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Tuesday, August 8, 2017
Abstract-Terahertz-pulse driven modulation of electronic spectra: Modeling electron-phonon coupling in charge-transfer crystals
Francesco Di Maiolo, Matteo Masino, and Anna Painelli
We calculate the optical spectra of a charge-transfer crystal modulated by a terahertz pulse, accounting for electron-vibration coupling. The model Hamiltonian is parametrized against first principle calculations and adiabatic results are validated against a fully non-adiabatic calculation where relaxation phenomena are introduced via the coupling of the quantum system to a dissipative bath of classic anharmonic oscillators. The experiment is well reproduced by the proposed model with no need to introduce any ad hoc assumption on the temporal dependence of model parameters, but just accounting for the quadratic dependence of the Hubbard U on non-totally symmetric molecular coordinates.