arXiv subjects

Smarajit Karmakar

Publications and source records attributed to Smarajit Karmakar.

At least 91 records · Page 5Linked to original sources

arXiv2015

Dynamics of Glass Forming Liquids with Randomly Pinned Particles

It is frequently assumed that in the limit of vanishing cooling rate, the glass transition phenomenon becomes a thermodynamic transition at a temperature $T_{K}$. However, with any finite cooling rate, the system falls out of equilibrium at temperatures near $T_g(>T_{K})$, implying that the very existence of the putative thermodynamic phase transition at $T_{K}$ can be questioned. Recent studies of systems with randomly pinned particles have hinted that the thermodynamic glass transition may be observed in simulations and experiments carried out for liquids with randomly pinned particles. This expectation is based on the results of approximate calculations that suggest that the temperature of the thermodynamic glass transition increases as the concentration of pinned particles is increased and it may be possible to equilibrate the system at temperatures near the increased transition temperature. We test the validity of this prediction through extensive molecular dynamics simulations of two model glass-forming liquids in the presence of random pinning. We fit the temperature-dependence of the structural relaxation time to the Vogel-Fulcher-Tammann form that predicts a divergence of the relaxation time at a temperature $T_{VFT}$ and identify this temperature with the thermodynamic transition temperature $T_K$. We find that $T_{VFT}$ does not show any sign of increasing with increasing concentration of pinned particles. The main effect of pinning is found to be a rapid decrease in the kinetic fragility of the system with increasing pin concentration. Implications of these observations for current theories of the glass transition are discussed.

cond-mat.stat-mech↗

arXiv2014

Glass-like slow dynamics in a colloidal solid with multiple ground states

We study the phase ordering dynamics of a two dimensional model colloidal solid using molecular dynamics simulations. The colloid particles interact with each other with a Hamaker potential modified by the presence of equatorial "patches" of attractive and negative regions. The total interaction potential between two such colloids is, therefore, strongly directional and has three-fold symmetry. Working in the canonical ensemble, we determine the tentative phase diagram in the density-temperature plane which features three distinct crystalline ground states viz, a low density honeycomb solid followed by a rectangular solid at higher density, which eventually transforms to a close packed triangular structure as the density is increased further. We show that when cooled rapidly from the liquid phase along isochores, the system undergoes a transition to a "strong glass" while slow cooling gives rise to crystalline phases. We claim that geometrical frustration arising from the presence of many crystalline ground states causes glassy ordering and dynamics in this solid. Our results may be easily confirmed by suitable experiments on patchy colloids.

cond-mat.dis-nn↗

arXiv2014

Distribution of Diffusion Constants and Stokes-Einstein Violation in supercooled liquids

It is widely believed that the breakdown of the Stokes-Einstein (SE) relation between the translational diffusivity and the shear viscosity in supercooled liquids is due to the development of dynamic heterogeneity i.e. the presence of both slow and fast moving particles in the system. In this study we \emph{directly} calculate the distribution of the diffusivity for a model system for different temperatures in the supercooled regime. We find that with decreasing temperature, the distribution evolves from Gaussian to bimodal indicating that on the time scale of the typical relaxation time, mobile (fluid like) and less mobile (solid like) particles in the system can be \emph{unambiguously} identified. We also show that less mobile particles obey the Stokes-Einstein relation even in the supercooled regime and it is the mobile particles which show strong violation of the Stokes-Einstein relation in agreement with the previous studies on different model glass forming systems. Motivated by some of the recent studies where an ideal glass transition is proposed by randomly pinning some fraction of particles, we then studied the SE breakdown as a function of random pinning concentration in our model system. We showed that degree of SE breakdown increases quite dramatically with increasing pinning concentration, thereby providing a new way to unravel the puzzles of SE violation in supercooled liquids in greater details.

cond-mat.stat-mech↗

arXiv2013

Comparison of Static Length-Scales Characterizing the Glass Transition

The dramatic dynamic slowing down associated with the glass transition is considered by many to be related to the existence of a static length scale that grows when temperature decreases. Defining, identifying and measuring such a length is a subtle and non-trivial problem. Recently, two proposals, based on very different insights regarding the relevant physics, were put forward. One approach is based on the point-to-set correlation technique and the other on the scale where the lowest eigenvalue of the Hessian matrix becomes sensitive to disorder. In this Letter we present numerical evidence that the two approaches might result in the same identical length scale. This provides further mutual support to their relevance and, at the same time, raise interesting theoretical questions, discussed in the conclusion, concerning the fundamental reason for their relationship.

cond-mat.stat-mech↗

arXiv2012

The nature of the β-peak in the loss modulus of amorphous solids

Glass formers exhibit, upon an oscillatory excitation, a response function whose imaginary and real parts are known as the loss and storage moduli respectively. The loss modulus typically peaks at a frequency known as the αfrequency which is associated with the main relaxation mechanism of the super-cooled liquid. In addition, the loss modulus is decorated by a smaller peak, shoulder or wing which is referred to as the β-peak. The physical origin of this secondary peak had been debated for decades, with proposed mechanisms ranging from highly localized relaxations to entirely cooperative ones. Using numerical simulations we bring an end to the debate, exposing a clear and unique cooperative mechanism for the said β-peak which is distinct from that of the $α$-peak.

cond-mat.mtrl-sci↗

arXiv2012

Breakdown of the Stokes-Einstein relation in two, three and four dimensions

The breakdown of the Stokes-Einstein (SE) relation between diffusivity and viscosity at low temperatures is considered to be one of the hallmarks of glassy dynamics in liquids. Theoretical analyses relate this breakdown with the presence of heterogeneous dynamics, and by extension, with the fragility of glass formers. We perform an investigation of the breakdown of the SE relation in 2, 3 and 4 dimensions, in order to understand these interrelations. Results from simulations of model glass formers show that the degree of the breakdown of the SE relation decreases with increasing spatial dimensionality. The breakdown itself can be rationalized via the difference between the activation free energies for diffusivity and viscosity (or relaxation times) in the Adam-Gibbs relation in three and four dimensions. The behavior in two dimensions also can be understood in terms of a generalized Adam-Gibbs relation that is observed in previous work. We calculate various measures of heterogeneity of dynamics and find that the degree of the SE breakdown and measures of heterogeneity of dynamics are generally well correlated but with some exceptions. The two dimensional systems we study show deviations from the pattern of behavior of the three and four dimensional systems both at high and low temperatures. The fragility of the studied liquids is found to increase with spatial dimensionality, contrary to the expectation based on the association of fragility with heterogeneous dynamics.

cond-mat.stat-mech↗

arXiv2012

Random Pinning Glass Model

Glass transition where viscosity of liquids increases dramatically upon decrease of temperature without any major change in structural properties, remains one of the most challenging problems in condensed matter physics (Cavagna, 2009; Berthier and Biroli, 2011) in spite of tremendous research efforts in last decades. On the other hand disordered freezing of spins in a magnetic materials with decreasing temperature, the so-called spin glass transition, is relatively better understood (Mezard, Parisi and Virasoro, 1987; Castellani and Cavagna, 2005). Previously found similarity between some spin glass models with the structural glasses (Kirkpatrick and Thirumalai, 1987; Kirkpatrick and Wolynes, 1987; Kirkpatrick and Wolynes, 1987; Franz and Parisi, 1999; Moore and Drossel, 2002) inspired development of theories of structural glasses (Kirkpatrick, Thirumalai and Wolynes, 1989; Barrat, Franz and Parisi, 1997; Mézard and Parisi, 1999; Lubchenko and Wolynes, 2007; Biroli and Bouchaud, 2012) based on the scenario of spin glass transition. This scenario though looks very appealing is still far from being well established. One of the main differences between standard spin systems to molecular systems is the absence of quenched disorder and the presence of translational invariance: it often assumed that this difference is not relevant, but this conjecture is still far from being established. The quantities, which are well defined and characterized for spin models, are not easily calculable for molecular glasses due to the lack of quenched disorder which breaks the translational invariance in the system and the characterization of the similarity between the spin and the structural glass transition remained an elusive subject still now. In this study we introduced a model structural glass with built in quenched disorder which alleviates this main difference between the spin and molecular glasses thereby helping us to compare these two systems: the possibility of producing a good thermalization at rather low temperatures is one of the advantages of this model.

cond-mat.stat-mech↗

arXiv2012

Finite Size Scaling for the Glass Transition: the Role of a Static Length Scale

Over the last decade computer simulations have had an increasing role in shedding light on difficult statistical physical phenomena and in particular on the ubiquitous problem of the glass transition. Here in a wide variety of materials the viscosity of a super-cooled liquid increases by many orders of magnitude upon decreasing the temperature over a modest range. A natural concern in these computer simulation is the very small size of the simulated systems compared to experimental ones, raising the issue of how to assess the thermodynamic limit. Here we offer a theory for the glass transition based on finite size scaling, a method that was found very useful in the context of critical phenomena and other interesting problems. As is known, the construction of such a theory rests crucially on the existence of a growing {\em static} length scale upon decreasing the temperature. We demonstrate that the static length scale that was discovered in Ref. \cite{12KLP} fits the bill extremely well, allowing us to provide a finite size scaling theory for the $α$ relaxation time of the glass transition, including predictions for the thermodynamic limit based on simulations in small systems.

cond-mat.stat-mech↗

arXiv2012

The Adam-Gibbs relation for glass-forming liquids in 2, 3 and 4 dimensions

The Adam-Gibbs relation between relaxation times and the configurational entropy has been tested extensively for glass formers using experimental data and computer simulation results. Although the form of the relation contains no dependence on the spatial dimensionality in the original formulation, subsequent derivations of the Adam-Gibbs relation allow for such a possibility. We test the Adam-Gibbs relation in 2, 3, and 4 spatial dimensions using computer simulations of model glass formers. We find that the relation is valid in 3 and 4 dimensions. But in 2 dimensions, the relation does not hold, and interestingly, no single alternate relation describes the results for the different model systems we study.

cond-mat.dis-nn↗

arXiv2012

Relaxation Mechanisms in Glassy Dynamics: the Arrhenius and Fragile Regimes

Generic glass formers exhibit at least two characteristic changes in their relaxation behavior, first to an Arrhenius-type relaxation at some characteristic temperature, and then at a lower characteristic temperature to a super-Arrhenius (fragile) behavior. We address these transitions by studying the statistics of free energy barriers for different systems at different temperatures and space dimensions. We present a clear evidence for changes in the dynamical behavior at the transition to Arrhenius and then to a super-Arrhenius behavior. A simple model is presented, based on the idea of competition between single-particle and cooperative dynamics. We argue that Arrhenius behavior can take place as long as there is enough free volume for the completion of a simple $T_1$ relaxation process. Once free volume is absent one needs a cooperative mechanism to `collect' enough free volume. We show that this model captures all the qualitative behavior observed in simulations throughout the considered temperature range.

cond-mat.dis-nn↗

arXiv2011

Universality of the Plastic Instability in Strained Amorphous Solids

By comparing the response to external strains in metallic glasses and in Lenard-Jones glasses we find a quantitative universality of the fundamental plastic instabilities in the athermal, quasistatic limit. Microscopically these two types of glasses are as different as one can imagine, the latter being determined by binary interactions, whereas the former by multiple interactions due to the effect of the electron gas that cannot be disregarded. In spite of this enormous difference the plastic instability is the same saddle-node bifurcation. As a result the statistics of stress and energy drops in the elasto-plastic steady state are universal, sharing the same system-size exponents.

cond-mat.soft↗

arXiv2011

Exposing the static scale of the glass transition by random pinning

The dramatic slowing down associated with the glass transition cannot be fully understood without an associated static length that is expected to increase rapidly as the temperature is reduced. The search for such a length was long and arduous, without a universally accepted candidate at hand. Recently a natural such length $ξ_s$ was proposed, stemming from a cross-over between plastic and elastic mechanical responses of the material. In this Letter we show that supercooled liquids in which there exists random pinning sites of density $ρ_{\rm im}\sim 1/ξ_s^d$ exhibit complete jamming of all dynamics. This is a direct demonstration that the proposed length scale is indeed {\em the} static length that was long sought-after.

cond-mat.stat-mech↗

arXiv2011

An Athermal Brittle to Ductile Transition in Amorphous Solids

Brittle materials exhibit sharp dynamical fractures when meeting Griffith's criterion, whereas ductile materials blunt a sharp crack by plastic responses. Upon continuous pulling ductile materials exhibit a necking instability which is dominated by a plastic flow. Usually one discusses the brittle to ductile transition as a function of increasing temperature. We introduce an athermal brittle to ductile transition as a function of the cut-off length of the inter-particle potential. On the basis of extensive numerical simulations of the response to pulling the material boundaries at a constant speed we offer an explanation of the onset of ductility via the increase in the density of plastic modes as a function of the potential cutoff length. Finally we can resolve an old riddle: in experiments brittle materials can be strained under grip boundary conditions, and exhibit a dynamic crack when cut with a sufficiently long initial slot. Mysteriously, in molecular dynamics simulations it appeared that cracks refused to propagate dynamically under grip boundary conditions, and continuous pulling was necessary to achieve fracture. We argue that this mystery is removed when one understands the distinction between brittle and ductile athermal amorphous materials.

cond-mat.stat-mech↗

arXiv2011

Direct Estimate of the Static Length-Scale Accompanying the Glass Transition

Characterizing the glass state remains elusive since its distinction from a liquid state is not obvious. Glasses are liquids whose viscosity has increased so much that they cannot flow. Accordingly there have been many attempts to define a static length-scale associated with the dramatic slowing down of supercooled liquid with decreasing temperature. Here we present a simple method to extract the desired length-scale which is highly accessible both for experiments and for numerical simulations. The fundamental idea is that low lying vibrational frequencies come in two types, those related to elastic response and those determined by plastic instabilities. The minimal observed frequency is determined by one or the other, crossing at a typical length-scale which is growing with the approach of the glass transition. This length-scale characterizes the correlated disorder in the system, where on longer length-scales the details of the disorder become irrelevant, dominated by the Debye model of elastic modes.

cond-mat.stat-mech↗

arXiv2011

Do Athermal Amorphous Solids Exist?

We study the elastic theory of amorphous solids made of particles with finite range interactions in the thermodynamic limit. For the elastic theory to exist one requires all the elastic coefficients, linear and nonlinear, to attain a finite thermodynamic limit. We show that for such systems the existence of non-affine mechanical responses results in anomalous fluctuations of all the nonlinear coefficients of the elastic theory. While the shear modulus exists, the first nonlinear coefficient B_2 has anomalous fluctuations and the second nonlinear coefficient B_3 and all the higher order coefficients (which are non-zero by symmetry) diverge in the thermodynamic limit. These results put a question mark on the existence of elasticity (or solidity) of amorphous solids at finite strains, even at zero temperature. We discuss the physical meaning of these results and propose that in these systems elasticity can never be decoupled from plasticity: the nonlinear response must be very substantially plastic.

cond-mat.stat-mech↗

arXiv2010

What Determines the Yield Stress in Amorphous Solids?

A crucially important material parameter for all amorphous solids is the yield stress, which is the value of the stress for which the material yields to plastic flow when it is strained quasi-statically at zero temperature. It is difficult in laboratory experiments to determine what parameters of the inter-particle potential effect the value of the yield stress. Here we use the versatility of numerical simulations to study the dependence of the yield stress on the parameters of the inter-particle potential. We find a very simple dependence on the fundamental scales which characterize the repulsive and attractive parts of the potential respectively, and offer a scaling theory that collapses the data for widely different potentials and in different space dimensions.

physics.comp-ph↗

arXiv2010

Statistical Physics of the Yielding Transition in Amorphous Solids

The art of making structural, polymeric and metallic glasses is rapidly developing with many applications. A limitation to their use is their mechanical stability: under increasing external strain all amorphous solids respond elastically to small strains but have a finite yield stress which cannot be exceeded without effecting a plastic response which typically leads to mechanical failure. Understanding this is crucial for assessing the risk of failure of glassy materials under mechanical loads. Here we show that the statistics of the energy barriers ΔE that need to be surmounted changes from a probability distribution function (pdf) that goes smoothly to zero to a pdf which is finite at ΔE=0. This fundamental change implies a dramatic transition in the mechanical stability properties with respect to external strain. We derive exact results for the scaling exponents that characterize the magnitudes of average energy and stress drops in plastic events as a function of system size.

cond-mat.soft↗

arXiv2010

Statistical Physics of Elasto-Plastic Steady States in Amorphous Solids: Finite Temperatures and Strain Rates

The effect of finite temperature $T$ and finite strain rate $\dotγ$ on the statistical physics of plastic deformations in amorphous solids made of $N$ particles is investigated. We recognize three regimes of temperature where the statistics are qualitatively different. In the first regime the temperature is very low, $T<T_{\rm cross}(N)$, and the strain is quasi-static. In this regime the elasto-plastic steady state exhibits highly correlated plastic events whose statistics are characterized by anomalous exponents. In the second regime $T_{\rm cross}(N)<T<T_{\rm max}(\dotγ)$ the system-size dependence of the stress fluctuations becomes normal, but the variance depends on the strain rate. The physical mechanism of the cross-over is different for increasing temperature and increasing strain rate, since the plastic events are still dominated by the mechanical instabilities (seen as an eigenvalue of the Hessian matrix going to zero), and the effect of temperature is only to facilitate the transition. A third regime occurs above the second cross-over temperature $T_{\rm max}(\dotγ)$ where stress fluctuations become dominated by thermal noise. Throughout the paper we demonstrate that scaling concepts are highly relevant for the problem at hand, and finally we present a scaling theory that is able to collapse the data for all the values of temperatures and strain rates, providing us with a high degree of predictability.

cond-mat.stat-mech↗