Numerically "exact" charge transport dynamics in a dissipative electron-phonon model rationalizing the success of the transient localization scenario

Abstract: Optical conductivity in molecular semiconductors is suppressed in the terahertz region, featuring the displaced Drude peak that reflects carriers' transient localization (TL) by slow intermolecular vibrations. Meanwhile, recent computations in minimal models evidence optical-conductivity enhancements below the characteristic vibrational frequency, which cannot be captured by the TL phenomenology. These models assume undamped vibrations, whereas atomistic simulations show that the vibrations most strongly modulating carrier's hopping amplitude are damped. Here, we use the dissipaton equations of motion (DEOM) method to compute finite-temperature real-time current autocorrelation function in a one-dimensional model with Brownian-oscillator spectral density of nonlocal carrier-phonon interaction. We exploit the dissipaton algebra to handle the phonon-assisted current, reduce the method's computational requirements by working in momentum space, and confirm that numerically stable transport dynamics are virtually independent of a specific DEOM closing scheme. With increasing damping, we find that DEOM optical-conductivity profiles become increasingly qualitatively similar to TL predictions. For parameters representative of room-temperature hole transport in single-crystal rubrene, we conclude that the TL phenomenology is established already in the underdamped-oscillator regime. Reasonable variations in the damping constant weakly affect the carrier mobility, which remains within experimental bounds. Overall, our results strongly suggest that optical-conductivity enhancements at very low frequencies are artifacts of undamped vibrations, and rationalize the success of the TL phenomenology in describing experimental data.