We demonstrate ultrafast magnetization dynamics in a 5d transition metal using circularly-polarized x-ray free electron laser in the hard x-ray region. A decay time of light-induced demagnetization of L1${}_0$-FePt was determined to be $tau_textrm{Pt} = 0.6 textrm{ps}$ using time-resolved x-ray magnetic circular dichroism at the Pt L${}_3$ edge, whereas magneto-optical Kerr measurements indicated the decay time for total magnetization as $tau_textrm{total} = 0.1 textrm{ps}$. A transient magnetic state with the photo-modulated magnetic coupling between the 3d and 5d elements is firstly demonstrated.
As a 3D topological insulator, bismuth selenide (Bi2Se3) has potential applications for electrically and optically controllable magnetic and optoelectronic devices. How the carriers interact with lattice is important to understand the coupling with its topological phase. It is essential to measure with a time scale smaller than picoseconds for initial interaction. Here we use an X-ray free-electron laser to perform time-resolved diffraction to study ultrafast carrier-induced lattice contractions and interlayer modulations in Bi2Se3 thin films. The lattice contraction depends on the carrier concentration and is followed by an interlayer expansion accompanied by oscillations. Using density functional theory (DFT) and the Lifshitz model, the initial contraction can be explained by van der Waals force modulation of the confined free carrier layers. Band inversion, related to a topological phase transition, is modulated by the expansion of the interlayer distance. These results provide insight into instantaneous topological phases on ultrafast timescales.
Using a time-resolved magneto-optical Kerr effect (TR-MOKE) microscope, we observed ultrafast demagnetization of inverse-spinel-type NiCo2O4 (NCO) epitaxial thin films of the inverse spinel type ferrimagnet NCO with perpendicular magnetic anisotropy. This microscope uses a pump-probe method, where the sample is pumped at 1030 nm, and magnetic domain images are acquired via MOKE microscopy at 515 nm (the second harmonic). We successfully observed the dynamics of the magnetic domain of the NCO thin film via laser irradiation, and obtained a demagnetization time constant of approximately 0.4 ps. This time constant was significantly smaller than the large time constants reported for other half-metallic oxides. These results, combined with the results of our x-ray photoemission spectroscopy study, indicate that this NCO thin film is a ferrimagnetic metal whose electronic structure deviates from the theoretically predicted half-metallic one.
We have investigated the spin and orbital magnetic moments of Fe in FePt nanoparticles in the $L$1$_{0}$-ordered phase coated with SiO$_{2}$ by x-ray absorption spectroscopy (XAS) and x-ray magnetic circular dichroism (XMCD) measurements at the Fe $L_{rm 2,3}$ absorption edges. Using XMCD sum rules, we evaluated the ratio of the orbital magnetic moment ($M_{rm orb}$) to the spin magnetic moment ($M_{rm spin}$) of Fe to be $M_{rm orb}/M_{rm spin}$ = 0.08. This $M_{rm orb}/M_{rm spin}$ value is comparable to the value (0.09) obtained for FePt nanoparticles prepared by gas phase condensation, and is larger than the values ($sim$0.05) obtained for FePt thin films, indicating a high degree of $L$1$_{0}$ order. The hysteretic behavior of the FePt component of the magnetization was measured by XMCD. The magnetic coercivity ($H_{rm c}$) was found to be as large as 1.8 T at room temperature, $sim$3 times larger than the thin film value and $sim$50 times larger than that of the gas phase condensed nanoparticles. The hysteresis curve is well explained by the Stoner-Wohlfarth model for non-interacting single-domain nanoparticles with the $H_{rm c}$ distributed from 1 T to 5 T.
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.
The strong perpendicular magnetic anisotropy of $L{rm1_0}$-ordered FePt has been the subject of extensive studies for a long time. However, it is not known which element, Fe or Pt, mainly contributes to the magnetic anisotropy energy (MAE). We have investigated the anisotropy of the orbital magnetic moments of Fe 3$d$ and Pt 5$d$ electrons in $L{rm1_0}$-ordered FePt thin films by Fe and Pt $L_{2,3}$-edge x-ray magnetic circular dichroism (XMCD) measurements for samples with various degrees of long-range chemical order $S$. Fe $L_{2,3}$-edge XMCD showed that the orbital magnetic moment was larger when the magnetic field was applied perpendicular to the film than parallel to it, and that the anisotropy of the orbital magnetic moment increased with $S$. Pt $L_{2,3}$-edge XMCD also showed that the orbital magnetic moment was smaller when the magnetic field was applied perpendicular to the film than parallel to it, opposite to the Fe $L_{2,3}$-edge XMCD results although the anisotropy of the orbital magnetic moment increases with $S$ like the Fe edge. These results are qualitatively consistent with the first-principles calculation by Solovyev ${it et al.}$ [Phys. Rev. B $bf{52}$, 13419 (1995).], which also predicts the dominant contributions of Pt 5$d$ to the magnetic anisotropy energy rather than Fe 3$d$ due to the strong spin-orbit coupling and the small spin splitting of the Pt 5$d$ bands in $L{rm1_0}$-ordered FePt.
Kohei Yamamoto
,Yuya Kubota
,Motohiro Suzuki
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(2018)
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"Ultrafast demagnetization of Pt magnetic moment in L1${}_0$-FePt probed by hard x-ray free electron laser"
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Kohei Yamamoto
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