Searcharxiv⌕ Search

arXiv subjects

Smarajit Karmakar

Publications and source records attributed to Smarajit Karmakar.

At least 73 records · Page 4Linked to original sources

Plastic deformation of a permanently bonded network: stress relaxation by pleats

We show that a flat two dimensional network of connected vertices, when stretched, may deform plastically by producing `pleats'; system spanning linear structures with width comparable to the lattice spacing, where the network overlaps on itself. To understand the pleating process, we introduce an external field that couples to local {\em non-affine} displacements, i.e. those displacements of neighbouring vertices that cannot be represented as a local affine strain. We obtain both zero and finite temperature phase diagrams in the strain -- field plane. Pleats occur here as a result of an equilibrium first-order transition from the homogeneous network to a heterogeneous phase where stress is localised within pleats and eliminated elsewhere. We show that in the thermodynamic limit the un-pleated state is always metastable at vanishing field for infinitesimal strain. Plastic deformation of the initially homogeneous network is akin to the decay of a metastable phase via a dynamical transition. We make predictions concerning local stress distributions and thermal effects associated with pleats which may be observable in suitable experimental systems.

cond-mat.soft↗

Effect of pinning on the yielding transition of amorphous solids

Using numerical simulations, we have studied the yielding response, in the athermal quasi static limit, of a model amorphous material having inclusions in the form of randomly pinned particles. We show that, with increasing pinning concentration, the plastic activity becomes more spatially localized, resulting in smaller stress drops, and corresponding increase in the magnitude of strain where yielding occurs. We demonstrate that, unlike the spatially heterogeneous and avalanche led yielding in the case of the unpinned glass, for the case of large pinning concentration, yielding takes place via a spatially homogeneous proliferation of localized events.

cond-mat.soft↗

Slow Relaxations of Chemically Confined Hydration Layers near Lipid Bilayers: Dynamical Heterogeneities above Supercooling

A hydrated 1,2-dimyristoyl-sn-glycero-3-phosphorylcholine (DMPC) lipid membrane is investigated using an all atom molecular dynamics simulation at 308K to find out the physical sources of universal slow relaxation of hydration layers. Continuously residing interface water (IW) hydrogen bonded to each other and concertedly to different moieties of lipid heads are identified. The non-gaussian parameter of all IW show a crossover from cage vibration to translational diffusion. A significant non-gaussianity is observed for the IW prevailing large length correlations in translational van Hove functions. Two time-scales for the ballisitic motions and hopping transitions are obtained from the self intermediate scattering functions of the IW with an additional long relaxation which disappears for the BW. This is attributed to the coupled dynamics of IW cages hydrogen bonded to lipid heads. Our calculations reveal that the water near membranes are slowed down due to dynamical heterogeneities above room temperature and have implications to bioprotection mechanism at freezing conditions.

cond-mat.soft↗

Non-Gaussianity of van Hove Function and Dynamic Heterogeneity Length Scale

Non-Gaussian nature of the probability distribution of particles' displacements in the supercooled temperature regime in glass-forming liquids are believed to be one of the major hallmarks of glass transition. It is already been established that this probability distribution which is also known as the van Hove function show universal exponential tail. The origin of such an exponential tail in the distribution function is attributed to the hopping motion of particles observed in the supercooled regime. The non-Gaussian nature can also be explained if one assumes that the system has heterogeneous dynamics in space and time. Thus exponential tail is the manifestation of dynamic heterogeneity. In this work we directly show that non-Gaussanity of the distribution of particles' displacements occur over the dynamic heterogeneity length scale and dynamical behaviour course grained over this length scale becomes homogeneous. We study the non-Gaussianity of van Hove function by systematically coarse graining at different length scale and extract the length scale of dynamic heterogeneity at which the shape of the van Hove function crosses over from non-Gaussian to Gaussian. The obtained dynamic heterogeneity scale is found to be in very good agreement with the scale obtained from other conventional methods.

cond-mat.stat-mech↗

Do thermodynamically stable rigid solids exist?

Customarily, crystalline solids are defined to be {\em rigid} since they resist changes of shape determined by their boundaries. However, rigid solids cannot exist in the thermodynamic limit where boundaries become irrelevant. Particles in the solid may rearrange to adjust to shape changes eliminating stress without destroying crystalline order. Rigidity is therefore valid only in the {\em metastable} state that emerges because these particle rearrangements in response to a deformation, or strain, are associated with slow collective processes. Here, we show that a thermodynamic collective variable may be used to quantify particle rearrangements that occur as a solid is deformed at zero strain rate. Advanced Monte Carlo simulation techniques are then employed to obtain the equilibrium free energy as a function of this variable. Our results lead to a new view on rigidity: While at zero strain a rigid crystal coexists with one that responds to infinitesimal strain by rearranging particles and expelling stress, at finite strain the rigid crystal is metastable, associated with a free energy barrier that decreases with increasing strain. The rigid phase becomes thermodynamically stable by switching on an external field, which penalises particle rearrangements. This produces a line of first-order phase transitions in the field - strain plane that intersects the origin. Failure of a solid once strained beyond its elastic limit is associated with kinetic decay processes of the metastable rigid crystal deformed with a finite strain rate. These processes can be understood in quantitative detail using our computed phase diagram as reference.

cond-mat.mtrl-sci↗

Possible Universal Relation Between Short time $β$-relaxation and Long time $α$-relaxation in Glass-forming Liquids

Relaxation processes in supercooled liquids are known to exhibit interesting as well as complex behavior. One of the hallmarks of this relaxation process observed in the measured auto correlation function is occurrence of multiple steps of relaxation. The shorter time relaxation is known as the $β$-relaxation which is believed to be due to the motion of particles in the cage formed by their neighbors. One the other hand longer time relaxation, the $α$-relaxation is believed to be the main relaxation process in the liquids. The timescales of these two relaxations processes dramatically separate out with supercooling. In spite of decades of researches, it is still not clearly known how these relaxation processes are related to each other. In this work we show that, there is a possible universal relation between short time $β$-relaxation and the long time $α$-relaxation. This relation is found to be quite robust across many different model systems. Finally we show that length scale obtained from the finite size scaling analysis of $β$ timescale is same as that of length scale associated with the dynamic heterogeneity in both two and three dimensions.

cond-mat.soft↗

Role of $α$ and $β$ relaxations in Collapsing Dynamics of a Polymer Chain in Supercooled Glass-forming Liquid

Understanding the effect of glassy dynamics on the stability of bio-macromolecules and investigating the underlying relaxation processes governing degradation processes of these macromolecules are of immense importance in the context of bio-preservation. In this work we have studied the stability of a model polymer chain in a supercooled glass-forming liquid at different amount of supercooling in order to understand how dynamics of supercooled liquids influence the collapse behavior of the polymer. Our systematic computer simulation studies find that apart from long time relaxation processes ($α$ relaxation), short time dynamics of the supercooled liquid, known as $β$ relaxation plays an important role in controlling the stability of the model polymer. This is in agreement with some recent experimental findings. These observations are in stark contrast with the common belief that only long time relaxation processes are the sole player. We find convincing evidence that suggest that one might need to review the the vitrification hypothesis which postulates that $α$ relaxations control the dynamics of biomolecules and thus $α$-relaxation time should be considered for choosing appropriate bio-preservatives. We hope that our results will lead to understand the primary factors in protein stabilization in the context of bio-preservation.

cond-mat.soft↗

Block Analysis for the Calculation of Dynamic and Static Length Scales in Glass-Forming Liquids

We present {\it block analysis}, an efficient method to perform finite-size scaling for obtaining the length scale of dynamic heterogeneity and the point-to-set length scale for generic glass-forming liquids. This method involves considering blocks of varying sizes embedded in a system of a fixed (large) size. The length scale associated with dynamic heterogeneity is obtained from a finite-size scaling analysis of the dependence of the four-point dynamic susceptibility on the block size. The block size dependence of the variance of the $α$-relaxation time yields the static point-to-set length scale. The values of the obtained length scales agree quantitatively with those obtained from other conventional methods. This method provides an efficient experimental tool for studying the growth of length scales in systems such as colloidal glasses for which performing finite-size scaling by carrying out experiments for varying system sizes may not be feasible.

cond-mat.soft↗

Glass Transition in Supercooled Liquids with Medium Range Crystalline Order

The origins of rapid dynamical slow down in glass forming liquids in the growth of static length scales, possibly associated with identifiable structural ordering, is a much debated issue. Growth of medium range crystalline order (MRCO) has been observed in various model systems to be associated with glassy behaviour. Such observations raise the question about the eventual state reached by a glass former, if allowed to relax for sufficiently long times. Is a slowly growing crystalline order responsible for slow dynamics? Are the molecular mechanisms for glass transition in liquids with and without MRCO the same? If yes, glass formers with MRCO provide a paradigm for understanding glassy behaviour generically. If not, systems with MRCO form a new class of glass forming materials whose molecular mechanism for slow dynamics may be easier to understand in terms of growing crystalline order, and should be approached in that manner, even while they will not provide generic insights. In this study we perform extensive molecular dynamics simulations of a number of glass forming liquids in two dimensions and show that the static and dynamic properties of glasses with MRCO are different from other glass forming liquids with no predominant local order. We also resolve an important issue regarding the so-called Point-to-set method for determining static length scales, and demonstrate it to be a robust, order agnostic, method for determining static correlation lengths in glass formers.

cond-mat.soft↗

Pinning Susceptibility : A Novel Method to Study Growth of Amorphous Order in Glass-forming Liquids

Existence and growth of amorphous order in supercooled liquids approaching glass transition is a subject of intense research. Even after decades of work, there is still no clear consensus on the molecular mechanisms that lead to a rapid slowing down of liquid dynamics approaching this putative transition. The existence of a correlation length associated with amorphous order has recently been postulated and also been estimated using multi-point correlation functions which cannot be calculated easily in experiments. Thus the study of growing amorphous order remains mostly restricted to systems like colloidal glasses and simulations of model glass-forming liquids. In this Letter, we propose an experimentally realizable yet simple correlation function to study the growth of amorphous order. We then demonstrate the validity of this approach for a few well-studied model supercooled liquids and obtain results which are consistent with other conventional methods.

cond-mat.stat-mech↗

Amorphization of a crystalline solid by plastic deformation

We demonstrate that plastic deformation in solids is associated with a dynamic transition that is reminiscent to the transition from a superconducting to a mixed phase in Type II superconductors. We report analytic calculations, extensive molecular dynamics and sequential umbrella sampling Monte Carlo simulations of a two dimensional triangular crystalline solid undergoing plastic deformation under strain. The solid consists of particles connected by harmonic springs. Non-affine displacement fluctuations of the solid are enhanced using an external field, causing a rich deformation behaviour. The external field leads to a mixed phase, where defect and stress-free crystallites are surrounded by a network of amorphous regions with large local internal stress --- a "stress Meissner" effect. The transition shows slow ageing dynamics caused by the presence of many competing, non-crystalline free-energy minima. Under uniform uniaxial strain, this amorphization transition gives rise to irreversible plastic deformation with the amorphous regions appearing as band-like structures. Our results may be checked by careful experiments on colloidal crystals using holographic optical tweezers.

cond-mat.soft↗

Equilibrium and dynamic pleating of a crystalline bonded network

We describe a phase transition that gives rise to structurally non-trivial states in a two-dimensional ordered network of particles connected by harmonic bonds. Monte Carlo simulations reveal that the network supports, apart from the homogeneous phase, a number of heterogeneous "pleated" phases, which can be stabilised by an external field. This field is conjugate to a global collective variable quantifying "non-affineness", i.e.~the deviation of local particle displacements from local affine deformation. In the pleated phase, stress is localised in ordered rows of pleats and eliminated from the rest of the lattice. The {\em kinetics} of the phase transition is unobservably slow in molecular dynamics simulation near coexistence, due to very large free energy barriers. When the external field is increased further to lower these barriers, the network exhibits rich dynamic behaviour: it transforms into a {\em metastable} phase with the stress now localised in a {\em disordered} arrangement of pleats. The pattern of pleats shows ageing dynamics and slow relaxation to equilibrium. Our predictions may be checked by experiments on tethered colloidal solids in dynamic laser traps.

cond-mat.soft↗

Understanding the Dynamics of Glass-forming Liquids with Random Pinning within the Random First Order Transition Theory

Extensive computer simulations are performed for a few model glass-forming liquids in both two and three dimensions to study their dynamics when a randomly chosen fraction of particles are frozen in their equilibrium positions. For all the studied systems, we find that the temperature-dependence of the $α$ relaxation time extracted from an overlap function related to the self part of the density autocorrelation function can be explained within the framework of the Random First Order Transition (RFOT) theory of the glass transition. We propose a scaling description to rationalize the simulation results and show that our data for the $α$ relaxation time for all temperatures and pin concentrations are consistent with this description. We find that the fragility parameter obtained from fits of the temperature dependence of the $α$ relaxation time to the Vogel-Fulcher-Tammann (VFT) form decreases by almost an order of magnitude as the pin concentration is increased from zero. Our scaling description relates the fragility parameter to the static length scale of RFOT and thus provides a physical understanding of fragility within the framework of the RFOT theory. Implications of these findings for the values of the exponents appearing in the RFOT theory are discussed.

cond-mat.stat-mech↗

Understanding Stokes-Einstein Relation in Supercooled Liquids using Random Pinning

Breakdown of Stokes-Einstein relation in supercooled liquids is believed to be one of the hallmarks of glass transition. The phenomena is studied in depth over many years to understand the microscopic mechanism without much success. Recently it was found that violation of Stokes-Einstein relation in supercooled liquids can be tuned very systematically by pinning randomly a set of particles in their equilibrium positions. This observation suggested a possible framework where breakdown of Stokes-Einstein relation in the dynamics of supercooled liquids can be studied with precise control. We have done extensive molecular dynamics simulations to understand this phenomena by analyzing the structure of appropriately defined set of dynamically slow and fast particles clusters. We have shown that the Stokes-Einstein breakdown actually become predominant once the cluster formed by the slow particles percolate the entire system size. Finally we proposed a possible close connection between fractal dimensions of these clusters and the exponents associated with the fractional Stokes-Einstein relation.

cond-mat.stat-mech↗

The Static Lengthscale Characterizing the Glass Transition at Lower Temperatures

The existence of a static lengthscale that grows in accordance with the dramatic slowing down observed at the glass transition is a subject of intense interest. A recent publication compared two proposals for this length scale, one 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. The conclusion was that both approaches lead to the same lengthscale, but the former is easier to measure at higher temperatures and the latter at lower temperatures. But even after using both methods together, the range of increase in the observed lengthscales was limited by the relaxation times reachable by standard molecular dynamics techniques (i.e. about 4-5 orders of magnitude). In this paper we therefore attempt to explore the typical scale at even lower temperatures, testing for this purpose two approaches, one based on the idea of vapor deposition and the other on a swap Monte Carlo technique. We conclude that the first approach does not help in getting to lower temperatures, but the second one does so quite effectively. We can reach a typical lengthscale that grows in accordance with at least $15$ orders of magnitude increase in the relaxation time, competing with the best experimental conditions. We conclude by discussing the relationship between the observed lengthscale and various models of the relaxation time.

cond-mat.stat-mech↗

Vanishing of configurational entropy may not imply an ideal glass transition in randomly pinned liquids

Ozawa et. al [1] presented numerical results for the configurational entropy density, $s_c$, of a model glass-forming liquid in the presence of random pinning. The location of a "phase boundary" in the pin density ($c$) - temperature ($T$) plane, that separates an "ideal glass" phase from the supercooled liquid phase, is obtained by finding the points at which $s_c(T,c) \to 0$. According to the theoretical arguments by Cammarota et. al. [2], an ideal glass transition at which the $α$-relaxation time $τ_α$ diverges takes place when $s_c$ goes to zero. We have studied the dynamics of the same system using molecular dynamics simulations. We have calculated the time-dependence of the self intermediate scattering function, $F_s(k,t)$ at three state points in the $(c-T)$ plane where $s_c(T,c) \simeq 0$ according to Ref. [1]. It is clear from the plots that the relaxation time is finite [$τ_α\sim \mathcal{O}(10^6)]$ at these state points. Similar conclusions have been obtained in Ref.[3] where an overlap function was used to calculate $τ_α$ at these state points.

cond-mat.stat-mech↗

Excess Vibrational Density of States and the Brittle to Ductile Transition in Crystalline and Amorphous Solids

The conditions which determine whether a material behaves in a brittle or ductile fashion on mechanical loading are still elusive and comprise a topic of active research among materials physicists and engineers. In this study, we present results of {\em in silico} mechanical deformation experiments from two very different model solids in two and three dimensions. The first consists of particles interacting with isotropic potentials and the other has strongly direction dependent interactions. We show that in both cases, the excess vibrational density of states is the fundamental quantity which characterises the ductility of the material. Our results can be checked using careful experiments on colloidal solids.

cond-mat.soft↗

Short-time $β$-relaxation in glass-forming liquids is cooperative in nature

Temporal relaxation of density fluctuations in supercooled liquids near the glass transition occurs in multiple steps. The short-time $β$-relaxation is generally attributed to spatially local processes involving the rattling motion of a particle in the transient cage formed by its neighbors. Using molecular dynamics simulations for three model glass-forming liquids, we show that the $β$-relaxation is actually cooperative in nature. Using finite-size scaling analysis, we extract a growing length-scale associated with $β$-relaxation from the observed dependence of the $β$-relaxation time on the system size. Remarkably, the temperature dependence of this length scale is found to be the same as that of the length scale that describes the spatial heterogeneity of local dynamics in the long-time $α$-relaxation regime. These results show that the conventional interpretation of $β$-relaxation as a local process is too simplified and provide a clear connection between short-time dynamics and long-time structural relaxation in glass-forming liquids.

cond-mat.stat-mech↗