, even for an extremely rigid material like graphene.

cond-mat.mtrl-sci

Intrinsic ripples in graphene

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 Åwhich is compatible with experimental findings (50-100 Å) 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.

cond-mat.mtrl-sci