385 research outputs found
The random first-order transition theory of active glass in the high-activity regime
No full textAbstractDense active matter, in the fluid or amorphous-solid form, has generated intense interest as a model for the dynamics inside living cells and multicellular systems. An extension of the random first-order transition theory (RFOT) to include activity was developed, whereby the activity of the individual particles was added to the free energy of the system in the form of the potential energy of an active particle, trapped by a harmonic potential that describes the effective confinement by the surrounding medium. This active-RFOT model was shown to successfully account for the dependence of the structural relaxation time in the active glass, extracted from simulations, as a function of the activity parameters: the magnitude of the active force (f
0) and its persistence time (τ
p
). However, significant deviations were found in the limit of large activity (large f
0 and/or τ
p
). Here we extend the active-RFOT model to high activity using an activity-dependent harmonic confining potential, which we solve self-consistently. The extended model predicts qualitative changes in the high activity regime, which agree with the results of simulations in both three-dimensional and two-dimensional models of active glass.Department of Atomic Energy, Government of Indiahttps://doi.org/10.13039/501100001502Marie Sklodowska-Curie Actionshttps://doi.org/10.13039/10001869
Numerical Studies Of Slow Dynamics And Glass Transition In Model Liquids
No full textAn increase in the co-operativity in the motion of particles and a growth of a suitably defined dynamical correlation length seem to be generic features exhibited by all liquids upon supercooling. These features have been observed both in experiments and in numerical simulations of glass-forming liquids. Specially designed NMR experiments have estimated that the rough magnitude of this correlation length is of the order of a few nanometers near the glass transition. Simulations also predict that there are regions in the system which are more liquid-like than other regions. A complete theoretical understanding of this behaviour is not available at present. In recent calculations, Berthier, Biroli and coworkers [1, 2] extended the simple mode coupling theory (MCT) to incorporate the effects of dynamic heterogeneity and predicted the existence of a growing dynamical correlation length associated with the cooperativity of the dynamics. MCT also predicts a power law divergence of different dynamical quantities at the mode coupling temperature and at temperatures somewhat higher than the mode coupling temperature, these predictions are found to be consistent with experimental and simulation results. The system size dependence of these quantities should exhibit finite size scaling (FSS) similar to that observed near a continuous phase transition in the temperature range where they show power law growth. Hence we have used the method of finite size scaling in the context of the dynamics of supercooled liquids. In chapter 2, we present the results of extensive molecular dynamics simulations of a model glass forming liquid and extract a dynamical correlation length ξ associated with dynamic heterogeneity by performing a detailed finite size scaling analysis of a four-point dynamic susceptibility χ4(t) [3] and the associated Binder cumulant. We find that although these quantities show the “normal” finite size scaling behaviour expected for a system with a growing correlation length, the relaxation time τ does not. Thus glassy dynamics can not be fully understood in terms of “standard” critical phenomena. Inspired by the success of the empirical Adam-Gibbs relation [4] which relates dynamics with the configurational entropy, we have calculated the configurational entropy for different system sizes and temperatures to explain the nontrivial scaling behaviour of the relaxation time. We find that the behaviour of the relaxation time τ can be explained in terms of the Adam-Gibbs relation [4] for all temperatures and system sizes. This observation raises serious questions about the validity of the mode coupling theory which does not include the effects of the potential energy (or free energy) landscape on the dynamics. On the other hand, in the “random first order transition” theory (RFOT), introduced by Wolynes and coworkers [5], the configurational entropy plays a central role in determining the dynamics. So we also tried to explain our simulation results in terms of RFOT. However, this interpretation has the drawback that the value of one of the exponents of this theory extracted from our numerical results does not satisfy an expected physical bound, and there is no clear explanation for the obtained values of other exponents. Thus we find puzzling values for the exponents relevant to the applicability of RFOT, which are in need of explanation. This can be due to the fact that RFOT focuses only near the glass transition, while all our simulation results are for temperatures far above the glass transition temperature (actually, above the mode coupling temperature). Interestingly, results similar to ours were obtained in a recent analysis [6] of experimental data near the laboratory glass transition, on a large class of glass-forming materials. Thus right now we do not have any theory which can explain our simulation data consistently from all perspectives. There have been some attempts to extend the RFOT analysis to temperatures above the mode coupling temperature [7, 8] and to estimate a length scale associated with the configurational entropy at such temperatures. We compare our results with the predictions arising from these analyses.
In chapter 3, we present simulation results that suggest that finite size scaling analysis is probably the only feasible method for obtaining reliable estimates of the dynamical correlation length for supercooled liquids. As mentioned before, although there exists a growing correlation length, the behaviour of all measured quantities (specifically, the relaxation time) is not in accordance with the behaviour expected in “standard” critical phenomena. So one might suspect the results for the correlation length extracted from the scaling analysis. To find out whether the results obtained by doing finite size scaling are correct, we have done simulations of very large system sizes for the same model glass forming liquid. In earlier studies, the correlation length has been extracted from the wave vector dependence of the dynamic susceptibility in the limit of zero wave vector, but to estimate the correlation length with reasonable accuracy one needs data in the small wave vector range. This implies that one needs to simulate very large systems. But as far as we know, in all previous studies typical system sizes of the order of 10, 000 particles have been used to do this analysis. In this chapter we show by comparing results for systems of 28, 000 and 350, 000 particles that these previous estimates are not reliable. We also show that one needs to simulate systems with at least a million particles to estimate the correlation length correctly near the mode coupling temperature and this size increases with decreasing temperature. We compare the correlation length obtained by analyzing the wave vector dependence of the dynamic susceptibility for a 350, 000particle system with the results obtained from the finite size scaling analysis. We were only able to compare the results in the high temperature range due to obvious reasons. However the agreement in the high temperature range shows that the finite size scaling analysis is robust and also establishes the fact that finite size scaling is the only practical method to extract reliable correlation lengths in supercooled liquids.
In chapter 4, we present a free energy landscape analysis of dynamic heterogeneity for a monodisperse hard sphere system. The importance of the potential energy landscape for particles interacting with soft potentials is well known in the glass community from the work of Sastry et al. [9] and others, but the hard sphere system which does not have any well defined potential energy landscape also exhibits similar slow dynamics in the high density limit. Thus it is not clear how to treat the hard sphere systems within the same energy landscape formalism. Dasgupta et al. [10, 11, 12, 13, 14, 15] showed that one can explain the slow dynamics of these hard core systems in term of a free energy landscape picture. They and other researchers showed that these system have many aperiodic local minima in its free energy landscape, with free energy lower than that of the liquid. Using the Ramkrishnan-Yussouff free energy functional, we have performed multi parameter variational minimizations to map out the detailed density distribution of glassy free energy minima. We found that the distribution of the widths of local density peaks at glassy minima is spatially heterogeneous. By performing hard sphere event driven molecular dynamics simulation, we show that there exists strong correlation between these density inhomogeneity and the local Debye-Waller factor which provides a measure of the dynamic heterogeneity observed in simulations. This result unifies the system of hard core particles with the other soft core particles in terms of a landscapebased description of dynamic heterogeneity.
In chapter 5, we extend the same free energy analysis to a polydisperse system and show that there is a critical polydispersity beyond which the crystal state is not stable and glassy states are thermodynamically stable. We also found a reentrant behaviour in the liquid-solid phase transition within this free-energy based formalism. These results are in qualitative agreement with experimental observations for colloidal systems
Collective Behaviour of Confined Equilibrium And Non Equilibrium Soft Matter Systems
Get PDFDue to their diversity, soft matter systems provide a convenient platform to study a variety of physical phenomena like phase transitions and collective motion. Encompassing a wide range of equilibrium and non-equilibrium systems, they often provide significant insight into the statistical mechanics of different kinds of many-body systems. Though large scale properties of such systems are of fundamental interest in their own accord, since most experimental realizations of soft matter systems are finite sized, there is a growing need to understand the effects of confinement or boundary conditions on the collective behaviour of such systems. The primary purpose of this thesis is to study the effects of boundary conditions or confinement on both equilibrium and non-equilibrium soft matter systems via theoretical modelling. For equilibrium systems we have studied a system of colloidal particles in harmonic confinement, and for non-equilibrium systems we consider a system of self-propelled rods in both harmonic and hard wall confinement.
In Chapter 1 we first lay down some basic concepts of stochastic dynamics and Brownian motion, before discussing some of the recent results on confinement effects on colloidal systems, showing how the properties of a finite sized colloidal system can be very different from those of large, un confined systems. Thereafter turning to non-equilibrium active systems, we discuss various fundamental problems posed by these systems due to their unique ability to generate and dissipate energy on their own. We also point out some instances of observed confinement effects in such systems, such as boundary aggregation and transient hedgehog-like clusters near the boundary.
Chapter 2 deals with the effect of harmonic confinement on a finite sized colloidal assembly, where we show that such finite size effects coupled with a confining potential can give rise to special features like initial position dependent expulsion of dopant particles. First we model experimentally studied small two-dimensional colloidal assemblies trapped by a defocussed laser beam by Langevin dynamics simulations in the presence of harmonic confinement and demonstrate how the system shows a crossover from liquid state to crystalline state as a function of the stiffness of the confinement. We also show that in the crystalline state the system can be effectively modelled as a rigid body under small force perturbations. Notably, while studying the dynamics of a defect particle inside these crystallites, we found evidence for the occurrence of self purification by the crystallites.
In this process, a dopant is spontaneously expelled out of the crystallite. Surprisingly, this phenomena has a strong dependence on the initial position of the dopant, which turns out to be the consequence of the non monotonic spatial variation of the free energy of the system as a function of the dopant position. This is caused by a difference in the rate of change of internal energy and entropy with the dopant position, with the entropy decreasing faster when the dopant is closer to the centre. This can be attributed to the amount of disruption of crystalline order in the assembly due to the incommensurate dimensions of the defect particle. In order to put these results in a general perspective, we verify in the last part of this chapter that the presence of this free energy barrier is independent of the exact functional forms of the confining potential and the interaction of a defect particle with the host particles, as well as the shape and size of the defect particle.
Moving to non-equilibrium systems, we consider, in Chapter 3, the effect of harmonic and hard wall confinement on a two-dimensional system of self-propelled rods (SPRs). Though there have been very limited studies of confinement effects on such systems, existing studies are adequate to show that their behaviour near a boundary wall can be very different, e.g. formation of hedgehog like clusters near a boundary wall. First we show that for harmonic confinement small systems show polar order, which decays with system size, eventually going away for large systems. But the effect of hard wall confinement turns out to be rather different, where the system shows isotropic and clustered states depending on the values of activity and density. We construct a complete activity-density phase diagram showing four distinct phases. For high density and high activity, the rods spontaneously arrange themselves into a stable vortex structure in which the rods exhibit global radial polar order.
Surprisingly this order does not decay with system size: the radial orientation of the rods exhibit strong spatial correlation even in large systems, ruling out the possibility that the radial order is a finite-size effect. Using other geometrical shapes of the hard wall boundary, we confirm this phase to be independent of the shape of the boundary. We also demonstrate how small modifications of the boundary conditions at the hard wall can collapse the clustered and vortex phases to a global flocking phase similar to that found in earlier studies of hydrodynamic active particles under confinement.
Based on these observations, we conclude that the bulk of the system is strongly affected by the subjected boundary condition, which is rather unusual for large systems.
In Chapter 4 this thesis concludes with a summary of the main results and suggestions for future work along similar line
Motility driven glassy dynamics in confluent epithelial monolayers
Get PDFAs wounds heal, embryos develop, cancer spreads, or asthma progresses, the cellular monolayer undergoes a glass transition between solid-like jammed and fluid-like flowing states. During some of these processes, the cells undergo an epithelial-to-mesenchymal transition (EMT): they acquire in-plane polarity and become motile. Thus, how motility drives the glassy dynamics in epithelial systems is critical for the EMT process. However, no analytical framework that is indispensable for deeper insights exists. Here, we develop such a theory inspired by a well-known glass theory. One crucial result of this work is that the confluency affects the effective persistence time-scale of active force, described by its rotational diffusivity, Deffr. Deffr differs from the bare rotational diffusivity, Dr, of the motile force due to cell shape dynamics, which acts to rectify the force dynamics: Deffr is equal to Dr when Dr is small and saturates when Dr is large. We test the theoretical prediction of Deffr and how it affects the relaxation dynamics in our simulations of the active Vertex model. This novel effect of Deffr is crucial to understanding the new and previously published simulation data of active glassy dynamics in epithelial monolayers
Glassy Dynamics in Active Matter
No full textThere has been much interest in the glassy dynamics of living systems at the scales
of subcellular structures, cells and tissues. This has motivated theoretical studies on
the approach to glassy behaviour in dense systems driven by activity, opening up new
questions, both in the physics of glass transitions and in active matter. A key issue is
whether active glasses are akin to passive ones with an effective temperature or whether
they are fundamentally different. In this thesis we address some of these issues using a
variety of simulation and analytical techniques
Numerical Study Of The Complex Dynamics Of Sheared Nematogenic Fluids
Get PDFIn this thesis, we have tried to explain the regular and irregular(chaotic) dynamics of worm like micellar solutions on applying shear, through a detailed study of the equation of motion of a nematic order parameter tensor coupled to a hydrodynamic velocity field. We have assumed spatial variations only along one direction i.e. the gradient direction(1D model). The resulting phase diagram shows various interesting steady states or phases such as spatiotemporal chaos, temporal and spatiotemporal periodicities, and alignment of the director axis along the imposed flow field. The coupling of the orientational degrees of freedom of the order parameter with the hydrodynamic flow field holds the key to the appearance of dynamic shear bands in the system. We have solved numerically a set of coupled nonlinear equations to obtain the order parameter stress developed in the system; the magnitude of the order parameter tensor, the biaxiality parameter and the orientation of the director axis of the nemato gens under shear have also been studied in detail. To study the phase diagram obtained by time integration of the equation of motion mathematically, a stability analysis of the fixed point of motion for various parameter values has been performed so that the location of the chaotic-to-aligned phase boundary is verified. Also in the periodic region of the phase diagram, the stability of limit cycles is tested by analysing the fixed point of the corresponding Poincare map. Stability analysis of the periodic orbits leads to the observation that in the parameter space, there are regions of phase coexistence where chaotic or spatiotemporally intermittent behaviour coexists with periodic behaviour.
When corrections in the imposed velocity field due to the order parameter stress were taken into account and the order parameter response was looked into at several points in the parameter space, the modified equations of motion were found to reproduce the earlier behaviour in all the different regimes if the value of a dimensionless viscosity parameter is taken to be such that the bare viscous stress overrides the order parameter stress. The phase boundaries are however different from the ones seen in the earlier model. However, for a choice of the viscosity parameter such that the order parameter stress and the bare viscous stress are comparable, we see two distinctly different attractors: a banded, periodic one that is common to both α1equalto 0, and not equal to 0 and a banded chaotic one for α1not equal to 0. Here, α1is a parameter that governs the nonlinearity in the stretching of the order parameter tensor along the direction of the applied shear. Quantitative analysis of the various chaotic attractors throws up not only positive Lyapunov exponents but also that the banded chaos is a “flip-flop” kind of chaos where the switching between two long-lived states of high and lows hear stress is chaotic, where as the behaviour in either of the two states is periodic, with either a single, isolated frequency or a bunch of harmonics. Also, the spatial correlation of the shear stress in the chaotic attractors is of much larger range than the temporal correlation, the latter being almost delta-function-like. On increasing the temperature of the system till it is above the isotropic–nematic transition temperature in the absence of shear, we find that under shear, similar attractors as those in the nematic case are observed, both for passive advection and for the full 1D hydrodynamics. This is an encouraging result since actual experiments are performed at a temperature for which the system is in the isotropic phase in the absence of shear. Thus for the 1D system, the parameter space has been explored quite extensively.
Considering spatial variations only along the gradient axis of the system under shear is not enough since experiments have observed interesting behaviour in the vorticity plane in which Taylor velocity rolls were noted. Hence taking the system to 2D was necessary. Our numerical study of the 2D system under shear is incomplete because we came across computational difficulties. However, on shorter time scales we have seen a two-banded state with an oscillating interface and Taylor velocity rolls as well. The methodology used for the 2D study can also be used to reproduce the 1D results by the simple step of taking initial condition with no variation in the vorticity direction. This automatically ensures that no variation in the vorticity direction ever builds up because the equations of motion ensure that these variations in the system do not grow by themselves unless fed in at the start. Using this method, we were able to reproduce all the attractors found in the 1D calculation. Thus the 1D attractors have been observed using two different methods of calculation. Further work on the full 2D numerics needs to be done because we believe that spatiotemporally complex steady-state attractor s exist in the 2D system also for appropriate values of the parameters
Phenomenological Theory Of Superconductivity And Low-Energy Electronic Spectra In The High-Tc Cuprates
Get PDFCondensed matter physics is a rapidly evolving field of research enriched with the synthesis of new materials exhibiting a bewildering variety of phenomena and advances in experimental techniques. Over the years, discoveries and innovations in electronic systems have emphasized the crucial role played by correlations among electrons behind many of the observed unusual properties and have posed serious challenges to the physics community by exposing the lack of well-controlled theoretical methods to study the class of materials known as strongly correlated electronic systems. In these systems, known theoretical techniques typically fail to capture the essential features of the many-body ground state and finite temperature properties of the systems as typical electronic interaction energies are of order of or larger than the kinetic energies.
The study of strongly correlated electronic systems went through a revolution in the 1980s and 1990s after the discovery of superconductivity inorganic compounds, in heavy fermion systems and ultimately in copper oxides, referred to as cuprates, by Bednorz and Muller. In particular, the pursuit of understanding the mysterious origin of superconductivity in the cuprates and other associated strange phenomena has fascinated the condensed matter community over last two and half decades leading to most of the important unsolved, and probably interconnected, problems of quantum condensed matter physics such as the metal-insulator transition in low dimensions breakdown of Fermi liquid theory, the origin and behavior of unconventional superconductivity, quantum critical points, electronic in homogeneities and localization in interacting systems. This thesis is devoted to the study of some of the aspects of high-temperature superconductivity and associated phenomena in cuprates. In what follows, I give an overview of the organization of the thesis in to different chapters and their contents.
For setting up the stage, in Chapter 1, I give a brief account of some of the remarkable phenomena and properties observed in strongly correlated electronic matter and their salient features, that continue to draw much attention and excitement in current times. The peculiarity of the state of affairs in these systems is emphasized and motivated in the background of the paradigmatic Landau Fermi liquid theory and Hubbard model, the minimal model that is expected to capture the quintessence of electronic strong correlation.
In Chapter 2, starting with a brief historical account of the discovery of superconductivity in cuprates, the crystal structure of these materials, their chemical realities and basic electronic details are reviewed. This is followed by a survey of the phase diagram of cuprates, doped with, say, x number of holes per copper site, and a plethora of experimental findings that constitute the high-c puzzle. Characteristics of various observed phases, such as the superconducting, pseudo gap and strange metal phases, are discussed on the basis off acts accumulated through various experimental probes, e.g. nuclear magnetic resonance(NMR), neutron scattering, specific heat, transport and optical conductivity measurements as well as photo emission, tunnelling and Raman spectroscopies. As elucidated, these experiments point toward the need for an unconventional mechanism of superconductivity in cuprates and, more so, for the description of the rather abnormal high-temperature normal state that is realized above the superconducting transition temperature c. Keeping in mind the fact that there is no consensus even about the minimal microscopic electronic model, I review two models, namely the three band model and the t - J model; various approximate treatments of these models have dominated the theoretical developments in this field. A large number of theoretical pictures have been proposed based on different microscopic, semi-microscopic and phenomenological approaches in the past two decades for explaining the genesis of the observed strange phenomena in high-c cuprates. I include brief discussions on only a few of them while citing relevant references.
As mentioned above, a variety of approximate microscopic theories, based on both strong and weak coupling approaches, as well as numerical techniques have been tried to understand the cuprate phase diagram and capture the aspects of strong correlations in-built in Hubbard and t -J models. On the other hand, in conventional superconductors and, in general, for the study of phase transitions, phenomenological Ginzburg-Landau(GL) functionals written down from very general symmetry grounds have provided useful description for a variety of systems. Specially, Ginzburg-Landau theory has been proven to be complementary to the BCS theory for attacking a plethora of situations in superconductors, e.g., in homogeneities, structures of an isolated vortex and the vortex lattice etc. The GL functional has found wide applicability for the study of vortex matter in high-c superconductors as well. Inspired by the success of this type of phenomenological route, we propose and develop in Chapter 3 an approach, analogous in spirit to that of Ginzburg and Landau, for the superconducting and pseudogap phases of cuprates. We encompass a large number of well known phenomenologies of cuprate superconductivity in the form of a low-energy effective lattice functional of complex spin-singlet pair amplitudes with magnitude Δm and phase m, i.e. m =Δm exp(i m), that resides on the Cu-Cubonds(indexed by m)of the CuO2 planes of cuprates. The functional respects general symmetry requirements, e.g. the -wave symmetry of the superconducting order parameter as found in experiments. The assumptions and the specific physical picture behind such an approach as well as the key empirical inputs that go into it are discussed in this chapter. We calculate the superconducting transition temperature c and the average magnitude of the local pair amplitude, Δ= (Δm), using single-site mean-field theory for the model. We show that this approximation leads to general features of the doping-temperature(x - T )phase diagram in agreement with experiment. In particular, we find a phase coherent superconducting state with d-wave symmetry below a parabolic Tc (x) dome and a phase incoherent state with a perceptible local gap that persists up to a temperature around which can be thought of as a measure of the pseudogap temperature scale T* . Further, effects of thermal fluctuations beyond the mean-field level are captured via Monte Carlo(MC) simulations of the model for a finite two-dimensional (2D) lattice. We exhibit results for Tc obtained from MC simulations as well as that estimated in a cluster mean field approximation. Based on our picture we remark on contrasting scenarios proposed for the doping dependence of the pseudogap temperature.
Chapter 4 describes fluctuation phenomena related to pairing degrees of freedom and manifestations of these effects in various quantities of interest, e.g. superfluid density, specific heat etc., at finite temperature. Fluctuation effects have been studied in detail in superconductors over the years and pursued mainly using either the conventional GL functional or the BCS-framework at a microscopic level. However, the picture, in which the pseudogap phase is viewed as one consisting of bond-pairs with a d-wave symmetry correlation length growing as T approaches Tc, implies fluctuation phenomena of quite a different kind, as we discuss here. The contribution of the bond-pair degrees of freedom to thermal properties is obtained here from the lattice free-energy functional using MC simulation, as mentioned in the preceding paragraph. The results for the superfluid density or superfluid stiffness ps, a quantity measured e.g. via the penetration depth, are discussed. As shown, its doping and temperature dependence compare well with experimental results. In this chapter, I also report the calculation of the fluctuation specific heat Cv(T) and find that there are two peaks in its temperature dependence, a sharp one connected with Tc (ordering of the phase of m)and a relatively broad one(hump)connected to T* (rapid growth of the magnitude of Δm). The former is specially sensitive to the presence of a magnetic field, as we find in agreement with experiment. Vortices are relevant excitations in a superconductor and, in particular, in 2D orquasi-2D systems vortices influence the finite temperature properties in a major way. The results for the temperature dependence of vortex density obtained in the MC simulation of the GL-like model are also mentioned in Chapter 4. I report an estimate of the correlation length as well. These results might have relevance for the large Nernst signal observed over a broad temperature range above c in cuprates, as pointed out there.
Properties of an isolated vortex and collective effects arising due to interaction between vortices are of much significance for understanding mixed state of type-II superconductors and thus of cuprates. The superconducting order is destroyed in the core region around the centre of a vortex and the vortex core carries signatures of the normal state in a temperature regime where it is generally unattainable due to occurrence of superconductivity. As mentioned in Chapter 5, vortex properties(e.g. electronic excitation spectrum at the vortex core) in BCS superconductors have been explored theoretically, at a microscopic level through the Bogoliubov-deGennes(BdG) theory as well as using the Ginzburg-Landau functional. However, properties of vortices in cuprate superconductors have been found to be much more unusual than could possibly be captured by straightforward extensions of BCS theory to a -wave symmetry case. Chapter 5 briefly reviews the experimental findings on vortices in the superconducting state of cuprates, mainly as probed by Scanning Tunnelling Microscopy(STM) as well as from other probes such as NMR, neutron scattering, SR etc. I discuss some of the consequences of our GL-like functional regarding vortex properties, namely that of the vortex core and the region around it. We use our model to find Δm and m at different sites m for a 2π vortex whose core is at the midpoint of a square plaquette of Cu lattice sites. The vortex is found to change character from being primarily a phase or Josephson vortex for small x to a more BCS-like or Abrikosov vortex with a large diminution in the magnitude Δm as one approaches the vortex core, for large . Here I do not make any direct comparison with experimental data but discuss implications of our results in the background of existing experimental facts.
Unravelling the mysteries of high-Tc cuprates should necessarily involve the understanding of electronic excitations over a broad regime of doping and temperature encompassing the pseudo gap, superconducting and strange metal states. A phenomenological theory which aims to describe the pseudo gap phase as one consisting of preformed bond-pairs, is required to include both unpaired electrons and Cooper pairs of the same electrons coexisting and necessarily coupled with each other. In our Ginzburg Landau approach only the latter are explicit, while the former are integrated out. However, effects connected with the pair degrees of freedom are often investigated via their coupling to electrons, one very prominent examples being Angle Resolved Photoemmision Spectroscopy(ARPES),in which the momentum and energy spectrum of electrons ejected from the metal impinged by photons is investigated. In Chapter 6, we develop a unified theory of electronic excitations in the superconducting and pseudo gap phases using a model of electrons quantum mechanically coupled to spatially and temporally fluctuating Cooper pairs(the nearest neighbour singlet bond pairs). We discuss the theory and a number of its predictions which seem to be in good agreement with high resolution ARPES measurements, which have uncovered a number of unusual spectral properties of electrons near the Fermi energy with definite in-plane momenta. We show here that the spectral function of electrons with momentum ranging over the putative Fermi surface(recovered at high temperatures above the pseudogap temperature scale) is strongly affected by their coupling to Cooper pairs. On approaching Tc i.e. the temperature at which the Cooper pair phase stiffness becomes nonzero, the inevitable coupling of electrons with long-wavelength(d-wave symmetry) phase fluctuations leads to the observed characteristic low-energy behavior as reported in Chapter 6. Collective d-wave symmetry superconducting correlations develop among the pairs with a characteristic correlation length ξ which diverges on approaching the continuous transition temperature Tc from above. These correlations have a generic form for distances much larger than the lattice spacing. As we show here, the effect of these correlations on the electrons leads, for example, to a pseudogap in electronic density of states for T > T c persisting till T* , temperature-dependent Fermi arcs i.e. regions on the Fermi surface where the quasiparticle spectral density is non zero for a zero energy excitation and to the filling of the antinodal pseudogap in the manner observed. Further, the observed long-range order(LRO) below c leads to a sharp antinodal spectral feature related to the non zero superfluid density, and thermal pair fluctuations cause a deviation(‘bending’) of the inferred ‘gap’ as a function of k from the expected d-wave form (cos kxa - cos kya). The bending, being of thermal origin, decreases with decreasing temperature, in agreement with recent ARPES measurements.
I conclude in Chapter 7 by mentioning some natural directions in which the functional and the approach used here could be taken forward. The phenomenological theory proposed and developed in this thesis reconciles and ties together a range of cuprate superconductivity phenomena qualitatively and confronts them quantitatively with experiment. The results, and their agreement with a large body of experimental findings, strongly support the mechanism based on nearest neighbor Cooper pairs, and emergence of long-range -wave symmetry order as a collective effect arising from short range interaction between these pairs. This probably points to the way in which high-c superconductivity will be understood
Dynamics of glass forming liquids with emphasis on vibrational modes
No full textThe potential energy landscape (PEL) description is regarded as one of the fundamental landmarks in the theory of glass transition, which has found wide applications not only in the understanding of disordered materials but also in other frontiers of research, such as bio-molecules, catalysis, machine learning, and neural networks. In this context, the mechanically stable local minimum energy configurations of the PEL, which are known as inherent structures (ISs), have a major role to play in elucidating various dynamical and thermodynamic properties of the system in terms of its sojourn over the complex multi-dimensional potential energy surface (PES). However contrary to the crystals, disordered materials pose a greater challenge in understanding their properties. Due to their ordered structures, the normal modes of collective vibrational excitations in crystals can be described by plane waves, which are known as phonons, and they play a fundamental role in determining the kinetic and thermodynamic properties of crystalline solids. Notwithstanding the difficulties presented by the inherent disorder in glass-forming materials, collective excitations associated with small-amplitude vibrations of the system about their ISs can be defined. This thesis presents a study of the dynamics of glass-forming liquids with emphasis on the collective vibrational excitations of the underlying disordered solid.
The vibrational spectrum of disordered harmonic solids consists of a coexisting region of extended phonon modes that obey the Debye scaling law in their density of states, g(ω) ∼ ω^(d−1) in d dimensions, and quasi-localized modes that obey a universal g(ω) ∼ ω^4 law. These excess quasi-localized modes, appearing in the boson peak region of the vibrational spectrum, are found to be substantially different in nature as compared to the modes in other parts of the spectrum. The first part of the thesis describes an investigation of the dynamics of model glass-forming systems based on the measurement of thermal transport properties, with emphasis on the role of the vibrational modes in determining the thermal conductivity. Depending on the protocol of preparation of the glass, the system explores different parts of the PEL. The distinct ISs visited by the system in its exploration of the PEL impact the thermal transport characteristics of the low-temperature glassy states significantly. The observation of lower values of thermal conductivity with slower cooling or growing age of the glass former can be rationalized in terms of the system’s exploration of ISs with progressively lower energy. This in turn has been linked to the presence of more localized normal mode excitations associated with the ISs. Further, the energy diffusivity d(ω) that measures the ability of an excitation to transport thermal energy, has been found to obey a generic d(ω) ∼ 1/(ω^3) law for the quasi-localized normal modes. The diffusivity of low-frequency delocalized phonon modes in two dimensions, on the other hand, follows a d(ω) ∼ 1/(ω^2) law, and it is possible to transform these extended modes to acquire quasi-localized character by the introduction of quenched disorder, which can be achieved via pinning a fraction of the particles. Notably, the boson peak coincides with the well-known Ioffee-Regel limit for phonons, which signals the crossover in terms of d(ω), from a regime populated by delocalized modes to a regime of quasi-localized modes.
In the second part of the thesis, the low-temperature short-time dynamics of a model glass forming system in metabasins of the PEL has been examined. A metabasin is an assembly of strongly correlated basins of ISs in the PEL. Our analysis in terms of the complete vibrational spectrum reveals that the harmonic approximation is not adequate for describing the short-time dynamics at temperatures near the glass transition point. The mean-square displacements computed within the harmonic approximation deviates from that obtained from molecular dynamics simulation at a time shorter than the β-relaxation timescale (τ_β ). With the added contribution of the anharmonic terms in the Hamiltonian via an approximate scheme, the mean- square displacement obtained from the modified calculation shows an agreement with that from both molecular dynamics and metabasin dynamics to a time extending beyond τ_β . The short-time dynamics appears as a combination of the dynamics within the basins of individual ISs and the system’s exploration of different basins inside a metabasin. Moreover, our study shows that the manifestation of the low-frequency quasi-localized excitations in the dynamical quantities depends on the nature of the microscopic dynamics (Newtonian or Langevin) of the system. Our studies in the thesis thus highlight a few important features of the low-temperature dynamics of glass formers and their close connection with the system’s potential energy landscape via the collective vibrational excitations
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