arXiv subjects

Smarajit Karmakar

Publications and source records attributed to Smarajit Karmakar.

At least 55 records · Page 3Linked to original sources

arXiv2022

A Novel Method to Probe the Pronounced Growth of Correlation Lengths in an Active Glass-forming Liquids using Elongated Probe

The growth of correlation lengths in equilibrium glass-forming liquids near the glass transition is considered a critical finding in the quest to understand the physics of glass formation. These understandings helped us understand various dynamical phenomena observed in supercooled liquids. It is known that at least two different length scales exist - one is of thermodynamic origin, while the other is dynamical in nature. Recent observations of glassy dynamics in biological and synthetic systems where the external or internal driving source controls the dynamics, apart from the usual thermal noise, led to the emergence of the field of active matter. A question of whether the physics of glass formation in these active systems is also accompanied by growing dynamic and static lengths is indeed timely. In this article, we probe the growth of dynamic and static lengths in a model active glass system using rod-like elongated probe particles, an experimentally viable method. We show that the dynamic and static lengths in these non-equilibrium systems grow much more rapidly than their passive counterparts. We then offer an understanding of the violation of the Stokes-Einstein relation and Stokes-Einstein-Debye relation using these lengths via a scaling theory.

cond-mat.soft↗

arXiv2022

Dependence of the glass transition and jamming densities on spatial dimension

We investigate the dynamics of soft sphere liquids through computer simulations for spatial dimensions from $d =3$ to $8$, over a wide range of temperatures and densities. Employing a scaling of density-temperature dependent relaxation times, we precisely identify the density $ϕ_0$ which marks the ideal glass transition in the hard sphere limit, and a crossover from sub- to super-Arrhenius temperature dependence. The difference between $ϕ_0$ and the athermal jamming density $ϕ_J$, small in 3 and 4 dimensions, increases with dimension, with $ϕ_0 > ϕ_J$ for $d > 4$. We compare our results with recent theoretical calculations.

cond-mat.soft↗

arXiv2021

Enhanced Phonon Peak in Four-point Dynamic Susceptibility in the Supercooled Active Glass-forming Liquids

Active glassy systems can be thought of as simple model systems that imitate complex biological systems. Sometimes, it becomes crucial to estimate the amount of the activity present in such biological systems, such as predicting the progression rate of the cancer cells or the healing time of the wound. In this work, we study a model active glassy system to understand a possible quantification of the degree of activity from the collective, long-range phonon response in the system. We find that the four-point dynamic susceptibility, $χ_4(t)$ at the phonon timescale, grows with increased activity. We then show how one can estimate the degree of the activity at such a small timescale by measuring the growth of $χ_4(t)$ with changing activity. A detailed finite size analysis of this measurement, shows that the peak height of $χ_4(t)$ at this phonon timescale increases strongly with increasing system size suggesting a possible existence of an intrinsic dynamic length scale that grows with increasing activity. Finally, we show that this peak height is a unique function of effective activity across all system sizes, serving as a possible parameter for characterizing the degree of activity in a system.

cond-mat.soft↗

arXiv2021

Annealing effects of multidirectional oscillatory shear in model glass formers

We study the effects of cyclic, athermal quasi-static shear on a model glass-forming system in three dimensions. We utilize the three available orthogonal shear planes, namely $XY, YZ \text{ and } XZ$ to better explore the energy landscape. Using measurements of the stroboscopic $(γ= 0)$ energy, we study the effects of using an orthogonal shear direction to perturb unidirectional steady-states. We find that that each sequence of the unidirectional protocol leads to compaction with the universal, $ΔE \sim N^{-1}$ behavior as a function of the number of cycles, $N$. Additionally we find that cyclic shear utilizing multiple shear planes presents hierarchical compaction, producing progressively lower steady state energies compared to a protocol involving unidirectional cyclic shear alone. Furthermore, with the periodicity of the stroboscopic energy as reference, we show that it is possible to achieve steady state limit-cycles of tunable periodicities using different combinations of the three orthogonal strain directions. We find that such protocols exhibit better annealing as compared to protocols with steady states created using unidirectional shear. Importantly, we find a non-trivial trend in the annealing energy and the period of the steady-state limit-cycle, with an aperiodic protocol appearing to produce the most well annealed states. Finally, we compare the phase diagram of the average steady state energy $\langle E_{\text{S.S.}} \rangle$, as a function of the shearing amplitude $γ_{\max}$, using unidirectional and multidirectional protocols, and find that the universal features are preserved.

cond-mat.dis-nn↗

arXiv2021

Universal non-Debye low-frequency vibrations in sheared amorphous solids

We study energy minimized configurations of amorphous solids with a simple shear degree of freedom. We show that the low-frequency regime of the vibrational density of states of structural glass formers is crucially sensitive to the stress-ensemble from which the configurations are sampled. In both two and three dimensions, a shear-stabilized ensemble displays a $D(ω_{\min}) \sim ω^{5}_{\min}$ regime, as opposed to the $ω^{4}_{\min}$ regime observed under unstrained conditions. We also study an ensemble of two dimensional, strained amorphous solids near a plastic event. We show that the minimum eigenvalue distribution at a strain $γ$ near the plastic event occurring at $γ_{P}$, displays a collapse when scaled by $\sqrt{γ_P - γ}$, and with the number of particles as $N^{-0.22}$. Notably, at low-frequencies, this scaled distribution displays a robust $D(ω_{\min}) \sim ω^{6}_{\min}$ power-law regime, which survives in the large $N$ limit. Finally, we probe the universal properties of this ensemble through a characterization of the second and third eigenvalues of the Hessian matrix near a plastic event.

cond-mat.dis-nn↗

arXiv2021

Non-trivial activity dependence of static length scale and critical tests of active random first-order transition theory

Effects of activity on glassy dynamics are fundamental in several biological processes. Active glasses extend the scope of the equilibrium problem and provide new control parameters to probe different theoretical aspects. In the theory of glassy dynamics, different length scales play pivotal roles. Here, for the first time, we present results for the static length scale, $ξ_S$, in an active glass via large-scale molecular dynamics simulations for model active glasses in three spatial dimensions. We show that although the relaxation dynamics are equilibrium-like, activity has non-trivial effects on $ξ_S$. $ξ_S$ plays the central role in the random first-order transition (RFOT) theory. Thus, our work provides critical tests for the active RFOT theory, a phenomenological extension of its equilibrium counterpart. We find that the two exponents, $θ$ and $ψ$, within the theory, become activity-dependent, exposing the non-trivial effects of activity on $ξ_S$. However, the combination of $θ$ and $ψ$, which controls the relaxation dynamics, remains nearly independent of activity leading to the effectively equilibrium-like behavior. Interestingly, $ξ_S$ shows higher growth in an active glass; this should help better comparison of theories with simulations and experiments.

cond-mat.soft↗

arXiv2021

Universal mechanical instabilities in the energy landscape of amorphous solids: evidence from athermal quasistatic expansion

Using numerical simulations, we study the failure of an amorphous solid under quasi-static expansion starting from a homogeneous high-density state. During the volume expansion, we demonstrate the existence of instabilities manifesting via saddle-node bifurcation in which a minimum meets a saddle. During all such events, the smallest eigenvalue of the Hessian matrix vanishes as a square-root singularity. The plastic instabilities are manifested via sudden jumps in pressure and energy, with the largest event happening when a cavity appears, leading to the yielding of the material. We show that during cavitation and prior to complete fracture, the statistics of pressure or energy jumps corresponding to the plastic events show sub-extensive finite-size scaling, similar to the case of simple shear but with different exponents. Thus, overall, our study reveals universality in the fundamental characteristics during mechanical failure in amorphous solids under any quasi-static deformation protocol.

cond-mat.soft↗

arXiv2021

Spatial Dimensionality Dependence of Heterogeneity, Breakdown of the Stokes-Einstein Relation and Fragility of a Model Glass-Forming Liquid

We investigate the heterogeneity of dynamics, the breakdown of the Stokes-Einstein relation and fragility in a model glass forming liquid, a binary mixture of soft spheres with a harmonic interaction potential, for spatial dimensions from 3 to 8. Dynamical heterogeneity is quantified through the dynamical susceptibility $χ_4$, and the non-Gaussian parameter $α_2$. We find that the fragility, the degree of breakdown of the Stokes-Einstein relation, as well as heterogeneity of dynamics, decrease with increasing spatial dimensionality. We briefly describe the dependence of fragility on density, and use it to resolve an apparent inconsistency with previous results.

cond-mat.soft↗

arXiv2021

Kinetic Fragility Directly Correlates with the Many-body Static Amorphous Order in Glass-Forming Liquids

The term "fragility" describes the rate at which viscosity grows when a supercooled liquid approaches its putative glass transition temperature. The field of glassy materials is actively searching for a structural origin that governs this dynamical slowing down in the supercooled liquid, which occurs without any discernible change in structure. Our work shows clear evidence that growing many-body static amorphous order is intimately correlated with the kinetic fragility of glass-forming liquids. It confirms that the system's dynamical response to temperature is concealed in its micro-structures. This finding may pave the way for a deeper understanding of the different temperature dependence of the relaxation time or viscosity in a wide variety of glass-forming liquids.

cond-mat.soft↗

arXiv2021

Thermodynamics and its correlation with dynamics in a mean-field model and pinned systems: A comparative study using two different methods of entropy calculation

Recently, some of us developed a novel model glass-forming liquid with k extra interactions with pseudo neighbours to each liquid particle over and above the regular interactions with its neighbours. Analysis of the structure and dynamics of these systems showed that with an increase in k the systems have more mean-field like properties. This work presents an extensive study of the thermodynamics of the above-mentioned model for several values of k and its correlation with the dynamics. We surprisingly find that the usual thermodynamic integration (TI) method of calculating the entropy provides unphysical results for this model. It predicts the vanishing of configurational entropy at state points at which both the collective and the single-particle dynamics of the system show complete relaxation. We then employ a new method known as the two-phase thermodynamics (2PT) method to calculate the entropy. We find that with an increase in k the difference in the entropy computed using the two methods (2PT and TI) increases. We also find that in the temperature range studied, the entropy calculated via the 2PT method satisfies the Adam-Gibbs (AG) relationship between the relaxation time and the configurational entropy, whereas the entropy calculated via the TI method shows a strong violation of the same. We then apply the 2PT method to calculate the entropy in another system where some fractions of particles are pinned randomly in their equilibrium positions. This system also shows a similar breakdown of the AG relationship as reported earlier. We show that the difference in entropy calculated via the 2PT and TI methods increases with an increase in pinning density. We also find that when the entropy is calculated using the 2PT method, the AG relationship between the dynamics and the entropy holds.

cond-mat.soft↗

arXiv2021

Soft-Pinning: Experimental Validation of Static Correlations in Supercooled Molecular Glass-forming Liquids

Enormous enhancement in the viscosity of a liquid near its glass transition is generally connected to the growing many-body static correlations near the transition, often coined as `amorphous ordering'. Estimating the length scales of such correlations in different glass-forming liquids is highly important to unravel the physics of glass formation. Experiments on molecular glass-forming liquids become pivotal in this scenario as the viscosity grows several folds ($\sim 10^{14}$), simulations or colloidal glass experiments fail to access the long-time scales required. Here we design an experiment to extract the static length scales in molecular liquids using dilute amounts of another large molecule as a pinning site. Results from dielectric relaxation experiments on supercooled glycerol with different pinning concentrations of sorbitol and the simulations on a few model glass-forming liquids with pinning sites indicate the robustness of the proposed method, opening a plethora of opportunity to study the physics of other glass-forming liquids.

cond-mat.soft↗

arXiv2021

Translational Dynamics of Rod-like Particles in Supercooled Liquids: Probing Dynamic Heterogeneity and Amorphous Order

The use of probe molecules to extract the local dynamical and structural properties of complex dynamical systems is an age-old technique both in simulations and experiments. A lot of important information which is not immediately accessible from the bulk measurements can be accessed via these local measurements. Still, a detailed understanding of how a probe particle's dynamics are affected by the surrounding liquid medium is not very well understood, especially in the supercooled temperature regime. This work shows how translational dynamics of a rod-like particle immersed in a supercooled liquid can give us information on the growth of the correlation length scale associated with dynamical heterogeneity and the multi-body static correlations in the medium. A unified scaling theory rationalizes all the observed results leading to the development of a novel yet simple method that is accessible in experiments to measure the growth of these important length-scales in molecular glass-forming liquids.

cond-mat.soft↗

arXiv2020

Singularities in Hessian element distributions of amorphous media

We show that the distribution of elements $H$ in the Hessian matrices associated with amorphous materials exhibit singularities $P(H) \sim {\lvert H \rvert}^γ$ with an exponent $γ< 0$, as $\lvert H \rvert \to 0$. We exploit the rotational invariance of the underlying disorder in amorphous structures to derive these exponents exactly for systems interacting via radially symmetric potentials. We show that $γ$ depends only on the degree of smoothness $n$ of the potential of interaction between the constituent particles at the cut-off distance, independent of the details of interaction in both two and three dimensions. We verify our predictions with numerical simulations of models of structural glass formers. Finally, we show that such singularities affect the stability of amorphous solids, through the distributions of the minimum eigenvalue of the Hessian matrix.

cond-mat.dis-nn↗

arXiv2020

Dynamics of Rod like Particles in Supercooled Liquids -- Probing Dynamic Heterogeneity and Amorphous Order

Probing dynamic and static correlation in glass-forming supercooled liquids has been a challenge for decades in spite of extensive research. Dynamic correlation which manifests itself as Dynamic Heterogeneity is ubiquitous in a vast variety of systems starting from molecular glass-forming liquids, dense colloidal systems to collections of cells. On the other hand, the mere concept of static correlation in these dense disordered systems remain somewhat elusive and its existence is still actively debated. We propose a novel method to extract both dynamic and static correlations using rod-like particles as probe. This method can be implemented in molecular glass-forming liquids in experiments as well as in other soft matter systems including biologically relevant systems. We also rationalize the observed log-normal like distribution of rotational decorrelation time of elongated probe molecules in reported experimental studies along with a proposal of a novel methodology to extract dynamic and static correlation lengths in experiments.

cond-mat.stat-mech↗

arXiv2019

Time Scales of Fickian Diffusion and the Lifetime of Dynamic Heterogeneity

Dynamic heterogeneity, believed to be one of the hallmarks of the dynamics of supercooled liquids, is expected to affect the diffusion of the particles comprising the liquid. We have carried out extensive molecular dynamics simulations of two model glass-forming liquids in three dimensions to study the time scales at which Fick's law of diffusion starts to set in. We have identified two different Fickian timescales: one at which the mean squared displacement begins to show a linear dependence on time, and another one at which the distribution of particle displacements becomes Gaussian. These two times scales are found to be very different from each other and from the $α$ relaxation time in both systems. An interesting connection is found between one of these Fickian time scales and the time scale obtained from the bond-breakage correlation function. We discuss the relationships between these different timescales and their connection to dynamic heterogeneity in the system.

cond-mat.soft↗

arXiv2019

Particle pinning suppresses spinodal criticality in the shear banding instability

Strained amorphous solids often fail mechanically by creating a shear-band. It had been understood that the shear banding instability is usefully described as crossing a spinodal point (with disorder) in an appropriate thermodynamic description. It remained contested however whether the spinodal is critical (with divergent correlation length) or not. Here we offer evidence for critical spinodal by using particle pinning. For a finite concentration of pinned particles the correlation length is bounded by the average distance between pinned particles, but without pinning it is bounded by the system size.

cond-mat.soft↗

arXiv2019

Geometry-controlled Failure Mechanisms of Amorphous Solids on the Nanoscale

Amorphous solids, confined on the nano-scale, exhibit a wealth of novel phenomena yet to be explored. In particular, the response of such solids to a mechanical load is not well understood and, as has been demonstrated experimentally, it differs strongly from bulk samples made of the same materials. Failure patterns and mechanisms are strongly affected by the geometry of the confinement and the interplay between interfacial effects in the sample and the time scale, imposed by an external mechanical field. Here, we present the mechanism of cavity formation in a confined model glass, subjected to expansion with a constant strain rate. This system is studied for varying geometric aspect ratio and sample size. Our results show that for a given temperature and straining condition, the sample shows cavitation when the aspect ratio reaches a critical value and below this aspect ratio the sample breaks by forming a neck. The critical aspect ratio is associated with a critical curvature of the neck that depends on strain rate and temperature. If this critical curvature is exceeded, the free energy of the system is minimized by the formation of a cavity. Our study reveals a novel mechanism of cavity formation on the nanoscale. This is probably a generic mechanism for material's failure in small confined systems under mechanical load.

cond-mat.stat-mech↗

arXiv2019

Signature of Dynamical Heterogeneity in Spatial Correlations of Particle Displacement and its Temporal Evolution in Supercooled Liquids

The existence of heterogeneity in the dynamics of supercooled liquids is believed to be one of the hallmarks of the glass transition. Intense research has been carried out in the past to understand the origin of this heterogeneity in dynamics and a possible length scale associated with it. We have done extensive molecular dynamics simulations of few model glass-forming liquids in three dimensions to understand the temporal evolution of the dynamic heterogeneity and the heterogeneity length scale. We find that although the strength of the dynamic heterogeneity is maximum at a timescale close to characteristic $α$-relaxation time of the system, dynamic heterogeneity itself is well-developed at timescale as short as $β$-relaxation time and survives up to a timescale as long as few tens of $α$-relaxation time. Moreover, we discovered that temperature dependence of heterogeneity length remains the same in the whole time window although its absolute value changes over time in a non-monotonic manner.

cond-mat.soft↗