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Nonequilibrium electron-lattice dynamics

Sharareh Sayyad

Published Jan 17, 2017• 0 citations
OpenAlex

Abstract

Optimizing various properties of materials have been under intensive focus for many decades. In recent years, the exposure of ultrafast techniques enhance the possibility of seizing this goal. As by employing these techniques, one can expose the system under strong short fields, and investigate the transient response of various low-lying excitations. Such studies will strengthen our understanding of interplays among various degrees of freedom in correlated materials, and thereby facilitate the chance to manipulate different properties of these systems. Of our particular attention is the electron-lattice dynamics, where modulating a particular vibrational mode of the crystal lattice, will lead to the emergence of new quasi stable'' lattice structures as well as novel transient phenomena. Aside from these experimental prospects, the above mentioned goals were also the subject of an extensive theoretical studies. In this thesis, we investigated the in and out of equilibrium dynamics of electronic systems which are interacting with lattice degrees of freedom. We employed the two-time Keldysh Green's function within the framework of the dynamical mean field theory to conduct our researches on this subject. In our first attempt, we studied the dynamical response of a one-electron system under a linear electron-lattice interaction. We explored the real-time formation of a bound quasiparticle, known as a polaron, under various parameter regimes of the model. We presented that when the carrier is suddenly coupled to the lattice degrees of freedom, the long-time response of the system in the strong coupling limit exhibits both bound, polaronic, and unbound, delocalized, states. We characterized the nature of such a mixed state using the adiabatic picture of the model. We also showed that the formed polaron is dressed by excited phononic states, in contrast to its equilibrium counterpart, where the ground-state phononic states are bounding the electron. We also addressed the response of a many-body electronic system, weakly coupled to a bosonic bath, under various time dependent excitations, which brings the system to a bad-metallic phase. We employed a model which treated the Coulomb repulsive interaction locally. We presented that the relaxation of this excited state varies by the strength of the electron-electron interaction. We demonstrated that, for both insulating and metallic regimes of the system, a slow relaxation dynamics can be observed close to the phase transition from the metallic to insulating regimes of the system. Our analysis revealed that in the metallic side, this slow evolution is rooted in the spin-related physics of the problem. However, in the insulating regimes of the model, our results showed that presence of a gap in the spectral density of the insulating system prohibits the relaxation of the excited particles. We also studied the associated timescale for the adiabatic dynamics near the Mott transition. Our results exhibited that there is a nonadiabatic window'' in the metallic side of the phase transition, in which the adiabatic timescale is extremely long. We pointed out that the presence of such a window is intertwined with the slow relaxation timescale of the spin-related dynamics close to the Mott transition. We also captured an induced metallic phase near metal-to-insulator transition out of equilibrium. We initiated this study using the slave-rotor impurity solver, which is been coupled to the self-energies obtained from the first-order Luttinger-Ward functional for the Phonon degrees of freedom. We presented the emergence of the larger spectral density at small frequencies both in metallic and insulating phases close to the phase transition, which is surrounded by pseudo gaps. We explored the physics of such spectral densities as well as their dependencies on the phononic parameters. We postulated that this response of the system is due to the evolution of the system, in a non-thermal mechanism, towards a temperature which is less than the initial temperature of the system, before coupling to the bath. We also pointed out that the associated very slow relaxation dynamics is the result of the formation of psuedo-gaps around the quasiparticle peak.

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Non-Equilibrium Correlated Quantum Dynamics of Lattice Trapped Finite Bosonic Ensembles

Symeon Mystakidis

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Alternatively, a sudden ramping down of the lattice depth which favors the spatial delocalization is employed to access the cradle mode for setups with filling smaller than unity. Following a multiple interaction quench protocol, we observe the rise of several lowest-band tunneling modes as well as the cradle and the breathing mode. Besides the cradle mode, all other excited modes are highly tunable possessing different frequencies during and in between the quenches. In the excitation dynamics a monotonic behavior with increasing quench amplitude and a non-linear dependence on the duration of the application of the quenched interaction strength is revealed. Additionally, a periodic population transfer between momenta for quenches of increasing interaction is observed, with a power-law frequency dependence on the quench amplitude. Linear interaction quenches from a superfluid to a Mott-insulator state excite various inter- and intraband tunneling modes. 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To relate our findings with possible experimental realizations, we simulate, for the first time for binary mixtures, single-shot images showcasing that the growth rate of the variance of a sample of single-shots probes the degree of entanglement inherent in the system. As a next step we investigate the expansion dynamics of a mass balanced Bose-Fermi mixture confined in a one-dimensional optical lattice upon quenching an imposed harmonic trap from strong-to-weak confinement. Tuning the interspecies interaction strength we realize the immiscible and miscible correlated ground state phases. We further show that the system's dynamical response crucially depends on the initial phase and consists of an expansion of each cloud and an interwell tunneling dynamics. Varying the quench amplitude and referring to a fixed phase a multitude of response regimes is unveiled, being richer within the immiscible phase, which are described by distinct expansion strengths and tunneling channels. 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•Apr 18, 2019•0 citations

Thermal dynamics of lattice modes near a polaronic crossover: from the dilute polaron limit to a charge ordered state

Sauri Bhattacharyya, Saurabh Pradhan, Pinaki Majumdar

We provide a comprehensive solution to the lattice dynamics problem in the two dimensional Holstein model at finite electron density and finite temperature. We work in the physically relevant adiabatic regime and vary the electron-phonon interaction from the weak coupling perturbative window to the strong coupling polaronic regime. We explore three typical electron densities, dilute - where spatial correlations between polarons is weak, intermediate - where correlations are significant, and half-filling - where there is long range checkerboard order at low temperature. We use two methods both of which exploit the "slowness" of the phonons to handle the problem. These are (i)~a standard random phase approximation (RPA), adapted to capture small quantum fluctuations on Monte Carlo generated classical thermal backgrounds, and (ii)~a Langevin dynamics scheme, with a simplified ``thermal noise'', that can address large amplitude dynamical fluctuations. The Langevin scheme, as we argue in the paper, is the superior method in the strong coupling part of the phase diagram, where lattice distortions are large. It reveals a non trivial multi-peak momentum resolved spectrum with a high energy part, on the scale of the bare phonon frequency $Ω$, and a low energy peak at $ω\ll Ω$. Below the polaronic threshold, the high energy dispersion changes only modestly with temperature $T$, while the broadening, arising from mode coupling, increases linearly with $T$ at low temperature. The low energy peak shows up at strong coupling and finite temperature and arises from the slow tunneling of polarons. The tunneling events become spatially correlated as electron density increases towards half-filling, and the weight becomes strongly momentum and temperature dependent. We suggest the analytic basis of these results.

arXiv:1711.08749•Nov 23, 2017•0 citations
Optimizing various properties of materials have been under intensive focus for many decades. In recent years, the exposure of ultrafast techniques enhance the possibility of seizing this goal. As by employing these techniques, one can expose the system under strong short fields, and investigate the transient response of various low-lying excitations. Such studies will strengthen our understanding of interplays among various degrees of freedom in correlated materials, and thereby facilitate the chance to manipulate different properties of these systems. Of our particular attention is the electron-lattice dynamics, where modulating a particular vibrational mode of the crystal lattice, will lead to the emergence of new quasi stable'' lattice structures as well as novel transient phenomena. Aside from these experimental prospects, the above mentioned goals were also the subject of an extensive theoretical studies. In this thesis, we investigated the in and out of equilibrium dynamics of electronic systems which are interacting with lattice degrees of freedom. We employed the two-time Keldysh Green's function within the framework of the dynamical mean field theory to conduct our researches on this subject. In our first attempt, we studied the dynamical response of a one-electron system under a linear electron-lattice interaction. We explored the real-time formation of a bound quasiparticle, known as a polaron, under various parameter regimes of the model. We presented that when the carrier is suddenly coupled to the lattice degrees of freedom, the long-time response of the system in the strong coupling limit exhibits both bound, polaronic, and unbound, delocalized, states. We characterized the nature of such a mixed state using the adiabatic picture of the model. We also showed that the formed polaron is dressed by excited phononic states, in contrast to its equilibrium counterpart, where the ground-state phononic states are bounding the electron. We also addressed the response of a many-body electronic system, weakly coupled to a bosonic bath, under various time dependent excitations, which brings the system to a bad-metallic phase. We employed a model which treated the Coulomb repulsive interaction locally. We presented that the relaxation of this excited state varies by the strength of the electron-electron interaction. We demonstrated that, for both insulating and metallic regimes of the system, a slow relaxation dynamics can be observed close to the phase transition from the metallic to insulating regimes of the system. Our analysis revealed that in the metallic side, this slow evolution is rooted in the spin-related physics of the problem. However, in the insulating regimes of the model, our results showed that presence of a gap in the spectral density of the insulating system prohibits the relaxation of the excited particles. We also studied the associated timescale for the adiabatic dynamics near the Mott transition. Our results exhibited that there is a nonadiabatic window'' in the metallic side of the phase transition, in which the adiabatic timescale is extremely long. We pointed out that the presence of such a window is intertwined with the slow relaxation timescale of the spin-related dynamics close to the Mott transition. We also captured an induced metallic phase near metal-to-insulator transition out of equilibrium. We initiated this study using the slave-rotor impurity solver, which is been coupled to the self-energies obtained from the first-order Luttinger-Ward functional for the Phonon degrees of freedom. We presented the emergence of the larger spectral density at small frequencies both in metallic and insulating phases close to the phase transition, which is surrounded by pseudo gaps. We explored the physics of such spectral densities as well as their dependencies on the phononic parameters. We postulated that this response of the system is due to the evolution of the system, in a non-thermal mechanism, towards a temperature which is less than the initial temperature of the system, before coupling to the bath. We also pointed out that the associated very slow relaxation dynamics is the result of the formation of psuedo-gaps around the quasiparticle peak.
Correlated systems are a wide class of materials in which the strong electron-electron repulsion is the origin of very fascinating and unusual properties, among which metal-to-insulator transitions and high temperature superconductivity are the most striking examples. In the recent years, the fast development of non-adiabatic probing techniques opened new interesting perspectives for the investigation of such materials in non-equilibrium conditions. In this thesis, we discuss the theoretical description of few relevant cases which represent different examples of non-equilibrium phenomena in correlated materials. In particular, we will focus on the dynamics following a sudden excitation and the coupling to an external driving field. As a first example we consider the dynamics across a phase transition, namely we explore the possibility of driving a phase transition as the result of a sudden excitation, as e.g. the coupling with a short light pulse. We consider systems showing different equilibrium phases and study the conditions under which the off-equilibrium dynamics may lead to non-trivial dynamical phase transitions. A different case is represented by the dynamics induced by a driving electric field. This problem is particularly relevant for the possible applications of correlated materials in electronic devices. Here we consider the paradigmatic case of a correlated material coupled to external sources which impose a finite bias across the system. We analyze the formation and the properties of the non-equilibrium stationary states in which a finite current flows through the system. This allows us to study the non-linear response properties of a correlated system. In this context, a particularly relevant aspect is the problem of the dielectric breakdown of a Mott insulator, namely the formation of conducting states in the Mott insulating phase. In this thesis we explore different mechanisms leading to such possibility. First we discuss a quantum tunneling mechanism of carriers driven across the insulating gap by the effect of strong electric-fields. Eventually, we discuss the possibility of a resistive transition from an insulating to a metallic state induced by the application of an external electric-field.
We study equilibrium and nonequilibrium properties of electron-phonon systems described by the Hubbard-Holstein model using dynamical mean-field theory. In equilibrium, we benchmark the results for impurity solvers based on the one-crossing approximation and slave-rotor approximation against non-perturbative numerical renormalization group reference data. We also examine how well the low-energy properties of the electron-boson coupled systems can be reproduced by an effective static electron-electron interaction. The one-crossing and slave-rotor approximations are then used to simulate insulator-to-metal transitions induced by a sudden switch-on of the electron-phonon interaction. The slave-rotor results suggest the existence of a critical electron-phonon coupling above which the system is transiently trapped in a nonthermal metallic state with coherent quasiparticles. The same quench protocol in the one-crossing approximation results in a bad metallic state.
Correlated electron systems represent a wide class of materials which at equilibrium display fascinating properties. Several recent experimental breakthroughs in the field of femtosecond spectroscopy and cold atomic gases allow nowadays to investigate the real time dynamics of these many-body quantum systems. Since strongly correlated systems usually escape single particle approaches, the theoretical study of their dynamics constitutes a formidable problem which necessitates the development of novel techniques. In this Thesis we investigate the out-of-equilibrium physics of simple paradigmatic models that are believed to capture some essential physics of interacting fermions by means of the time dependent extension of the Gutzwiller Variational Approach. After an introductory Chapter on the recent results in this field, in Chapter 2 we present the Gutzwiller Approach in-and-out of equilibrium. In Chapter 3 we investigate the dynamics for the single band Hubbard model after a linear ramp of the Coulomb interaction. We will show that a dynamical transition appears for any duration of the ramp; this dynamical point is adiabatically connected to the zero temperature Metal-to-Insulator transition. We will then consider the role of quantum fluctuations beyond mean field. In Chapter 4 we consider the dynamics of an initial antiferromagnetic state under a quench of the interaction in the single band fermionic Hubbard model. We will show that non-thermal ordered states survive more than expected and that two different nonequilibrium antiferromagnets can be distinguished. Finally in Chapter 5 we will consider a two-band Hubbard model which we believe captures the main physics of the paradigmatic compound vanadium sesquioxide, V2 O3 . After an investigation of the equilibrium properties for this model, we will provide evidences that non-thermal metallic phases can emerge upon an excitation of a Mott insulator.
We examine electron-electron mediated relaxation following ultrafast electric field pump excitation of the fermionic degrees of freedom in the Falicov-Kimball model for correlated electrons. The results reveal a dichotomy in the temporal evolution of the system as one tunes through the Mott metal-to-insulator transition: in the metallic regime relaxation can be characterized by evolution toward a steady state well described by Fermi-Dirac statistics with an increased effective temperature; however, in the insulating regime this quasithermal paradigm breaks down with relaxation toward a nonthermal state with a complicated electronic distribution as a function of momentum. We characterize the behavior by studying changes in the energy, photoemission response, and electronic distribution as functions of time. This relaxation may be observable qualitatively on short enough time scales that the electrons behave like an isolated system not in contact with additional degrees of freedom which would act as a thermal bath, especially when using strong driving fields and studying materials whose physics may manifest the effects of correlations.
Ultracold atoms in optical lattices constitute a versatile many-body platform with highly tunable parameters, allowing us to emulate a multitude of complex quantum systems, in the laboratory, even those eluding analytical treatment. In particular, the nonequilibrium dynamics of strongly correlated many-body systems represents one of the most challenging problems of modern quantum physics, with applications ranging from thermalization dynamics and transport properties to the management of correlations and the control of the dynamics. Understanding nonequilibrium phenomena of strongly correlated systems is a formidable task. A very promising route to gain insight into such systems is to examine few-body setups which contain only a few relevant degrees of freedom, yet incorporating the quantum correlations between the particles. The present dissertation contributes to the understanding of the nonequilibrium dynamics of strongly-correlated quantum many-body systems by exploring systems of few-bosons −-− of one or two species −-− trapped in optical lattices. The systems are driven out-of-equilibrium either by performing a quench of a Hamiltonian parameter or by considering a time-periodic modulation of the external confinement. In the course of several consecutive works, we showcase different ways to couple the nonequilibrium modes, while unveiling their correlated nature and microscopic origin. To simulate the nonequilibrium dynamics, a sophisticated, highly flexible ab-initio method for numerically solving the time-dependent many-body Schrodinger equation is utilized, namely the Multi-Layer Multi-Configuration Time-Dependent Hartree Method for Atomic Mixtures (ML-MCTDHX). Within the first part we study in six consecutive works the correlated nonequilibrium dynamics of few-boson systems in one-dimensional finite lattices. Starting from weak interactions, it is shown that a sudden increase of the interaction strength generates a global density-wave tunneling dynamics as well as intrawell breathing and cradle-like excited-band processes. The cradle process is a dipole-like process generated by the quench-induced over-barrier transport and it is one of the central results of the present thesis. Remarkably enough, the interaction quenches couple the density-wave and cradle modes, inducing resonance phenomena between the inter and intrawell dynamics. We further show that the cradle mode is inherently related to the initial delocalization and, following a quench from strong-to-weak interactions, can be excited only for incommensurate setups with filling larger than unity. Alternatively, a sudden ramping down of the lattice depth which favors the spatial delocalization is employed to access the cradle mode for setups with filling smaller than unity. Following a multiple interaction quench protocol, we observe the rise of several lowest-band tunneling modes as well as the cradle and the breathing mode. Besides the cradle mode, all other excited modes are highly tunable possessing different frequencies during and in between the quenches. In the excitation dynamics a monotonic behavior with increasing quench amplitude and a non-linear dependence on the duration of the application of the quenched interaction strength is revealed. Additionally, a periodic population transfer between momenta for quenches of increasing interaction is observed, with a power-law frequency dependence on the quench amplitude. Linear interaction quenches from a superfluid to a Mott-insulator state excite various inter- and intraband tunneling modes. The competition between the quench rate and the interparticle repulsion leads to a resonant dynamical response, at moderate ramp times, being related to avoided-crossings in the many-body eigenspectrum. The resultant higher-band excitation dynamics is shown to obey an exponential decay possessing two distinct time scales with varying ramp time. Inspecting the crossover from shallow to deep lattices we find that for a diabatic quench the excited-band fraction decreases, while approaching the adiabatic limit it exhibits a nonlinear behavior for increasing height of the potential barrier. Quenching from strong-to-weak interactions leads to a melting of the Mott-insulator and negligible higher-band excitations. Performing quenches either on the wavevector or the phase of a spatially dependent interaction profile triggers various tunneling channels and a rich excitation dynamics which is amplified for increasing inhomogeneity amplitude. Most importantly, the phase quench is shown to induce a directional transport enabling us to discern, otherwise, energetically degenerate tunneling pathways. Finally, a periodic population transfer between distinct momenta for quenches of increasing wavevector and a directed occupation of higher momenta following a phase quench is observed. Employing a quench of an additional harmonic trap from strong-to-weak confinement, we find that the competition between the initial localization and the repulsive interaction leads to a resonant response of the system related to avoided-crossings in the many-body eigenspectrum with varying final trap frequency. Furthermore, we show that these avoided-crossings can be utilized to prepare the system in a desired state. The second part comprises two efforts and is devoted to the study of the nonequilibrium dynamics of finite ultracold bosonic ensembles in periodically driven one-dimensional optical lattices. For a shaken lattice, a wide range of driving frequencies is covered and a resonant behavior of the intrawell dynamics is revealed and found to be related to a rich intraband excitation spectrum. Moreover, it is shown that for increasing repulsion a strong suppression of the interwell tunneling and an enhanced excitation dynamics occurs. For a vibrating lattice, an additional interaction quench gives rise to admixtures of different excitations in the outer wells, an enhanced breathing in the center and an amplification of the emerging tunneling dynamics. The occurence of multiple resonances between the inter- and intrawell dynamics at different quench amplitudes is revealed, with the position of the resonances being tunable via the driving frequency and thus allowing for further control of the mode coupling in optical lattices. In the third and final part of this thesis we unravel the quench dynamics of a Bose-Bose and a Bose-Fermi mixture. Utilizing an interspecies interaction quench we cross the miscibility-immiscibility threshold in a harmonically confined Bose-Bose mixture. We show that increasing the interspecies repulsion coefficient results in a filamentation of the density of each species, with the spontaneously generated filaments being strongly correlated and exhibiting domain-wall structures. Strikingly, by following the reverse quench protocol, i.e., upon decreasing the interspecies interaction strength, the formation of multiple dark-antidark solitary waves is observed. These solitary wave structures are found to decay into the many-body environment, soon after their generation in sharp contrast to the predictions of the mean-field approximation. To relate our findings with possible experimental realizations, we simulate, for the first time for binary mixtures, single-shot images showcasing that the growth rate of the variance of a sample of single-shots probes the degree of entanglement inherent in the system. As a next step we investigate the expansion dynamics of a mass balanced Bose-Fermi mixture confined in a one-dimensional optical lattice upon quenching an imposed harmonic trap from strong-to-weak confinement. Tuning the interspecies interaction strength we realize the immiscible and miscible correlated ground state phases. We further show that the system's dynamical response crucially depends on the initial phase and consists of an expansion of each cloud and an interwell tunneling dynamics. Varying the quench amplitude and referring to a fixed phase a multitude of response regimes is unveiled, being richer within the immiscible phase, which are described by distinct expansion strengths and tunneling channels. Finally, in the expansion dynamics a two-body anti-correlated behavior between the predominantly occupied wells is unveiled.
We provide a comprehensive solution to the lattice dynamics problem in the two dimensional Holstein model at finite electron density and finite temperature. We work in the physically relevant adiabatic regime and vary the electron-phonon interaction from the weak coupling perturbative window to the strong coupling polaronic regime. We explore three typical electron densities, dilute - where spatial correlations between polarons is weak, intermediate - where correlations are significant, and half-filling - where there is long range checkerboard order at low temperature. We use two methods both of which exploit the "slowness" of the phonons to handle the problem. These are (i)~a standard random phase approximation (RPA), adapted to capture small quantum fluctuations on Monte Carlo generated classical thermal backgrounds, and (ii)~a Langevin dynamics scheme, with a simplified ``thermal noise'', that can address large amplitude dynamical fluctuations. The Langevin scheme, as we argue in the paper, is the superior method in the strong coupling part of the phase diagram, where lattice distortions are large. It reveals a non trivial multi-peak momentum resolved spectrum with a high energy part, on the scale of the bare phonon frequency ΩΩΩ, and a low energy peak at ω≪Ωω\ll Ωω≪Ω. Below the polaronic threshold, the high energy dispersion changes only modestly with temperature TTT, while the broadening, arising from mode coupling, increases linearly with TTT at low temperature. The low energy peak shows up at strong coupling and finite temperature and arises from the slow tunneling of polarons. The tunneling events become spatially correlated as electron density increases towards half-filling, and the weight becomes strongly momentum and temperature dependent. We suggest the analytic basis of these results.