The non-equilibrium dynamics of matter excited by light may produce electronic phases, such as laser-induced high-transition-temperature superconductivity, that do not exist in equilibrium. Here we simulate the dynamics of a metal driven at initial time by a spatially uniform pump that excites dipole-active vibrational modes which couple nonlinearly to electrons. We provide evidence for rapid loss of spatial coherence, leading to emergent effective disorder in the dynamics, which arises in a system unitarily evolving under a translation-invariant Hamiltonian, and dominates the electronic behavior as the system evolves towards a correlated electron-phonon long-time state, possibly explaining why transient superconductivity is not observed. Our framework provides a basis within which to understand correlation dynamics in current pump-probe experiments of vibrationally coupled electrons, highlight the importance of the evolution of phase coherence, and demonstrate that pumped electron-phonon systems provide a means of realizing dynamically induced disorder in translation-invariant systems.
The non-equilibrium dynamics of matter excited by light may produce electronic phases, such as laser-induced high-transition-temperature superconductivity, that do not exist in equilibrium. Here we simulate the dynamics of a metal driven at initial time by a spatially uniform pump that excites dipole-active vibrational modes which couple nonlinearly to electrons. We provide evidence for rapid loss of spatial coherence, leading to emergent effective disorder in the dynamics, which arises in a system unitarily evolving under a translation-invariant Hamiltonian, and dominates the electronic behavior as the system evolves towards a correlated electron-phonon long-time state, possibly explaining why transient superconductivity is not observed. Our framework provides a basis within which to understand correlation dynamics in current pump-probe experiments of vibrationally coupled electrons, highlight the importance of the evolution of phase coherence, and demonstrate that pumped electron-phonon systems provide a means of realizing dynamically induced disorder in translation-invariant systems.
Light offers a route to engineer new phases of matter far from equilibrium, including transient states suggestive of superconducting, charge-ordered, and excitonic ordering behavior. Yet it remains unclear how optical excitation can dynamically produce long-range phase coherence-a defining feature of true order such as superconductivity-rather than merely enhancing local pairing. Here we show that impulsively driven low-frequency phonons enhance long-range electronic correlations in a low-dimensional metal. Through numerically exact simulations, we demonstrate that slow phonons suppress dynamical disorder, enabling buildup of coherence and enhancement of charge (and pairing) orders. These findings provide direct evidence that light can mediate enhancement of long-range order and suggest that future experimental strategies-such as the design of selective excitations of narrow phonon distributions to limit dephasing-may offer viable routes to design and stabilize transient superconducting states.
We investigate an exact nonequilibrium solution of a two-site electron-phonon model, where an infrared-active phonon that is nonlinearly coupled to the electrons is driven by a laser field. The time-resolved electronic spectrum shows coherence-incoherence spectral weight transfer, a clear signature of light-enhanced electron-phonon coupling. The present study is motivated by recent evidence for enhanced electron-phonon coupling in pump-probe terahertz and angle-resolved photoemission spectroscopy in bilayer graphene when driven near resonance with an infrared-active phonon mode [E. Pomarico et al., Phys. Rev. B 95, 024304 (2017)], and by a theoretical study suggesting that transient electronic attraction arises from nonlinear electron-phonon coupling [D. M. Kennes et al., Nat. Phys. 13, 479 (2017)]. We show that a linear scaling of light-enhanced electron-phonon coupling with the pump field intensity emerges, in accordance with a time-nonlocal self-energy based on a mean-field decoupling using quasiclassical phonon coherent states. Finally, we demonstrate that this leads to enhanced double occupancies in accordance with an effective electron-electron attraction. Our results suggest that materials with strong phonon nonlinearities provide an ideal playground to achieve light-enhanced electron-phonon coupling and possibly light-induced superconductivity.
Studies on out-of-equilibrium dynamics have paved a way to realize a new state of matter. Superconductor-like properties above room temperatures recently suggested to be in copper oxides achieved by selectively exciting vibrational phonon modes by laser have inspired studies on an alternative and general strategy to be pursued for high-temperature superconductivity. We show that the superconductivity can be enhanced by irradiating laser to correlated electron systems owing to two mechanisms: First, the effective attractive interaction of carriers is enhanced by the dynamical localization mechanism, which drives the system into strong coupling regions. Second, the irradiation allows reaching uniform and enhanced superconductivity dynamically stabilized without deteriorating into equilibrium inhomogeneities that suppress superconductivity. The dynamical superconductivity is subject to the Higgs oscillations during and after the irradiation. Our finding sheds light on a way to enhance superconductivity that is inaccessible in equilibrium in strongly correlated electron systems.
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.
We study, by means of the time-dependent Gutzwiller approximation, the out-of-equilibrium dynamics of a half-filled Hubbard-Holstein model of correlated electrons interacting with local phonons. Inspired by pump-probe experiments, where intense light pulses selectively induce optical excitations that trigger a transient out-of-equilibrium dynamics, here we inject energy in the Hubbard bands by a nonequilibrium population of empty and doubly-occupied sites. We first consider the case of a global perturbation, acting over the whole sample, and find evidence of a mean-field dynamical transition where the lattice gets strongly distorted above a certain energy threshold, despite the weak strength of the electron-phonon coupling by comparison with the Hubbard repulsion. Next, we address a slab geometry for a correlated heterostructure and study the relaxation dynamics across the system when the perturbation acts locally on the first layer. While for weak deviations from equilibrium the excited surface is able to relax by transferring its excess energy to the bulk, for large deviations, the excess energy stays instead concentrated in the surface layer. This self-trapping occurs both in the absence as well as in the presence of electron-phonon coupling. Phonons actually enforce the trapping by distorting at the surface.
The time evolution of two classes of systems is studied with real time molecular dynamics simulations. The first consists of a coupled electron-lattice system. For a periodic system, we present results for the time evolution of a one-dimensional system consisting of an electron, described by a tight-binding Hamiltonian, and a harmonic lattice, coupled by a deformation-type potential. We solve numerically the nonlinear system of equations of motion for this model in order to study the effects of varying the electronic effective mass for several initial conditions and coupling strengths. A large effective mass favors localized polaron formation for initially localized electrons. For initially extended electronic states, increasing the effective mass of an electron initially close to the bottom of the band makes localization more difficult, while for an initially highly excited electron, localized polaron formation is possible only when the electronic effective mass and the atomic masses of the lattice become of the same order. For a small parameter range, we find an impressive recurrence, a periodic and a complete exchange between the electronic and vibrational degrees of freedom of a small part of the initial electronic energy. The disordered case, described by a tight-binding model exhibiting metal-insulator transition (the diagonal matrix elements having a spatial variation incommensurate with the lattice), demonstrates the combined effects of disorder and electron-phonon interaction. The el-ph interaction has profound effects, especially on one-electron extended states just above the mobility edge, where the electronic states change from extended to localized. Polaron formation is facilitated close to the mobility edge and, in most cases, the localization length (lc) decreases upon increasing the disorder or el-ph coupling, as expected. However, for strongly localized states due to disorder or el-ph interaction, increase of el-ph coupling or disorder, respectively, results in an increase of lc. This increase is due to phonon assisted hopping. The second class of systems studied consists of carbon and hydrogen. We calculate phonon anharmonic effects in diamond and graphite using a tight-binding molecular dynamics scheme. Using one-phonon spectral intensities that have been calculated through the Fourier transform of the velocity-velocity correlation function, we study the temperature dependence of the phonon frequency shift and phonon linewidth. In the case of the zone-center optical mode of diamond where experimental data are available, our results are in good agreement with experiment. A tight-binding model for carbon-hydrogen interaction is developed and used in molecular dynamics simulations. The parameters are obtained by fitting to the electronic and vibrational properties of methane. The results obtained for hydrocarbon molecules are in good agreement with experimental data and first-principles results. Interstitial hydrogen in diamond is also studied with this model and the results are compared with available experimental and ab initio results. The case of hydrogenated amorphous carbon is considered as well.