Finite Temperature TD-DMRG for the Carrier Mobility of Organic Semiconductors

A large number of non-adiabatic dynamical studies have been applied to reveal the nature of carrier transport in organic semiconductors with different approximations. We present here a “nearly exact” graphical process unit (GPU) based finite temperature TD-DMRG method to evaluate the carrier mobility in organic semiconductors as described by electron-phonon model, in particular to rubrene crystal, one of the prototypical organic semiconductors, with parameters derived from first-principles. We find that (i) TD-DMRG is a general and robust method that can bridge the gap between hopping and band picture covering a wide range of electronic coupling strength; and (ii) with realistic parameters, TD-DMRG is able to account for the experimentally observed “band-like” transport behavior ($\mathrm{\partial }\mu \mathrm{/}\mathrm{\partial }T<0$) in rubrene. We further study the long-standing puzzle of isotope effect for charge transport and unambiguously demonstrate that the negative isotope effect ($\partial \mu / \partial m < 0$where$m$ is the atomic mass) should be universal.