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arXiv:2201.06879 · Physical Review A

Correlation effects in high-order harmonic generation from finite systems

Thomas Hansen, Simon Vendelbo Bylling Jensen, Lars Bojer Madsen

Published May 23, 2022• 28 citations
arXivHTMLPDF

Abstract

Using the Hubbard model we study how the process of high-order harmonic generation (HHG) is modified by electron-electron correlation for both finite and bulk systems. A finite-size enhancement of the HHG signal is found and attributed to electrons backscattering off the lattice edges. Additionally, with the increasing strength of the electron-electron correlation an enhancement of the high-frequency regime of the HHG spectrum is found. This is attributed to the on-site Coulomb repulsion between electrons giving rise to a localized correlation-induced quiver motion of the electrons. The finite-lattice enhancement dominates the HHG spectra from a few harmonic orders until a threshold from which the correlational enhancement dominates. This threshold is determined by the degree of correlation and decreases into the low-frequency regime for increasing electron-electron correlation. This infers that as the electron-electron correlation increases, the finite-size effect on the electron dynamics decreases.

DOI
10.1103/physreva.105.053118

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Using the Hubbard model we study how the process of high-order harmonic generation (HHG) is modified by electron-electron correlation for both finite and bulk systems. A finite-size enhancement of the HHG signal is found and attributed to electrons backscattering off the lattice edges. Additionally, with the increasing strength of the electron-electron correlation an enhancement of the high-frequency regime of the HHG spectrum is found. This is attributed to the on-site Coulomb repulsion between electrons giving rise to a localized correlation-induced quiver motion of the electrons. The finite-lattice enhancement dominates the HHG spectra from a few harmonic orders until a threshold from which the correlational enhancement dominates. This threshold is determined by the degree of correlation and decreases into the low-frequency regime for increasing electron-electron correlation. This infers that as the electron-electron correlation increases, the finite-size effect on the electron dynamics decreases.
The key optical and electronic functionalities in condensed materials are determined by the band filling of electrons and their Coulomb correlations. To directly capture how many-body correlations influence the correlated electron dynamics under the driving of laser pulses, the comprehensible quasiparticle picture is desired to distinguish the ultrafast creation and annihilation of doublon-holon pairs in attosecond timescale. Here, we adopt the one-dimensional non-half-filling Hubbard model to study the high-harmonic generation (HHG) in correlated electron systems. As the value of Hubbard UUU increases, the cutoff energy and spectral features in HHG spectra have been revealed and their scaling laws are explained by the characteristic energy gaps obtained from the electronic bands under the quasiparticle picture. The adjustable degree of band filling in correlated systems paves a way to enhance high-harmonic emissions by regulating the creation of doublon-holon pairs. The complex temporal profile of HHG is elucidated in this work by the light-induced evolution of quasiparticle bands in correlated materials. In addition, the dephasing of the HHG spectrum caused by the vibration-induced disorder or lattice temperature is affirmed in the correlated electron systems and this dephasing process is attributed to quasiparticle-lattice scattering during the doublons and holons propagating among the disordered lattice sites.
The spectra produced by high-order harmonic generation (HHG) typically exhibit well-defined peaks at odd integers times the laser frequency. However, in recent investigations of HHG from correlated materials, spectra exhibit signals at noninteger harmonics which do not conform to the well-known symmetry-based selection rules for HHG spectra. Here, we use the Fermi-Hubbard model to study HHG from a linear chain of atoms. This model allows us to study both the correlated and uncorrelated phases through a specification of the amount of onsite electron-electron repulsion. The presence of signal at noninteger harmonics can be interpreted as originating from the population of multiple Floquet states. We show how this coupling to different Floquet states depends on the characteristics of the driving pulse and the strength of the electron-electron interaction in the system.
Using the one-dimensional Fermi-Hubbard model we study the effects of lattice imperfections on high-harmonic generation (HHG) from correlated systems. We simulate such imperfections by randomly modifying the chemical potential across the individual lattice sites. We control the degree of correlation by varying the Hubbard UUU. In the limit of vanishing UUU, this approach results in Anderson localization. For non-vanishing UUU, we explain the spectral observations using a qualitative picture in which correlation and the imperfections may balance each other out, causing Bloch-like transitions, i.e., transitions similar to those occurring in the case with small or vanishing UUU and with vanishing imperfection-induced energy gaps, even though the dynamics take place under conditions of high UUU and severe imperfections. We verify this picture by studying HHG spectra where imperfections are found to cause gain in the HHG spectra. The spectral gain is mainly in high harmonic orders for low correlation and low harmonic orders for high correlation. We explain this using the following qualitative picture. For low correlation, the addition of imperfections gives rise to significant energy gaps in the system, corresponding to high harmonics, and when the correlation is massive the addition of imperfections balances out the correlation, resulting in smaller energy gaps, meaning lower harmonic orders. We further demonstrate how in the unbalanced cases, i.e., high UUU and relatively small amount of imperfection or vice versa, the dynamics are largely adiabatic, and how in the balanced cases, with similar magnitude of correlation and imperfection, the dynamics are qualitatively similar.
Using the one-dimensional Hubbard model, which is commonly used for describing, e.g., high-Tc{T}_{c}Tc​ superconducting cuprates, we study high-harmonic generation (HHG) from doped, correlated materials. Doping is modeled by changing the number of electrons in the lattice from the conventional half-filling case. For relatively small Hubbard UUU, i.e., small electron-electron correlation, we find little to no effect of doping on the dynamics and the HHG spectra. For increasing UUU the degree of doping has a marked effect on the dynamics and spectra. We explain these findings through the quasiparticle-based doublon-holon picture. The dynamics are separated into two types, first, doublon and holon movement, and, second, doublon-holon pair creation and annihilation. Doping results in all configurations containing doublons or holons. Those quasiparticles can move at no extra cost in energy regardless of the correlation level. This motion at no energy cost increases the high-harmonic gain for low- and medium-harmonic orders. We discuss that in the high-UUU limit, antiferromagnetic ordering becomes increasingly unlikely with increasing doping rates and explain an associated drop in the high-order harmonics relative to the case of half-filling.
Abstract We study effects of lattice imperfections on high-harmonic generation from correlated systems using the Fermi–Hubbard model. We simulate such imperfections by randomly modifying the chemical potential across the individual lattice sites. We control the degree of electron–electron interaction by varying the Hubbard U. In the limit of vanishing U, this approach results in Anderson localization. For nonvanishing U, we rationalize the spectral observations in terms of qualitative k-space and real-space pictures. When the interaction and imperfection terms are of comparable magnitude, they may balance each other out, causing Bloch-like transitions. If the terms differ significantly, each electron transition requires a relatively large amount of energy and the current is reduced. We find that imperfections result in increased high-harmonic gain. The spectral gain is mainly in high harmonic orders for low U and low orders for high U.
High harmonic generation in crystalline solids has been examined so far on the basis of one-body energy-band structures arising from electron itineracy in a periodic potential. Here, we show the emergence of high harmonic generation signals which are attributed to the dynamics of many-body states in a low-dimensional correlated electron system. An interacting fermion model and its effective pseudospin model on a one-dimensional dimer-type lattice are analyzed. Observed high harmonic generation signals in a spontaneously symmetry-broken state, where charge densities are polarized inside of dimer units, show threshold behavior with respect to light amplitude and are interpreted in terms of tunneling and recombination of kink-antikink excitations in an electric field.