Ultrafast terahertz Stark spectroscopy reveals the excited-state dipole moments of retinal in bacteriorhodopsin.

The photoinduced all-trans to 13-cis isomerization of the retinal Schiff base represents the ultrafast first step in the reaction cycle of bacteriorhodopsin (BR). Extensive experimental and theoretical work has addressed excited-state dynamics and isomerization via a conical intersection with the ground state. In conflicting molecular pictures, the excited state potential energy surface has been modeled as a pure S[Formula: see text] state that intersects with the ground state, or in a 3-state picture involving the S[Formula: see text] and S[Formula: see text] states. Here, the photoexcited system passes two crossing regions to return to the ground state. The electric dipole moment of the Schiff base in the S[Formula: see text] and S[Formula: see text] state differs strongly and, thus, its measurement allows for assessing the character of the excited-state potential. We apply the method of ultrafast terahertz (THz) Stark spectroscopy to measure electric dipole changes of wild-type BR and a BR D85T mutant upon electronic excitation. A fully reversible transient broadening and spectral shift of electronic absorption is induced by a picosecond THz field of several megavolts/cm and mapped by a 120-fs optical probe pulse. For both BR variants, we derive a moderate electric dipole change of 5 [Formula: see text] 1 Debye, which is markedly smaller than predicted for a neat S[Formula: see text]-character of the excited state. In contrast, S[Formula: see text]-admixture and temporal averaging of excited-state dynamics over the probe pulse duration gives a dipole change in line with experiment. Our results support a picture of electronic and nuclear dynamics governed by the interaction of S[Formula: see text] and S[Formula: see text] states in a 3-state model.

Exploring the Fundamental Spatial Limits of Magnetic All-Optical Switching.

All-optical switching (AOS) results in ultrafast and deterministic magnetization reversal upon single laser pulse excitation, potentially supporting faster and more energy-efficient data storage. To explore the fundamental limits of achievable bit densities in AOS, we have used soft X-ray transient grating spectroscopy to study the ultrafast magnetic response of a GdFe alloy after a spatially structured excitation with a periodicity of 17 nm. The ultrafast spatial evolution of the magnetization in combination with atomistic spin dynamics and microscopic temperature model calculations allows us to derive a detailed phase diagram of AOS as a function of both the absorbed energy density and the nanoscale excitation period. Our results suggest that the minimum size for AOS in GdFe alloys, induced by a nanoscale periodic excitation, is around 25 nm and that this limit is governed by ultrafast lateral electron diffusion and by the threshold for optical damage.

Transient Terahertz Stark Effect: A Dynamic Probe of Electric Interactions in Polar Liquids.

Electric forces acting on molecules in liquids at ambient temperature fluctuate at terahertz (THz) frequencies with a direct impact on their electronic and optical properties. We introduce the transient THz Stark effect to modify the electronic absorption spectra of dye molecules and, thus, elucidate and determine the underlying molecular interactions and dynamics. Picosecond electric fields of megavolts/cm induce a nonequilibrium response of the prototypical Betaine-30 in polar solution that is probed via transient absorption changes. The field-induced broadening of the absorption band follows the THz intensity in time, with a minor impact of solvent dynamics. The ground and excited state dipole energies in the THz field govern this response, allowing for a quantification of electric forces in a structurally frozen molecular environment.

Pump-probe x-ray microscopy of photo-induced magnetization dynamics at MHz repetition rates.

We present time-resolved scanning x-ray microscopy measurements with picosecond photo-excitation via a tailored infrared pump laser at a scanning transmission x-ray microscope. Specifically, we image the laser-induced demagnetization and remagnetization of thin ferrimagnetic GdFe films proceeding on a few nanoseconds timescale. Controlling the heat load on the sample via additional reflector and heatsink layers allows us to conduct destruction-free measurements at a repetition rate of 50 MHz. Near-field enhancement of the photo-excitation and controlled annealing effects lead to laterally heterogeneous magnetization dynamics which we trace with 30 nm spatial resolution. Our work opens new opportunities to study photo-induced dynamics on the nanometer scale, with access to picosecond to nanosecond time scales, which is of technological relevance, especially in the field of magnetism.

Deterministic Generation and Guided Motion of Magnetic Skyrmions by Focused He+-Ion Irradiation.

Magnetic skyrmions are quasiparticles with nontrivial topology, envisioned to play a key role in next-generation data technology while simultaneously attracting fundamental research interest due to their emerging topological charge. In chiral magnetic multilayers, current-generated spin-orbit torques or ultrafast laser excitation can be used to nucleate isolated skyrmions on a picosecond time scale. Both methods, however, produce randomly arranged skyrmions, which inherently limits the precision on the location at which the skyrmions are nucleated. Here, we show that nanopatterning of the anisotropy landscape with a He+-ion beam creates well-defined skyrmion nucleation sites, thereby transforming the skyrmion localization into a deterministic process. This approach allows control of individual skyrmion nucleation as well as guided skyrmion motion with nanometer-scale precision, which is pivotal for both future fundamental studies of skyrmion dynamics and applications.

All-Optical Switching on the Nanometer Scale Excited and Probed with Femtosecond Extreme Ultraviolet Pulses.

Ultrafast control of magnetization on the nanometer length scale, in particular all-optical switching, is key to putting ultrafast magnetism on the path toward future technological application in data storage technology. However, magnetization manipulation with light on this length scale is challenging due to the wavelength limitations of optical radiation. Here, we excite transient magnetic gratings in a GdFe alloy with a periodicity of 87 nm by the interference of two coherent femtosecond light pulses in the extreme ultraviolet spectral range. The subsequent ultrafast evolution of the magnetization pattern is probed by diffraction of a third, time-delayed pulse tuned to the Gd N-edge at a wavelength of 8.3 nm. By examining the simultaneously recorded first and second order diffractions and by performing reference real-space measurements with a wide-field magneto-optical microscope with femtosecond time resolution, we can conclusively demonstrate the ultrafast emergence of all-optical switching on the nanometer length scale.

The patterning toolbox FIB-o-mat: Exploiting the full potential of focused helium ions for nanofabrication.

Focused beams of helium ions are a powerful tool for high-fidelity machining with spatial precision below 5 nm. Achieving such a high patterning precision over large areas and for different materials in a reproducible manner, however, is not trivial. Here, we introduce the Python toolbox FIB-o-mat for automated pattern creation and optimization, providing full flexibility to accomplish demanding patterning tasks. FIB-o-mat offers high-level pattern creation, enabling high-fidelity large-area patterning and systematic variations in geometry and raster settings. It also offers low-level beam path creation, providing full control over the beam movement and including sophisticated optimization tools. Three applications showcasing the potential of He ion beam nanofabrication for two-dimensional material systems and devices using FIB-o-mat are presented.

Observation of fluctuation-mediated picosecond nucleation of a topological phase.

Topological states of matter exhibit fascinating physics combined with an intrinsic stability. A key challenge is the fast creation of topological phases, which requires massive reorientation of charge or spin degrees of freedom. Here we report the picosecond emergence of an extended topological phase that comprises many magnetic skyrmions. The nucleation of this phase, followed in real time via single-shot soft X-ray scattering after infrared laser excitation, is mediated by a transient topological fluctuation state. This state is enabled by the presence of a time-reversal symmetry-breaking perpendicular magnetic field and exists for less than 300 ps. Atomistic simulations indicate that the fluctuation state largely reduces the topological energy barrier and thereby enables the observed rapid and homogeneous nucleation of the skyrmion phase. These observations provide fundamental insights into the nature of topological phase transitions, and suggest a path towards ultrafast topological switching in a wide variety of materials through intermediate fluctuating states.

A tabletop setup for ultrafast helicity-dependent and element-specific absorption spectroscopy and scattering in the extreme ultraviolet spectral range.

Further advances in the field of ultrafast magnetization dynamics require experimental tools to measure the spin and electron dynamics with element-specificity and femtosecond temporal resolution. We present a new laboratory setup for two complementary experiments with light in the extreme ultraviolet (XUV) spectral range. One experiment is designed for polarization-dependent transient spectroscopy, particularly for simultaneous measurements of magnetic circular dichroism (MCD) at the 3p resonances of the 3d transition metals Fe, Co, and Ni. The second instrument is designed for resonant small-angle scattering experiments with monochromatic light allowing us to monitor spin dynamics with spatial information on the nanometer scale. We combine a high harmonic generation (HHG) source with a phase shifter to obtain XUV pulses with variable polarization and a flux of about (3 ± 1) × 1010 photons/s/harmonic at 60 eV at the source. A dedicated reference spectrometer effectively reduces the intensity fluctuations of the HHG spectrum to below 0.12% rms. We demonstrate the capabilities of the setup by capturing the energy- and polarization-dependent absorption of a thin Co film as well as the time-resolved small-angle scattering in a magnetic-domain network of a Co/Pt multilayer. The new laboratory setup allows systematic studies of optically induced spin and electron dynamics with element-specificity, particularly with MCD as the contrast mechanism with femtosecond temporal resolution and an unprecedented signal-to-noise ratio.

Spatial distribution of electric-field enhancement across the gap of terahertz bow-tie antennas.

The electric-field enhancement in terahertz (THz) antennas designed for nonlinear THz spectroscopy of soft matter is characterized by spatially resolved electrooptic sampling. To mimic the relevant interaction geometry, metallic, resonant bow-tie antennas are deposited on a thin zinc telluride crystal of 10 µm thickness. The THz electric field transmitted through the antenna gap is recorded by electrooptic sampling. By focusing the 800 nm, sub-20 fs sampling pulses, we achieve a spatial resolution of some 3 µm, which is 1/3 to 1/8 of the antenna-gap width. The THz field in the gap displays an enhancement by a factor of up to 4.5 with a pronounced spectral variation, depending sensitively on the antenna-arm length and the gap width. By scanning the 800 nm probe spot laterally through the antenna gap, the spatial variation of the enhancement is determined, reaching the highest values at the edges of the gap. The results are in agreement with simulations of the electric-field distributions by finite-element calculations.

Optical inter-site spin transfer probed by energy and spin-resolved transient absorption spectroscopy.

Optically driven spin transport is the fastest and most efficient process to manipulate macroscopic magnetization as it does not rely on secondary mechanisms to dissipate angular momentum. In the present work, we show that such an optical inter-site spin transfer (OISTR) from Pt to Co emerges as a dominant mechanism governing the ultrafast magnetization dynamics of a CoPt alloy. To demonstrate this, we perform a joint theoretical and experimental investigation to determine the transient changes of the helicity dependent absorption in the extreme ultraviolet spectral range. We show that the helicity dependent absorption is directly related to changes of the transient spin-split density of states, allowing us to link the origin of OISTR to the available minority states above the Fermi level. This makes OISTR a general phenomenon in optical manipulation of multi-component magnetic systems.

Fast current-driven domain walls and small skyrmions in a compensated ferrimagnet.

Spintronics is a research field that aims to understand and control spins on the nanoscale and should enable next-generation data storage and manipulation. One technological and scientific key challenge is to stabilize small spin textures and to move them efficiently with high velocities. For a long time, research focused on ferromagnetic materials, but ferromagnets show fundamental limits for speed and size. Here, we circumvent these limits using compensated ferrimagnets. Using ferrimagnetic Pt/Gd44Co56/TaOx films with a sizeable Dzyaloshinskii-Moriya interaction, we realize a current-driven domain wall motion with a speed of 1.3 km s-1 near the angular momentum compensation temperature (TA) and room-temperature-stable skyrmions with minimum diameters close to 10 nm near the magnetic compensation temperature (TM). Both the size and dynamics of the ferrimagnet are in excellent agreement with a simplified effective ferromagnet theory. Our work shows that high-speed, high-density spintronics devices based on current-driven spin textures can be realized using materials in which TA and TM are close together.

Field-free deterministic ultrafast creation of magnetic skyrmions by spin-orbit torques.

Magnetic skyrmions are stabilized by a combination of external magnetic fields, stray field energies, higher-order exchange interactions and the Dzyaloshinskii-Moriya interaction (DMI). The last favours homochiral skyrmions, whose motion is driven by spin-orbit torques and is deterministic, which makes systems with a large DMI relevant for applications. Asymmetric multilayers of non-magnetic heavy metals with strong spin-orbit interactions and transition-metal ferromagnetic layers provide a large and tunable DMI. Also, the non-magnetic heavy metal layer can inject a vertical spin current with transverse spin polarization into the ferromagnetic layer via the spin Hall effect. This leads to torques that can be used to switch the magnetization completely in out-of-plane magnetized ferromagnetic elements, but the switching is deterministic only in the presence of a symmetry-breaking in-plane field. Although spin-orbit torques led to domain nucleation in continuous films and to stochastic nucleation of skyrmions in magnetic tracks, no practical means to create individual skyrmions controllably in an integrated device design at a selected position has been reported yet. Here we demonstrate that sub-nanosecond spin-orbit torque pulses can generate single skyrmions at custom-defined positions in a magnetic racetrack deterministically using the same current path as used for the shifting operation. The effect of the DMI implies that no external in-plane magnetic fields are needed for this aim. This implementation exploits a defect, such as a constriction in the magnetic track, that can serve as a skyrmion generator. The concept is applicable to any track geometry, including three-dimensional designs.

Colloidal domain lithography in multilayers with perpendicular anisotropy: an experimental study and micromagnetic simulations.

Currently, much attention is being paid to patterned multilayer systems in which there exists a perpendicular magnetic anisotropy, because of their potential applications in spintronics devices and in a new generation of magnetic storage media. To further improve their performance, different patterning techniques can be used, which render them suitable also for other applications. Here we show that He(+) 10 keV and Ar(+) 100 keV ion bombardment of (Ni(80)Fe(20)-2 nm/Au-2 nm/Co-0.6 nm/Au-2 nm)(10) multilayers through colloidal mask enables magnetic patterning of regularly arranged cylindrical magnetic domains, with perpendicular anisotropy, embedded in a non-ferromagnetic matrix or in a ferromagnetic matrix with magnetization oriented along the normal. These domains form an almost perfect two-dimensional hexagonal lattice with a submicron period and a large correlation length in a continuous and flat multilayer system. The magnetic anisotropy of these artificial domains remains unaffected by the magnetic patterning process, however the magnetization configuration of such a system depends on the magnetic properties of the matrix. The micromagnetic simulations were used to explain some of the features of the investigated patterned structures.

Plasma ion source for in situ ion bombardment in a soft x-ray magnetic scattering diffractometer.

A new plasma ion source for in situ keV He ion bombardment of solid state samples or thin films was designed and built for ion fluences between 1 × 10(12) and 1 × 10(17) ions/cm(2). The system was designed to be mounted to different diffraction chambers for soft x-ray resonant magnetic scattering. Without breaking the vacuum due to He-ion bombardment, structural and magnetic modifications of the samples can be studied in situ and element specifically.

Asymmetric magnetization reversal of stripe-patterned exchange bias layer systems for controlled magnetic particle transport.

Domain wall movement assisted transport of particles: exchange-biased samples with designed stripe-domains show strong stray fields and an asymmetric magnetization reversal. Using these characteristics superparamagnetic particles can be trapped and transported directly on the sample over large-scale areas. High particle velocities, small external fields, and automatically reduced particle clustering allow broad applicability of this transport method.

Colloidal domain lithography for regularly arranged artificial magnetic out-of-plane monodomains in Au/Co/Au layers.

Regularly arranged magnetic out-of-plane patterns in continuous and flat films are promising for applications in data storage technology (bit patterned media) or transport of individual magnetic particles. Whereas topographic magnetic structures are fabricated by standard lithographical techniques, the fabrication of regularly arranged artificial domains in topographically flat films is difficult, since the free energy minimization determines the existence, shape, and regularity of domains. Here we show that keV He(+) ion bombardment of Au/Co/Au layer systems through a colloidal mask of hexagonally arranged spherical polystyrene beads enables magnetic patterning of regularly arranged cylindrical magnetic monodomains with out-of-plane magnetization embedded in a ferromagnetic matrix with easy-plane anisotropy. This colloidal domain lithography creates artificial domains via periodic lateral anisotropy variations induced by periodic defect density modulations. Magnetization reversal of the layer system observed by magnetic force microscopy shows individual disc switching indicating monodomain states.