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Intra-atomic exchange couplings (IEC) between $5d6s$ and $4f$ electrons areubiquitous in rare-earth metals and play a critical role in spin dynamics.However, detecting them in real time domain has been difficult. Here we showthe direct evidence of IEC between $5d6s$ and $4f$ electrons in gadolinium.Upon femtosecond laser excitation, $5d6s$ electrons are directly excited, theirmajority bands shift toward the Fermi level while their minority bands do theopposite. For the first time, our first-principles minority shift now agreeswith the experiment quantitatively. Excited $5d6s$ electrons lower the exchangepotential barrier for $4f$ electrons, so the $4f$ states are also shifted inenergy, a prediction that can be tested experimentally. Although a significantnumber of $5d6s$ electrons, some several eV below the Fermi level, are excitedout of the Fermi sea, there is no change in the $4f$ states, a clearmanifestation of intra-atomic exchange coupling. Based on our results, wepropose that the demagnetization time of a material be inversely proportionalto the density of states at the Fermi level and the excited, not the whole,spin moment. This can be tested experimentally.

Manifestation of intra-atomic 5d6s-4f exchange coupling in photoexcited gadolinium