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arXiv:2312.09668

Two-particle correlation effects on nonlinear optical responses in the 1d interacting Rice-Mele model

Akira Kofuji, Robert Peters

Published Dec 15, 2023• 0 citations
arXivHTMLPDF

Abstract

Nonlinear responses in crystalline solids are attracting a great deal of attention because of exciting phenomena, such as the bulk photovoltaic effect in noncentrosymmetric crystals and the third harmonic generation related to Higgs modes in superconductors, and their potential applicability to electronic devices. Recently, nonlinear responses have also been studied in strongly correlated electron systems. Experimental evidence has revealed that correlations play a significant role in nonlinear responses. However, most theoretical calculations only consider excitonic effects or involve numerically demanding approaches, making interpreting the results challenging. In this paper, we adopt another approach, which is based on real-time evolution using the correlation expansion method. Particularly, we focus on the 1d interacting Rice-Mele model. We analyze the impact of the density-density interaction on the linear and nonlinear conductivities and demonstrate that two-particle correlations beyond the mean-field level enhance second-order nonlinear responses, especially the second harmonic generation, while the linear response is not strongly affected. Furthermore, by decomposing the current into a one-particle contribution and six two-particle contributions, we show that the ``biexciton transition" term and its nonlinear oscillations is the most dominant two-particle contribution to the nonlinear response. In addition, we also show that the intercell charge-charge correlation is strongly enhanced when the system is driven with the frequency corresponding to the excitonic peak and can even exceed the intracell correlation. This implies the possibility of manipulating two-particle correlations with external fields.

DOI
10.48550/arxiv.2312.09668

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Nonlinear responses in crystalline solids are attracting a great deal of attention because of exciting phenomena, such as the bulk photovoltaic effect in noncentrosymmetric crystals and the third harmonic generation related to Higgs modes in superconductors, and their potential applicability to electronic devices. Recently, nonlinear responses have also been studied in strongly correlated electron systems. Experimental evidence has revealed that correlations play a significant role in nonlinear responses. However, most theoretical calculations only consider excitonic effects or involve numerically demanding approaches, making interpreting the results challenging. In this paper, we adopt another approach, which is based on real-time evolution using the correlation expansion method. Particularly, we focus on the 1d interacting Rice-Mele model. We analyze the impact of the density-density interaction on the linear and nonlinear conductivities and demonstrate that two-particle correlations beyond the mean-field level enhance second-order nonlinear responses, especially the second harmonic generation, while the linear response is not strongly affected. Furthermore, by decomposing the current into a one-particle contribution and six two-particle contributions, we show that the ``biexciton transition" term and its nonlinear oscillations is the most dominant two-particle contribution to the nonlinear response. In addition, we also show that the intercell charge-charge correlation is strongly enhanced when the system is driven with the frequency corresponding to the excitonic peak and can even exceed the intracell correlation. This implies the possibility of manipulating two-particle correlations with external fields.
Nonlinear responses in crystalline solids are attracting a great deal of attention because of exciting phenomena, such as the bulk photovoltaic effect in noncentrosymmetric crystals and the third-harmonic generation related to Higgs modes in superconductors, and their potential applicability to electronic devices. Recently, nonlinear responses have also been studied in strongly correlated electron systems. Experimental evidence has revealed that correlations play a significant role in nonlinear responses. However, most theoretical calculations only consider excitonic effects or involve numerically demanding approaches, making interpreting the results challenging. In this paper, we adopt another approach, which is based on real-time evolution using the correlation expansion method. We focus in particular on the one-dimensional interacting Rice-Mele model. We analyze the impact of the density-density interaction on the linear and nonlinear conductivities, and we demonstrate that two-particle correlations beyond the mean-field level enhance second-order nonlinear responses, especially the second-harmonic generation, while the linear response is not strongly affected. Furthermore, by decomposing the current into a one-particle contribution and six two-particle contributions, we show that the ``biexciton transition'' term and its nonlinear oscillations are the most dominant two-particle contribution to the nonlinear response. In addition, we also show that the intercell charge-charge correlation is strongly enhanced when the system is driven with the frequency corresponding to the excitonic peak, and it can even exceed the intracell correlation. This implies the possibility of manipulating two-particle correlations with external fields.
For both, fundamental physics and novel applications, nonlinear effects are crucial.Powerful laser fields require to treat mobile electrons beyond linear response theory.Phenomena familiar from nonlinear optics are manifest in ultracold Rydberg systems, which have a high potential for advancing the understanding of many-body physics via quantum simulations and promote progress in quantum computation and -information.Various devices and plasmonics systems are based on thin, nearly two dimensional (2D) layers, such as quantum wells, graphene-like structures or transition metal dichalcogenides.We here derive an expression for nonlinear response functions in arbitrary order, and evaluate it explicitly in 2D for the quadratic and the cubic density response of non-interacting fermions.As correlations are of enhanced importance in low dimensions, we next incorporate screened interactions.This results in the generation of 2nd and 3rd harmonics of the collective modes (zero sound and plasmons), damped by multiple particle-hole continua.
Summary form only given. The ultrafast nonlinear optical response of semiconductor-microcavities (SMCs) in the nonperturbative regime is attracting growing interest for exploring fundamental light-matter interactions in many-particle quantum systems, as well as for the future implementations of ultrafast photonic devices. In spite of many investigations, the coherent dynamics of excitonic nonlinear-response in the nonperturbative regime has not been fully understood. Open questions are how strong exciton-cavity coupling affects exciton-exciton (X-X) interactions, and how in turn the X-X correlation influences the nonlinear response of SmCs. We investigate these open questions and show that the nonperturbative regime provides an unprecedented tool for investigating four-particle correlations.We start from the equations for the third order exciton polarization and cavity field describing quantum optical effects and coherent nonlinear optics in SMCs, perform the semiclassical factorization and include multiple scattering processes.
Nonlinear responses in condensed matter are intensively studied because they provide rich information about materials and hold the possibility of being applied in diodes or high-frequency optical devices. While nonlinear responses in noninteracting models have been explored widely, the effect of strong correlations on the nonlinear response is still poorly understood, even though it has been suggested that correlations can enhance the nonlinear response. In this work, we first give an analytical derivation of nonlinear responses using the Green's function methods at finite temperature. Then, we discuss the difficulties of considering dissipation using conventional methods, such as the reduced density matrix method. We reveal that the relaxation time approximation leads to severe limitations when considering optical responses. Finally, we demonstrate that correlation effects, such as the renormalization of the band structure and different lifetime in orbitals or sublattices, can significantly enhance nonlinear responses and can even change the sign of the nonlinear conductivity.
Nonlinear responses in condensed matter are intensively studied because they provide rich information about the materials and hold the possibility of being applied in diodes or high-frequency optical devices. While nonlinear responses in noninteracting models have been explored widely, the effect of strong correlations on the nonlinear response is still poorly understood, even though it has been suggested that correlations can enhance the nonlinear response. In this work, we first give an analytical derivation of nonlinear responses using Green's function methods at finite temperature. Then, we discuss the difficulties of considering dissipation using conventional methods, such as the reduced density matrix method. We reveal that the relaxation time approximation leads to severe limitations when considering optical responses. Finally, we demonstrate that correlation effects, such as the renormalization of the band structure and different lifetimes in orbitals or sublattices, can significantly enhance nonlinear responses and even change the sign of the nonlinear conductivity.
In recent years, the study of phenomena pertaining to non-linear properties of materials has seen a major upswing - especially in the context of High Harmonic Generation (HHG). In this thesis, an account of the current state of research in this area will be given. In addition, we seek to combine two seemingly disparate areas of research, both of which have been the subject of numerous years of intense research - namely those of HHG in solid state materials, and the optical response of strongly correlated quantum systems. To this end we will rely on solving the Fermi-Hubbard model coupled to an electromagnetic field under time propagation. With the aid of both numerical work and simple energy level analyses, we are able to explain most of the characteristics of our calculated spectra. High field strength will induce a Mott insulator to metal phase transition whose imprints will be established through time resolved high harmonic emission and doublon and spin correlation functions. The various HHG spectra, together with said correlation functions will be studied through an Exact diagonalization algorithm in conjunction with an Arnoldi-Lanczos time propagator. The parameter space considered is comprised of the electron-electron repulsion energy, U, and peak electric field strength. Additionally, the study is not restricted to half-filling, and results for doped materials will be presented. We find that the high U-induced energy gap in the Fermi-Hubbard model plays the same role as the valence-conduction bandgap in models like for instance the Semiconductor Bloch Equations when it comes to generating high harmonic radiation through multiphoton processes. The central part of this thesis aims at providing insight to and making further contributions to an article published in Nature Photonics in March 2018. [1]