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Register a new userStructural dynamics during laser induced ultrafast demagnetization
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The mechanism underlying femtosecond laser pulse induced ultrafast magnetization dynamics remains elusive despite two decades of intense research on this phenomenon. Most experiments focused so far on characterizing magnetization and charge carrier dynamics, while first direct measurements of structural dynamics during ultrafast demagnetization were reported only very recently. We here present our investigation of the infrared laser pulse induced ultrafast demagnetization process in a thin Ni film, which characterizes simultaneously magnetization and structural dynamics. This is achieved by employing femtosecond time resolved X-ray resonant magnetic reflectivity (tr-XRMR) as probe technique. The experimental results reveal unambiguously that the sub-picosecond magnetization quenching is accompanied by strong changes in non-magnetic X-ray reflectivity. These changes vary with reflection angle and changes up to 30$%$ have been observed. Modeling the X-ray reflectivity of the investigated thin film, we can reproduce these changes by a variation of the apparent Ni layer thickness of up to 1$%$. Extending these simulations to larger incidence angles we show that tr-XRMR can be employed to discriminate experimentally between currently discussed models describing the ultrafast demagnetization phenomenon.
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Spin and orbital angular momenta are two intrinsic properties of an electron and are responsible for the physics of a solid. How the spin and orbital evolve with respect to each other on several hundred femtoseconds is largely unknown, but it is at the center of laser-induced ultrafast demagnetization. In this paper, we introduce a concept of the spin-orbital correlation diagram, where spin angular momentum is plotted against orbital angular momentum, much like the position-velocity phase diagram in classical mechanics. We use four sets of highly accurate time-resolved x-ray magnetic circular dichroism (TR-XMCD) data to construct four correlation diagrams for iron and cobalt. To our surprise, a pattern emerges. The trace on the correlation diagram for iron is an arc, and at the end of demagnetization, it has a pronounced cusp. The correlation diagram for cobalt is different and appears more linear, but with kinks. We carry out first-principles calculations with two different methods: time-dependent density functional theory (TDDFT) and time-dependent Liouville density functional theory (TDLDFT). These two methods agree that the experimental findings for both Fe and Co are not due t experimental errors. It is the spin-orbit coupling that correlates the spin dynamics to the orbital dynamics.Microscopically, Fe and Co have different orbital occupations, which leads to distinctive correlation diagrams. We believe that this correlation diagram presents a useful tool to better understand spin and orbital dynamics on an ultrafast time scale. A brief discussion on the magnetic anisotropy energy is also provided.
Ni$_{0.8}$Fe$_{0.2}$ (Py) and Py alloyed with Cu exhibit intriguing ultrafast demagnetization behavior, where the Ni magnetic moment shows a delayed response relative to the Fe, an effect which is strongly enhanced by Cu alloying. We have studied a broad range of Cu concentrations to elucidate the effects of Cu alloying in Py. The orbital/spin magnetic moment ratios are largely unaffected by Cu alloying, signifying that Cu-induced changes in the ultrafast demagnetization are not related to spin-orbit interactions. We show that magnon diffusion can explain the delayed Ni response, which we attribute to an enhanced magnon generation rate in the Fe sublattice relative to the Ni sublattice. Furthermore, Py exhibits prominent RKKY-like exchange interactions, which are strongly enhanced between Fe atoms and diminished between Ni atoms by Cu alloying. An increased Fe magnon scattering rate is expected to occur concurrently with this increased Fe-Fe exchange interaction, supporting the results obtained from the magnon diffusion model.
Here we carry out a first-principles time-dependent calculation to investigate how fast electrons actually move under laser excitation and how large the electron transport affects demagnetization on the shortest time scale. To take into account the transport effect, we implement the intraband transition in our theory. In the bulk fcc Ni, we find the effect of the spin transport on the demagnetization is extremely small, no more than 1%. The collective electron velocity in Ni is 0.4 $rm AA/fs$, much smaller than the Fermi velocity, and the collective displacement is no more than 0.1 $rm AA$. But this does not mean that electrons do not travel fast; instead we find that electron velocities at two opposite crystal momenta cancel each other. We follow the $Gamma$-X line and find a huge dispersion in the velocities in the crystal momentum space. In the Fe/W(110) thin film, the overall demagnetization is larger than Ni, and the Fermi velocity is higher than Ni. However, the effect of the spin transport is still small in the Fe/W(110) thin film. Based on our numerical results and existing experimental findings, we propose a different mechanism that can explain two latest experimental results. Our finding sheds new light on the effect of ballistic transport on demagnetization.
The temperature evolution of GdFeCo electrons following optical heating plays a key role in all optical switching of GdFeCo and is primarily governed by the strength of coupling between electrons and phonons. Typically, the strength of electron-phonon coupling in a metal is deduced by monitoring changes in reflectance following optical heating and then analyzing the transient reflectance with a simple two-temperature thermal model. In a magnetic metal, the change in reflectance cannot be assumed to depend only the electron and phonon temperatures because a metals reflectance also depends on the magnetization. To deduce the electron-phonon coupling constant in GdFeCo, we analyze thermal transport in Au and GdFeCo bilayers following optical heating of the GdFeCo electrons. We use the reflectance of the Au layer to monitor the temperature evolution of the Au phonons. By interpreting the response of the bilayer to heating with a thermal model, we determine the electron-phonon coupling constant in GdFeCo to be 6 x 10^17 W/(m^3-K) corresponding to an electron-phonon relaxation time in GdFeCo of ~150 fs.
We study how the color and polarization of ultrashort pulses of visible light can be used to control the demagnetization processes of the antiferromagnetic insulator Cr$_2$O$_3$. We utilize time-resolved second harmonic generation (SHG) to probe how changes in the magnetic and structural state evolve in time. We show that, varying the pump photon-energy to excite either localized transitions within the Cr or charge transfer states, leads to markedly different dynamics. Through a full polarization analysis of the SHG signal, symmetry considerations and density functional theory calculations, we show that, in the non-equilibrium state, SHG is sensitive to {em both} lattice displacements and changes to the magnetic order, which allows us to conclude that different excited states couple to phonon modes of different symmetries. Furthermore, the spin-scattering rate depends on the induced distortion, enabling us to control the timescale for the demagnetization process. Our results suggest that selective photoexcitation of antiferromagnetic insulators allows fast and efficient manipulation of their magnetic state.
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