@article { ISI:000325780800062, title = {Interplay between crystallization and glass transition in binary lennard-Jones mixtures (vol 139, 104501, 2013)}, journal = {Journal of Chemical Physics}, volume = {139}, number = {14}, year = {2013}, month = {OCT}, pages = {Article No. 149902}, publisher = {AMER INST PHYSICS}, type = {Article}, address = {CIRCULATION \& FULFILLMENT DIV, 2 HUNTINGTON QUADRANGLE, STE 1 N O 1, MELVILLE, NY 11747-4501 USA}, issn = {0021-9606}, doi = {10.1063/1.4824740}, author = {Banerjee, Atreyee and Chakraborty, Suman and Bhattacharyya, Sarika Maitra} } @article { ISI:000324387400035, title = {Interplay between crystallization and glass transition in binary Lennard-Jones mixtures}, journal = {Journal of Chemical Physics}, volume = {139}, number = {10}, year = {2013}, month = {SEP}, pages = {Article No. 104501}, publisher = {AMER INST PHYSICS}, type = {Article}, address = {CIRCULATION \& FULFILLMENT DIV, 2 HUNTINGTON QUADRANGLE, STE 1 N O 1, MELVILLE, NY 11747-4501 USA}, abstract = {

In this work we explore the interplay between crystallization and glass transition in different binary mixtures by changing their inter-species interaction length and also the composition. We find that only those systems which form bcc crystal in the equimolar mixture and whose global structure for larger x(A) (x(A) = 0.6, where x(A) is the mole fraction of the bigger particles) is a mixed fcc + bcc phase, do not crystallize at this higher composition. However, the systems whose equimolar structure is a variant of fcc (NaCl type crystal) and whose global structure at larger xA is a mixed NaCl + fcc phase, crystallize easily to this mixed structure. We find that the stability against crystallization of this {\textquoteleft}{\textquoteleft}bcc zone{\textquoteright}{\textquoteright} is due to the frustration between the locally preferred structure (LPS) and the mixed bcc + fcc crystal. Our study suggests that when the global structure is a mixed crystal where a single species contributes to both the crystal forms and where the two crystal forms have large difference in some order parameter related to that species then this induces frustration between the LPS and the global structure. This frustration makes the systems good glass former. When x(A) is further increased (0.70 \<= x(A) \< 0.90) the systems show a tendency towards mixed fcc crystal formation. However, the {\textquoteleft}{\textquoteleft}bcc zone{\textquoteright}{\textquoteright} even for this higher composition is found to be sitting at the bottom of a V shaped phase diagram formed by two different variants of the fcc crystal structure, leading to its stability against crystallization. (C) 2013 AIP Publishing LLC.

}, issn = {0021-9606}, doi = {10.1063/1.4820402}, author = {Banerjee, Atreyee and Chakrabarty, Suman and Bhattacharyya, Sarika Maitra} } @article { ISI:000316969500085, title = {Non-monotonic size dependence of diffusion and levitation effect: a mode-coupling theory analysis}, journal = {Journal of Chemical Physics}, volume = {138}, number = {12}, year = {2013}, month = {MAR}, pages = {124505}, publisher = {AMER INST PHYSICS}, type = {Article}, address = {CIRCULATION \& FULFILLMENT DIV, 2 HUNTINGTON QUADRANGLE, STE 1 N O 1, MELVILLE, NY 11747-4501 USA}, abstract = {

We present a study of diffusion of small tagged particles in a solvent, using mode coupling theory (MCT) analysis and computer simulations. The study is carried out for various interaction potentials. For the first time, using MCT, it is shown that only for strongly attractive interaction potential with allowing interpenetration between the solute-solvent pair the diffusion exhibits a non-monotonic solute size dependence which has earlier been reported in simulation studies [P. K. Ghorai and S. Yashonath, J. Phys. Chem. B 109, 5824-5835 (2005)]. For weak attractive and repulsive potential the solute size dependence of diffusion shows monotonic behaviour. It is also found that for systems where the interaction potential does not allow solute-solvent interpenetration, the solute cannot explore the neck of the solvent cage. Thus these systems even with strong attractive interaction will never show any non-monotonic size dependence of diffusion. This non-monotonic size dependence of diffusion has earlier been connected to levitation effect [S. Yashonath and P. Santikary, J. Phys. Chem. 98, 6368 (1994)]. We also show that although levitation is a dynamic phenomena, the effect of levitation can be obtained in the static radial distribution function. (C) 2013 American Institute of Physics. [http://dx.doi.org/10.1063/1.4796232]

}, issn = {0021-9606}, doi = {10.1063/1.4796232}, author = {Nandi, Manoj Kumar and Banerjee, Atreyee and Bhattacharyya, Sarika Maitra} } @article { ISI:000350657700011, title = {Role of structure and entropy in determining differences in dynamics for glass formers with different interaction potentials}, journal = {Physical Review Letters}, volume = {113}, number = {22}, year = {2014}, month = {NOV}, pages = {225701}, publisher = {AMER PHYSICAL SOC}, address = {ONE PHYSICS ELLIPSE, COLLEGE PK, MD 20740-3844 USA}, abstract = {

We present a study of two model liquids with different interaction potentials, exhibiting similar structure but significantly different dynamics at low temperatures. By evaluating the configurational entropy, we show that the differences in the dynamics of these systems can be understood in terms of their thermodynamic differences. Analyzing their structure, we demonstrate that differences in pair correlation functions between the two systems, through their contribution to the entropy, dominate the differences in their dynamics, and indeed overestimate the differences. Including the contribution of higher order structural correlations to the entropy leads to smaller estimates for the relaxation times, as well as smaller differences between the two studied systems.

}, issn = {0031-9007}, doi = {10.1103/PhysRevLett.113.225701}, author = {Banerjee, Atreyee and Sengupta, Shiladitya and Sastry, Srikanth and Bhattacharyya, Sarika Maitra} } @article { ISI:000364585200026, title = {Unraveling the success and failure of mode coupling theory from consideration of entropy}, journal = {Journal of Chemical Physics}, volume = {143}, number = {17}, year = {2015}, month = {NOV}, pages = {174504}, publisher = {AMER INST PHYSICS}, address = {1305 WALT WHITMAN RD, STE 300, MELVILLE, NY 11747-4501 USA}, abstract = {

We analyze the dynamics of model supercooled liquids in a temperature regime where predictions of mode coupling theory (MCT) are known to be valid qualitatively. In this regime, the Adam-Gibbs (AG) relation, based on an activation picture of dynamics, also describes the dynamics satisfactorily, and we explore the mutual consistency and interrelation of these descriptions. Although entropy and dynamics are related via phenomenological theories, the connection between MCT and entropy has not been argued for. In this work, we explore this connection and provide a microscopic derivation of the phenomenological Rosenfeld theory. At low temperatures, the overlap between the MCT power law regime and AG relation implies that the AG relation predicts an avoided divergence at T-c, the origin of which can be related to the vanishing of pair configurational entropy, which we find occurring at the same temperature. We also show that the residual multiparticle entropy plays an important role in describing the relaxation time. (C) 2015 AIP Publishing LLC.

}, issn = {0021-9606}, doi = {10.1063/1.4934986}, author = {Nandi, Manoj Kumar and Banerjee, Atreyee and Sengupta, Shiladitya and Sastry, Srikanth and Bhattacharyya, Sarika Maitra} } @article { ISI:000381384300031, title = {Composition dependence of the glass forming ability in binary mixtures: the role of demixing entropy}, journal = {Journal of Chemical Physics}, volume = {145}, number = {3}, year = {2016}, month = {JUL}, pages = {Article Number: 034503}, publisher = {AMER INST PHYSICS}, address = {1305 WALT WHITMAN RD, STE 300, MELVILLE, NY 11747-4501 USA}, abstract = {

We present a comparative study of the glass forming ability of binary systems with varying composition, where the systems have similar global crystalline structure (CsCl+fcc). Biased Monte Carlo simulations using umbrella sampling technique show that the free energy cost to create a CsCl nucleus increases as the composition of the smaller particles is decreased. We find that systems with comparatively lower free energy cost to form CsCl nucleus exhibit more pronounced pre-crystalline demixing near the liquid/crystal interface. The structural frustration between the CsCl and fcc crystal demands this demixing. We show that closer to the equimolar mixture, the entropic penalty for demixing is lower and a glass forming system may crystallize when seeded with a nucleus. This entropic penalty as a function of composition shows a non-monotonic behaviour with a maximum at a composition similar to the well known Kob-Anderson (KA) model. Although the KA model shows the maximum entropic penalty and thus maximum frustration against CsCl formation, it also shows a strong tendency towards crystallization into fcc lattice of the larger {\textquoteleft}{\textquoteleft}A{\textquoteright}{\textquoteright} particles which can be explained from the study of the energetics. Thus for systems closer to the equimolar mixture although it is the requirement of demixing which provides their stability against crystallization, for KA model it is not demixing but slow dynamics and the presence of the {\textquoteleft}{\textquoteleft}B{\textquoteright}{\textquoteright} particles make it a good glass former. The locally favoured structure around {\textquoteleft}{\textquoteleft}B{\textquoteright}{\textquoteright} particles is quite similar to the CsCl structure and the incompatibility of CsCl and fcc hinders the fcc structure growth in the KA model. Although the glass forming binary systems studied here are quite similar, differing only in composition, we find that their glass forming ability cannot be attributed to a single phenomenon. Published by AIP Publishing.

}, issn = {0021-9606}, doi = {10.1063/1.4958630}, author = {Nandi, Ujjwal Kumar and Banerjee, Atreyee and Chakrabarty, Suman and Bhattacharyya, Sarika Maitra} } @article { ISI:000381384300030, title = {Effect of total and pair configurational entropy in determining dynamics of supercooled liquids over a range of densities}, journal = {Journal of Chemical Physics}, volume = {145}, number = {3}, year = {2016}, month = {JUL}, pages = {Article Number: 034502}, publisher = {AMER INST PHYSICS}, address = {1305 WALT WHITMAN RD, STE 300, MELVILLE, NY 11747-4501 USA}, abstract = {

In this paper, we present a study of supercooled liquids interacting with the Lennard Jones potential and the corresponding purely repulsive (Weeks-Chandler-Andersen) potential, over a range of densities and temperatures, in order to understand the origin of their different dynamics in spite of their structures being similar. Using the configurational entropy as the thermodynamic marker via the Adam Gibbs relation, we show that the difference in the dynamics of these two systems at low temperatures can be explained from thermodynamics. At higher densities both the thermodynamical and dynamical difference between these model systems decrease, which is quantitatively demonstrated in this paper by calculating different parameters. The study also reveals the origin of the difference in pair entropy despite the similarity in the structure. Although the maximum difference in structure is obtained in the partial radial distribution function of the B type of particles, the rdf of AA pairs and AB pairs gives rise to the differences in the entropy and dynamics. This work supports the observation made in an earlier study [A. Banerjee et al., Phys. Rev. Lett. 113, 225701 (2014)] and shows that they are generic in nature, independent of density. Published by AIP Publishing.

}, issn = {0021-9606}, doi = {10.1063/1.4958627}, author = {Banerjee, Atreyee and Nandi, Manoj Kumar and Sastry, Srikanth and Bhattacharyya, Sarika Maitra} } @article {43845, title = {Determination of onset temperature from the entropy for fragile to strong liquids}, journal = {Journal of Chemical Physics}, volume = {147}, year = {2017}, month = {JUL}, pages = {Article Number: 024504}, type = {Article}, abstract = {

In this paper, we establish a connection between the onset temperature of glassy dynamics with the change in the entropy for a wide range of model systems. We identify the crossing temperature of pair and excess entropies as the onset temperature. Below the onset temperature, the residual multiparticle entropy, the difference between excess and pair entropies, becomes positive. The positive entropy can be viewed as equivalent to the larger phase space exploration of the system. The new method of onset temperature prediction from entropy is less ambiguous, as it does not depend on any fitting parameter like the existing methods. Published by AIP Publishing.

}, doi = {10.1063/1.4991848}, author = {Banerjee, Atreyee and Nandi, Manoj Kumar and Sastry, Srikanth and Bhattacharyya, Sarika Maitra} } @article {44109, title = { Role of the pair correlation function in the dynamical transition predicted by mode coupling theory}, journal = {Physical Review Letters}, volume = {119}, year = {2017}, month = {DEC}, type = {Article}, abstract = {In a recent study, we have found that for a large number of systems the configurational entropy at the pair level S-c2, which is primarily determined by the pair correlation function, vanishes at the dynamical transition temperature T-c. Thus, it appears that the information of the transition temperature is embedded in the structure of the liquid. In order to investigate this, we describe the dynamics of the system at the mean field level and, using the concepts of the dynamical density functional theory, show that the dynamical transition temperature depends only on the pair correlation function. Thus, this theory is similar in spirit to the microscopic mode coupling theory (MCT). However, unlike microscopic MCT, which predicts a very high transition temperature, the present theory predicts a transition temperature that is similar to T-c. This implies that the information of the dynamical transition temperature is embedded in the pair correlation function.}, doi = {10.1103/PhysRevLett.119.265502}, author = {Nandi, Manoj Kumar and Banerjee, Atreyee and Dasgupta, Chandan and Bhattacharyya, Sarika Maitra} } @article {43859, title = {Validity of the Rosenfeld relationship: a comparative study of the network forming NTW model and other simple liquids}, journal = {Journal of Chemical Sciences}, volume = {129}, year = {2017}, month = {JUL}, pages = {793-800}, type = {Article}, abstract = {In this paper we explore the validity of the Rosenfeld and the Dzugutov relation for the Lennard-Jones (LJ) system, its repulsive counterpart, the WCA system and a network forming liquid, the NTW model. We find that for all the systems both the relations are valid at high temperature regime with an universal exponent close to 0.8. Similar to that observed for the simple liquids, the LJ and the WCA systems show a breakdown of the scaling laws at the low temperature regime. However for the NTW model, which is a simple liquid, these scaling laws are valid even at lower temperature regime similar to that found for ionic melts. Thus we find that the NTW model has mixed characteristics of simple liquids and ionic melts. Our study further reveals a quantitative relationship between the Rosenfeld and the Arrhenius relations. For strong liquids, the validity of the Rosenfeld relation in the low temperature regime is connected to it following the Arrhenius behaviour in that regime. Finally we explore the role of pair entropy and residual multiparticle entropy in the dynamics as a function of fragility of the systems.}, doi = {10.1007/s12039-0}, author = {Banerjee, Atreyee and Nandi, Manoj Kumar and Bhattacharyya, Sarika Maitra} }