An excitonic model for the electron–hole plasma relaxation in proton-irradiated insulators

The relaxation of free electron–hole pairs generated after proton irradiation is modelled by means of a simplified set of hydrodynamic equations. The model describes the coupled evolution of the electron–hole pair and self-trapped exciton (STE) densities, along with the electronic and lattice temperatures. The equilibration of the electronic and lattice excitations is based on the two-temperature model, while two mechanisms for the relaxation of free electron–hole pairs are considered: STE formation and Auger recombination. Coulomb screening and band gap renormalisation are also taken into account. Our numerical results show an ultrafast ($${\ll }\,{\mathrm {1}}$$ ≪ 1 ps) free electron–hole pair relaxation time in amorphous $${{\mathrm {SiO}}_{\mathrm {2}}}$$ SiO 2 for initial carrier densities either below or above the exciton Mott transition. Coulomb screening alone is not found to yield the long relaxation time ($${\mathrm {\gg }}{\mathrm {10}}$$ ≫ 10 ps) experimentally observed in amorphous $${{\mathrm {SiO}}_{\mathrm {2}}}$$ SiO 2 and borosilicate crown glass BK7 irradiated with high-intensity laser pulses or BK7 irradiated by short proton pulses. Another mechanism, e.g. thermal detrapping of STEs, is required to correctly model the long free electron–hole pair relaxation time observed experimentally. Graphical Abstract

Revealing generation, migration, and dissociation of electron-hole pairs and current emergence in an organic photovoltaic cell

Using an innovative quantum mechanical method for an open quantum system, we observe in real time and space the generation, migration, and dissociation of electron-hole pairs, transport of electrons and holes, and current emergence in an organic photovoltaic cell. Ehrenfest dynamics is used to study photoexcitation of thiophene:fullerene stacks coupled with a time-dependent density functional tight-binding method. Our results display the generation of an electron-hole pair in the donor and its subsequent migration to the donor-acceptor interface. At the interface, electrons transfer from the lowest unoccupied molecular orbitals (LUMOs) of thiophenes to the second LUMOs of fullerene. Further migration of electrons and holes leads to the emergence of current. These findings support previous experimental evidence of coherent couplings between electronic and vibrational degrees of freedom and are expected to stimulate further work toward exploring the interplay between electron-hole pair (exciton) binding and vibronic coupling for charge separation and transport.