The interaction of subpicosecond laser pulses with magnetically ordered materials has developed into a fascinating research topic in modern magnetism. From the discovery of subpicosecond demagnetization over a decade ago to the recent demonstration of magnetization reversal by a single 40 fs laser pulse, the manipulation of magnetic order by ultrashort laser pulses has become a fundamentally challenging topic with a potentially high impact for future spintronics, data storage and manipulation, and quantum computation. Understanding the underlying mechanisms implies understanding the interaction of photons with charges, spins, and lattice, and the angular momentum transfer between them. This paper will review the progress in this field of laser manipulation of magnetic order in a systematic way. Starting with a historical introduction, the interaction of light with magnetically ordered matter is discussed. By investigating metals, semiconductors, and dielectrics, the roles of nearly free electrons, charge redistributions, and spin-orbit and spin-lattice interactions can partly be separated, and effects due to heating can be distinguished from those that are not. It will be shown that there is a fundamental distinction between processes that involve the actual absorption of photons and those that do not. It turns out that for the latter, the polarization of light plays an essential role in the manipulation of the magnetic moments at the femtosecond time scale. Thus, circularly and linearly polarized pulses are shown to act as strong transient magnetic field pulses originating from the nonabsorptive inverse Faraday and inverse Cotton-Mouton effects, respectively. The recent progress in the understanding of magneto-optical effects on the femtosecond time scale together with the mentioned inverse, optomagnetic effects promises a bright future for this field of ultrafast optical manipulation of magnetic order or femtomagnetism.

/pdf/ultrafast-optical-manipulation-of-magnetic-order-2ms2t5k1zo.pdf

Ultrafast optical manipulation of magnetic order

The dynamics of spin ordering in magnetic materials is of interest for both fundamental understanding and progress in information-processing and recording technology. Radu et al. study spin dynamics in a ferrimagnetic gadolinium–iron–cobalt (GdFeCo) alloy that is optically excited at a timescale shorter than the characteristic magnetic exchange interaction between the Gd and Fe spins. Using element-specific X-ray magnetic circular dichroism spectroscopy, they show that the Gd and Fe spins switch directions at very different timescales. As a consequence, an unexpected transient ferromagnetic state emerges. These surprising observations, supported by simulations, provide a possible new concept of manipulating magnetic order on a timescale of the exchange interaction. Ferromagnetic or antiferromagnetic spin ordering is governed by the exchange interaction, the strongest force in magnetism1,2,3,4. 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.

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

Demagnetization in metals occurs on very different timescales depending on the material. It is now shown that electron–phonon-mediated spin scattering describes the process of demagnetization well in every case, and the differences in timescale are mainly determined by the ratio between Curie temperature and the atomic magnetic moment.

Explaining the paradoxical diversity of ultrafast laser-induced demagnetization

This article reviews static and dynamic interfacial effects in magnetism, focusing on interfacially-driven magnetic effects and phenomena associated with spin-orbit coupling and intrinsic symmetry breaking at interfaces. It provides a historical background and literature survey, but focuses on recent progress, identifying the most exciting new scientific results and pointing to promising future research directions. It starts with an introduction and overview of how basic magnetic properties are affected by interfaces, then turns to a discussion of charge and spin transport through and near interfaces and how these can be used to control the properties of the magnetic layer. Important concepts include spin accumulation, spin currents, spin transfer torque, and spin pumping. An overview is provided to the current state of knowledge and existing review literature on interfacial effects such as exchange bias, exchange spring magnets, spin Hall effect, oxide heterostructures, and topological insulators. The article highlights recent discoveries of interface-induced magnetism and non-collinear spin textures, non-linear dynamics including spin torque transfer and magnetization reversal induced by interfaces, and interfacial effects in ultrafast magnetization processes.

https://link.aps.org/accepted/10.1103/RevModPhys.89.025006

Interface-induced phenomena in magnetism

X-ray absorption spectroscopy is a powerful probe of molecular structure, but it has previously been too slow to track the earliest dynamics after photoexcitation. We investigated the ultrafast formation of the lowest quintet state of aqueous iron(II) tris(bipyridine) upon excitation of the singlet metal-to-ligand-charge-transfer ( 1 MLCT) state by femtosecond optical pump/x-ray probe techniques based on x-ray absorption near-edge structure (XANES). By recording the intensity of a characteristic XANES feature as a function of laser pump/x-ray probe time delay, we find that the quintet state is populated in about 150 femtoseconds. The quintet state is further evidenced by its full XANES spectrum recorded at a 300-femtosecond time delay. These results resolve a long-standing issue about the population mechanism of quintet states in iron(II)-based complexes, which we identify as a simple 1 MLCT→ 3 MLCT→ 5 T cascade from the initially excited state. The time scale of the 3 MLCT→ 5 T relaxation corresponds to the period of the iron-nitrogen stretch vibration.

https://science.sciencemag.org/content/sci/323/5913/489.full.pdf

Femtosecond XANES Study of the Light-Induced Spin Crossover Dynamics in an Iron(II) Complex

The rapidly increasing information density required of modern magnetic data storage devices raises the question of the fundamental limits in bit size and writing speed At present, the magnetization reversal of a bit can occur as quickly as 200 ps (ref 1) A fundamental limit has been explored by using intense magnetic-field pulses of 2 ps duration leading to a non-deterministic magnetization reversal For this process, dissipation of spin angular momentum to other degrees of freedom on an ultrafast timescale is crucial An even faster regime down to 100 fs or below might be reached by non-thermal control of magnetization with femtosecond laser radiation Here, we show that an efficient novel channel for angular momentum dissipation to the lattice can be opened by femtosecond laser excitation of a ferromagnet For the first time, the quenching of spin angular momentum and its transfer to the lattice with a time constant of 120+/-70 fs is determined unambiguously with X-ray magnetic circular dichroism We report the first femtosecond time-resolved X-ray absorption spectroscopy data over an entire absorption edge, which are consistent with an unexpected increase in valence-electron localization during the first 120+/-50 fs, possibly providing the driving force behind femtosecond spin-lattice relaxation

Femtosecond modification of electron localization and transfer of angular momentum in nickel.

We present the first X-ray absorption spectrum over an entire absorption edge using femtosecond pulses from a synchrotron-based slicing source. An ultrafast laser pulse excited a nickel film, and a succeeding X-ray pulse from the BESSY femtoslicing facility probed the Ni L3-edge. By choosing either linear or circular X-ray polarization, the spectra represent snapshots of the electronic or the magnetic state, respectively, with an exposure time of about 100 fs. We find an almost instantaneous response of the electronic system to the laser pulse, and provide a first direct measurement of the quenching of magnetic moments within 120 fs.

C. Lupulescu

Papers

Femtosecond modification of electron localization and transfer of angular momentum in nickel.

Ultrafast Electron and Spin Dynamics in Nickel Probed With Femtosecond X-Ray Pulses