We propose a semi-classical model for femtosecond-laser induced demagnetization due to spinpolarized excited electron diffusion in the super-diffusive regime. Our approach treats the finite elapsed time and transport in space between multiple electronic collisions exactly, as well as the presence of several metal films in the sample. Solving the derived transport equation numerically we show that this mechanism accounts for the experimentally observed demagnetization within 200 fs in Ni, without the need to invoke any angular momentum dissipation channel.Excitation with femtosecond laser pulses is known for more than a decade to cause an ultrafast quenching of the magnetization in metallic ferromagnets [1]. The achieved demagnetization times are typically 100-300 fs for ferromagnets such as Ni [1,2]. Hence, laser-induced demagnetization opens up new, interesting routes for magnetic recording with hitherto unprecedented speeds [3]. However, in spite of the technological importance the mechanism underlying the femtosecond demagnetization remains highly controversial. A common belief is that there should exist an ultrafast channel for the dissipation of spin angular momentum [4][5][6][7][8]. Several such mechanisms through which an excited electron can undergo a spinflip in a ferromagnetic metal are currently being debated. The main proposed mechanisms for a fast spin-flip process are a Stoner excitation, an inelastic magnon scattering, an Elliott-Yafet-type of phonon scattering [4,5], spin-flip Coulomb scattering [6], laser-induced spin-flips [7], or relativistic quantum electrodynamic processes [8]. An effect that, until recently [9], has been regarded to play only a marginal role is the spin-polarized transport of laser-excited hot electrons.In this Letter we show that spin-dependent transport of laser-excited electrons provides a considerable contribution to the ultrafast demagnetization process and can even completely explain it. We demonstrate this by developing a transport equation for the super-diffusive flow of spin-polarized electrons. A few approaches to describe the electron motion have been attempted previously [10,11]. In our theory, however, we take into account the whole process of multiple, spin-conserving electron scattering events and electron cascades created by inelastic electron scattering. Also the presence of different metallic films in the probed material is treated. We solve the developed theory numerically for ferromagnetic Ni, for which the femtosecond demagnetization is well documented [1,2,12], and show that a large demagnetization in a few hundred femtoseconds is generated.The typical geometry for a femtosecond laser experiment is depicted in Fig. 1. The intense laser beam creates excited hot electrons in the ferromagnetic film, which will start to move in a random direction. Our goal is to compute the time-dependent magnetization resulting from the super-diffusive motion in the laser spot. Due to the fact that the electronic mean-free-path (up to a few tens of nm) is much smaller tha...

In spin-based electronics, information is encoded by the spin state of electron bunches 1,2,3,4 . Processing this information requires the controlled transport of spin angular momentum through a solid 5,6 , preferably at frequencies reaching the so far unexplored terahertz (THz) regime 7,8,9 . Here, we demonstrate, by experiment and theory, that the temporal shape of femtosecond spin-current bursts can be manipulated by using specifically designed magnetic heterostructures. A laser pulse is employed to drive spins 10,11,12 from a ferromagnetic Fe thin film into a nonmagnetic cap layer that has either low (Ru) or high (Au) electron mobility. The resulting transient spin current is detected by means of an ultrafast, contactless amperemeter 13 based on the inverse spin Hall effect 14,15 that converts the spin flow into a THz electromagnetic pulse. We find that the Ru cap layer yields a considerably longer spin-current pulse because electrons are injected in Ru d states that have a much smaller mobility than Au sp states 16 . Thus, spin current pulses and the resulting THz transients can be shaped by tailoring magnetic heterostructures, which opens the door for engineering high-speed spintronic devices as well as broadband THz emitters 7,8,9 , in particular covering the elusive range from 5 to 10THz.Contemporary electronics is based on the electron charge as information carrier whose presence or absence encodes the value of a bit. Much more efficient devices for low-power data storage and processing could be realized if the spin degree of freedom were used in addition 1,2,3,4 . The spintronics approach requires the generation and control of spin currents, that is, the transport of spin angular momentum through space 5,6 . Spintronic operations should be performed at a pace exceeding that of today's computers, which ultimately requires the generation of spin current pulses with terahertz (1 THz = 10 12 Hz) bandwidths 7,8 as well as the possibility to manipulate them in novel structures 17,18 . To date, femtosecond spin-current pulses have been successfully launched by optically exciting electrons in semiconductors 10 or ferromagnetic metals 11,12 . However, to enable ultrafast basic operations on these transients (such as buffering or delaying), their shape and propagation have to be controlled on subpicosecond time scales.Here, we employ magnetic heterostructures containing an optimally chosen nonmagnetic metallic layer whose electron mobility allows us either to trap or to transmit electrons and, thus, to engineer ultrafast spin pulses. The spin flow is probed in a contactless manner using the inverse spin Hall effect 14,15 (ISHE) that converts the spin current into a detectable THz electromagnetic pulse 13 . Our findings open up a route to device-oriented femtosecond spintronics as well as novel broadband emitters of THz radiation 7,8,9 .Our idea is illustrated in Fig. 1a, which shows a schematic of a ferromagnetic Fe film capped by a thin layer of Ru or Au. Absorption of a femtosecond laser pulse (photon energy 1...

Irradiating a ferromagnet with a femtosecond laser pulse is known to induce an ultrafast demagnetization within a few hundred femtoseconds. Here we demonstrate that direct laser irradiation is in fact not essential for ultrafast demagnetization, and that electron cascades caused by hot electron currents accomplish it very efficiently. We optically excite a Au/Ni layered structure in which the 30 nm Au capping layer absorbs the incident laser pump pulse and subsequently use the X-ray magnetic circular dichroism technique to probe the femtosecond demagnetization of the adjacent 15 nm Ni layer. A demagnetization effect corresponding to the scenario in which the laser directly excites the Ni film is observed, but with a slight temporal delay. We explain this unexpected observation by means of the demagnetizing effect of a superdiffusive current of non-equilibrium, non-spin-polarized electrons generated in the Au layer.

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