We theoretically investigate the effect of static disorder on the dynamics of photoexcited states in one-dimensional Mott insulators. We numerically calculate the time development of the state excited by a light pulse in the Pariser-Parr-Pople model, where disorder is introduced in the site energy and the transfer integral. In the weaker excitation case, the spin-charge coupling is induced by the disorder in the transfer integral. The effects of the disorder in the site energy on the spin-charge coupling are much weaker than those in the transfer integral. In the stronger excitation case, the spin and the charge degrees of freedom are coupled in the photoexcited states even in regular systems. The spin relaxations are enhanced by the disorders, and there are no significant differences in the effects of disorders on the spin relaxations between these two kinds of disorders.
We theoretically investigate the effect of static disorder on the dynamics of photoexcited states in one-dimensional Mott insulators. We numerically calculate the time development of the state excited by a light pulse in the Pariser-Parr-Pople model, where disorder is introduced in the site energy and the transfer integral. In the weaker excitation case, the spin-charge coupling is induced by the disorder in the transfer integral. The effects of the disorder in the site energy on the spin-charge coupling are much weaker than those in the transfer integral. In the stronger excitation case, the spin and the charge degrees of freedom are coupled in the photoexcited states even in regular systems. The spin relaxations are enhanced by the disorders, and there are no significant differences in the effects of disorders on the spin relaxations between these two kinds of disorders.
We theoretically investigate the dynamics of insulator-metal transition induced by light-pulse excitation in one-dimensional (1D) and two-dimensional (2D) Mott insulators. We adopt the Pariser-Parr-Pople model, and pump-probe signal is obtained by numerically calculating the time development of the state excited by a light pulse. In the 1D case, when photoexcitation density is below about 10%, an extremely small portion of the energy eigenstates dominates the optical process, and the spin-charge separation holds in these dominant energy eigenstates. As a result, the Mott gap and the short-range antiferromagnetic (AF) spin order are preserved, and the spin relaxation does not occur. When the density is above the value, a metallic state without the Mott gap is photogenerated, and the magnitude of the short-range AF spin order is significantly reduced by photoexcitation. This is consistent with the experimentally observed photoinduced Mott transition. Furthermore, the spin relaxation occurs in the metallic state. This photoinduced Mott transition is a manifestation of the spin-charge coupling in the intensely photoexcited states. In the 2D case, the spin and the charge degrees of freedom are coupled even in the weakly photoexcited states, and the characteristic crossover associated with the excitation density is not observed.
We theoretically investigate the dynamics of insulator-metal transition induced by light-pulse excitation in one-dimensional Mott insulators. We adopt the Pariser--Parr--Pople model and the pump-probe signal is obtained by numerically calculating the time development of the state excited by light pulse. When the photoexcitation density is below about 10%, an extremely small portion of the energy eigenstates dominates the optical process and the spin-charge separation holds in these dominant energy eigenstates. As a result, the Mott gap and the short-range antiferromagnetic (AF) spin order are preserved and spin relaxation does not occur. When the density is above the value, a metallic state without the Mott gap is photogenerated and the magnitude of the short-range AF spin order is significantly reduced by photoexcitation. This is consistent with the experimentally observed photoinduced Mott transition. Furthermore, spin relaxation occurs in the metallic state. This photoinduced Mott transition is a manifestation of the spin-charge coupling in the intensely photoexcited states.
We theoretically investigate the dynamics of photoexcited states in one-dimensional Mott insulators. We adopt the Pariser–Parr–Pople model, and numerically calculate the time development of the nonequilibrium state excited by a light pulse. In the weaker light excitation case where the maximum photoexcitation density is below about 18%, the charge carriers in the photoexcited states are holons and doublons, and the geminate recombination of bound doublon–holon pairs, namely, the Auger recombination process dominates the decay of the photogenerated holons and doublons with the realistic Coulomb parameters. In the stronger light excitation case where the density is above the value, the charge carriers of the photoexcited states cannot be described by holons and doublons. As a result, the Auger recombination process of doublon–holon pairs is not the main decay route of the photogenerated charges. Furthermore, the spin and the charge degrees of freedom are coupled, and spin relaxation occurs in the photoexcited states. As the density of the photogenerated charge carriers becomes larger, the decay time decreases. This tendency is consistent with experiments.
Ultra-fast spectroscopy can reveal the interplay of charges with low energy degrees of freedom, which underlies the rich physics of correlated materials. As a potential glue for superconductivity, spin fluctuations in Mott insulators are of particular interest. A theoretical description of the coupled spin and charge degrees of freedom is challenging, because magnetic order is often only short-lived and short-ranged. In this work we theoretically investigate how the spin-charge interactions influence the relaxation of a two-dimensional Mott-Hubbard insulator after photo-excitation. We use a nonequilibrium variant of the dynamical cluster approximation, which, in contrast to single-site dynamical mean-field theory, captures the effect of short-range correlations. The relaxation time is found to scale with the strength of the nearest-neighbor spin correlations, and can be 10-20 fs in the cuprates. Increasing the temperature or excitation density decreases the spin correlations and thus implies longer relaxation times. This may help to distinguish the effect of spin-fluctuations on the charge relaxation from the influence of other bosonic modes in the solid.
We theoretically investigate the dynamics of the photoexcited state in the strongly correlated low-dimensional electron systems. In the two-dimensional case, the ultrafast relaxation originating from the transfer of photogenerated charges in the antiferromagnetic background is followed by the slower one originating from the spin structure rearrangement with the new charge distributions. This clearly shows the difference in the relaxation between charge and spin degrees of freedom. In the one-dimensional case, spin-charge separation holds and the mechanical coherence is preserved.