arXiv subjects

Chandan Dasgupta

Publications and source records attributed to Chandan Dasgupta.

At least 55 records · Page 3Linked to original sources

arXiv2016

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↗

arXiv2015

Spatial modulation of the composition of a binary liquid near a repulsive wall

When a binary liquid is confined by a strongly repulsive wall, the local density is depleted near the wall and an interface similar to that between the liquid and its vapor is formed. This analogy suggests that the composition of the binary liquid near this interface should exhibit spatial modulation similar to that near a liquid-vapor interface even if the interactions of the wall with the two components of the liquid are the same. The Guggenheim adsorption relation quantifies the concentrations of two components of a binary mixture near a liquid-vapor interface and qualitatively states that the majority (minority) component enriches the interface for negative (positive) mixing energy if the surface tensions of the two components are not very different. From molecular dynamics simulations of binary mixtures with different compositions and interactions, we find that the Guggenheim relation is qualitatively satisfied at wall-induced interfaces for systems with negative mixing energy at all state points considered. For systems with positive mixing energy, this relation is found to be qualitatively valid at low densities, while it is violated at state points with high density where correlations in the liquid are strong. This observation is validated by a calculation of the density profiles of the two components of the mixture using density functional theory with the Ramakrishnan-Yussouff free-energy functional. Possible reasons for the violation of the Guggenheim relation are discussed.

cond-mat.soft↗

arXiv2015

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↗

arXiv2015

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↗

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↗

arXiv2015

Tunable mechanical and thermal properties of ZnS/CdS core/shell nanowires

Using all atom molecular dynamics (MD) simulations, we have studied the mechanical properties of ZnS/CdS core/shell nanowires. Our results show that the coating of a few atomic layer CdS shell on the ZnS nanowire leads to a significant change in the stiffness of the core/shell nanowires compared to the stiffness of pure ZnS nanowires. The binding energy between the core and shell region decreases due to the lattice mismatch at the core-shell interface. This reduction in binding energy plays an important role in determining the stiffness of a core/shell nanowire. We have also investigated the effects of the shell on the thermal conductivity and melting behavior of the nanowires.

cond-mat.mtrl-sci↗

arXiv2015

Driving force of water entry into hydrophobic channels of carbon nanotubes: entropy or energy?

Spontaneous entry of water molecules inside single-wall carbon nanotubes (SWCNTs) has been confirmed by both simulations and experiments. Using molecular dynamics simulations, we have studied the thermodynamics of filling of a (6,6) carbon nanotube in a temperature range from 273 to 353 K and with different strengths of the nanotube-water interaction. From explicit energy and entropy calculations using the two-phase thermodynamics method, we have presented a thermodynamic understanding of the filling behaviour of a nanotube. We show that both the energy and the entropy of transfer decrease with increasing temperature. On the other hand, scaling down the attractive part of the carbon-oxygen interaction results in increased energy of transfer while the entropy of transfer increases slowly with decreasing the interaction strength. Our results indicate that both energy and entropy favour water entry into (6,6) SWCNTs. Our results are compared with those of several recent studies of water entry into carbon nanotubes.

cond-mat.mes-hall↗

arXiv2014

Nature of the Effective Interaction Between Dendrimers

We have performed fully atomistic classical molecular dynamics (MD) simulations to calculate the effective interaction between two polyamidoamine (PAMAM) dendrimers. Using the umbrella sampling (US) technique, we have obtained the potential of mean force (PMF) between the dendrimers and investigated the effects of protonation level and dendrimer size on the PMF. Our results show that the interaction between the dendrimers can be tuned from purely repulsive to partly attractive by changing the protonation level. The PMF profiles are well-fitted by the sum of an exponential and a Gaussian function with the weight of the exponential function dominating over that of the Gaussian function. This observation is in disagreement with the results obtained in previous analytic [Macromolecules 34, 2914 (2001)] and coarse-grained simulation [J. Chem. Phys. 120, 7761 (2004)] studies which predicted the effective interaction to be Gaussian.

physics.comp-ph↗

arXiv2014

Ising Model on a random network with annealed or quenched disorder

We study the equilibrium properties of an Ising model on a disordered random network where the disorder can be quenched or annealed. The network consists of four-fold coordinated sites connected via variable length one-dimensional chains. Our emphasis is on nonuniversal properties and we consider the transition temperature and other equilibrium thermodynamic properties, including those associated with one dimensional fluctuations arising from the chains. We use analytic methods in the annealed case, and a Monte Carlo simulation for the quenched disorder. Our objective is to study the difference between quenched and annealed results with a broad random distribution of interaction parameters. The former represents a situation where the time scale associated with the randomness is very long and the corresponding degrees of freedom can be viewed as frozen, while the annealed case models the situation where this is not so. We find that the transition temperature and the entropy associated with one dimensional fluctuations are always higher for quenched disorder than in the annealed case. These differences increase with the strength of the disorder up to a saturating value. We discuss our results in connection to physical systems where a broad distribution of interaction strengths is present.

cond-mat.stat-mech↗

arXiv2014

Hydrodynamics of compressible superfluids in confined geometries

We present a study of the hydrodynamics of compressible superfluids in confined geometries. We use a perturbative procedure in terms of the dimensionless expansion parameter $(v/v_s)^2$ where $v$ is the typical speed of the flow and $v_s$ the speed of sound. A zero value of this parameter corresponds to the incompressible limit. We apply the procedure to two specific problems: the case of a trapped superfluid with a gaussian profile of the local density, and that of a superfluid confined in a rotating obstructed cylinder. We find that the corrections due to finite compressibility which are, as expected, negligible for liquid He, are important but amenable to the perturbative treatment for typical ultracold atomic systems.

cond-mat.quant-gas↗

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

Annealing of supersolidity in plastically deformed solid $^4$He

We present a numerical study of a continuum plasticity field coupled to a Ginzburg-Landau model for superfluidity. The results suggest that a supersolid fraction may appear as a long-lived transient during the time evolution of the plasticity field at higher temperatures where both dislocation climb and glide are allowed. Supersolidity, however, vanishes with annealing. As the temperature is decreased, dislocation climb is arrested and any residual supersolidity due to incomplete annealing remains frozen. Our results provide a resolution of many perplexing issues concerning a variety of experiments on solid $^4$He.

cond-mat.mtrl-sci↗

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↗

arXiv2011

Characterization of the Dynamics of Glass-forming Liquids from the Properties of the Potential Energy Landscape

We develop a framework for understanding the difference between strong and fragile behavior in the dynamics of glass-forming liquids from the properties of the potential energy landscape. Our approach is based on a master equation description of the activated jump dynamics among the local minima of the potential energy (the so-called inherent structures) that characterize the potential energy landscape of the system. We study the dynamics of a small atomic cluster using this description as well as molecular dynamics simulations and demonstrate the usefulness of our approach for this system. Many of the remarkable features of the complex dynamics of glassy systems emerge from the activated dynamics in the potential energy landscape of the atomic cluster. The dynamics of the system exhibits typical characteristics of a strong supercooled liquid when the system is allowed to explore the full configuration space. This behavior arises because the dynamics is dominated by a few lowest-lying minima of the potential energy and the potential energy barriers between these minima. When the system is constrained to explore only a limited region of the potential energy landscape that excludes the basins of attraction of a few lowest-lying minima, the dynamics is found to exhibit the characteristics of a fragile liquid.

cond-mat.dis-nn↗

arXiv2010

Phenomenological Ginzburg-Landau-like theory for superconductivity in the cuprates

We propose a phenomenological Ginzburg-Landau-like theory of cuprate superconductivity. The free energy is expressed as a functional F of the spin-singlet pair amplitude psi_ij=psi_m=Delta_m exp(i phi_m); i and j are nearest-neighbor sites of the Cu lattice in which the superconductivity is believed to primarily reside and m labels the site at the center of the bond between i and j. The system is modeled as a weakly coupled stack of such planes. We hypothesize a simple form, F[Delta,phi]=sum_m (A Delta_m^2+ B Delta_m^4/2)+C sum_ Delta_m Delta_n cos(phi_m-phi_n), for the functional. The coefficients A, B and C are determined from comparison with experiments. We work out a number of consequences of the proposed functional for specific choices of A, B and C as functions of hole density x and temperature T. There can be a rapid crossover of from small to large values as A changes sign on lowering T and the crossover temperatures is identified with the observed pseudogap temperature. The superconducting phase-coherence transition occurs at a different temperature T_c, and describes superconductivity with d-wave symmetry for C>0. We calculate T_c(x) which has the observed parabolic shape, being strongly influenced by the coupling between Delta_m and phi_m present in F. The superfluid density, the local gap magnitude, the specific heat (with and without a magnetic field) and vortex properties are obtained using F. We compare our results successfully with experiments. We also obtain the electron spectral density as influenced by the coupling between the electrons and the pair correlation function calculated from F. Features such as temperature dependent Fermi arcs, antinodal pseudogap filling temperature, pseudogapped density of states in different momentum regions of the Fermi surface and `bending' of the energy gap versus momentum on the Fermi surface emerge from the theory.

cond-mat.supr-con↗

arXiv2010

Non-classical Rotational Inertia in a Two-dimensional Bosonic Solid Containing Grain Boundaries

We study the occurrence of non-classical rotational inertia (NCRI) arising from superfluidity along grain boundaries in a two-dimensional bosonic system. We make use of a standard mapping between the zero-temperature properties of this system and the statistical mechanics of interacting vortex lines in the mixed phase of a type-II superconductor. In the mapping, the liquid phase of the vortex system corresponds to the superfluid bosonic phase. We consider numerically obtained polycrystalline configurations of the vortex lines in which the microcrystals are separated by liquid-like grain boundary regions which widen as the vortex system temperature increases. The NCRI of the corresponding zero-temperature bosonic systems can then be numerically evaluated by solving the equations of superfluid hydrodynamics in the channels near the grain boundaries. We find that the NCRI increases very abruptly as the liquid regions in the vortex system (equivalently, superfluid regions in the bosonic system) form a connected, system-spannig structure with one or more closed loops. The implications of these results for experimentally observed supersolid phenomena are discussed.

cond-mat.quant-gas↗

arXiv2010

Banded spatiotemporal chaos in sheared nematogenic fluids

We present the results of a numerical study of a model of the hydrodynamics of a sheared nematogenic fluid, taking into account the effects of order parameter stresses on the velocity profile, but allowing spatial variations only in the gradient direction. When parameter values are such that the stress from orientational distortions is comparable to the bare viscous stress, the system exhibits steady states with the characteristics of shear banding. In addition, nonlinearity in the coupling of extensional flow to orientation leads to the appearance of a new steady state in which the features of both spatiotemporal chaos and shear banding are present.

cond-mat.soft↗

arXiv2009

The phase diagram of vortex matter in layered superconductors with tilted columnar pinning centers

We study the vortex matter phase diagram of a layered superconductor in the presence of columnar pinning defects, {\it tilted} with respect to the normal to the layers. We use numerical minimization of the free energy written as a functional of the time averaged vortex density of the Ramakrishnan-Yussouff form, supplemented by the appropriate pinning potential. We study the case where the pin density is smaller than the areal vortex density. At lower pin concentrations, we find, for temperatures of the order of the melting temperature of the unpinned lattice, a Bose glass type phase which at lower temperatures converts, via a first order transition, to a Bragg glass, while, at higher temperatures, it crosses over to an interstitial liquid. At somewhat higher concentrations, no transition to a Bragg glass is found even at the lowest temperatures studied. While qualitatively the behavior we find is similar to that obtained using the same procedures for columnar pins normal to the layers, there are important and observable quantitative differences, which we discuss.

cond-mat.supr-con↗