C. Stamm

Transient ferromagnetic-like state mediating ultrafast reversal of antiferromagnetically coupled spins

Ferromagnetic or antiferromagnetic spin ordering is governed by the exchange interaction, the strongest force in magnetism. Understanding spin dynamics in magnetic materials is an issue of crucial importance for progress in information processing and recording technology. Usually the dynamics are studied by observing the collective response of exchange-coupled spins, that is, spin resonances, after an external perturbation by a pulse of magnetic field, current or light. The periods of the corresponding resonances range from one nanosecond for ferromagnets down to one picosecond for antiferromagnets. However, virtually nothing is known about the behaviour of spins in a magnetic material after being excited on a timescale faster than that corresponding to the exchange interaction (10–100 fs), that is, in a non-adiabatic way. Here we use the element-specific technique X-ray magnetic circular dichroism to study spin reversal in GdFeCo that is optically excited on a timescale pertinent to the characteristic time of the exchange interaction between Gd and Fe spins. We unexpectedly find that the ultrafast spin reversal in this material, where spins are coupled antiferromagnetically, occurs by way of a transient ferromagnetic-like state. Following the optical excitation, the net magnetizations of the Gd and Fe sublattices rapidly collapse, switch their direction and rebuild their net magnetic moments at substantially different timescales; the net magnetic moment of the Gd sublattice is found to reverse within 1.5 picoseconds, which is substantially slower than the Fe reversal time of 300 femtoseconds. Consequently, a transient state characterized by a temporary parallel alignment of the net Gd and Fe moments emerges, despite their ground-state antiferromagnetic coupling. These surprising observations, supported by atomistic simulations, provide a concept for the possibility of manipulating magnetic order on the timescale of the exchange interaction.

Ultrafast spin transport as key to femtosecond demagnetization

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.

Femtosecond x-ray absorption spectroscopy of spin and orbital angular momentum in photoexcited Ni films during ultrafast demagnetization

BESSY II, Helmholtz-Zentrum Berlin fu¨r Materialien und Energie GmbH,Albert-Einstein-Strasse 15, 12489 Berlin, Germany(Dated: March 19, 2010)We follow for the first time the evolution of the spin and orbital angular momentum of a thinNi film during ultrafast demagnetization, by means of x-ray magnetic circular dichroism. Bothcomponents decrease with a 130 ± 40 fs time constant upon excitation with a femtosecond laserpulse. Additional x-ray absorption measurements reveal an increase in the spin-orbit interaction by6±2 % during this process. This is the experimental observation of a transient change in spin-orbitinteraction during ultrafast demagnetization.

A novel monochromator for experiments with ultrashort X‐ray pulses

Aiming at advancing storage-ring-based ultrafast X-ray science, over the past few years many upgrades have been undertaken to continue improving beamline performance and photon flux at the Femtoslicing facility at BESSY II. In this article the particular design upgrade of one of the key optical components, the zone-plate monochromator (ZPM) beamline, is reported. The beamline is devoted to optical pump/soft X-ray probe applications with 100 fs (FWHM) X-ray pulses in the soft X-ray range at variable polarization. A novel approach consisting of an array of nine off-axis reflection zone plates is used for a gapless coverage of the spectral range between 410 and 1333 eV at a designed resolution of E/ΔE = 500 and a pulse elongation of only 30 fs. With the upgrade of the ZPM the following was achieved: a smaller focus, an improved spectral resolution and bandwidth as well as excellent long-term stability. The beamline will enable a new class of ultrafast applications with variable optical excitation wavelength and variable polarization.

Ultrafast and Distinct Spin Dynamics in Magnetic Alloys

Controlling magnetic order on ultrashort timescales is crucial for engineering the next-generation magnetic devices that combine ultrafast data processing with ultrahigh-density data storage. An appealing scenario in this context is the use of femtosecond (fs) laser pulses as an ultrafast, external stimulus to fully set the orientation and the magnetization magnitude of a spin ensemble. Achieving such control on ultrashort timescales, e.g., comparable to the excitation event itself, remains however a challenge due to the lack of understanding the dynamical behavior of the key parameters governing magnetism: The elemental magnetic moments and the exchange interaction. Here, we investigate the fs laser-induced spin dynamics in a variety of multi-component alloys and reveal a dissimilar dynamics of the constituent magnetic moments on ultrashort timescales. Moreover, we show that such distinct dynamics is a general phenomenon that can be exploited to engineer new magnetic media with tailor-made, optimized dynamic properties. Using phenomenological considerations, atomistic modeling and time-resolved X-ray magnetic circular dichroism (XMCD), we demonstrate demagnetization of the constituent sub-lattices on significantly different timescales that depend on their magnetic moments and the sign of the exchange interaction. These results can be used as a “recipe” for manipulation and control of magnetization dynamics in a large class of magnetic materials.

Ultrafast reduction of the total magnetization in iron

Surprisingly, if a ferromagnet is exposed to an ultrafast laser pulse, its apparent magnetization is reduced within less than a picosecond. Up to now, the total magnetization, i.e., the average spin polarization of the whole valence band, was not detectable on a sub-picosecond time scale. Here, we present experimental data, confirming the ultrafast reduction of the total magnetization. Soft x-ray pulses from the free electron laser in Hamburg (FLASH) extract polarized cascade photoelectrons from an iron layer excited by a femtosecond laser pulse. The spin polarization of the emitted electrons is detected by a Mott spin polarimeter.

The role of space charge in spin-resolved photoemission experiments

Spin-resolved photoemission is one of the most direct ways of measuring the magnetization of a ferromagnet. If all valence band electrons contribute, the measured average spin polarization is proportional to the magnetization. This is even the case if electronic excitations are present, and thus is of particular interest for studying the response of the magnetization to a pump laser pulse. Here, we demonstrate the feasibility of ultrafast spin-resolved photoemission using free electron laser (FEL) radiation and investigate the effect of space charge on the detected spin polarization. The sample is exposed to the radiation of the FEL FLASH in Hamburg. Surprisingly, the measured spin polarization depends on the fluence of the FEL radiation: a higher FEL fluence reduces the measured spin polarization. Space-charge simulations can explain this effect. These findings have consequences for future spin-polarized photoemission experiments using pulsed photon sources.

Ultrafast Magnetism as Seen by X-rays

Revealing the ultimate speed limit at which magnetic order can be controlled, is a fundamental challenge of modern magnetism having far reaching implications for magnetic recording industry. Exchange interaction is the strongest force in magnetism, being responsible for ferromagnetic or antiferromagnetic spin order. How do spins react after being optically perturbed on an ultrashort timescales pertinent to the characteristic time of the exchange interaction? Here we demonstrate that femtosecond measurements of X-ray magnetic circular dichroism provide revolutionary new insights into the problem of ultrafast magnetism. In particular, we show that upon femtosecond optical excitation the ultrafast spin reversal of Gd(FeCo) - a material with antiferromagnetic coupling of spins - occurs via a transient ferromagnetic state. The latter one emerges due to different dynamics of Gd and Fe magnetic moments: Gd switches within 1.5 ps while it takes only 300 fs for Fe. Thus, by using a single fs laser pulse one can force the spin system to evolve via an energetically unfavorable way and temporary switch from an antiferromagnetic to ferromagnetic type of ordering. These observations supported by atomistic simulations, present a novel concept of manipulating magnetic order on different classes of magnetic materials on timescales of the exchange interaction.

Engineering Ultrafast Magnetism

We employ time-resolved X-ray magnetic circular dichroism with fs time resolution to investigate the ultrafast, laser-driven dynamics of multi-sublattice materials, with both ferromagnetic and antiferromagnetic coupling. These measurements provide evidence for a demagnetization time that scales with the elemental magnetic moment and varies with the exchange interaction symmetry.

A novel monochromator for ultrashort soft x-ray pulses

Reflection zone plates (RZP), which consist of elliptical zone plates fabricated on a total external reflection mirror surface, can be effectively used to produce a monochromatic x-ray beam and to focus it at photon energies below 1400 eV. However, as RZPs are highly chromatic, they can be designed only for one specific photon energy. We alleviate this problem by using a novel approach: a Reflection Zone Plate Array (RZPA). Here, we report about successful implementation of novel monochromator based on RZPAs for experiments with 100 fs time resolution at the upgraded Femtoslicing facility at BESSY-II. Aiming at minimum losses in x-ray flux up to 2000 resolution, we fabricated and used an RZPA as a single optical element for diffraction and focusing. Nine Fresnel lenses, designed for the energies of 410 eV, 543 eV, 644 eV, 715 eV, 786 eV, 861 eV, 1221 eV and 1333 eV which correspond to the absorption edges of NK, O-K, Mn-L, Fe-L, Co-L, Ni-L, Gd-M and Dy-M, were fabricated on the same substrate with a diameter of 100 mm. At resolution E/ΔE up to 2000 all edges of other elements in that range (400-1400 eV) are covered, too.