The role of ultrafast magnon generation in the magnetization dynamics of rare-earth metals.

Ultrafast demagnetization of rare-earth metals is distinct from that of 3d ferromagnets, as rare-earth magnetism is dominated by localized 4f electrons that cannot be directly excited by an optical laser pulse. Their demagnetization must involve excitation of magnons, driven either through exchange coupling between the 5d6s-itinerant and 4f-localized electrons or by coupling of 4f spins to lattice excitations. Here, we disentangle the ultrafast dynamics of 5d6s and 4f magnetic moments in terbium metal by time-resolved photoemission spectroscopy. We show that the demagnetization time of the Tb 4f magnetic moments of 400 fs is set by 4f spin-lattice coupling. This is experimentally evidenced by a comparison to ferromagnetic gadolinium and supported by orbital-resolved spin dynamics simulations. Our findings establish coupling of the 4f spins to the lattice via the orbital momentum as an essential mechanism driving magnetization dynamics via ultrafast magnon generation in technically relevant materials with strong magnetic anisotropy.

Grueneisen-approach for the experimental determination of transient spin and phonon energies from ultrafast x-ray diffraction data: gadolinium.

We study gadolinium thin films as a model system for ferromagnets with negative thermal expansion. Ultrashort laser pulses heat up the electronic subsystem and we follow the transient strain via ultrafast x-ray diffraction. In terms of a simple Grueneisen approach, the strain is decomposed into two contributions proportional to the thermal energy of spin and phonon subsystems. Our analysis reveals that upon femtosecond laser excitation, phonons and spins can be driven out of thermal equilibrium for several nanoseconds.

Ultrafast Spin Density Wave Transition in Chromium Governed by Thermalized Electron Gas.

The energy and momentum selectivity of time- and angle-resolved photoemission spectroscopy is exploited to address the ultrafast dynamics of the antiferromagnetic spin density wave (SDW) transition photoexcited in epitaxial thin films of chromium. We are able to quantitatively extract the evolution of the SDW order parameter Δ through the ultrafast phase transition and show that Δ is governed by the transient temperature of the thermalized electron gas, in a mean field description. The complete destruction of SDW order on a sub-100 fs time scale is observed, much faster than for conventional charge density wave materials. Our results reveal that equilibrium concepts for phase transitions such as the order parameter may be utilized even in the strongly nonadiabatic regime of ultrafast photoexcitation.

Disparate ultrafast dynamics of itinerant and localized magnetic moments in gadolinium metal.

The Heisenberg-Dirac intra-atomic exchange coupling is responsible for the formation of the atomic spin moment and thus the strongest interaction in magnetism. Therefore, it is generally assumed that intra-atomic exchange leads to a quasi-instantaneous aligning process in the magnetic moment dynamics of spins in separate, on-site atomic orbitals. Following ultrashort optical excitation of gadolinium metal, we concurrently record in photoemission the 4f magnetic linear dichroism and 5d exchange splitting. Their dynamics differ by one order of magnitude, with decay constants of 14 versus 0.8 ps, respectively. Spin dynamics simulations based on an orbital-resolved Heisenberg Hamiltonian combined with first-principles calculations explain the particular dynamics of 5d and 4f spin moments well, and corroborate that the 5d exchange splitting traces closely the 5d spin-moment dynamics. Thus gadolinium shows disparate dynamics of the localized 4f and the itinerant 5d spin moments, demonstrating a breakdown of their intra-atomic exchange alignment on a picosecond timescale.

A high-order harmonic generation apparatus for time- and angle-resolved photoelectron spectroscopy.

We present a table top setup for time- and angle-resolved photoelectron spectroscopy to investigate band structure dynamics of correlated materials driven far from equilibrium by femtosecond laser pulse excitation. With the electron-phonon equilibration time being in the order of 1-2 ps it is necessary to achieve sub-picosecond time resolution. Few techniques provide both the necessary time and energy resolution to map non-equilibrium states of the band structure. Laser-driven high-order harmonic generation is such a technique. In our experiment, a grating monochromator delivers tunable photon energies up to 40 eV. A photon energy bandwidth of 150 meV and a pulse duration of 100 fs FWHM allow us to cover the k-space necessary to map valence bands at different kz and detect outer core states.

Role of spin-flip exchange scattering for hot-electron lifetimes in cobalt.

The spin-dependent lifetimes of hot electrons in fcc Co films were studied by spin- and time-resolved two-photon photoemission. Even for excitation energies close to the Fermi level, we find almost identical lifetimes for majority and minority electrons. This result contradicts ab initio theories predicting 5 to 10 times longer lifetimes for the majority electrons in 3d ferromagnets. We provide direct experimental evidence that this discrepancy is caused by the dominance of exchange scattering in inelastic electron decay, in combination with the excitation of secondary electrons. The latter are inherent for all real materials and devices.

Magnetic exchange splitting in Fe above the Curie temperature.

The magnetic exchange splitting of electronic states in a 7 monolayer Fe film on Cu(001) was investigated below and above the Curie temperature T(C), using image-potential surface states as sensor. At T(C), the long-range magnetic order breaks down as reflected by a vanishing spin splitting and vanishing spin polarization. The exchange splitting, in contrast, does not change abruptly at T(C) but persists up to T=1.2T(C). Equally, the spin-integrated linewidth shows no signature of the magnetic phase transition but smoothly decreases with increasing temperature. Our experimental results confirm theoretical expectations that, at T(C), the long-range magnetic order disappears but the local magnetic moments and, in particular, the valence electronic structure are unaffected by the phase transition.

Ultrafast magnon generation in an Fe film on Cu(100).

We report on a combined experimental and theoretical study of the spin-dependent relaxation processes in the electron system of an iron film on Cu(100). Spin-, time-, energy- and angle-resolved two-photon photoemission shows a strong characteristic dependence of the lifetime of photoexcited electrons on their spin and energy. Ab initio calculations as well as a many-body treatment corroborate that the observed properties are determined by relaxation processes involving magnon emission. Thereby we demonstrate that magnon emission by hot electrons occurs on the femtosecond time scale and thus provides a significant source of ultrafast spin-flip processes. Furthermore, engineering of the magnon spectrum paves the way for tuning the dynamic properties of magnetic materials.

Ferromagnetic Fe on Cu(001) throughout the fcc-like phase: arguing from the viewpoint of the electronic structure.

The scientific enthusiasm for ultrathin Fe films on Cu(001) has now lasted for more than 20 years. Is there ferromagnetic iron with a face-centred cubic (fcc) structure? Does ferromagnetism in Fe hinge on the body-centred cubic (bcc) structure? In this contribution, we try to establish that the electron system gives evidence of ferromagnetic behaviour with fcc-like electronic bands. We examine a crystal-induced surface state, which is characteristic of fcc surface order. Furthermore, we compare electronic signatures of fcc and bcc: the d-band exchange splitting, image-potential-state energies and the work function. We conclude that, from the viewpoint of the electronic structure, Fe on Cu(001) is found to be ferromagnetic throughout the fcc-like phase. This result raises a new question: how much deviation from the relaxed fcc order is acceptable without losing the electronic signature of fcc?

Electronic structure of CoSi(2) films on Si(111) studied using time-resolved two-photon photoemission.

The occupied and unoccupied electronic structure of thin epitaxial CoSi(2) films grown on Si(111) substrates was studied using time-resolved two-photon photoemission and valence-band photoemission spectroscopy. The work function of the sample surfaces and the Schottky barrier height at the metal-semiconductor interface were measured as a function of annealing temperature. The photoemission data reveal several occupied and unoccupied electronic states which exhibit a high sensitivity to the annealing temperature. Time-resolved measurements show a behavior typical for a short-lived hot-electron gas and indications for an image-potential resonance.

Spin-orbit hybridization points in the face-centered-cubic cobalt band structure.

Linear magnetic dichroism is observed in spin-, time-, and energy-resolved two-photon photoemission from valence bands of epitaxial fcc cobalt on Cu(001). With image-potential states as spectator states we identify initial bulk and surface states with minority spin character as the source for dichroic intensities and apparent dichroic lifetimes. Excellent agreement with ab initio fully relativistic calculations of the cobalt fcc band structure allows us to precisely determine spin-orbit hybridization points close to the Fermi level. These spin hot spots enhance spin-flip scattering by several orders of magnitude and are therefore assumed to be crucial in ultrafast demagnetization.

Nonequilibrium magnetization dynamics of gadolinium studied by magnetic linear dichroism in time-resolved 4f core-level photoemission.

The magnetic linear dichroism of the gadolinium 4f core level is studied in a time-resolved photoemission experiment employing laser pump- and synchrotron-radiation probe pulses. Upon optical excitation of the 5d6s valence electrons with femtosecond laser pulses, the magnetic order in the 4f spin system is reduced. Remarkably, the linear dichroism remains at 80% of the equilibrium contrast while the lattice temperature reaches the Curie temperature due to electron-phonon scattering. Contrasting itinerant ferromagnets, this shows that equilibration between the lattice and spin subsystems takes in Gd about 80 ps and is established in parallel with heat diffusion.

Auger resonant Raman scattering in itinerant electron systems: continuum excitation in Cu.

The role of electron localization for resonant photoemission and Auger resonant Raman scattering to occur in an extended system was studied by polarization dependent resonant photoemission at the Cu L edges. Auger resonant Raman scattering was observed for continuum excitation into van Hove singularities at the L(1) and X(1) points, 4.2 and 7.7 eV above threshold. These findings show that resonant photoemission and Auger resonant Raman scattering are general features of photoemission independent of the degree of electron localization.