Laser-Induced Skyrmion Writing and Erasing in an Ultrafast Cryo-Lorentz Transmission Electron Microscope

Gabriele Berruto, Fabrizio Carbone, Ping Huang, Ivan Madan, Yoshie Murooka, Enrico Pomarico, Henrik Moodysson Rønnow, Giovanni Maria Vanacore
2018
Journal paper

Abstract

We demonstrate that light-induced heat pulses of different duration and energy can write Skyrmions in a broad range of temperatures and magnetic field in FeGe. Using a combination of camera-rate and pump- probe cryo-Lorentz transmission electron microscopy, we directly resolve the spatiotemporal evolution of the magnetization ensuing optical excitation. The Skyrmion lattice was found to maintain its structural properties during the laser-induced demagnetization, and its recovery to the initial state happened in the sub-μs to μs range, depending on the cooling rate of the system.

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In my thesis, transport measurements such as resistivity and, more importantly, thermopower S, were used to explore the phase diagram of bad metals. Bad metals are electronically correlated systems whose ground state lies close to a quantum phase transition. By tuning the control parameters, such as temperature (T ), magnetic field (B), hydrostatic pressure (p) or chemical substitution (x), we can induce phase transitions between the various electronic, magnetic and structural phases. Here, the thermopower is presented as a unique tool for probing quantum phase transition because it is a measure of the entropy of conducting electrons. The main part of the thesis is dedicated to the study of Fe-based superconductors (FeSC) discovered in 2008. Their parent compound has an antiferromagnetic (AF) ground state, where the itinerant electrons form a spin-density wave (SDW), a periodic modulation of spin density. This coincides or is preceded by a structural, tetragonal-to-orthorhombic transition. The nesting between the electron and hole Fermi surface is believed to be the driving mechanism for the SDW state. By changing the structural or chemical properties the AF ground state of FeSC is suppressed, giving way to superconductivity (SC). The remaining antiferromagnetic fluctuations above the transition can provide a glue for SC pairing. Here, the analysis of the thermopower S/T of BaFe1−xCoxAs2 (BFCA) in the x-T phase diagram shows the signatures of the spin fluctuation which have a dome-like dependence and follow the trend of superconducting Tc . The logarithmic increase of S/T upon decreasing T is ascribed to the proximity of the spin-density-wave quantum critical point. It can be understood as an increase of entropy due to the incommensurate AF spin fluctuations. We can ascribe the high values of thermopower in BFCA at intermediate- and room-temperatures to the influence of low-T quantum criticality. To probe the response of the electronic system in FeSC to structural changes, we performed measurements under pressure of the parent compound BaFe2As2 (BFA), the SC electron-doped BFCA, and hole-doped Ba1−xKxFe2As2 (BKFA). In the parent compound pressure suppresses the structural/SDW transition, similar to the effect of doping. For doped systems, in order to describe the behavior of thermopower in the high-T range (above 100K) we used a semi-metallic two-band model which was fitted to the data in order to extract the pressure dependence of the band parameters. In both doping cases the effect of pressure was similar, an increase of the band overlap and of the effective number of charge carriers. With this model we can explain the high-T , x and p dependence of thermopower in both electron- and hole-doped BFA. In a structurally simpler Fe-chalcogenide Fe1+yTe1−xSex compound, the excess of Fe has a Kondo-like influence on the charge carriers which dramatically changes the physics of the normal state. To probe the normal state, pressure, doping, magnetic Fe-excess concentration (y) and temperature were used as control parameters. At low-T a characteristic upturn of resistivity (ρmag ) is observed, followed by an increase of thermopower (Smag ), which we identify as the magnetic contribution caused by the spin-flip scattering events. Increasing the y resulted in an increase of ρmag , and a decrease of Smag , which is in agreement with the behavior of canonical Kondo-systems. Pressure suppresses the magnetic contribution to transport, thus increasing the itinerancy of the system. MnSi is another system in which the sensitivity of thermopower to entropy brings new information related to the complex magnetic structure. Pressure was used to drive the system from a helically ordered, canonical Fermi-liquid (FL) phase with T 2-resistivity to the intrinsically disordered, non-Fermi-liquid (NFL) phase above pc with T3/2-dependence. Our contour plot of S/T demonstrated how powerful the thermopower technique is, by reproducing the whole previously established T -p phase diagram. At the phase transition from the magnetically-ordered FL phase to the disordered NFL, the thermopower is dramatically enhanced. We bring useful information about the mysterious partial order (PO) phase inside the NFL phase, previously detected only by neutron scattering. The fluctuating helices scenario can describe the observed increase of entropy/thermopower in the PO phase. At ambient pressure, close to the helical transition of MnSi, a moderate magnetic field can stabilize the skyrmion lattice - the lattice of topological magnetic whirls, vortices. We observe a signature of the skyrmion lattice as a minute drop in thermopower. It is located exactly in the same region of the T − B phase diagram where an increase in magnetoresistance and Hall effect was reported previously. This feature originates from the additional scattering of conducting electrons on magnetic vortices, while the change in S is dominated by the decrease of entropy as the stable skyrmion lattice is formed. Overall, resistivity was used to confirm the established phase diagram, while thermopower, as an interesting and not sufficiently understood technique, was used to probe the sensitive changes of the charge carriers at the Fermi surface. We explored various phases showing how useful thermopower is to probe the entropy of electronic system on the verge of quantum phase transition.

EPFL2012

Magnetic skyrmions, topologically non-trivial chiral whirl-like spin configurations, have been under massive investigations in both fundamental and application aspects. In some special compounds, these quasi-particles can formtriangular skrymion lattice (SkL) exhibiting abundant unique properties. This thesis presents my comprehensive studies on the SkL in the magnetoelectric (ME) coupling helimagnet Cu2OSeO3. Starting from measurements on single crystal bulk Cu2OSeO3 samples, including dc magnetization, magnetoelectric susceptibility and neutron scattering, so as to get the general understanding of this system, the main work of this thesis focused on the investigation of quasi-two dimensional thin slab samples by the state-of-the-art Lorentz electron transmission electron microscopy (LTEM). Variousmagnetic textures including the spin helices and skyrmions were observed and analyzed. What separates the work presented here from literatures is the special emphasis on the dynamics of the SkL under various excitations in real space and real time, such as thermal fluctuation, magnetic field and electric field. Specifically, the magnetic field induced melting of the SkL in Cu2OSeO3 was, for the first time, observed and analyzed quantitatively. Two-step melting process was observed and demonstrated to follow the Kosterlitz-Thouless-Halperin-Nelson-Young (KTHNY) theory. The application of electric field can not only rotate the SkL, but also create skyrmions fromthe helical phase. My studies, especially those focused on the emergent properties induced by external fields, are intended to provide deeper insight into the fundamental knowledge of the SkL in Cu2OSeO3 and to promote the the development of skyrmion based spintronic applications.

EPFL2017

There once was a harsh competition between different computer memory technologies, and now we cheer triumph for the Random Access-Memory (RAM) devices, -- cheap, fast, tiny, stable. The competing Magnetic Bubble Memory had faded away as magnetic bubbles are undesirably large and pretty much not robust, manifesting both low data density and high operational costs. However, what we do possess now are nanosize objects of topological nature, magnetic skyrmions, which are protected from continuous field variations and take very little energy cost to be moved. Thus, skyrmions are considered as promising information carriers for future memory devices and ultradense data storage, while skyrmion phases in bulk materials are interesting from fundamental point of view in exploring topological states of matter. In this thesis, I develop and advance several effective theoretical approaches, diverse both in their methods and use, which were of appeal for several skyrmionic experiments in our lab (LQM/EPFL). We were and are primarily interested in the open issues in the applied field of skyrmionics, which may be taken under the umbrella of creation, stabilization and control of magnetic skyrmions under electric fields, mechanical strains, thermal gradients, etc. For the goals achieved and yet to be achieved, the magnetoelectric insulator Cu2OSeO3, which uniquely responses to all the above mentioned fields, is a highly advantageous candidate. Magnetoelectric here means that the spins of a magnetic material are coupled to external electric fields, while insulating properties are very advantageous to preserve both the state and the very existence of skyrmions by eliminating the Joule heating. The novel results in this thesis are calculations for both individual and arrayed skyrmions under electric fields, mechanical strains and uniform pressures, and thermal gradients. Furthermore, several fundamental questions were addressed by developing an extended formalism for calculation skyrmion-pocket phase diagrams, studying the topologically-governed crossover between skyrmions and magnetic bubbles, and discussing the possible role of merons (half-skyrmions) in skyrmion phase formation. The result with the most immediate appeal is probably the theoretical and experimental study of skyrmion lattices in electric fields, with a direct demonstration of writing and erasing of the full skyrmion phase under electric fields of few Volts per micrometer, as compatible with modern microelectronic devices.

EPFL2017

EPFL2012

EPFL2017