Charge, Lattice, and Spin Dynamics in Photoinduced Phase Transitions from Charge-Order-Insulator to Metal in Quasi-Two-Dimensional Organic Conductors

Abstract

To elucidate different photoinduced melting dynamics of charge orders observed in quasi-two-dimensional organic conductors $\theta$-(BEDT-TTF)${}_2$RbZn(SCN)${}_4$ and $\alpha$-(BEDT-TTF)${}_2$I${}_3$ [BEDT-TTF=bis(ethylenedithio)tetrathiafulvalene], we theoretically study photoinduced time evolution of charge and spin correlation functions on the basis of exact many-electron wave functions coupled with classical phonons in extended Peierls-Hubbard models on anisotropic triangular lattices. In both salts, the so-called horizontal-stripe charge order is stabilized by nearest-neighbor repulsive interactions and by electron-lattice interactions. In $\theta$-(BEDT-TTF)${}_2$RbZn(SCN)${}_4$ (abbreviated as $\theta$-RbZn), the stabilization energy due to lattice distortion is larger, so that larger quantity of energy needs to be absorbed for the melting of the charge and lattice orders. The photoinduced charge dynamics shows a complex behavior owing to a substantial number of nearly degenerate eigenstates involved. This is related to the high structural symmetry when the lattice is undistorted. In $\alpha$-(BEDT-TTF)${}_2$I${}_3$ (abbreviated as $\alpha$-I${}_3$), the lattice stabilization energy is smaller, and smaller quantity of energy is sufficient to melt the charge and lattice orders leading to a metallic phase. The photoinduced charge dynamics shows a sinusoidal oscillation. In $\alpha$-I${}_3$, the low structural symmetry ensures nearly spin-singlet bonds between hole-rich sites, where the spin correlation survives even after photoexcitation.

10 pages, 9 figures, twocolumn version

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Cited by in corpus (18)

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• Photoinduced Enhancement of Anisotropic Charge Correlations on Triangular Lattices with Trimers
• Charge and spin correlations of a Peierls insulator after a quench
• Effects of Lattice and Molecular Phonons on Photoinduced Neutral-to-Ionic Transition Dynamics in Tetrathiafulvalene-$p$-Chloranil
• Quench dynamics in higher-dimensional Holstein models: Insights from Truncated Wigner Approaches
• Real-time evolution of static electron-phonon models in time-dependent electric fields
• Predicted photoinduced pair annihilation of emergent magnetic charges in the organic salt $\alpha$-(BEDT-TTF)${}_2$I${}_3$ irradiated by linearly polarized light
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• Dynamical phase transitions in the photodriven charge-ordered Dirac-electron system
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• Photoinduced dynamics of excitonic order and Rabi oscillation in the two-orbital Hubbard model
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• Role of hydrogen bonding in charge-ordered organic conductor $\alpha$-(BEDT-TTF)${}_2$I${}_3$ probed by ${}^{127}$I nuclear quadrupole resonance