The rapidly increasing information density required of modern magnetic data storage devices raises the question of the fundamental limits in bit size and writing speed. At present, the magnetization reversal of a bit can occur as quickly as 200 ps (ref. 1). A fundamental limit has been explored by using intense magnetic-field pulses of 2 ps duration leading to a non-deterministic magnetization reversal. For this process, dissipation of spin angular momentum to other degrees of freedom on an ultrafast timescale is crucial. An even faster regime down to 100 fs or below might be reached by non-thermal control of magnetization with femtosecond laser radiation. Here, we show that an efficient novel channel for angular momentum dissipation to the lattice can be opened by femtosecond laser excitation of a ferromagnet. For the first time, the quenching of spin angular momentum and its transfer to the lattice with a time constant of 120+/-70 fs is determined unambiguously with X-ray magnetic circular dichroism. We report the first femtosecond time-resolved X-ray absorption spectroscopy data over an entire absorption edge, which are consistent with an unexpected increase in valence-electron localization during the first 120+/-50 fs, possibly providing the driving force behind femtosecond spin-lattice relaxation.
Femtosecond x-ray magnetic circular dichroism was used to study the time-dependent magnetic moment of 4f electrons in the ferromagnets Gd and Tb, which are known for their different spin-lattice coupling. We observe a two-step demagnetization with an ultrafast demagnetization time of 750 fs identical for both systems and slower times which differ sizeably with 40 ps for Gd and 8 ps for Tb. We conclude that spin-lattice coupling in the electronically excited state is enhanced up to 50 times compared to equilibrium.
We follow for the first time the evolution of the spin and orbital angular momentum of a thin Ni film during ultrafast demagnetization, by means of x-ray magnetic circular dichroism. Both components decrease with a 130 ± 40 fs time constant upon excitation with a femtosecond laser pulse. Additional x-ray absorption measurements reveal an increase in the spin-orbit interaction by 6 ± 2 % during this process. This is the experimental observation of a transient change in spin-orbit interaction during ultrafast demagnetization.
Employing spin-, time-, and energy-resolved photoemission spectroscopy, we present the first study on the spin polarization of a single electronic state after ultrafast optical excitation. Our investigation concentrates on the majority-spin component of the d-band-derived Gd(0001) surface state d(z(2))(↑). While its binding energy shows a rapid Stoner-like shift by 90 meV with an exponential time constant of τ(E)=0.6±0.1 ps, the d(z(2))(↑) spin polarization remains nearly constant within the first picoseconds and decays with τ(S)=15±8 ps. This behavior is in clear contrast to the equilibrium phase transition, where the spin polarization vanishes at the Curie temperature.
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