The photoexcited state in a correlated electron system with a spin-state degree of freedom is studied. We start from the two-orbital extended Hubbard model where the energy difference between the two orbitals is introduced. The photoexcited metastable state is examined based on the effective model Hamiltonian derived using the two-orbital Hubbard model. Spin-state change is induced by photoirradiation in the low-spin band insulator near the phase boundary, and it is found that a high-spin state is stabilized by creating a ferromagnetic bound state with photodoped hole carriers. An optical absorption occurs between the bonding and antibonding orbitals inside the bound state. The time evolution of photoexcited states is simulated in the time-dependent mean-field scheme. It is found that pair annihilations of photodoped electrons and holes generate the high-spin state in a low-spin band insulator. We propose that this process is directly observed by the time-resolved photoemission experiments.
The photoexcited state in a correlated electron system with a spin-state degree of freedom is studied. We start from the two-orbital extended Hubbard model where the energy difference between the two orbitals is introduced. The photoexcited metastable state is examined based on the effective model Hamiltonian derived using the two-orbital Hubbard model. Spin-state change is induced by photoirradiation in the low-spin band insulator near the phase boundary, and it is found that a high-spin state is stabilized by creating a ferromagnetic bound state with photodoped hole carriers. An optical absorption occurs between the bonding and antibonding orbitals inside the bound state. The time evolution of photoexcited states is simulated in the time-dependent mean-field scheme. It is found that pair annihilations of photodoped electrons and holes generate the high-spin state in a low-spin band insulator. We propose that this process is directly observed by the time-resolved photoemission experiments.
Photoinduced carrier dynamics in a correlated electron system on a coupled two-leg ladder lattice are studied. The two-leg ladder Hubbard model is analyzed utilizing the exact diagonalization method based on the Lanczos algorithm in finite-size clusters. In order to reveal the transient carrier dynamics after photoirradiation, we calculate the low-energy components of the hole kinetic energy, the pair-field correlation function, the optical conductivity spectra, and other characteristics. It is shown that the photoinduced metallic-like state appears in a half-filled Mott insulating state, while the low-energy carrier motion is suppressed by photoirradiation in the case of hole-doped metallic states. These photoinduced changes in the electron dynamics are associated with changes in the carrier-pair coherence; they are not attributed to a naive thermalization, and are associated with a ladder-lattice effect instead. Based on the numerical results, optical control of hole pairs using double-pulse pumping is demonstrated. Implications for recent optical pump-probe experiments are presented.
The search for hidden orders in photoexcited lattice systems is an active research field driven by experimental reports of light-induced or light-stabilized phases. In this study, we investigate hidden electronic orders in strongly correlated two-orbital Hubbard models with orbital-dependent bandwidths. In equilibrium, the half-filled systems are antiferromagnetically ordered. Using nonequilibrium dynamical mean field theory we demonstrate the appearance of nonthermal ferromagnetic order in the photodoped state, if the two bandwidths are sufficiently different, and its coexistence with spin-singlet $\ensuremath{\eta}$ superconductivity in the high photodoping region. Spin-triplet $\ensuremath{\eta}$-superconducting order appears instead if the two bandwidths are comparable. The rich nonequilibrium phasediagram uncovered in this work shows that Mott insulating multiorbital systems provide an interesting platform for the realization of nonthermal electronic orders.
By employing the time-dependent exact diagonalization method, we investigate the photoexcited states of the excitonic insulator in the extended Falicov-Kimball model (EFKM). We here show that the pulse irradiation can induce the interband electron-electron pair correlation in the photoexcited states, while the excitonic electron-hole pair correlation in the initial ground state is strongly suppressed. We also show that the photoexcited states contain the eigenstates of the EFKM with a finite number of interband electron-electron pairs, which are responsible for the enhancement of the electron-electron pair correlation. The mechanism found here is due to the presence of the internal SU(2) pairing structure in the EFKM and thus it is essentially the same as that for the photoinduced $\ensuremath{\eta}$ pairing in the repulsive Hubbard model reported recently [T. Kaneko et al., Phys. Rev. Lett. 122, 077002 (2019)]. This also explains why the nonlinear optical response is effective to induce the electron-electron pairs in the photoexcited states of the EFKM. Furthermore, we show that, unlike the $\ensuremath{\eta}$ pairing in the Hubbard model, the internal SU(2) structure is preserved even for a nonbipartite lattice when the EFKM has the direct-type band structure, in which the pulse irradiation can induce the electron-electron pair correlation with momentum $\mathbit{q}=\mathbit{0}$ in the photoexcited states. We also discuss briefly the effect of a perturbation that breaks the internal SU(2) structure.
Nonequilibrium control of electronically ordered hidden phases may lead to the development of ultrafast switches and memory devices. In this study, we demonstrate tunable hidden orders in the half-filled photodoped two-orbital extended Hubbard model. Using steady-state nonequilibrium dynamical mean-field theory, we clarify the coexistence and interplay of nonthermal charge, spin, and orbital order. The hidden state at low effective temperature and sufficiently high photodoping is reminiscent of Kugel-Khomskii order in the two-orbital Hubbard model at 41 and 43 filling, but it emerges out of a nonequilibrium charge-ordered state and exhibits a different magnetic structure. A low-energy effective Hamiltonian is used to analyze the exchange processes that stabilize the nonthermal order.
We theoretically study photoemission spectra for photodoped one-dimensional Mott insulators that can host excitons, and show that their spectral characteristics differ qualitatively from those of photodoped semiconductors. In conventional semiconductors, photoemission spectra are well understood; free charge carriers generate spectral weight near the bottom of the conduction band, while the formation of excitons leads to replica features of the valence band appearing inside the band gap. In one-dimensional Mott insulators, on the other hand, strong correlations give rise to fractionalized elementary excitations-spinons, holons, and doublons-which fundamentally modify the photoemission response. We find that when photodoped carriers, i.e., doublons and holons, remain unbound, the photoemission spectrum directly reflects the dispersion of spinons, i.e., magnetic elementary excitations. In contrast, when a doublon and a holon form an excitonic bound state, replica structures of the lower Hubbard band emerge inside the Mott gap, carrying contributions from both spinon and holon excitations. Importantly, the distribution of the in-gap signal depends sensitively on the degree of doublon-holon binding. The origin of these spectral features is clarified through a combination of exact diagonalization and the slave-particle approach. These results indicate that photoemission from photoinduced carriers and excitons in strongly correlated electron systems can provide information on magnetic properties and carrier-binding properties.
We study the relaxation dynamics of photocarriers in the paramagnetic Mott insulating phase of the half-filled two-band Hubbard model. Using nonequilibrium dynamical mean-field theory, we excite charge carriers across the Mott gap by a short hopping modulation, and simulate the evolution of the photodoped population within the Hubbard bands. We observe an ultrafast charge-carrier relaxation driven by the emission of local spin excitations with an inverse relaxation time proportional to the Hund's coupling. The photodoping generates additional side-bands in the spectral function, and for strong Hund's coupling, the photodoped population also splits into several resonances. The dynamics of the local many-body states reveals two effects, thermal blocking and kinetic freezing, which manifest themselves when the Hund's coupling becomes of the order of the temperature or the bandwidth, respectively. These effects, which are absent in the single-band Hubbard model, should be relevant for the interpretation of experiments on correlated materials with multiple active orbitals. In particular, the features revealed in the nonequilibrium energy distribution of the photocarriers are experimentally accessible, and provide information on the role of the Hund's coupling in these materials.