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arXiv:1206.0110 · Physical Review Letters

Quantum Dynamics of the Hubbard-Holstein Model in Equilibrium and Nonequilibrium: Application to Pump-Probe Phenomena

G. De Filippis, V. Cataudella, Elizabeth Nowadnick, Thomas Devereaux, Andrei S. Mishchenko, Naoto Nagaosa

Published Oct 23, 2012• 81 citations
arXivHTMLPDF

Abstract

The spectral response and physical features of the 2D Hubbard-Holstein model are calculated both in equilibrium at zero and low chemical dopings, and after an ultrashort powerful light pulse, in undoped systems. At equilibrium and at strong charge-lattice couplings, the optical conductivity reveals a three-peak structure in agreement with experimental observations. After an ultrashort pulse and at nonzero electron-phonon interaction, phonon and spin subsystems oscillate with the phonon period T(ph)≈80 fs. The decay time of the phonon oscillations is about 150-200 fs, similar to the relaxation time of the charge system. We propose a criterion for observing these oscillations in high T(c) compounds: the time span of the pump light pulse τ(pump) has to be shorter than the phonon oscillation period T(ph).

DOI
10.1103/physrevlett.109.176402

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The spectral response and physical features of the 2D Hubbard-Holstein model are calculated both in equilibrium at zero and low chemical dopings, and after an ultrashort powerful light pulse, in undoped systems. At equilibrium and at strong charge-lattice couplings, the optical conductivity reveals a three-peak structure in agreement with experimental observations. After an ultrashort pulse and at nonzero electron-phonon interaction, phonon and spin subsystems oscillate with the phonon period T(ph)≈80 fs. The decay time of the phonon oscillations is about 150-200 fs, similar to the relaxation time of the charge system. We propose a criterion for observing these oscillations in high T(c) compounds: the time span of the pump light pulse τ(pump) has to be shorter than the phonon oscillation period T(ph).
Nonequilibrium dynamics of interacting quantum many-body physics has recently attracted great attention. The authors address here the nonequilibrium dynamics of a single electron interacting through a Holstein-like coupling with dispersionless phonons on a one dimensional lattice. Using diagonalization in a limited functional space, they identify two different regimes: (1) the relaxation regime where, during a characteristic time scale, a net energy is transferred between the electronic and the phononic subsystem; and (2) the stationary regime, characterized by zero energy transfer and by persisting coherent oscillations in the dynamics of observables.
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.
Ultrafast pump-probe spectroscopy provides a powerful means to investigate electron-phonon (e-ph) interactions in strongly correlated systems. Nevertheless, the question of how different microscopic e-ph coupling mechanisms influence the lattice's nonequilibrium response has not been widely addressed. We perform time-dependent density matrix renormalization group simulations on a pumped one-dimensional Mott insulator coupled to phonons through either Holstein or Su-Schrieffer-Heeger (SSH) interactions. The electronic responses of the two models are qualitatively similar in the Mott-insulating regime and are governed by the same excitations and resonance conditions of the Hubbard model. In contrast, the lattice dynamics of the two models differ substantially. While the Hubbard-Holstein model exhibits long-lived coherent phonon oscillations when the pump resonates with the bare phonon frequency, no such oscillations are observed for the Hubbard-SSH model. These contrasting responses remain robust against changes in phonon frequency and pump parameters, suggesting that coherent lattice dynamics can provide a direct nonequilibrium probe of the microscopic form of e-ph coupling.
We theoretically study the pump-probe response of nonequilibrium BCS superconductors coupled to optical phonons. For ultrashort pump pulses a nonadiabatic regime emerges, which is characterized by oscillations of the superconducting order parameter as well as by the generation of coherent phonons. Using the density-matrix formalism, we compute the pump-probe response in the nonadiabatic regime of the coupled Bogoliubov quasiparticle-phonon system and determine the signatures of the order parameter and the phonon oscillations in the pump-probe conductivity. We find that the nonadiabatic dynamics of the BCS superconductor reflects itself in oscillations of the pump-probe response as functions of delay time $\ensuremath{\delta}t$ between pump and probe pulses. We argue that from the analysis of this oscillatory behavior both frequency and decay time of the algebraically decaying order-parameter oscillations can be inferred. Similarly, the coherent phonons are evidenced in the pump-probe conductivity by oscillations with the frequency of the phonons. Remarkably, we find that the oscillatory response in the pump-probe conductivity is resonantly enhanced when the frequency of the order-parameter oscillations is tuned to the phonon energy.
We calculate the spectral function of the one-dimensional Hubbard-Holstein model using the time-dependent density matrix renormalization group, focusing on the regime of large local Coulomb repulsion, and away from electronic half-filling. We argue that, from weak to intermediate electron-phonon coupling, phonons interact only with the electronic charge, and not with the spin degrees of freedom. For strong electron-phonon interaction, spinon and holon bands are not discernible anymore and the system is well described by a spinless polaronic liquid. In this regime, we observe multiple peaks in the spectrum with an energy separation corresponding to the energy of the lattice vibrations (i.e., phonons). We support the numerical results by introducing a well controlled analytical approach based on Ogata-Shiba's factorized wave function, showing that the spectrum can be understood as a convolution of three contributions, originating from charge, spin, and lattice sectors. We recognize and interpret these signatures in the spectral properties and discuss the experimental implications.
Pump-probe experiments have turned out as a powerful tool in order to study the dynamics of competing orders in a large variety of materials. The corresponding analysis of the data often relies on standard linear-response theory generalized to nonequilibrium situations. Here we examine the validity of such an approach for the charge and pairing response of systems with charge-density wave and (or) superconducting (SC) order. Our investigations are based on the attractive Hubbard model which we study within the time-dependent Hartree-Fock approximation. In particular, we calculate the quench and pump-probe dynamics for SC and charge order parameters in order to analyze the frequency spectra and the coupling of the probe field to the specific excitations. Our calculations reveal that the ``linear-response assumption'' is justified for small to moderate nonequilibrium situations (i.e., pump pulses) in the case of a purely charge-ordered ground state. However, the pump-probe dynamics on top of a superconducting ground state is determined by phase and amplitude modes which get coupled far from the equilibrium state indicating the failure of the linear-response assumption.