Ultrafast Amplification and Nonlinear Magnetoelastic Coupling of Coherent Magnon Modes in an Antiferromagnet.

We investigate the role of domain walls in the ultrafast magnon dynamics of an antiferromagnetic NiO single crystal in a pump-probe experiment with variable pump photon energy. Analyzing the amplitude of the energy-dependent photoinduced ultrafast spin dynamics, we detect a yet unreported coupling between the material's characteristic terahertz- and gigahertz-magnon modes. We explain this unexpected coupling between two orthogonal eigenstates of the corresponding Hamiltonian by modeling the magnetoelastic interaction between spins in different domains. We find that such interaction, in the nonlinear regime, couples the two different magnon modes via the domain walls and it can be optically exploited via the exciton-magnon resonance.

Wide spectral range ultrafast pump-probe magneto-optical spectrometer at low temperature, high-magnetic and electric fields.

We developed a table-top setup to perform magneto-optical pump-probe measurements with the possibility to independently tune the photon-energy of both pump and probe beams in the 0.5 eV-3.5 eV range. Our apparatus relies on a commercial turn-key amplified laser system, able to generate light pulses with duration shorter than or comparable to 100 fs throughout the whole spectral range. The repetition rate of the source can be modified via the computer in the 1 kHz to 1 MHz range. A commercial balanced detector is connected to a high-frequency digitizer, allowing for a highly-sensitive detection scheme: rotations of the probe polarization as small as 70 µdeg can be measured. Additionally, a DC magnetic field as high as 9 T and voltages in the kV regime can be applied on the sample. A cryostat allows us to precisely set the temperature of the specimen in the 4 K-420 K interval. We prove the performance of our setup by measuring the ultrafast demagnetization of a cobalt crystal as a function of a wide variety of experimental parameters.

Ultrafast optically induced spin transfer in ferromagnetic alloys.

The vision of using light to manipulate electronic and spin excitations in materials on their fundamental time and length scales requires new approaches in experiment and theory to observe and understand these excitations. The ultimate speed limit for all-optical manipulation requires control schemes for which the electronic or magnetic subsystems of the materials are coherently manipulated on the time scale of the laser excitation pulse. In our work, we provide experimental evidence of such a direct, ultrafast, and coherent spin transfer between two magnetic subsystems of an alloy of Fe and Ni. Our experimental findings are fully supported by time-dependent density functional theory simulations and, hence, suggest the possibility of coherently controlling spin dynamics on subfemtosecond time scales, i.e., the birth of the research area of attomagnetism.

Tuning the charge flow between Marcus regimes in an organic thin-film device.

Marcus's theory of electron transfer, initially formulated six decades ago for redox reactions in solution, is now of great importance for very diverse scientific communities. The molecular scale tunability of electronic properties renders organic semiconductor materials in principle an ideal platform to test this theory. However, the demonstration of charge transfer in different Marcus regions requires a precise control over the driving force acting on the charge carriers. Here, we make use of a three-terminal hot-electron molecular transistor, which lets us access unconventional transport regimes. Thanks to the control of the injection energy of hot carriers in the molecular thin film we induce an effective negative differential resistance state that is a direct consequence of the Marcus Inverted Region.

All-optical control of ferromagnetic thin films and nanostructures.

The interplay of light and magnetism allowed light to be used as a probe of magnetic materials. Now the focus has shifted to use polarized light to alter or manipulate magnetism. Here, we demonstrate optical control of ferromagnetic materials ranging from magnetic thin films to multilayers and even granular films being explored for ultra-high-density magnetic recording. Our finding shows that optical control of magnetic materials is a much more general phenomenon than previously assumed and may have a major impact on data memory and storage industries through the integration of optical control of ferromagnetic bits.

Engineered materials for all-optical helicity-dependent magnetic switching.

The possibility of manipulating magnetic systems without applied magnetic fields have attracted growing attention over the past fifteen years. The low-power manipulation of the magnetization, preferably at ultrashort timescales, has become a fundamental challenge with implications for future magnetic information memory and storage technologies. Here we explore the optical manipulation of the magnetization in engineered magnetic materials. We demonstrate that all-optical helicity-dependent switching (AO-HDS) can be observed not only in selected rare earth-transition metal (RE-TM) alloy films but also in a much broader variety of materials, including RE-TM alloys, multilayers and heterostructures. We further show that RE-free Co-Ir-based synthetic ferrimagnetic heterostructures designed to mimic the magnetic properties of RE-TM alloys also exhibit AO-HDS. These results challenge present theories of AO-HDS and provide a pathway to engineering materials for future applications based on all-optical control of magnetic order.

Feedback effect during ultrafast demagnetization dynamics in ferromagnets.

Motivated by the recent controversy about the importance of spin-flip scattering for ultrafast demagnetization in ferromagnets, we study the spin-dependent electron dynamics based on a dynamical Elliott-Yafet mechanism. The key improvement to earlier approaches is the use of a modified Stoner model with a dynamic exchange splitting between majority and minority bands. In the framework of our microscopic model, we find a novel feedback effect between the time-dependent exchange splitting and the spin-flip scattering. This feedback effect allows us to reproduce important properties of the demagnetization dynamics quantitatively. Our results demonstrate that in general Elliott-Yafet spin-flip scattering needs to be taken into account to obtain a microscopic picture of demagnetization dynamics.

Explaining the paradoxical diversity of ultrafast laser-induced demagnetization.

Pulsed-laser-induced quenching of ferromagnetic order has intrigued researchers since pioneering works in the 1990s. It was reported that demagnetization in gadolinium proceeds within 100 ps, but three orders of magnitude faster in ferromagnetic transition metals such as nickel. Here we show that a model based on electron-phonon-mediated spin-flip scattering explains both timescales on equal footing. Our interpretation is supported by ab initio estimates of the spin-flip scattering probability, and experimental fluence dependencies are shown to agree perfectly with predictions. A phase diagram is constructed in which two classes of laser-induced magnetization dynamics can be distinguished, where the ratio of the Curie temperature to the atomic magnetic moment turns out to have a crucial role. We conclude that the ultrafast magnetization dynamics can be well described disregarding highly excited electronic states, merely considering the thermalized electron system.

Spin-flip processes and ultrafast magnetization dynamics in Co: Unifying the microscopic and macroscopic view of femtosecond magnetism.

The femtosecond magnetization dynamics of a thin cobalt film excited with ultrashort laser pulses has been studied using two complementary pump-probe techniques, namely, spin-, energy-, and time-resolved photoemission and the time-resolved magneto-optical Kerr effect. Combining the two methods, it is possible to identify the microscopic electron spin-flip mechanisms responsible for the ultrafast macroscopic magnetization dynamics of the cobalt film. In particular, we show that electron-magnon excitation does not affect the overall magnetization even though it is an efficient spin-flip channel on the sub-200 fs time scale. Instead, we find experimental evidence for the relevance of Elliott-Yafet-type spin-flip processes for the ultrafast demagnetization taking place on a time scale of 300 fs.

Photoemission electron microscopy as a tool for the investigation of optical near fields.

Photoemission electron microscopy was used to image the electrons photoemitted from specially tailored Ag nanoparticles deposited on a Si substrate (with its native oxide SiO(x)). Photoemission was induced by illumination with a Hg UV lamp (photon energy cutoff homega(UV) = 5.0 eV, wavelength lambda(UV) = 250 nm) and with a Ti:sapphire femtosecond laser (homega(l) = 3.1 eV, lambda(l) = 400 nm, pulse width below 200 fs), respectively. While homogeneous photoelectron emission from the metal is observed upon illumination at energies above the silver plasmon frequency, at lower photon energies the emission is localized at tips of the structure. This is interpreted as a signature of the local electrical field therefore providing a tool to map the optical near field with the resolution of emission electron microscopy.