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Femtosecond laser excitation of solid-state systems creates non-equilibriumhot electrons that cool down by transferring their energy to other degrees offreedom and ultimately to lattice vibrations of the solid. By combining abinitio calculations with ultrafast diffuse electron scattering we gain adetailed understanding of the complex non-equilibrium energy transfer betweenelectrons and phonons in laser-excited Ni metal. Our experimental results showthat the wavevector resolved population dynamics of phonon modes is distinctlydifferent throughout the Brillouin zone and are in remarkable agreement withour theoretical results. We find that zone-boundary phonon modes becomeoccupied first. As soon as the energy in these modes becomes larger than theaverage electron energy a backflow of energy from lattice to electronic degreesof freedom occurs. Subsequent excitation of lower-energy phonon modes drivesthe thermalization of the whole system on the picosecond timescale. Wedetermine the evolving non-equilibrium phonon occupations which we find todeviate markedly from thermal occupations.

Tracking the Ultrafast Non-Equilibrium Energy Flow between Electronic and Lattice Degrees of Freedom in Crystalline Nickel