Dynamical Slowing-Down in an Ultrafast Photoinduced Phase Transition
Alfred Zong, Pavel E. Dolgirev, Anshul Kogar, Emre Ergeçen, Mehmet Burak Yilmaz, Ya‐Qing Bie, Timm Rohwer, I‐Cheng Tung, Joshua A. W. Straquadine, Xirui Wang, Yafang Yang, Xiaozhe Shen, Renkai Li, Jie Yang, Suji Park, Matthias C. Hoffmann, Benjamin K. Ofori-Okai, M. Kozina, Haidan Wen, Xijie J. Wang, I. R. Fisher, Pablo Jarillo‐Herrero, Nuh Gedik
Complex systems, which consist of a large number of interacting constituents, often exhibit universal behavior near a phase transition. A slowdown of certain dynamical observables is one such recurring feature found in a vast array of contexts. This phenomenon, known as critical slowing-down, is well studied mostly in thermodynamic phase transitions. However, it is less understood in highly nonequilibrium settings, where the time it takes to traverse the phase boundary becomes comparable to the timescale of dynamical fluctuations. Using transient optical spectroscopy and femtosecond electron diffraction, we studied a photoinduced transition of a model charge-density-wave (CDW) compound LaTe_{3}. We observed that it takes the longest time to suppress the order parameter at the threshold photoexcitation density, where the CDW transiently vanishes. This finding can be captured by generalizing the time-dependent Landau theory to a system far from equilibrium. The experimental observation and theoretical understanding of dynamical slowing-down may offer insight into other general principles behind nonequilibrium phase transitions in many-body systems.
Complex systems, which consist of a large number of interacting constituents, often exhibit universal behavior near a phase transition. A slowdown of certain dynamical observables is one such recurring feature found in a vast array of contexts. This phenomenon, known as critical slowing-down, is well studied mostly in thermodynamic phase transitions. However, it is less understood in highly nonequilibrium settings, where the time it takes to traverse the phase boundary becomes comparable to the timescale of dynamical fluctuations. Using transient optical spectroscopy and femtosecond electron diffraction, we studied a photoinduced transition of a model charge-density-wave (CDW) compound LaTe_{3}. We observed that it takes the longest time to suppress the order parameter at the threshold photoexcitation density, where the CDW transiently vanishes. This finding can be captured by generalizing the time-dependent Landau theory to a system far from equilibrium. The experimental observation and theoretical understanding of dynamical slowing-down may offer insight into other general principles behind nonequilibrium phase transitions in many-body systems.
We investigate the laser-induced dynamics of electronically driven charge-density-wave (CDW) order. A comprehensive mean-field analysis of the attractive Hubbard model in the weak-coupling regime reveals ultrafast switching and ultrafast melting of the order via a nonthermal pathway. The resulting nonequilibrium phase diagram exhibits multiple distinct regimes of the order parameter dynamics upon increasing field strength, indicative of multiple dynamical phase transitions. Using an intuitive pseudospin picture, we show how the distinct dynamical regimes can be connected to the spin precession angle. We furthermore study the effects of electron-electron interactions beyond mean field to show that the main features of the phase diagram are robust against scattering or thermalization processes. For example, the nonthermal state with switched order is characterized by a particularly slow relaxation. The nonthermal phases can be stabilized by tailoring the pulse shape with optimal control theory. We also demonstrate how the dynamics allows to distinguish an electron-electron interaction driven CDW from an electron-phonon interaction driven CDW.
We investigate the out-of-equilibrium dynamics of a photoexcited charge-density-wave (CDW) state in the square-lattice Holstein model, in a setup similar to a pump-probe experiment. At half-filling, the ground state of this system is characterized by a checkerboard modulation of particle densities, accompanied by a concomitant lattice distortion. An efficient real-space dynamics method integrating the von Neumann equation for electron density matrix and Newton equation for classical lattice dynamics is developed to simulate the dynamical evolution of a photoexcited Holstein system. We find that the energy injected by a short pump pulse results in the reduction of the CDW order and the generation of coherent phonons. At strong photoexcitations, while the CDW order is melted in the sense that the time-averaged order parameter vanishes, a dynamical CDW state is self-sustained by the strong coherent phonon oscillations. Our large-scale simulations further uncover a dynamical regime of intermediate fluence where complex pattern formation is induced by the pump pulse. The emergent spatial textures are characterized by super density modulations on top of the short-range checkerboard CDW order. Our demonstration of pattern formation highlights the significance of dynamical inhomogeneity in quantum many-body systems in pump-probe experiments.
We investigate the nonequilibrium dynamics of the spinless Haldane model with nearest-neighbor interactions on the honeycomb lattice by employing an unbiased numerical method. In this system, a first-order transition from the Chern insulator at weak coupling to the charge-density-wave (CDW) phase at strong coupling can be characterized by a level crossing of the lowest energy levels. Here we show that if adiabatically following the eigenstates across this level crossing, their Chern numbers are preserved, leading to the identification of a topologically nontrivial low-energy excited state in the CDW regime. By promoting a resonant energy excitation via an ultrafast circularly polarized pump pulse, we find that the system acquires a nonvanishing Hall response as a result of the large overlap enhancement between the time-dependent wave function and the topologically nontrivial excited state. This response is suggestive of a photoinduced topological phase transition via unitary dynamics, despite a proper definition of the Chern number remaining elusive for an out-of-equilibrium interacting system. We contrast these results with more common quench protocols in which such features are largely absent in the dynamics even if the postquench Hamiltonian displays a topologically nontrivial ground state.
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.
The interaction of time-dependent electromagnetic fields with electrons in quantum materials can give rise to many both fundamentally interesting as well as technologically relevant phenomena like transient band structure manipulations or the emergence of prethermal states of matter, which are not a result of heating. This thesis contributes theoretical insights to both these topics: We model the interference of Floquet and Volkov side bands, which are a result of the dressing of electron states by light, in a time-resolved angle-resolved photoemission spectroscopy (ARPES) experiment. Furthermore, we analyze the emergence of a band-like feature in the non-equilibrium spectral function of a one-dimensional charge-density wave insulator upon periodic driving. Secondly, we use the fermionic truncated Wigner approximation (fTWA), a phase space method for the time evolution of interacting fermions, to study the light-induced order parameter dynamics in SU(N)-symmetric fermionic lattice models. By comparison with exact analytical results for an interaction quench in the Hubbard model, we find that dephasing-induced prethermalization is correctly described by fTWA. We discuss photoinduced prethermal transitions between competing phases of matter in the large-N Hubbard-Heisenberg model and find a pronounced frequency-dependence of the transition. This work contributes to a better understanding of photoinduced order parameter dynamics from a microscopic perspective.
We theoretically investigate the transient spectral function during the photoinduced melting of charge order in a correlated electron system, to unravel the dynamical processes triggered by different initial excitations. We employ a one-dimensional interacting spinless fermion model introducing a pulsed laser light, and perform a comparative study by the Hartree-Fock approximation and by the exact diagonalization method to numerically solve the time-dependent Schrödinger equation. We find characteristic behavior in the transient spectral function, whose features strongly depend on the pump light frequency ωp. When ωp is resonant with the collective phase mode of frequency Ωc≃ΔCO/2, where ΔCO is the charge gap, the transient spectral function exhibits a photoinduced in-gap weight which triggers large responses. With increasing the laser intensity, the development of in-gap weight directly turns into the collapse of the gap. This charge-order destabilization process is in sharp contrast to the case of ωp>ΔCO, where the photoirradiation induces interband electron-hole excitations giving rise to a shrinkage of the gap. The impact of quantum fluctuations and spatial inhomogeneity on the photoinduced dynamics is also discussed.