| 1. |
- Chen, Cong, et al.
(författare)
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Distinguishing attosecond electron-electron scattering and screening in transition metals
- 2017
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Ingår i: Proceedings of the National Academy of Sciences of the United States of America. - : National Academy of Sciences. - 0027-8424 .- 1091-6490. ; 114:27, s. E5300-E5307
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Tidskriftsartikel (refereegranskat)abstract
- Electron-electron interactions are the fastest processes in materials, occurring on femtosecond to attosecond timescales, depending on the electronic band structure of the material and the excitation energy. Such interactions can play a dominant role in light-induced processes such as nano-enhanced plasmonics and catalysis, light harvesting, or phase transitions. However, to date it has not been possible to experimentally distinguish fundamental electron interactions such as scattering and screening. Here, we use sequences of attosecond pulses to directly measure electron-electron interactions in different bands of different materials with both simple and complex Fermi surfaces. By extracting the time delays associated with photoemission we show that the lifetime of photoelectrons from the d band of Cu are longer by similar to 100 as compared with those from the same band of Ni. We attribute this to the enhanced electron-electron scattering in the unfilled d band of Ni. Using theoretical modeling, we can extract the contributions of electron-electron scattering and screening in different bands of different materials with both simple and complex Fermi surfaces. Our results also show that screening influences high-energy photoelectrons (approximate to 20 eV) significantly less than low-energy photoelectrons. As a result, high-energy photoelectrons can serve as a direct probe of spin-dependent electron-electron scattering by neglecting screening. This can then be applied to quantifying the contribution of electron interactions and screening to low-energy excitations near the Fermi level. The information derived here provides valuable and unique information for a host of quantum materials.
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| 2. |
- 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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| 3. |
- 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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| 4. |
- Kfir, Ofer, et al.
(författare)
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Generation of bright phase-matched circularly-polarized extreme ultraviolet high harmonics
- 2015
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Ingår i: Nature Photonics. - 1749-4885 .- 1749-4893. ; 9:2, s. 99-105
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Tidskriftsartikel (refereegranskat)abstract
- Circularly-polarized extreme ultraviolet and X-ray radiation is useful for analysing the structural, electronic and magnetic properties of materials. To date, such radiation has only been available at large-scale X-ray facilities such as synchrotrons. Here, we demonstrate the first bright, phase-matched, extreme ultraviolet circularly-polarized high harmonics source. The harmonics are emitted when bi-chromatic counter-rotating circularly-polarized laser pulses field-ionize a gas in a hollow-core waveguide. We use this new light source for magnetic circular dichroism measurements at the M-shell absorption edges of Co. We show that phase-matching of circularly-polarized harmonics is unique and robust, producing a photon flux comparable to linearly polarized high harmonic sources. This work represents a critical advance towards the development of table-top systems for element-specific imaging and spectroscopy of multiple elements simultaneously in magnetic and other chiral media with very high spatial and temporal resolution.
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| 5. |
- Kfir, Ofer, et al.
(författare)
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Helicity-selective phase-matching and quasi-phase matching of circularly polarized high-order harmonics : towards chiral attosecond pulses
- 2016
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Ingår i: Journal of Physics B: Atomic, Molecular and Optical Physics. - : IOP Publishing. - 0953-4075 .- 1361-6455. ; 49:12
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Tidskriftsartikel (refereegranskat)abstract
- Phase matching of circularly polarized high-order harmonics driven by counter-rotating bi-chromatic lasers was recently predicted theoretically and demonstrated experimentally. In that work, phase matching was analyzed by assuming that the total energy, spin angular momentum and linear momentum of the photons participating in the process are conserved. Here we propose a new perspective on phase matching of circularly polarized high harmonics. We derive an extended phase matching condition by requiring a new propagation matching condition between the classical vectorial bi-chromatic laser pump and harmonics fields. This allows us to include the influence of the laser pulse envelopes on phase matching. We find that the helicity dependent phase matching facilitates generation of high harmonics beams with a high degree of chirality. Indeed, we present an experimentally measured chiral spectrum that can support a train of attosecond pulses with a high degree of circular polarization. Moreover, while the degree of circularity of the most intense pulse approaches unity, all other pulses exhibit reduced circularity. This feature suggests the possibility of using a train of attosecond pulses as an isolated attosecond probe for chiral-sensitive experiments.
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| 6. |
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| 7. |
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| 8. |
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| 9. |
- 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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| 10. |
- Tao, Zhensheng, et al.
(författare)
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The nature of the ultrafast magnetic phase transition in nickel revealed by correlating EUV-MOKE and ARPES spectroscopies
- 2019
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Ingår i: XXI International Conference on Ultrafast Phenomena 2018 (UP 2018). - : EDP Sciences.
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Konferensbidrag (refereegranskat)abstract
- By correlating time- and angle-resolved photoemission (Tr-ARPES) and time-resolved transverse- magneto-optical Kerr effect (Tr-TMOKE) measurements, both at extreme ultraviolet (EUV) wavelengths, we uncover the nature of the ultrafast photoinduced magnetic phase transition in Ni. This allows us to explain the ultrafast magnetic response of Ni at all laser fluences - from a small reduction of the magnetization at low laser fluences, to complete quenching at high laser fluences. We provide an alternative explanation to the fluence-dependent recovery timescales commonly observed in ultrafast magneto-optical spectroscopies on ferromagnets: it is due to the bulk-averaging effect and different depths of sample exhibit distinct dynamics, depending on whether a magnetic phase transition is induced. We also show evidence of two competing channels with two distinct timescales in the recovery process, that suggest the presence of coexisting phases in the material.
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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. |
- You, Wenjing, et al.
(författare)
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Revealing the Nature of the Ultrafast Magnetic Phase Transition in Ni by Correlating Extreme Ultraviolet Magneto-Optic and Photoemission Spectroscopies
- 2018
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Ingår i: Physical Review Letters. - : AMER PHYSICAL SOC. - 0031-9007 .- 1079-7114. ; 121:7
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Tidskriftsartikel (refereegranskat)abstract
- By correlating time-and angle-resolved photoemission and time-resolved transverse magneto-optical Kerr effect measurements, both at extreme ultraviolet wavelengths, we uncover the universal nature of the ultrafast photoinduced magnetic phase transition in Ni. This allows us to explain the ultrafast magnetic response of Ni at all laser fluences-from a small reduction of the magnetization at low laser fluences, to complete quenching at high laser fluences. Both probe methods exhibit the same demagnetization and recovery timescales. The spin system absorbs the energy required to proceed through a magnetic phase transition within 20 fs after the peak of the pump pulse. However, the spectroscopic signatures of demagnetization of the material appear only after approximate to 200 fs and the subsequent recovery of magnetization on timescales ranging from 500 fs to >70 ps. We also provide evidence of two competing channels with two distinct timescales in the recovery process that suggest the presence of coexisting phases in the material.
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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. |
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| 17. |
- 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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