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We present pump-probe measurements on the single-molecule magnet Fe_8 withmicrowave pulses having a length of several nanoseconds. The microwaveradiation in the experiments is located in the frequency range between 104 GHzand 118 GHz. The dynamics of the magnetization of the single Fe_8 crystal ismeasured using micrometer-sized Hall sensors. This technique allows us todetermine the level lifetimes of excited spin states, that are found to be ingood agreement with theoretical calculations. The theory, to which we compareour experimental results, is based on a general spin-phonon coupling formalism,which involves spin transitions between nearest and next-nearest energy levels.We show that good agreement between theory and experiments is only obtainedwhen using both the Delta m_S = +-1 transition as well as Delta m_S = +-2,where Delta m_S designates a change in the spin quantum number m_S. Temperaturedependent studies of the level lifetimes of several spin states allow usfinally to determine experimentally the spin-phonon coupling constants.

Energy Level Lifetimes in the Single-Molecule Magnet Fe_8 : Experiments and Simulations