T.H.M. Rasing

Ultrafast non-thermal control of magnetization by instantaneous photomagnetic pulses

The demand for ever-increasing density of information storage and speed of manipulation has triggered an intense search for ways to control the magnetization of a medium by means other than magnetic fields. Recent experiments on laser-induced demagnetization and spin reorientation use ultrafast lasers as a means to manipulate magnetization, accessing timescales of a picosecond or less. However, in all these cases the observed magnetic excitation is the result of optical absorption followed by a rapid temperature increase. This thermal origin of spin excitation considerably limits potential applications because the repetition frequency is limited by the cooling time. Here we demonstrate that circularly polarized femtosecond laser pulses can be used to non-thermally excite and coherently control the spin dynamics in magnets by way of the inverse Faraday effect. Such a photomagnetic interaction is instantaneous and is limited in time by the pulse width (∼200 fs in our experiment). Our finding thus reveals an alternative mechanism of ultrafast coherent spin control, and offers prospects for applications of ultrafast lasers in magnetic devices.

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

Ferromagnetic or antiferromagnetic spin ordering is governed by the exchange interaction, the strongest force in magnetism. 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.

Ultrafast precessional magnetization reversal by picosecond magnetic field pulse shaping

Since the invention of the first magnetic memory disk in 1954, much effort has been put into enhancing the speed, bit density and reliability of magnetic memory devices. In the case of magnetic random access memory (MRAM) devices, fast coherent magnetization rotation by precession of the entire memory cell is desired, because reversal by domain-wall motion is much too slow. In principle, the fundamental limit of the switching speed via precession is given by half of the precession period. However, under-critically damped systems exhibit severe ringing and simulations show that, as a consequence, undesired back-switching of magnetic elements of an MRAM can easily be initiated by subsequent write pulses, threatening data integrity. We present a method to reverse the magnetization in under-critically damped systems by coherent rotation of the magnetization while avoiding any ringing. This is achieved by applying specifically shaped magnetic field pulses that match the intrinsic properties of the magnetic elements. We demonstrate, by probing all three magnetization components, that reliable precessional reversal in lithographically structured micrometre-sized elliptical permalloy elements is possible at switching times of about 200 ps, which is ten times faster than the natural damping time constant.

Magnetic photonic crystals

In this paper we outline a new direction in the area of photonic crystals (PCs), or photonic band gap materials, i.e. one-, two-, or three-dimensional superstructures with periods that are comparable with the wavelengths of electromagnetic radiation. The main (and principal) characteristic of this new class of PCs is the presence of magnetically ordered components (or external magnetic field). The linear and nonlinear optical properties of such magnetic PCs are discussed.

Macroscopic Hierarchical Surface Patterning of Porphyrin Trimers via Self-Assembly and Dewetting

The use of bottom-up approaches to construct patterned surfaces for technological applications is appealing, but to date is applicable to only relatively small areas (∼10 square micrometers). We constructed highly periodic patterns at macroscopic length scales, in the range of square millimeters, by combining self-assembly of disk-like porphyrin dyes with physical dewetting phenomena. The patterns consisted of equidistant 5-nanometer-wide lines spaced 0.5 to 1 micrometers apart, forming single porphyrin stacks containing millions of molecules, and were formed spontaneously upon drop-casting a solution of the molecules onto a mica surface. On glass, thicker lines are formed, which can be used to align liquid crystals in large domains of square millimeter size.

Laser-induced ultrafast spin reorientation in the antiferromagnet TmFeO3.

All magnetically ordered materials can be divided into two primary classes: ferromagnets and antiferromagnets. Since ancient times, ferromagnetic materials have found vast application areas, from the compass to computer storage and more recently to magnetic random access memory and spintronics. In contrast, antiferromagnetic (AFM) materials, though representing the overwhelming majority of magnetically ordered materials, for a long time were of academic interest only. The fundamental difference between the two types of magnetic materials manifests itself in their reaction to an external magnetic field—in an antiferromagnet, the exchange interaction leads to zero net magnetization. The related absence of a net angular momentum should result in orders of magnitude faster AFM spin dynamics. Here we show that, using a short laser pulse, the spins of the antiferromagnet TmFeO3 can indeed be manipulated on a timescale of a few picoseconds, in contrast to the hundreds of picoseconds in a ferromagnet. Because the ultrafast dynamics of spins in antiferromagnets is a key issue for exchange-biased devices, this finding can expand the now limited set of applications for AFM materials.

Laser-induced magnetization dynamics and reversal in ferrimagnetic alloys

This review discusses the recent studies of magnetization dynamics and the role of angular momentum in thin films of ferrimagnetic rare-earth-transition metal (RE-TM) alloys, e.g. GdFeCo, where both magnetization and angular momenta are temperature dependent. It has been experimentally demonstrated that the magnetization can be manipulated and even reversed by a single 40 fs laser pulse, without any applied magnetic field. This switching is found to follow a novel reversal pathway, that is shown however to depend crucially on the net angular momentum, reflecting the balance of the two opposite sublattices. In particular, optical excitation of ferrimagnetic GdFeCo on a time scale pertinent to the characteristic time of the exchange interaction between the RE and TM spins, i.e. on the time scale of tens of femtoseconds, pushes the spin dynamics into a yet unexplored regime, where the two exchange-coupled magnetic sublattices demonstrate substantially different dynamics. As a result, the reversal of spins appears to proceed via a novel transient state characterized by a ferromagnetic alignment of the Gd and Fe magnetic moments, despite their ground-state antiferromagnetic coupling.Thus, optical manipulation of magnetic order by femtosecond laser pulses has developed into an exciting and still expanding research field that keeps being fueled by a continuous stream of new and sometimes counterintuitive results. Considering the progress in the development of plasmonic antennas and compact ultrafast lasers, optical control of magnetic order may also potentially revolutionize data storage and information processing technologies.

Ultrafast heating as a sufficient stimulus for magnetization reversal in a ferrimagnet

The question of how, and how fast, magnetization can be reversed is a topic of great practical interest for the manipulation and storage of magnetic information. It is generally accepted that magnetization reversal should be driven by a stimulus represented by time-non-invariant vectors such as a magnetic field, spin-polarized electric current, or cross-product of two oscillating electric fields. However, until now it has been generally assumed that heating alone, not represented as a vector at all, cannot result in a deterministic reversal of magnetization, although it may assist this process. Here we show numerically and demonstrate experimentally a novel mechanism of deterministic magnetization reversal in a ferrimagnet driven by an ultrafast heating of the medium resulting from the absorption of a sub-picosecond laser pulse without the presence of a magnetic field.

Nanoscale spin reversal by non-local angular momentum transfer following ultrafast laser excitation in ferrimagnetic GdFeCo

Ultrafast laser techniques have revealed extraordinary spin dynamics in magnetic materials that equilibrium descriptions of magnetism cannot explain. Particularly important for future applications is understanding non-equilibrium spin dynamics following laser excitation on the nanoscale, yet the limited spatial resolution of optical laser techniques has impeded such nanoscale studies. Here we present ultrafast diffraction experiments with an X-ray laser that probes the nanoscale spin dynamics following optical laser excitation in the ferrimagnetic alloy GdFeCo, which exhibits macroscopic all-optical switching. Our study reveals that GdFeCo displays nanoscale chemical and magnetic inhomogeneities that affect the spin dynamics. In particular, we observe Gd spin reversal in Gd-rich nanoregions within the first picosecond driven by the non-local transfer of angular momentum from larger adjacent Fe-rich nanoregions. These results suggest that a magnetic materials microstructure can be engineered to control transient laser-excited spins, potentially allowing faster (~ 1 ps) spin reversal than in present technologies.

Complete Chiral Symmetry Breaking of an Amino Acid Derivative Directed by Circularly Polarized Light

Circularly polarized light (CPL) emitted from star-forming regions is an attractive candidate as a cause of single chirality in nature. It has remained difficult, however, to translate the relatively small chemical effects observed on irradiation of molecular systems with CPL into high enantiomeric excesses. Here we demonstrate that irradiation of a racemic amino acid derivative with CPL leads to a small amount of chiral induction that can be amplified readily to give an enantiopure solid phase. A racemate composed of equal amounts of left- and right-handed crystals in contact with the irradiated solution is converted completely into crystals of single-handedness through abrasive grinding when racemization is effected in the solution. The rotation sense of the CPL fully determines the handedness of the final solid state. These findings illustrate the potential effectiveness of CPL in the control of molecular asymmetry, which is relevant for the origin of the single chirality inherent to many biological molecules.