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Paul Herrgen

Publications and source records attributed to Paul Herrgen.

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Unlocking ultrafast spin dynamics in a rare-earth magnet

The speed of optically driven magnetization dynamics is fundamentally determined by how efficiently angular momentum can be transferred between electronic, spin and lattice degrees of freedom. In rare-earth magnets, this process is typically slow because optical excitation primarily addresses itinerant electrons, whereas the magnetic moment resides in localized 4f states. Here we show that selective optical excitation of localized magnetic states can overcome this limitation. Using femtosecond pump-probe magneto-optical spectroscopy of ferrimagnetic gadolinium iron garnet, we resonantly excite an intra-4f transition of Gd3+ at 4.65 eV and resolve the ensuing dynamics of the antiferromagnetically coupled Gd and Fe sublattices. Direct excitation of the 4f manifold induces an ultrafast demagnetization of the Gd sublattice with a characteristic time of 38 fs, more than two orders of magnitude faster than in elemental gadolinium and even faster than the response of the Fe sublattice in the same material. By contrast, off-resonant excitation strongly suppresses the acceleration of the Gd dynamics while leaving the Fe response largely unchanged. These results demonstrate that the ultrafast magnetic response of rare-earth systems is governed not only by intrinsic material properties but also by the optical excitation pathway. Selective access to localized magnetic states therefore provides a powerful photonic handle for engineering angular-momentum flow and controlling magnetism far from equilibrium.

cond-mat.mtrl-sci

Dynamic interfacial effects in ultrathin ferromagnetic bilayers

We investigate the magnetization dynamics of an ultrathin Co (1.5 nm) /Py (1.5 nm) bilayer system from femtosecond (fs) to nanosecond (ns) timescales. Magnetization dynamics in the fs timescales is characterized as a highly non-equilibrium regime due to an ultrafast reduction of magnetization by laser excitation. On the other hand, the dynamics in the ns timescales is characterized as a close-to-equilibrium regime involving the excitation of coherent magnons. We demonstrate that the interfacial interaction between the Co and Py layers in these two non-equilibrium regimes across the timescales is dynamic and simultaneously influences the magnetization loss in the fs timescales and the magnon dynamics in the ns timescales. On ultrafast (fs) timescales, comparison between time-resolved magneto-optical Kerr effect (TR-MOKE) measurements and temperature-based {\mu}T model simulations reveals that the bilayer exhibits demagnetization dynamics intermediate between those of its individual layers. When driven far from equilibrium by ultrashort laser pulse excitation, the magnetization dynamics of the individual Co and Py layers appear to remain decoupled and evolve independently in the initial stages of the ultrafast response. On the other hand, in the ns regime, the two individual layers of the bilayer precess together at the same frequency in a coupled manner as one effective single layer. Furthermore, by correlating the ultrafast demagnetization to precessional damping we attempt to bridge the two non-equilibrium regimes across fs to ns timescales. These results improve our understanding of magnetization dynamics across timescales in ultrathin exchanged-coupled ferromagnetic bilayers and provide valuable insights for the design of high-frequency and energy efficient spintronic device concepts.

cond-mat.mtrl-sci

All optical excitation of spin polarization in d-wave altermagnets

The recently discovered altermagnets exhibit collinear magnetic order with zero net magnetization but with unconventional spin-polarized d/g/i-wave band structures, expanding the known paradigms of ferromagnets and antiferromagnets. In addition to novel current-driven electronic transport effects, the unconventional time-reversal symmetry breaking in these systems also makes it possible to obtain a spin response to \emph{linearly polarized} fields in the optical frequency domain. We show through ab-initio calculations of the prototypical d-wave altermagnet RuO$_2$, with a symmetry combining twofold spin rotation with fourfold lattice rotation, $[C_2\|C_{4z}]$, that there is an optical analogue of a spin splitter effect, as the coupling to a linearly polarized exciting laser field makes the d-wave character of the altermagnet directly visible. By magneto-optical measurements on RuO$_2$ films of different thicknesses ranging from $2$ to $8\,$nanometers, we demonstrate the predicted connection of the linear polarization of an ultrashort pump pulse to the sign and magnitude of the optically excited electronic spin polarization in the ultrathin RuO$_2$ films. The possibility of exciting and controlling an electronic spin polarization by linearly polarized optical pulses in a compensated system is a unique consequence of the altermagnetic material properties. Our experimental results therefore establish an optical pump-probe based protocol for detection of altermagnetic characteristics in ultrathin RuO$_2$ films, but our all-optical approach should apply more generally to materials in this altermagnetic symmetry class.

cond-mat.mtrl-sci

Laser-induced Creation of antiferromagnetic 180-degree domains in NiO/Pt bilayers

We demonstrate how the antiferromagnetic order in heterostructures of NiO/Pt thin films can be modified by optical pulses. We irradiate our samples with laser light and identify an optically induced creation of antiferromagnetic domains by imaging the created domain structure utilizing the X-ray magnetic linear dichroism effect. We study the effect of different laser polarizations on the domain formation and identify a polarization-independent creation of 180{\deg} domain walls and domains with 180{\deg} different N\'eel vector orientation. By varying the irradiation parameters, we determine the switching mechanism to be thermally induced and demonstrate the reversibility. We thus demonstrate experimentally the possibility to optically create antiferromagnetic domains, an important step towards future functionalization of all optical switching mechanisms in antiferromagnets.

cond-mat.mtrl-sci

Indirect optical manipulation of the antiferromagnetic order of insulating NiO by ultrafast interfacial energy transfer

We report the ultrafast, (sub)picosecond reduction of the antiferromagnetic order of the insulating NiO thin film in a Pt/NiO bilayer. This reduction of the antiferromagnetic order is not present in pure NiO thin films after a strong optical excitation. This ultrafast phenomenon is attributed to an ultrafast and highly efficient energy transfer from the optically excited electron system of the Pt layer into the NiO spin system. We propose that this energy transfer is mediated by a stochastic exchange scattering of hot Pt electrons at the Pt/NiO interface.

cond-mat.mtrl-sci