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arXiv:2007.16201 · Physical review. B./Physical review. B

Impact ionization and multiple photon absorption in the two-dimensional photoexcited Hubbard model

Florian Maislinger, Hans Gerd Evertz

Published Jan 11, 2022• 9 citations
arXivHTMLPDF

Abstract

We study the nonequilibrium response of a $4\ifmmode\times\else\texttimes\fi{}3$ Hubbard model at $U=8$ under the influence of a short electric field pulse, with the main focus on multiple photon excitations and on the change of double occupancy after the pulse. The behavior mainly depends on the driving frequency of the electric field. The largest change of double occupancy occurs during the pulse. For frequencies below the Mott gap, we observe multiphoton excitations at large field intensities. For frequencies beyond the gap energy, there is a region where Auger recombination reduces the double occupancy after the pulse. Impact ionization (multiexciton generation), namely, a growing double occupancy after the pulse, occurs for frequencies larger than twice the Mott gap. From the Loschmidt amplitude, we compute the eigenstate spectrum of the quantum state after the pulse, observing multiple distinct photon excitation peaks, in line with expectations from a quasiparticle picture. We introduce a technique with which we analyze the time evolution of double occupancy in each peak individually. The long-term behavior of the double occupancy almost only depends on the absorbed energy, and we explore the connection of this property to the eigenstate thermalization hypothesis.

DOI
10.1103/physrevb.105.045114

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We study the nonequilibrium response of a 4\ifmmode×\else\texttimes\fi34\ifmmode\times\else\texttimes\fi{}34\ifmmode×\else\texttimes\fi3 Hubbard model at U=8U=8U=8 under the influence of a short electric field pulse, with the main focus on multiple photon excitations and on the change of double occupancy after the pulse. The behavior mainly depends on the driving frequency of the electric field. The largest change of double occupancy occurs during the pulse. For frequencies below the Mott gap, we observe multiphoton excitations at large field intensities. For frequencies beyond the gap energy, there is a region where Auger recombination reduces the double occupancy after the pulse. Impact ionization (multiexciton generation), namely, a growing double occupancy after the pulse, occurs for frequencies larger than twice the Mott gap. From the Loschmidt amplitude, we compute the eigenstate spectrum of the quantum state after the pulse, observing multiple distinct photon excitation peaks, in line with expectations from a quasiparticle picture. We introduce a technique with which we analyze the time evolution of double occupancy in each peak individually. The long-term behavior of the double occupancy almost only depends on the absorbed energy, and we explore the connection of this property to the eigenstate thermalization hypothesis.
Using the time-dependent Lanczos method, we study the nonequilibrium dynamics of the half-filled one-dimensional ionic Hubbard model, deep within the Mott insulating regime, under the influence of a transient laser pulse. In equilibrium, increasing the staggered potential in the Mott regime reduces the Mott gap and broadens the Hubbard bands, creating favorable conditions for impact ionization. After laser excitation, impact ionization is observed, with its occurrence depending on both the staggered potential and the laser pump frequency. By analyzing the time evolution of the kinetic, ionic, and Coulomb interaction energies, we identify a novel mechanism for impact ionization, in which excess ionic potential energy is converted into additional double occupancy-distinct from the conventional mechanism where excess kinetic energy drives this process. We further reveal that impact ionization arises from interference between excited states driven by photon excitations of the same order. These results present a new pathway for realizing impact ionization in strongly correlated electron systems.
We study photoexcitations in small Hubbard clusters of up to 12 sites. After the electric field pulse some of these clusters show an increase of the double occupation through impact ionization. We treat the time-dependent electromagnetic field classically and calculate time evolution by exact diagonalization. As a tool for better analyzing the out-of-equilibrium dynamics, we generalize the Loschmidt amplitude. In this way we are able to resolve which many-body energy eigenstates are responsible for impact ionization and which ones show pronounced changes in the double occupation and spin energy. Our analysis reveals that the increase of spin energy is of little importance for impact ionization. We further demonstrate that, for one-dimensional chains, the optical conductivity has a characteristic peak structure originating solely from vertex corrections.
We study the influence of the pulse energy and fluence on the thermalization of photodoped Mott insulators. If the Mott gap is smaller than the width of the Hubbard bands, the kinetic energy of individual carriers can be large enough to produce additional doublon-hole pairs via a process analogous to impact ionization. The thermalization dynamics, which involves an adjustment of the doublon and hole densities, thus changes as a function of the energy of the photo-doped carriers and exhibits two time scales: a fast relaxation related to the impact ionization of high-energy carriers and a slower time scale associated with higher-order scattering processes. The slow dynamics depends more strongly on the gap size and the photodoping concentration.
Abstract Motivated by the recent progress in time-resolved nonequilibrium spectroscopy in condensed matter, we study an optically excited one-dimensional ionic Hubbard model by exact diagonalization. The model is relevant to organic crystals, transition metal oxides, or ultracold atoms in optical lattices. We implement numerical pump-probe measurements to calculate time-dependent conductivity and single-particle spectral functions. In general, short optical excitation induces a metallic behavior imprinted as a Drude peak in conductivity or an in-gap density of states. In a Mott insulator, we find that the induced Drude peak oscillates at the pump frequency and its second harmonic. The former comes from the oscillation of currents, and the latter from the interference of single- and three-photon excited states. In a band insulator, the Drude peak oscillates only at the pump frequency, and quantities such as the double occupancy do not oscillate. The absence of the second harmonic oscillation is due to the degeneracy of multi-photon excited states. The in-gap density of states in both insulators correlates with the Drude weight and the energy absorption for weak pumping. Strong pumping leads to saturation of the in-gap density of states and to suppression of the Drude weight in the Mott regime. We have also checked that the above features are robust for insulators in the intermediate parameter range. Our study demonstrates the distinct natures of the multi-photon excited states in two different insulators.
We use nonequilibrium dynamical mean-field theory in combination with a recently implemented strong-coupling impurity solver to investigate the relaxation of a Mott insulator after a laser excitation with frequency comparable to the Hubbard gap. The time evolution of the double occupancy exhibits a crossover from a strongly damped transient at short times toward an exponential thermalization at long times. In the limit of strong interactions, the thermalization time is consistent with the exponentially small decay rate for artificially created doublons, which was measured in ultracold atomic gases. When the interaction is comparable to the bandwidth, however, the double occupancy thermalizes within a few times the inverse bandwidth along a rapid thermalization path in which the exponential tail is absent. Similar behavior can be observed in time-resolved photoemission spectroscopy. Our results show that a simple quasi-equilibrium description of the electronic state breaks down for pump-excited Mott insulators characterized by strong interactions.
Doublon-holon dynamics is investigated in a pumped one-dimensional Hubbard model with a staggered on-site Coulomb interaction at half-filling. When the system parameters are set to be in the Mott-insulating regime the equilibrium sublattice density of states exhibits several characteristic peaks, corresponding to the lower and upper Hubbard bands as well as hybridization bands. We study the linear absorption spectrum and find two main peaks characterizing the photon frequencies which excite the ground state to an excited state. For a system driven by a laser pulse with general intensity and frequency, both the energy absorption and the doublon-holon dynamics exhibit distinct behaviors as a function of laser amplitude and frequency. Single-photon processes are observed at low laser intensity where the energy is absorbed for resonant laser frequencies. For strong laser intensity multiphoton-induced dynamics are observed in the system that are confirmed by an evaluation of the Loschmidt amplitude. The contribution of multiphoton processes to site-resolved double occupancy is also characterized by the generalized Loschmidt amplitude. The site-resolved doublon-holon dynamics are observed in both the one and multiphoton processes and the site-resolved behavior is explained within a quasiparticle picture. Our study suggests strategies to optically engineer the doublon-holon dynamics in one-dimensional strongly correlated many-body systems.