Phonon driven charge dynamics in polycrystalline acetylsalicylic acid mapped by ultrafast x-ray diffraction

Abstract

The coupled lattice and charge dynamics induced by phonon excitation in polycrystalline acetylsalicylic acid (aspirin) are mapped by femtosecond x-ray powder diffraction. The hybrid-mode character of the 0.9 ± 0.1 THz methyl rotation in the aspirin molecules is evident from collective charge relocations over distances of some 100 pm, much larger than the sub-picometer nuclear displacements. Oscillatory charge relocations around the methyl group generate a torque on the latter, thus coupling electronic and nuclear motions.