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We measure magnetization changes in a single crystal of the single-molecule magnet Fe8 when exposed to intense, short (<20 s) pulses of microwave radiation resonant with the m = 10 to 9 transition. We find that radiation induces a phonon bottleneck in the system with a time scale of ~5 s. The phonon bottleneck, in turn, drives the spin dynamics, allowing observation of thermally assisted resonant tunneling between spin states at the 100-ns time scale. Detailed numerical simulations quantitatively reproduce the data and yield a spin-phonon relaxation time of T1 ~ 40 ns.

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