By employing an unbiased numerical method, we investigate the ultrafast dynamics of the correlated systmes in one and two dimensions. For the extended Hubbard model on a periodic chain, the high-harmonic generation (HHG) of system close to the quantum critical point (QCP) is more intense than HHG in the neighboring two gapped phases, i.e., charge-density-wave and spin-density-wave states, especially in low-frequencies. The reason can be attributed to that the system in QCP is more sensitive to the external field and there are more optical-allowed excited states available to furnish photon-absorbing channels for this nonlinear processes. This feature provides a possibility of detecting the quantum phase transition by means of high-harmonic spectroscopy. We also expect to generate stronger HHG by irradiating materials with parameter settings close to QCP. In addition, we find that the even- or odd-order components of HHG can be used to distinguish the topologically ordered phases from locally ordered ones in a two-dimensional interacting Haldane model.
By employing an unbiased numerical method, we investigate the ultrafast dynamics of the correlated systmes in one and two dimensions. For the extended Hubbard model on a periodic chain, the high-harmonic generation (HHG) of system close to the quantum critical point (QCP) is more intense than HHG in the neighboring two gapped phases, i.e., charge-density-wave and spin-density-wave states, especially in low-frequencies. The reason can be attributed to that the system in QCP is more sensitive to the external field and there are more optical-allowed excited states available to furnish photon-absorbing channels for this nonlinear processes. This feature provides a possibility of detecting the quantum phase transition by means of high-harmonic spectroscopy. We also expect to generate stronger HHG by irradiating materials with parameter settings close to QCP. In addition, we find that the even- or odd-order components of HHG can be used to distinguish the topologically ordered phases from locally ordered ones in a two-dimensional interacting Haldane model.
By employing the exact diagonalization method, we investigate the high-harmonic generation (HHG) of the correlated systems under the strong laser irradiation. For the extended Hubbard model on a periodic chain, HHG close to the quantum critical point (QCP) is more significant compared to two neighboring gapped phases (i.e., charge-density-wave and spin-density wave states), especially in low frequencies. We confirm that the systems in the vicinity of the QCP are supersensitive to the external field and more optical-transition channels via excited states are responsible for HHG. This feature holds the potential of obtaining high-efficiency harmonics by making use of materials approaching QCP. Based on the two-dimensional Haldane model, we further propose that the even- or odd-order components of generated harmonics can be promisingly regarded as spectral signals to distinguish the topologically ordered phases from locally ordered ones. Our findings in this Letter pave the way to achieve ultrafast light source from HHG in strongly correlated materials and to study quantum phase transition by nonlinear optics in strong laser fields.
We report on the nonlinear optical signatures of quantum phase transitions in the high-temperature superconductor YBCO, observed through high harmonic generation. While the linear optical response of the material is largely unchanged when cooling across the phase transitions, the nonlinear optical response sensitively imprints two critical points, one at the critical temperature of the cuprate with the exponential growth of the surface harmonic yield in the superconducting phase and another critical point, which marks the transition from strange metal to pseudogap phase. To reveal the underlying microscopic quantum dynamics, a strong-field quasi-Hubbard model was developed, which describes the measured optical response dependent on the formation of Cooper pairs. Further, the theory provides insight into the carrier scattering dynamics and allows us to differentiate between the superconducting, pseudogap, and strange metal phases. The direct connection between nonlinear optical response and microscopic dynamics provides a powerful methodology to study quantum phase transitions in correlated materials. Further implications are light wave control over intricate quantum phases, light-matter hybrids, and application for optical quantum computing.
Different insulator phases compete with each other in strongly correlated materials with simultaneous local and non-local interactions. It is known that the homogeneous Mott insulator converts into a charge density wave (CDW) phase when the non-local interactions are increased, but there is ongoing debate on whether and in which parameter regimes this transition is of first order, or of second order with an intermediate bond-order wave phase. Here we show that strong-field optics applied to an extended Fermi-Hubbard system can serve as a powerful tool to reveal the nature of the quantum phase transition. Specifically, we show that in the strongly interacting regime characteristic excitations such as excitons, biexcitons, excitonic strings, and charge droplets can be tracked by the non-linear optical response to an ultrafast and intense laser pulse. Subcycle analysis of high harmonic spectra unravels the ultrafast dynamics of these increasingly complex objects, which partially escape the scrutiny of linear optics. Their appearance in the high harmonic spectrum provides striking evidence of a first-order transition into the CDW phase, and makes a strong case for using strong-field optics as a powerful tool to reveal the nature of quasiparticles in strongly correlated matter, and to track the electron dynamics during a first-order quantum phase transition.
High harmonic spectroscopy of quantum phase transitions in a high-Tc superconductor
We report on the new non--linear optical signatures of quantum phase transitions in the high-temperature superconductor YBCO, observed through high harmonic generation. While the linear optical response of the material is largely unchanged when cooling across the phase transitions, the nonlinear optical response sensitively imprints two critical points, one at the critical temperature of the cuprate with the exponential growth of the surface harmonic yield in the superconducting phase, and another critical point, which marks the transition from strange metal to pseudo gap phase. To reveal the underlying microscopic quantum dynamics, a novel strong-field quasi-Hubbard model was developed, which describes the measured optical response dependent on the formation of Cooper pairs. Further, the new theory provides insight into the carrier scattering dynamics and allows to differentiate between the superconducting, pseudo gap, and strange metal phases. The direct connection between non--linear optical response and microscopic dynamics provides a powerful new methodology to study quantum phase transitions in correlated materials. Further implications are light-wave control over intricate quantum phases, light-matter hybrids, and application for optical quantum computing.
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]
The strong-field process of high-harmonic generation (HHG) has, in recent years, been treated from a quantum optical perspective in the emerging research area of strong-field quantum optics. These investigations show that HHG radiation is, in general, in a nonclassical state of light. However, the quantum optical treatment of HHG from topological nontrivial materials is missing. Here, we aim to address this gap in current knowledge and consider the quantum optical HHG response from the Su-Schrieffer-Heeger model, a finite chain of atoms with both a topologically trivial and nontrivial insulating phase, the latter supporting edge states. We find that HHG from both topological phases is squeezed at the band-gap frequency. Interestingly, while the harmonic spectrum discriminates the two topological phases of the system, the degree of squeezing only discriminates the phases for smaller chain lengths. We attribute this difference to a relative increase in overlap between bulk and edge states in the topological nontrivial phase for smaller systems. Our findings reveal how the strength of dipole couplings governs the nonclassical HHG response and define new research questions on topologically protected generation of quantum light in strong-field physics.