Martin Aeschlimann

Adaptive subwavelength control of nano-optical fields.

Adaptive shaping of the phase and amplitude of femtosecond laser pulses has been developed into an efficient tool for the directed manipulation of interference phenomena, thus providing coherent control over various quantum-mechanical systems. Temporal resolution in the femtosecond or even attosecond range has been demonstrated, but spatial resolution is limited by diffraction to approximately half the wavelength of the light field (that is, several hundred nanometres). Theory has indicated that the spatial limitation to coherent control can be overcome with the illumination of nanostructures: the spatial near-field distribution was shown to depend on the linear chirp of an irradiating laser pulse. An extension of this idea to adaptive control, combining multiparameter pulse shaping with a learning algorithm, demonstrated the generation of user-specified optical near-field distributions in an optimal and flexible fashion. Shaping of the polarization of the laser pulse provides a particularly efficient and versatile nano-optical manipulation method. Here we demonstrate the feasibility of this concept experimentally, by tailoring the optical near field in the vicinity of silver nanostructures through adaptive polarization shaping of femtosecond laser pulses and then probing the lateral field distribution by two-photon photoemission electron microscopy. In this combination of adaptive control and nano-optics, we achieve subwavelength dynamic localization of electromagnetic intensity on the nanometre scale and thus overcome the spatial restrictions of conventional optics. This experimental realization of theoretical suggestions opens a number of perspectives in coherent control, nano-optics, nonlinear spectroscopy, and other research fields in which optical investigations are carried out with spatial or temporal resolution.

Topological states on the gold surface

Gold surfaces host special electronic states that have been understood as a prototype of Shockley surface states. These surface states are commonly employed to benchmark the capability of angle-resolved photoemission spectroscopy (ARPES) and scanning tunnelling spectroscopy. Here we show that these Shockley surface states can be reinterpreted as topologically derived surface states (TDSSs) of a topological insulator (TI), a recently discovered quantum state. Based on band structure calculations, the Z2-type invariants of gold can be well-defined to characterize a TI. Further, our ARPES measurement validates TDSSs by detecting the dispersion of unoccupied surface states. The same TDSSs are also recognized on surfaces of other well-known noble metals (for example, silver, copper, platinum and palladium), which shines a new light on these long-known surface states.

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.

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.

All-optical control of ferromagnetic thin films and nanostructures

All-optical magnetic state switching Magneto-optical memory storage media, such as hard drives, use magnetic fields to change the magnetization of memory bits, but the process is slow. Light can often reveal information about the magnetization state of a sample, such as its field direction. Lambert et al. show that under the right circumstances, light can also switch the magnetization state of a thin ferromagnetic film. Using light pulses instead of magnetic fields led to ultrafast data memory and data storage. Science, this issue p. 1337 The all-optical control of magnetization in thin ferromagnetic films is demonstrated. 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.

Determination of spin injection and transport in a ferromagnet/organic semiconductor heterojunction by two-photon photoemission

A fundamental prerequisite for the implementation of organic semiconductors (OSCs) in spintronics devices is the still missing basic knowledge about spin injection and transport in OSCs. Here, we consider a model system consisting of a high-quality interface between the ferromagnet cobalt and the OSC copper phthalocyanine (CuPc). We focus on interfacial effects on spin injection and on the spin transport properties of CuPc. Using spin-resolved two-photon photoemission, we have measured directly and in situ the efficiency of spin injection at the cobalt-CuPc interface. We report a spin injection efficiency of 85-90% for injection into unoccupied molecular orbitals of CuPc. Moreover, we estimate an electron inelastic mean free path in CuPc in the range of 1 nm and a 10-30 times higher quasi-elastic spin-flip length. We demonstrate that quasi-elastic spin-flip processes with energy loss < or = 200 meV are the dominant microscopic mechanism limiting the spin diffusion length in CuPc.

Ultrafast magnetization enhancement in metallic multilayers driven by superdiffusive spin current

Uncovering the physical mechanisms that govern ultrafast charge and spin dynamics is crucial for understanding correlated matter as well as the fundamental limits of ultrafast spin-based electronics. Spin dynamics in magnetic materials can be driven by ultrashort light pulses, resulting in a transient drop in magnetization within a few hundred femtoseconds. However, a full understanding of femtosecond spin dynamics remains elusive. Here we spatially separate the spin dynamics using Ni/Ru/Fe magnetic trilayers, where the Ni and Fe layers can be ferro- or antiferromagnetically coupled. By exciting the layers with a laser pulse and probing the magnetization response simultaneously but separately in Ni and Fe, we surprisingly find that optically induced demagnetization of the Ni layer transiently enhances the magnetization of the Fe layer when the two layer magnetizations are initially aligned parallel. Our observations are explained by a laser-generated superdiffusive spin current between the layers.

Coherent Two-Dimensional Nanoscopy

Coherent electronic states excited by ultrafast laser pulses were imaged at subwavelength resolution with photoelectrons. We introduce a spectroscopic method that determines nonlinear quantum mechanical response functions beyond the optical diffraction limit and allows direct imaging of nanoscale coherence. In established coherent two-dimensional (2D) spectroscopy, four-wave–mixing responses are measured using three ingoing waves and one outgoing wave; thus, the method is diffraction-limited in spatial resolution. In coherent 2D nanoscopy, we use four ingoing waves and detect the final state via photoemission electron microscopy, which has 50-nanometer spatial resolution. We recorded local nanospectra from a corrugated silver surface and observed subwavelength 2D line shape variations. Plasmonic phase coherence of localized excitations persisted for about 100 femtoseconds and exhibited coherent beats. The observations are best explained by a model in which coupled oscillators lead to Fano-like resonances in the hybridized dark- and bright-mode response.

Probing the timescale of the exchange interaction in a ferromagnetic alloy

The underlying physics of all ferromagnetic behavior is the cooperative interaction between individual atomic magnetic moments that results in a macroscopic magnetization. In this work, we use extreme ultraviolet pulses from high-harmonic generation as an element-specific probe of ultrafast, optically driven, demagnetization in a ferromagnetic Fe-Ni alloy (permalloy). We show that for times shorter than the characteristic timescale for exchange coupling, the magnetization of Fe quenches more strongly than that of Ni. Then as the Fe moments start to randomize, the strong ferromagnetic exchange interaction induces further demagnetization in Ni, with a characteristic delay determined by the strength of the exchange interaction. We can further enhance this delay by lowering the exchange energy by diluting the permalloy with Cu. This measurement probes how the fundamental quantum mechanical exchange coupling between Fe and Ni in magnetic materials influences magnetic switching dynamics in ferromagnetic materials relevant to next-generation data storage technologies.

Competing nonradiative channels for hot electron induced surface photochemistry

We report experiments in which we investigated the ultrafast dynamics of competing nonradiative channels for hot electron mechanisms in various polycrystalline metal samples. Time resolved two-photon photoemission, based on the equal pulse correlation technique, is used to measure the energy relaxation and the transport of the photoexcited carriers. In these studies the role of coherent effects in auto- and crosscorrelation experiments has been considered. While the inelastic lifetime of Ag is in qualitative and quantitative agreement with the Fermi liquid theory, the result obtained for Au is very different. The measured inelastic relaxation time for transition metals with unoccupied d orbitals is shorter as compared to the noble metals. The results demonstrate the feasibility of studying electron relaxation in noble and transition metals directly in the time domain and provide a framework for understanding the dynamics of hot electron transfer from a metal surface to the adsorbate.