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

TL;DR

This study investigates the ultrafast charge, lattice, and spin dynamics in photoinduced phase transitions of quasi-two-dimensional organic conductors, revealing how different lattice symmetries and stabilization energies influence melting of charge order and resulting metallic states.

Contribution

It provides a theoretical analysis of charge and spin dynamics during photoinduced phase transitions in two organic conductors, highlighting the role of lattice symmetry and stabilization energy in these processes.

Findings

Larger lattice stabilization energy in RbZn requires more energy to melt charge order.

Charge dynamics in RbZn is complex due to nearly degenerate eigenstates.

In I3, smaller stabilization energy allows easier melting and results in sinusoidal charge oscillations.

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.