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arXiv:2211.08694 · Physical review. B./Physical review. B

Controlling inversion and time-reversal symmetries by subcycle pulses in the one-dimensional extended Hubbard model

Kazuya Shinjo, Shigetoshi Sota, Seiji Yunoki, Takami Tohyama

Published May 2, 2023• 3 citations
arXivHTMLPDF

Abstract

Owning to their high controllability, laser pulses have contributed greatly to our understanding of strongly correlated electron systems. However, typical multicycle pulses do not control the symmetry of systems, which plays an important role in the emergence of novel quantum phases. Here, we demonstrate that subcycle pulses whose oscillation is less than one period within a pulse envelope can control inversion and time-reversal symmetries in the electronic states of the one-dimensional extended Hubbard model. Using an ultrashort subcycle pulse, one can generate a steady electric current (SEC) in a photoexcited state due to an Aharonov-Bohm flux instantaneously introduced through the phase of an electric field. Consequently, time-reversal symmetry is broken. In contrast, a broad subcycle pulse does not induce SEC but instead generates electric polarization, thus breaking inversion symmetry. Both symmetry breakings in a photoexcited state can be monitored by second-harmonic generation. These findings provide a new methodology for designing the symmetries of electronic states and open up a new field of subcycle-pulse engineering.

DOI
10.1103/physrevb.107.195103

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Owning to their high controllability, laser pulses have contributed greatly to our understanding of strongly correlated electron systems. However, typical multicycle pulses do not control the symmetry of systems, which plays an important role in the emergence of novel quantum phases. Here, we demonstrate that subcycle pulses whose oscillation is less than one period within a pulse envelope can control inversion and time-reversal symmetries in the electronic states of the one-dimensional extended Hubbard model. Using an ultrashort subcycle pulse, one can generate a steady electric current (SEC) in a photoexcited state due to an Aharonov-Bohm flux instantaneously introduced through the phase of an electric field. Consequently, time-reversal symmetry is broken. In contrast, a broad subcycle pulse does not induce SEC but instead generates electric polarization, thus breaking inversion symmetry. Both symmetry breakings in a photoexcited state can be monitored by second-harmonic generation. These findings provide a new methodology for designing the symmetries of electronic states and open up a new field of subcycle-pulse engineering.
The development of high-intensity ultrashort laser pulses unlocks the potential of pump-probe spectroscopy in sub-femtosecond timescale. Notably, subcycle pump pulses can generate electronic states unreachable by conventional multicycle pulses, leading to a phenomenon that we refer to as subcycle-pulse engineering. In this study, we employ the time-dependent density-matrix renormalization group method to unveil the transient absorption spectra of superconducting and metallic states in nearly half-filled one-dimensional and two-dimensional Hubbard models excited by an ultrashort half-cycle pulse, which can induce a current with inversion-symmetry breaking. In a superconducting state realized in attractive on-site interactions, we find the transient activation of absorptions at energies corresponding to the amplitude modes of superconducting and charge-density-wave states. On the other hand, in a metallic state realized in the two-dimensional model with repulsive on-site interactions, we obtain another type of absorption enhancements, which are distributed broadly in spin excitation energies. These findings indicate that superconducting and metallic states are sensitive to an ultrashort half-cycle pulse, leading to the transient activations of optical absorptions with their respective mechanisms.
Abstract Strongly correlated solids are complex and fascinating quantum systems, where new electronic states continue to emerge, especially when interaction with light triggers interplay between them. In this interplay, a sub-laser-cycle electronic response is particularly attractive as a tool for the ultrafast manipulation of matter at the petahertz scale. Here we introduce a new type of nonlinear multidimensional spectroscopy, which allows us to unravel charge and energy flows in strongly correlated systems interacting with few-cycle infrared pulses and the complex interplay between different correlated states evolving on the sub-femtosecond timescale. We demonstrate that the sub-cycle spectroscopy of a single-particle electronic response is extremely sensitive to correlated many-body dynamics and provides direct access to many-body response functions. For the two-dimensional Hubbard model under the influence of ultrashort, intense electric-field transients, we resolve the sub-femtosecond pathways of charge and energy flows between localized and delocalized many-body states and the creation of a highly correlated state surviving after the end of the laser pulse. Our findings open the way towards a regime of imaging and manipulating strongly correlated materials at optical rates, beyond the multicycle approach employed in Floquet engineering, with the sub-cycle response being a key tool for accessing many-body phenomena.
The most typical way to optically control population of atomic and molecular systems is to illuminate them with radiation, resonant to the relevant transitions. Here we consider a possibility to control populations with the subcycle and even unipolar pulses, containing less than one oscillation of electric field. Despite the spectrum of such pulses covers several levels at once, we show that it is possible to selectively excite the levels of our choice by varying the driving pulse shape, duration or time delay between consecutive pulses. The pulses which are not unipolar, but have a peak of electric field of one polarity much higher (and shorter) than of the opposite one, are also capable for such control.
The excited state dynamics of correlated electron and electron-phonon systems triggered by an oscillating electric-field pulse of large amplitude are theoretically investigated. A "negative-temperature" state and inversion of electron-electron and electron-phonon interactions are induced even by a symmetric monocycle pulse. This fact is numerically demonstrated, using the exact diagonalization method, in a band-insulator phase of one-dimensional three-quarter-filled strongly dimerized extended Peierls-Hubbard and Holstein models. When the total-energy increment is maximized as a function of the electric field amplitude, the occupancy of the bonding and antibonding orbitals is inverted to produce a negative-temperature state. Around this state, the dependences of time-averaged electron-electron and electron-phonon correlation functions on interaction parameters are opposite to those in the ground state.
In any atomic species, the spherically symmetric potential originating from the charged nucleus results in fundamental symmetry properties governing the structure of atomic states and transition rules between them. If atoms are exposed to external electric fields, these properties are modified giving rise to energy shifts such as the AC Stark-effect in varying fields and, contrary to this in a constant (DC) electric field for high enough field strengths, the breaking of the atomic symmetry which causes fundamental changes in the atom's properties. This has already been observed for atomic Rydberg states with high principal quantum numbers. Here, we report on the observation of effects linked to symmetry breaking in helium within the optical cycle of the utilized strong visible laser fields for states with principal quantum number n=2. These findings were enabled by temporally resolving the dynamics better than the sub-optical cycle of the applied laser field, utilizing the method of attosecond transient absorption spectroscopy (ATAS). We identify the spectroscopic fingerprint of instantaneous polarization and breaking of the symmetry of the atom in the intense visible femtosecond pulse used in an ATAS experiment and develop a time domain picture describing the dipole response that leads to these signatures. In the future, this general experimental approach can be used to measure strong-field induced symmetry-breaking effects in other atomic or molecular systems also consisting of two or more active electrons and thus to examine new routes to their bound-state and transition-state control by laser fields.
High-harmonic generation (HHG) in inversion-symmetric systems is typically restricted to odd harmonics by symmetry. Here, we show that this selection rule can be broken without modifying the underlying Hamiltonian. We investigate a boundary-driven Su-Schrieffer-Heeger (SSH) chain coupled to source and sink reservoirs and demonstrate that dissipative dynamics generates a nonequilibrium steady state carrying a finite DC current. While the SSH Hamiltonian retains inversion symmetry, the current-carrying steady-state density matrix does not, leading to the emergence of even harmonics in the emitted spectrum. Using a correlation-matrix approach based on the Lindblad master equation, we obtain the steady state and calculate the resulting HHG response. We find that the intensity of the even harmonics is directly controlled by the transport current, establishing a link between nonequilibrium charge transport and HHG selection rules. Our results uncover a mechanism for even-harmonic generation that relies solely on nonequilibrium steady-state symmetry breaking and provide a route to probing transport currents through ultrafast nonlinear spectroscopy in centrosymmetric quantum systems.