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Journal of the Physical Society of Japan

Auger Recombination of Photogenerated Charges in One-Dimensional Mott Insulators

Mami Segawa, Akira Takahashi, Hiroki Gomi, Masaki Aihara

Published Aug 15, 2011• 8 citations
Publisher

Abstract

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.

DOI
10.1143/jpsj.80.084721

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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.
We theoretically investigate the relaxation of photogenerated charge carriers 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 weak light pulse. We investigate the dependence of the dynamics on the Coulomb correlation strength in the case where the binding effect between photogenerated opposite charges is significant. In the strong-correlation region (U≫WU \gg WU≫W), where U is the onsite Coulomb interaction energy and W is the bandwidth, the Auger recombination where two bound holon–doublon pairs decay into one unbound holon–doublon pair dominates the decay dynamics. From the strong- to intermediate (U≃WU \simeq WU≃W)-correlation regions, the Auger recombination is always dominant, but the charge carriers involved in the process cannot be described by a holon and a doublon in the intermediate-correlation region. In the crossover region between these two regions, the Auger coefficient is strongly enhanced, and the decay time constant is consistent with those obtained in recent experiments.
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 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.
Abstract We theoretically investigate the effect of static disorder on the dynamics of photoexcited states in onedimensional Mott insulators. We adopt the Pariser‐Parr‐Pople model, where disorder is introduced in the site energy and the transfer integral. We numerically calculate the time development of the state excited by a light pulse, and investigate the time dependence of the nearest‐neighbor spin‐spin interaction energy, the on‐site Coulomb interaction energy, and the kinetic energy of photogenerated charges. In the weaker excitation case, the energy transfer from the charge degrees of freedom to the spin degrees of freedom does not occur in the regular systems as a result of the spin‐charge separation. When the disorder in the transfer integral is introduced, the spin‐spin interaction energy changes with time after photoexcitation, showing that the spin‐charge coupling is induced in this case. The effects of the disorder in the site energy on the spincharge coupling are much weaker than those in the transfer integral. On the contrary, the energy transfer from the on‐site Coulomb interaction energy to the kinetic energy is strongly suppressed by these two kinds of disorders. In the stronger excitation case, the spin and the charge degrees of freedom are coupled in the photoexcited states, and the two kinds of energy transfers occur even in regular systems. Furthermore, these energy transfers occur in irreversible way, suggesting that these transfers are relaxation phenomena. These relaxations are enhanced by the disorders. There are no significant differences in the effects of disorders on these relaxations between the disorder in the site energy and that in the transfer integral. (© 2009 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)
We theoretically analyze the process of charge recombination in the planar Mott-Hubbard insulators with the aim to explain the short picosecond-range lifetimes of photoexcited carriers, experimentally studied via pump-probe experiments on the undoped cuprates. The recombination mechanism consists of two essential ingredients: the formation of a metastable sss-type bound holon-doublon pair, i.e., the Mott exciton, and the decay of such an excitonic state via the multimagnon emission. In spite of the large gap that requires many bosons to be emitted, the latter process is fast due to a large exchange scale and strong charge-spin coupling in planar systems. As the starting microscopic model we consider the single-band Hubbard model and then a more realistic three-band model for cuprates, both leading to the same minimal one. The decay rate of the exciton is evaluated numerically via the Fermi golden rule, having consistency also with the direct time-evolution calculation. The decay rate reveals exponential dependence on the ratio of the Mott-Hubbard gap and the exchange coupling, the result qualitatively reproduced also within a toy exciton-boson model.