Uncovering the physical mechanisms that govern ultrafast charge and spin dynamics is crucial for understanding correlated matter as well as the fundamental limits of ultrafast spin-based electronics. Spin dynamics in magnetic materials can be driven by ultrashort light pulses, resulting in a transient drop in magnetization within a few hundred femtoseconds. However, a full understanding of femtosecond spin dynamics remains elusive. Here we spatially separate the spin dynamics using Ni/Ru/Fe magnetic trilayers, where the Ni and Fe layers can be ferro- or antiferromagnetically coupled. By exciting the layers with a laser pulse and probing the magnetization response simultaneously but separately in Ni and Fe, we surprisingly find that optically induced demagnetization of the Ni layer transiently enhances the magnetization of the Fe layer when the two layer magnetizations are initially aligned parallel. Our observations are explained by a laser-generated superdiffusive spin current between the layers.

Ultrafast Magnetization Enhancement in Metallic Multilayers Driven by Superdiffusive Spin Current

This year the discovery of femtosecond demagnetization by laser pulses is 20 years old. For the first time, this milestone work by Bigot and coworkers gave insight directly into the time scales of microscopic interactions that connect the spin and electron system. While intense discussions in the field were fueled by the complexity of the processes in the past, it now became evident that it is a puzzle of many different parts. Rather than providing an overview that has been presented in previous reviews on ultrafast processes in ferromagnets, this perspective will show that with our current depth of knowledge the first applications are developed: THz spintronics and all-optical spin manipulation are becoming more and more feasible. The aim of this perspective is to point out where we can connect the different puzzle pieces of understanding gathered over 20 years to develop novel applications. Based on many observations in a large number of experiments. Differences in the theoretical models arise from the localized and delocalized nature of ferromagnetism. Transport effects are intrinsically non-local in spintronic devices and at interfaces. We review the need for multiscale modeling to address the processes starting from electronic excitation of the spin system on the picometer length scale and sub-femtosecond time scale, to spin wave generation, and towards the modeling of ultrafast phase transitions that altogether determine the response time of the ferromagnetic system. Today, our current understanding gives rise to the first usage of ultrafast spin physics for ultrafast magnetism control: THz spintronic devices. This makes the field of ultrafast spin-dynamics an emerging topic open for many researchers right now.

/pdf/perspective-ultrafast-magnetism-and-thz-spintronics-4cicss3bvz.pdf

Perspective: Ultrafast magnetism and THz spintronics

This year the discovery of femtosecond demagnetization by laser pulses is 20 years old. For the first time this milestone work by Bigot and coworkers gave insight in a very direct way into the time scales of microscopic interactions that connect the spin and electron system. While intense discussions in the field were fueled by the complexity of the processes in the past, it now became evident that it is a puzzle of many different parts. Rather than giving an overview that has been presented in previous reviews on ultrafast processes in ferromagnets, this perspective will show that with our current depth of knowledge the first real applications are on their way: THz spintronics and all-optical spin manipulation are becoming more and more feasible. The aim of this perspective is to point out where we can connect the different puzzle pieces of understanding gathered over 20 years to develop novel applications. based on many observations in a large number of experiments. Differences in the theoretical models arise from the localized and delocalized nature of ferromagnetism. Transport effects are intrinsically non-local in spintronic devices and at interfaces. We review the need for multiscale modeling to address processes starting from electronic excitation of the spin system on the picometer length scale and sub-femtosecond time scale, to spin wave generation, and towards the modeling of ultrafast phase transitions that altogether determine the response time of the ferromagnetic system. Today, our current understanding gives rise to the first real applications of ultrafast spin physics for ultrafast magnetism control: THz spintronic devices. This makes the field of ultrafast spin-dynamics an emerging topic open for many researchers right now.

Electronic interactions underlie the exchange interaction responsible for the magnetic ordering and dynamics of magnetic materials. Here, Mentink et al. theoretically demonstrate the ultrafast and reversible tuning of the exchange interaction in Mott insulators driven by a time-periodic electric field.

/pdf/ultrafast-and-reversible-control-of-the-exchange-interaction-3ek28vw8g7.pdf

Ultrafast and reversible control of the exchange interaction in Mott insulators

Ultrafast non-thermal manipulation of magnetization by light relies on either indirect coupling of the electric field component of the light with spins via spin-orbit interaction or direct coupling between the magnetic field component and spins. Here we propose a scenario for coupling between the electric field of light and spins via optical modification of the exchange interaction, one of the strongest quantum effects with strength of 10(3) Tesla. We demonstrate that this isotropic opto-magnetic effect, which can be called inverse magneto-refraction, is allowed in a material of any symmetry. Its existence is corroborated by the experimental observation of terahertz emission by spin resonances optically excited in a broad class of iron oxides with a canted spin configuration. From its strength we estimate that a sub-picosecond modification of the exchange interaction by laser pulses with fluence of about 1 mJ cm(-2) acts as a pulsed effective magnetic field of 0.01 Tesla.

http://johanmentink.com/index.php/download_file/view/33/1/

Ultrafast optical modification of exchange interactions in iron oxides

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.

/pdf/disparate-ultrafast-dynamics-of-itinerant-and-localized-1krj85t3ac.pdf

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

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.

/pdf/a-high-order-harmonic-generation-apparatus-for-time-and-3zgr8s126x.pdf

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

The temporal evolution of the exchange-split Δ(2)-like Σ valence bands of the 4f-ferromagnet gadolinium after femtosecond laser excitation has been studied using angle-resolved photoelectron spectroscopy based on high-order harmonic generation. The ultrafast drop of the exchange splitting reflects the magnetic response seen in femtosecond magnetic dichroism experiments. However, while the minority valence band reacts immediately, the response of the majority counterpart is delayed by 1 picosecond and is only half as fast. These findings demonstrate that laser excitation drives the valence band structure out of magnetic equilibrium.

/pdf/femtosecond-laser-excitation-drives-ferromagnetic-gadolinium-4bfxg8bjlz.pdf

Femtosecond laser excitation drives ferromagnetic gadolinium out of magnetic equilibrium.

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.

https://advances.sciencemag.org/content/advances/6/39/eabb1601.full.pdf

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

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 $\mathrm{\ensuremath{\Delta}}$ through the ultrafast phase transition and show that $\mathrm{\ensuremath{\Delta}}$ 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.

/pdf/ultrafast-spin-density-wave-transition-in-chromium-governed-1ognovpahe.pdf

Björn Frietsch

Papers

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

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

Femtosecond laser excitation drives ferromagnetic gadolinium out of magnetic equilibrium.

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

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