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 (approximately 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.

Ferroelectromagnets are an interesting group of compounds that complement purely (anti-)ferroelectric or (anti-)ferromagnetic materials--they display simultaneous electric and magnetic order. With this coexistence they supplement materials in which magnetization can be induced by an electric field and electrical polarization by a magnetic field, a property which is termed the magnetoelectric effect. Aside from its fundamental importance, the mutual control of electric and magnetic properties is of significant interest for applications in magnetic storage media and 'spintronics'. The coupled electric and magnetic ordering in ferroelectromagnets is accompanied by the formation of domains and domain walls. However, such a cross-correlation between magnetic and electric domains has so far not been observed. Here we report spatial maps of coupled antiferromagnetic and ferroelectric domains in YMnO3, obtained by imaging with optical second harmonic generation. The coupling originates from an interaction between magnetic and electric domain walls, which leads to a configuration that is dominated by the ferroelectromagnetic product of the order parameters.

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.

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Optical second harmonic spectroscopy is introduced as a powerful supplement for the determination of complex magnetic structures. Experimental efforts are simplified and new degrees of freedom are opened. Thereby, some principal or technical restrictions of neutron or magnetic x-ray diffraction experiments are overcome. High spatial resolution leads to additional information about magnetically ordered matter. As an example, the noncollinear magnetic structure of the hexagonal manganites RMnO3 ( R = Sc, Y, Ho, Er, Tm, Yb, Lu) is analyzed. The results show that some earlier conclusions on their magnetic symmetry and properties should be revised.

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 103 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.

Magnetic phase diagrams of the hexagonal RMnO3 (with R=Sc, Y, Ho, In, Er, Tm, Yb, Lu) compounds in the magnetic-field/temperature plane are established by linear and nonlinear magneto-optical techniques. Eight different magnetic phases of the Mn3+ sublattice and at least three different phases of the R3+ sublattices are distinguished. Phase coexistence and photoinduced modification of the magnetic structure are observed. Magnetic reorientations of the Mn3+ lattice can occur via in-phase or antiphase rotation of the triangularly frustrated spins in the adjacent crystallographic planes.