Charge-induced chemical dynamics in glycine probed with time-resolved Auger electron spectroscopy.

In the present contribution, we use x-rays to monitor charge-induced chemical dynamics in the photoionized amino acid glycine with femtosecond time resolution. The outgoing photoelectron leaves behind the cation in a coherent superposition of quantum mechanical eigenstates. Delayed x-ray pulses track the induced coherence through resonant x-ray absorption that induces Auger decay. Temporal modulation of the Auger electron signal correlated with specific ions is observed, which is governed by the initial electronic coherence and subsequent vibronic coupling to nuclear degrees of freedom. In the time-resolved x-ray absorption measurement, we monitor the time-frequency spectra of the resulting many-body quantum wave packets for a period of 175 fs along different reaction coordinates. Our experiment proves that by measuring specific fragments associated with the glycine dication as a function of the pump-probe delay, one can selectively probe electronic coherences at early times associated with a few distinguishable components of the broad electronic wave packet created initially by the pump pulse in the cation. The corresponding coherent superpositions formed by subsets of electronic eigenstates and evolving along parallel dynamical pathways show different phases and time periods in the range of ( - 0.3 ± 0.1 ) π ≤ ϕ ≤ ( 0.1 ± 0.2 ) π and 18.2 - 1.4 + 1.7 ≤ T ≤ 23.9 - 1.1 + 1.2 fs. Furthermore, for long delays, the data allow us to pinpoint the driving vibrational modes of chemical dynamics mediating charge-induced bond cleavage along different reaction coordinates.

Electronic quantum coherence in glycine molecules probed with ultrashort x-ray pulses in real time.

Here, we use x-rays to create and probe quantum coherence in the photoionized amino acid glycine. The outgoing photoelectron leaves behind the cation in a coherent superposition of quantum mechanical eigenstates. Delayed x-ray pulses track the induced coherence through resonant x-ray absorption that induces Auger decay and by photoelectron emission from sequential double photoionization. Sinusoidal temporal modulation of the detected signal at early times (0 to 25 fs) is observed in both measurements. Advanced ab initio many-electron simulations allow us to explain the first 25 fs of the detected coherent quantum evolution in terms of the electronic coherence. In the kinematically complete x-ray absorption measurement, we monitor its dynamics for a period of 175 fs and observe an evolving modulation that may implicate the coupling of electronic to vibronic coherence at longer time scales. Our experiment provides a direct support for the existence of long-lived electronic coherence in photoionized biomolecules.

Novel Tunnel Magnetoresistive Sensor Functionalities via Oblique-Incidence Deposition.

Controlling the magnetic properties of ultrathin films remains one of the main challenges to the further development of tunnel magnetoresistive (TMR) device applications. The magnetic response in such devices is mainly governed by extending the primary TMR trilayer with the use of suitable contact materials. The transfer of magnetic anisotropy to ferromagnetic electrodes consisting of CoFeB layers results in a field-dependent TMR response, which is determined by the magnetic properties of the CoFeB as well as the contact materials. We flexibly apply oblique-incidence deposition (OID) to introduce arbitrary intrinsic in-plane anisotropy profiles into the magnetic layers. The OID-induced anisotropy shapes the magnetic response and eliminates the requirement of additional magnetic contact materials. Functional control is achieved via an adjustable shape anisotropy that is selectively tailored for the ultrathin CoFeB layers. This approach circumvents previous limitations on TMR devices and allows for the design of new sensing functionalities, which can be precisely customized to a specific application, even in the high field regime. The resulting sensors maintain the typical TMR signal strength as well as a superb thermal stability of the tunnel junction, revealing a striking advantage in functional TMR design using anisotropic interfacial roughness.

Bulk, cascaded pulse compression scheme and its application to spin emitter characterization.

The 35-fs-long pulses of a commercial Ti:sapphire amplifier are compressed to ∼20fs via self-phase modulation in bulk glass substrates. The cascading of both nonlinear broadening and dispersion compensation stages makes use of the increasing peak power in the successive nonlinear stages. As an application example, the compressed pulses are used for electro-optical sampling of terahertz waves created by optically pumped thin-film spin emitters.

Coherent control of collective nuclear quantum states via transient magnons.

Ultrafast and precise control of quantum systems at x-ray energies involves photons with oscillation periods below 1 as. Coherent dynamic control of quantum systems at these energies is one of the major challenges in hard x-ray quantum optics. Here, we demonstrate that the phase of a quantum system embedded in a solid can be coherently controlled via a quasi-particle with subattosecond accuracy. In particular, we tune the quantum phase of a collectively excited nuclear state via transient magnons with a precision of 1 zs and a timing stability below 50 ys. These small temporal shifts are monitored interferometrically via quantum beats between different hyperfine-split levels. The experiment demonstrates zeptosecond interferometry and shows that transient quasi-particles enable accurate control of quantum systems embedded in condensed matter environments.

Incoherent Nuclear Resonant Scattering from a Standing Spin Wave.

We introduce a method to study the spatial profiles of standing spin waves in ferromagnetic microstructures. The method relies on Nuclear Resonant Scattering of 57Fe using a microfocused beam of synchrotron radiation, the transverse coherence length of which is smaller than the length scale of lateral variations in the magnetization dynamics. Using this experimental method, the nuclear resonant scattering signal due to a confined spin wave is determined on the basis of an incoherent superposition model. From the fits of the Nuclear Resonant Scattering time spectra, the precessional amplitude profile across the stripe predicted by an analytical model is reconstructed. Our results pave the way for studying non-homogeneous dynamic spin configurations in microstructured magnetic systems using nuclear resonant scattering of synchrotron light.

Coherent THz Transient Spin Currents by Spin Pumping.

The generation of short spin current pulses is the basis for fast spintronic devices. In thin bilayer systems consisting of a nonmagnetic metal and a ferromagnet, a pure spin current is induced by a precessing magnetization into the nonmagnetic layer by spin pumping. This effect has been experimentally demonstrated at ferromagnetic resonance at GHz frequencies. Here, it is theoretically shown that transient magnetization dynamics efficiently generates short spin current pulses that exhibit two transient contributions. An effective coherent spin current generation is found far above the ferromagnetic resonance up to THz frequencies although dynamic magnetization amplitudes are very small in this regime. The results provide a concept for coherent THz spin current generation.

Nuclear Resonant Surface Diffraction of Synchrotron Radiation.

Nuclear resonant x-ray diffraction in grazing incidence geometry is used to determine the lateral magnetic configuration in a one-dimensional lattice of ferromagnetic nanostripes. During magnetic reversal, strong nuclear superstructure diffraction peaks appear in addition to the electronic ones due to an antiferromagnetic order in the nanostripe lattice. We show that the analysis of the angular distribution together with the time dependence of the resonantly diffracted x rays reveals surface spin structures with very high sensitivity. This scattering technique provides unique access to laterally correlated spin configurations in magnetically ordered nanostructures and, in perspective, also to their dynamics.

Model of THz Magnetization Dynamics.

Magnetization dynamics can be coherently controlled by THz laser excitation, which can be applied in ultrafast magnetization control and switching. Here, transient magnetization dynamics are calculated for excitation with THz magnetic field pulses. We use the ansatz of Smit and Beljers, to formulate dynamic properties of the magnetization via partial derivatives of the samples free energy density, and extend it to solve the Landau-Lifshitz-equation to obtain the THz transients of the magnetization. The model is used to determine the magnetization response to ultrafast multi- and single-cycle THz pulses. Control of the magnetization trajectory by utilizing the THz pulse shape and polarization is demonstrated.

Tunable Subluminal Propagation of Narrow-band X-Ray Pulses.

Group velocity control is demonstrated for x-ray photons of 14.4 keV energy via a direct measurement of the temporal delay imposed on spectrally narrow x-ray pulses. Subluminal light propagation is achieved by inducing a steep positive linear dispersion in the optical response of 57Fe Mössbauer nuclei embedded in a thin film planar x-ray cavity. The direct detection of the temporal pulse delay is enabled by generating frequency-tunable spectrally narrow x-ray pulses from broadband pulsed synchrotron radiation. Our theoretical model is in good agreement with the experimental data.

Spin precession mapping at ferromagnetic resonance via nuclear resonant scattering of synchrotron radiation.

We probe the spin dynamics in a thin magnetic film at ferromagnetic resonance by nuclear resonant scattering of synchrotron radiation at the 14.4 keV resonance of ^{57}Fe. The precession of the magnetization leads to an apparent reduction of the magnetic hyperfine field acting at the ^{57}Fe nuclei. The spin dynamics is described in a stochastic relaxation model adapted to the ferromagnetic resonance theory by Smit and Beljers to model the decay of the excited nuclear state. From the fits of the measured data, the shape of the precession cone of the spins is determined. Our results open a new perspective to determine magnetization dynamics in layered structures with very high depth resolution by employing ultrathin isotopic probe layers.

Spin waves and domain wall modes in curved magnetic nanowires.

The confinement of spin waves in inhomogeneous fields and spin wave interaction with domain walls has attracted interest due to possible applications in magnonics. We investigate spin waves in curved ferromagnetic nanowires. The field dispersion and localization of spin waves is revealed by comparison to known modes in stripes and taking into account the specific field reversal of the curved wire. In small wires we find a strongly altered mode spectrum in a certain field regime. Micromagnetic simulations show an extended domain wall within the wire in this field region. The domain wall shows several dynamic modes and changes the remaining spin wave modes. We find mode suppression as well as newly arising modes due to the strong inhomogenous internal field of the wall.

Magnetic soft x-ray microscopy of the domain wall depinning process in permalloy magnetic nanowires.

Full-field magnetic transmission x-ray microscopy at high spatial resolution down to 20 nm is used to directly observe field-driven domain wall motion in notch-patterned permalloy nanowires. The depinning process of a domain wall around a notch exhibits a stochastic nature in most nanowires. The stochasticity of the domain wall depinning sensitively depends on the geometry of the nanowire such as the wire thickness, the wire width, and the notch depth. We propose an optimized design of the nanowire for deterministic domain wall depinning field at a notch.

Tunable negligible-loss energy transfer between dipolar-coupled magnetic disks by stimulated vortex gyration.

A wide variety of coupled harmonic oscillators exist in nature. Coupling between different oscillators allows for the possibility of mutual energy transfer between them and the information-signal propagation. Low-energy input signals and their transport with negligible energy loss are the key technological factors in the design of information-signal processing devices. Here, utilizing the concept of coupled oscillators, we experimentally demonstrated a robust new mechanism for energy transfer between spatially separated dipolar-coupled magnetic disks - stimulated vortex gyration. Direct experimental evidence was obtained by a state-of-the-art experimental time-resolved soft X-ray microscopy probe. The rate of energy transfer from one disk to the other was deduced from the two normal modes' frequency splitting caused by dipolar interaction. This mechanism provides the advantages of tunable energy transfer rates, low-power input signals and negligible energy loss in the case of negligible intrinsic damping. Coupled vortex-state disks might be implemented in applications for information-signal processing.

Direct observation of stochastic domain-wall depinning in magnetic nanowires.

The stochastic field-driven depinning of a domain wall pinned at a notch in a magnetic nanowire is directly observed using magnetic x-ray microscopy with high lateral resolution down to 15 nm. The depinning-field distribution in Ni80Fe20 nanowires considerably depends on the wire width and the notch depth. The difference in the multiplicity of domain-wall types generated in the vicinity of a notch is responsible for the observed dependence of the stochastic nature of the domain-wall depinning field on the wire width and the notch depth. Thus the random nature of the domain-wall depinning process is controllable by an appropriate design of the nanowire.

Dependence of magnetic domain-wall motion on a fast changing current.

A dependence of current-induced domain-wall motion in nanowires on the temporal shape of current pulses is observed. The results show that the motion of the wall is amplified for alterations of the current on a time scale smaller than the intrinsic time scale of the domain wall which is a few nanoseconds in permalloy. This effect arises from an additional force on the wall by the spin-transfer torque due to a fast changing current and improves the efficiency of domain-wall motion. The observations provide an understanding for the efficient domain-wall motion with nanosecond current pulses.

Time-resolved x-ray microscopy of spin-torque-induced magnetic vortex gyration.

Time-resolved x-ray microscopy is used to image the influence of alternating high-density currents on the magnetization dynamics of ferromagnetic vortices. Spin-torque-induced vortex gyration is observed in micrometer-sized permalloy squares. The phases of the gyration in structures with different chirality are compared to an analytical model and micromagnetic simulations, considering both alternating spin-polarized currents and the current's Oersted field. In our case the driving force due to spin-transfer torque is about 70% of the total excitation while the remainder originates from the current's Oersted field. This finding has implications to magnetic storage devices using spin-torque driven magnetization switching and domain-wall motion.