Polaronic quantum diffusion in dynamic localization regime

Abstract

We investigate the quantum dynamics in a disordered electronic lattice with Fibonacci sequence of site energy and off-diagonal electron-phonon coupling within a sub-Ohmic bath by the timedependent density matrix renormalization group algorithm. It is found that, the slope of the inverse participation ratio versus the coupling strength undergoes a sudden change indicating a transition from the static to the dynamic localization. In the dynamic localization regime, the generated polarons coherently diffuse via hopping-like processes evidenced by the saturated entanglement entropy, providing a novel scenario for the transportation mechanism in strongly disordered systems. The mean-square displacement is revealed to be insensitive to the coupling strength, implying the quantum diffusion behavior survives the energy disorder that prevails in real organic materials.

Time‐dependent density matrix renormalization group method for quantum dynamics in complex systems

“…The developments of TD-DMRG methodology in recent years have enabled its application to a variety of significant scientific problems. 58,59,63,64,[70][71][72][73][74][75][76][77][78][79][80][81][82][83][84][85] Among them, the majority are focused on open quantum systems, especially with harmonic bath and linear system-bath coupling, to study the quantum dissipation in the condensed phase. Only a few of them are focused on molecular systems.…”

“…68 In addition to the rapid development of TD-DMRG algorithms, 69 the application scope of TD-DMRG is becoming more and more widespread. For quantum dynamics in the condensed phase, TD-DMRG has been used to study the dynamics of spin-boson model (SBM), 70 the exciton/charge transfer 64,[71][72][73][74][75] and linear/nonlinear spectroscopy in natural and artificial molecular aggregates, 59,76 carrier transport mobility in molecular solids, 77,78 singlet fission, 79,80 and so on. For molecular dynamics in the gas phase, TD-DMRG has been used to study the ultrafast interconversion dynamics of pyrazine described by more general vibronic models, 58,63,80 and radiationless decay rate of azulene including the anharmonic effect.…”

Disorder-free dynamic localization in non-adiabatic processes: entanglement entropy and OTOC

“…In order to see how the disorder in uences the dynamic localization, in this section, the Monte Carlo approach is combined with the non-adiabatic dynamic method to discuss the cases in presence of nite temperature [26,27]. The thermal motion presents in the lattice, and the initial deformations of lattice sites are disordered.…”

Impact of electron–phonon coupling on the quantum yield of photovoltaic devices

“…Accordingly, the consideration of electron-hole interaction, geminate recombination, and electron-phonon coupling is unavoidable for a fully microscopic understanding of the charge separation mechanism in organic photovoltaic devices. To tackle this problem, various numerical methods such as exact diagonalization, 11 diagrammatic Monte Carlo, 12 timedependent density functional theory, 13 the Dirac-Frenkel's timedependent variational principle, 14 quantum master equation, 15 and other approaches [16][17][18] have been developed. However, these methods are quite demanding from a computational point of view, which makes the comprehensive treatment of the charge separation process a challenging task.…”

“…35,36 In particular, the present formalism extends on previous work by Galperin and Nitzan in the context of molecular junctions 37 and by including the impact of electron-hole interaction, electron-phonon coupling and geminate recombination adds important highly non-trivial aspects to that model. Among the interesting novelties of this method compared to prior studies [11][12][13][14][15][16][17][18] is that it provides an energy domain framework which, on the one hand, enables one to have access to detailed spectral information, a suitable framework to interpret the results, and, on the other hand, provides an efficient inexpensive numerical approach to treat all parameters of interest on the same footing. The outline of this paper is as follows: In Sec.…”