| 1. |
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| 2. |
- Ryan, Sinéad A., et al.
(författare)
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Optically controlling the competition between spin flips and intersite spin transfer in a Heusler half-metal on sub-100-fs time scales
- 2023
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Ingår i: Science Advances. - : American Association for the Advancement of Science (AAAS). - 2375-2548. ; 9:45, s. 1428-
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Tidskriftsartikel (refereegranskat)abstract
- The direct manipulation of spins via light may provide a path toward ultrafast energy-efficient devices. However, distinguishing the microscopic processes that can occur during ultrafast laser excitation in magnetic alloys is challenging. Here, we study the Heusler compound Co2MnGa, a material that exhibits very strong light-induced spin transfers across the entire M-edge. By combining the element specificity of extreme ultraviolet high-harmonic probes with time-dependent density functional theory, we disentangle the competition between three ultrafast light-induced processes that occur in Co2MnGa: same-site Co-Co spin transfer, intersite Co-Mn spin transfer, and ultrafast spin flips mediated by spin-orbit coupling. By measuring the dynamic magnetic asymmetry across the entire M-edges of the two magnetic sublattices involved, we uncover the relative dominance of these processes at different probe energy regions and times during the laser pulse. Our combined approach enables a comprehensive microscopic interpretation of laser-induced magnetization dynamics on time scales shorter than 100 femtoseconds.
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| 3. |
- Fan, Tingting, et al.
(författare)
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Bright circularly polarized soft X-ray high harmonics for X-ray magnetic circular dichroism
- 2015
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Ingår i: Proceedings of the National Academy of Sciences of the United States of America. - : Proceedings of the National Academy of Sciences. - 0027-8424 .- 1091-6490. ; 112:46, s. 14206-14211
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Tidskriftsartikel (refereegranskat)abstract
- We demonstrate, to our knowledge, the first bright circularly polarized high-harmonic beams in the soft X-ray region of the electromagnetic spectrum, and use them to implement X-ray magnetic circular dichroism measurements in a tabletop-scale setup. Using counterrotating circularly polarized laser fields at 1.3 and 0.79 mu m, we generate circularly polarized harmonics with photon energies exceeding 160 eV. The harmonic spectra emerge as a sequence of closely spaced pairs of left and right circularly polarized peaks, with energies determined by conservation of energy and spin angular momentum. We explain the single-atom and macroscopic physics by identifying the dominant electron quantum trajectories and optimal phase-matching conditions. The first advanced phase-matched propagation simulations for circularly polarized harmonics reveal the influence of the finite phase-matching temporal window on the spectrum, as well as the unique polarization-shaped attosecond pulse train. Finally, we use, to our knowledge, the first tabletop X-ray magnetic circular dichroism measurements at the N-4,N-5 absorption edges of Gd to validate the high degree of circularity, brightness, and stability of this light source. These results demonstrate the feasibility of manipulating the polarization, spectrum, and temporal shape of high harmonics in the soft X-ray region by manipulating the driving laser waveform.
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| 4. |
- Hickstein, Daniel D., et al.
(författare)
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Direct Visualization of Laser-Driven Electron Multiple Scattering and Tunneling Distance in Strong-Field Ionization
- 2012
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Ingår i: Physical Review Letters. - 1079-7114. ; 109:7
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Tidskriftsartikel (refereegranskat)abstract
- Using a simple model of strong-field ionization of atoms that generalizes the well-known 3-step model from 1D to 3D, we show that the experimental photoelectron angular distributions resulting from laser ionization of xenon and argon display prominent structures that correspond to electrons that pass by their parent ion more than once before strongly scattering. The shape of these structures can be associated with the specific number of times the electron is driven past its parent ion in the laser field before scattering. Furthermore, a careful analysis of the cutoff energy of the structures allows us to experimentally measure the distance between the electron and ion at the moment of tunnel ionization. This work provides new physical insight into how atoms ionize in strong laser fields and has implications for further efforts to extract atomic and molecular dynamics from strong-field physics.
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| 5. |
- Hickstein, Daniel D., et al.
(författare)
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Non-collinear generation of angularly isolated circularly polarized high harmonics
- 2015
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Ingår i: Nature Photonics. - 1749-4885 .- 1749-4893. ; 9:11, s. 743-750
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Tidskriftsartikel (refereegranskat)abstract
- We generate angularly isolated beams of circularly polarized extreme ultraviolet light through the first implementation of non-collinear high harmonic generation with circularly polarized driving lasers. This non-collinear technique offers numerous advantages over previous methods, including the generation of higher photon energies, the separation of the harmonics from the pump beam, the production of both left and right circularly polarized harmonics at the same wavelength and the capability of separating the harmonics without using a spectrometer. To confirm the circular polarization of the beams and to demonstrate the practicality of this new light source, we measure the magnetic circular dichroism of a 20 nm iron film. Furthermore, we explain the mechanisms of non-collinear high harmonic generation using analytical descriptions in both the photon and wave models. Advanced numerical simulations indicate that this non-collinear mixing enables the generation of isolated attosecond pulses with circular polarization.
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| 6. |
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| 7. |
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| 8. |
- Rudolf, Dennis, et al.
(författare)
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Element Selective Investigation of Spin Dynamics in Magnetic Multilayers
- 2015
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Ingår i: Ultrafast Magnetism I. - Cham : Springer International Publishing. - 9783319077437 - 9783319077420 ; , s. 307-309
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Konferensbidrag (refereegranskat)abstract
- Our understanding of ultrafast switching processes in novel spin-based electronics depends on our detailed knowledge of interactions between spin, charge and phonons in magnetic structures. We present element-selective studies, using extreme ultraviolet (XUV) light, to gain insight into spin dynamics in exchange coupled magnetic multilayers on the femtosecond time scale.
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| 9. |
- Rudolf, Dennis, et al.
(författare)
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Ultrafast magnetization enhancement in metallic multilayers driven by superdiffusive spin current
- 2012
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Ingår i: Nature Communications. - : Springer Science and Business Media LLC. - 2041-1723. ; 3, s. 1037-
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Tidskriftsartikel (refereegranskat)abstract
- 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 ferroor 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.
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| 10. |
- Tao, Zhensheng, et al.
(författare)
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The nature of non-equilibrium ultrafast demagnetization in ferromagnetic nickel
- 2019
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Ingår i: Eleventh International Conference On Information Optics And Photonics (CIOP 2019). - : SPIE. - 9781510631748
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Konferensbidrag (refereegranskat)abstract
- It has long been known that ferromagnets undergo a phase transition from ferromagnetic to paramagnetic at the Curie temperature, associated with critical phenomena such as a divergence in the heat capacity. A ferromagnet can also be transiently demagnetized by heating it with an ultrafast laser pulse. However, to date the connection between out-of-equilibrium and equilibrium phase transitions was not known, nor how fast the out-of-equilibrium phase transitions can proceed. In this work, by combining time- and angle-resolved photoemission (Tr-ARPES) with time-resolved transverse magneto-optical Kerr (Tr-TMOKE) spectroscopies, we show that the same critical behavior also governs the ultrafast magnetic phase transition in nickel. This is evidenced by several observations. First, we observe a divergence of the transient heat capacity of the electron spin system preceding material demagnetization. Second, when the electron temperature is transiently driven above the Curie temperature, we observe an extremely rapid change in the material response: the spin system absorbs sufficient energy within the first 20 fs to subsequently proceed through the phase transition, while demagnetization and the collapse of the exchange splitting occur on much longer timescales. Third, we find that the transient electron temperature alone dictates the magnetic response. By comparing results obtained from different methods, we show that the critical behaviors are essential for fully explaining the fluence-dependent magnetization dynamics measured using magneto-optical spectroscopy.
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| 11. |
- Tengdin, Phoebe, et al.
(författare)
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Critical behavior within 20 fs drives the out-of-equilibrium laser-induced magnetic phase transition in nickel
- 2018
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Ingår i: Science Advances. - : AMER ASSOC ADVANCEMENT SCIENCE. - 2375-2548. ; 4:3
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Tidskriftsartikel (refereegranskat)abstract
- It has long been known that ferromagnets undergo a phase transition from ferromagnetic to paramagnetic at the Curie temperature, associated with critical phenomena such as a divergence in the heat capacity. A ferromagnet can also be transiently demagnetized by heating it with an ultrafast laser pulse. However, to date, the connection between out-of-equilibrium and equilibrium phase transitions, or how fast the out-of-equilibrium phase transitions can proceed, was not known. By combining time-and angle-resolved photoemission with time-resolved transverse magneto-optical Kerr spectroscopies, we show that the same critical behavior also governs the ultrafast magnetic phase transition in nickel. This is evidenced by several observations. First, we observe a divergence of the transient heat capacity of the electron spin system preceding material demagnetization. Second, when the electron temperature is transiently driven above the Curie temperature, we observe an extremely rapid change in the material response: The spin system absorbs sufficient energy within the first 20 fs to subsequently proceed through the phase transition, whereas demagnetization and the collapse of the exchange splitting occur on much longer, fluence-independent time scales of similar to 176 fs. Third, we find that the transient electron temperature alone dictates the magnetic response. Our results are important because they connect the out-of-equilibrium material behavior to the strongly coupled equilibrium behavior and uncover a new time scale in the process of ultrafast demagnetization.
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| 12. |
- Tengdin, Phoebe, et al.
(författare)
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Direct light–induced spin transfer between different elements in a spintronic Heusler material via femtosecond laser excitation
- 2020
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Ingår i: Science Advances. - : American Association for the Advancement of Science. - 2375-2548. ; 6:3
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Tidskriftsartikel (refereegranskat)abstract
- Heusler compounds are exciting materials for future spintronics applications because they display a wide range of tunable electronic and magnetic interactions. Here, we use a femtosecond laser to directly transfer spin polarization from one element to another in a half-metallic Heusler material, Co2MnGe. This spin transfer initiates as soon as light is incident on the material, demonstrating spatial transfer of angular momentum between neighboring atomic sites on time scales < 10 fs. Using ultrafast high harmonic pulses to simultaneously and independently probe the magnetic state of two elements during laser excitation, we find that the magnetization of Co is enhanced, while that of Mn rapidly quenches. Density functional theory calculations show that the optical excitation directly transfers spin from one magnetic sublattice to another through preferred spin-polarized excitation pathways. This direct manipulation of spins via light provides a path toward spintronic devices that can operate on few-femtosecond or faster time scales.
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| 13. |
- Turgut, Emrah, et al.
(författare)
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Stoner versus Heisenberg : Ultrafast exchange reduction and magnon generation during laser-induced demagnetization
- 2016
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Ingår i: PHYSICAL REVIEW B. - 2469-9950. ; 94:22
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Tidskriftsartikel (refereegranskat)abstract
- Understanding how the electronic band structure of a ferromagnetic material is modified during laser-induced demagnetization on femtosecond time scales has been a long-standing question in condensed matter physics. Here, we use ultrafast high harmonics to measure time-, energy-, and angle-resolved M-edge magnetic asymmetry spectra for Co films after optical pumping to induce ultrafast demagnetization. This provides a complete data set that we can compare with advanced ab initio magneto-optical calculations. Our analysis identifies that the dominant mechanisms contributing to ultrafast demagnetization on time scales up to several picoseconds are a transient reduction in the exchange splitting and the excitation of ultrafast magnons. Surprisingly, we find that the magnon contribution to ultrafast demagnetization is already strong on subpicosecond time scales, while the reduction in exchange splitting persists to several picoseconds.
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| 14. |
- Young, Linda, et al.
(författare)
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Roadmap of ultrafast x-ray atomic and molecular physics
- 2018
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Ingår i: Journal of Physics B: Atomic, Molecular and Optical Physics. - : IOP Publishing. - 0953-4075 .- 1361-6455. ; 51:3
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Forskningsöversikt (refereegranskat)abstract
- X-ray free-electron lasers (XFELs) and table-top sources of x-rays based upon high harmonic generation (HHG) have revolutionized the field of ultrafast x-ray atomic and molecular physics, largely due to an explosive growth in capabilities in the past decade. XFELs now provide unprecedented intensity (1020 W cm-2) of x-rays at wavelengths down to ∼1 Ångstrom, and HHG provides unprecedented time resolution (∼50 attoseconds) and a correspondingly large coherent bandwidth at longer wavelengths. For context, timescales can be referenced to the Bohr orbital period in hydrogen atom of 150 attoseconds and the hydrogen-molecule vibrational period of 8 femtoseconds; wavelength scales can be referenced to the chemically significant carbon K-edge at a photon energy of ∼280 eV (44 Ångstroms) and the bond length in methane of ∼1 Ångstrom. With these modern x-ray sources one now has the ability to focus on individual atoms, even when embedded in a complex molecule, and view electronic and nuclear motion on their intrinsic scales (attoseconds and Ångstroms). These sources have enabled coherent diffractive imaging, where one can image non-crystalline objects in three dimensions on ultrafast timescales, potentially with atomic resolution. The unprecedented intensity available with XFELs has opened new fields of multiphoton and nonlinear x-ray physics where behavior of matter under extreme conditions can be explored. The unprecedented time resolution and pulse synchronization provided by HHG sources has kindled fundamental investigations of time delays in photoionization, charge migration in molecules, and dynamics near conical intersections that are foundational to AMO physics and chemistry. This roadmap coincides with the year when three new XFEL facilities, operating at Ångstrom wavelengths, opened for users (European XFEL, Swiss-FEL and PAL-FEL in Korea) almost doubling the present worldwide number of XFELs, and documents the remarkable progress in HHG capabilities since its discovery roughly 30 years ago, showcasing experiments in AMO physics and other applications. Here we capture the perspectives of 17 leading groups and organize the contributions into four categories: ultrafast molecular dynamics, multidimensional x-ray spectroscopies; high-intensity x-ray phenomena; attosecond x-ray science.
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| 15. |
- Zusin, Dmitriy, et al.
(författare)
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Direct measurement of the static and transient magneto-optical permittivity of cobalt across the entire M-edge in reflection geometry by use of polarization scanning
- 2018
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Ingår i: Physical Review B. - : AMER PHYSICAL SOC. - 2469-9950 .- 2469-9969. ; 97:2
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Tidskriftsartikel (refereegranskat)abstract
- The microscopic state of amagnetic material is characterized by its resonant magneto-optical response through the off-diagonal dielectric tensor component epsilon(xy). However, the measurement of the full complex epsilon(xy) in the extreme ultraviolet spectral region covering the M absorption edges of 3d ferromagnets is challenging due to the need for either a careful polarization analysis, which is complicated by a lack of efficient polarization analyzers, or scanning the angle of incidence in fine steps. Here, we propose and demonstrate a technique to extract the complex resonant permittivity epsilon(xy) simply by scanning the polarization angle of linearly polarized high harmonics to measure the magneto-optical asymmetry in reflection geometry. Because this technique is more practical and faster to experimentally implement than previous approaches, we can directly measure the full time evolution of epsilon(xy)(t) during laser-induced demagnetization across the entire M-2,M-3 absorption edge of cobalt with femtosecond time resolution. We find that for polycrystalline Co films on an insulating substrate, the changes in epsilon(xy) are uniform throughout the spectrum, to within our experimental precision. This result suggests that, in the regime of strong demagnetization, the ultrafast demagnetization response is primarily dominated by magnon generation. We estimate the contribution of exchange-splitting reduction to the ultrafast demagnetization process to be no more than 25%.
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| 16. |
- Zusin, Dmitriy, et al.
(författare)
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Ultrafast perturbation of magnetic domains by optical pumping in a ferromagnetic multilayer
- 2022
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Ingår i: Physical Review B. - : American Physical Society. - 2469-9950 .- 2469-9969. ; 106:14
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Tidskriftsartikel (refereegranskat)abstract
- Ultrafast optical pumping of spatially nonuniform magnetic textures is known to induce far-from-equilibrium spin transport effects. Here, we use ultrafast x-ray diffraction with unprecedented dynamic range to study the laser-induced dynamics of labyrinth domain networks in ferromagnetic CoFe/Ni multilayers. We detected azimuthally isotropic, odd order, magnetic diffraction rings up to fifth order. The amplitudes of all three diffraction rings quench to different degrees within 1.6 ps. In addition, all three of the detected diffraction rings both broaden by 15% and radially contract by 6% during the quench process. We are able to rigorously quantify a 31% ultrafast broadening of the domain walls via Fourier analysis of the order-dependent quenching of the three detected diffraction rings. The broadening of the diffraction rings is interpreted as a reduction in the domain coherence length, but the shift in the ring radius, while unambiguous in its occurrence, remains unexplained. In particular, we demonstrate that a radial shift explained by domain-wall broadening can be ruled out. With the unprecedented dynamic range of our data, our results provide convincing evidence that labyrinth domain structures are spatially perturbed at ultrafast speeds under far-from-equilibrium conditions, albeit the mechanism inducing the perturbations remains yet to be clarified.
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