| 1. |
- Chen, Z., et al.
(författare)
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Ultrafast Self-Induced X-Ray Transparency and Loss of Magnetic Diffraction
- 2018
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Ingår i: Physical Review Letters. - : AMER PHYSICAL SOC. - 0031-9007 .- 1079-7114. ; 121:13
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Tidskriftsartikel (refereegranskat)abstract
- Using ultrafast similar or equal to 2.5 fs and similar or equal to 25 fs self-amplified spontaneous emission pulses of increasing intensity and a novel experimental scheme, we report the concurrent increase of stimulated emission in the forward direction and loss of out-of-beam diffraction contrast for a Co/Pd multilayer sample. The experimental results are quantitatively accounted for by a statistical description of the pulses in conjunction with the optical Bloch equations. The dependence of the stimulated sample response on the incident intensity, coherence time, and energy jitter of the employed pulses reveals the importance of increased control of x-ray free electron laser radiation.
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| 2. |
- Durr, Hermann A., et al.
(författare)
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A Closer Look Into Magnetism : Opportunities With Synchrotron Radiation
- 2009
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Ingår i: IEEE transactions on magnetics. - 0018-9464 .- 1941-0069. ; 45:1, s. 15-57
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Forskningsöversikt (refereegranskat)abstract
- The unique properties of synchrotron radiation, such as broad energy spectrum, variable light polarization, and flexible time structure, have made it an enormously powerful tool in the study of magnetic phenomena and materials. The refinement of experimental techniques has led to many new research opportunities, keeping up with the challenges put up by modern magnetism research. In this contribution, we review some of the recent developments in the application of synchrotron radiation and particularly soft X-rays to current problems in magnetism, and we discuss future perspectives.
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| 3. |
- Dürr, Hermann A., et al.
(författare)
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Revealing momentum-dependent electron-phonon and phonon-phonon coupling in complex materials with ultrafast electron diffuse scattering
- 2021
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Ingår i: MRS bulletin. - : Springer Nature. - 0883-7694 .- 1938-1425. ; 46:8, s. 731-737
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Tidskriftsartikel (refereegranskat)abstract
- Despite their fundamental role in determining many important properties of materials, detailed momentum-dependent information on the strength of electron–phonon and phonon–phonon coupling across the entire Brillouin zone has remained elusive. Ultrafast electron diffuse scattering (UEDS) is a recently developed technique that is making a significant contribution to these questions. Here, we describe both the UEDS methodology and the information content of ultrafast, photoinduced changes in phonon-diffuse scattering from single-crystal materials. We present results obtained from Ni, WSe2, and TiSe2, materials that are characterized by a complex interplay between electronic (charge, spin) and lattice degrees of freedom. We demonstrate the power of this technique by unraveling carrier–phonon and phonon–phonon interactions in both momentum and time and following nonequilibrium phonon dynamics in detail on ultrafast time scales. By combining ab initio calculations with ultrafast diffuse electron scattering, insights into electronic and magnetic dynamics that impact UEDS indirectly can also be obtained.
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| 4. |
- Engel, Robin Y., et al.
(författare)
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Parallel Broadband Femtosecond Reflection Spectroscopy at a Soft X-Ray Free-Electron Laser
- 2020
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Ingår i: Applied Sciences. - : MDPI. - 2076-3417. ; 10:19
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Tidskriftsartikel (refereegranskat)abstract
- Featured Application Exploiting the full flux and temporal resolution of SASE-FELs for highly sensitive X-ray absorption measurements. X-ray absorption spectroscopy (XAS) and the directly linked X-ray reflectivity near absorption edges yield a wealth of specific information on the electronic structure around the resonantly addressed element. Observing the dynamic response of complex materials to optical excitations in pump-probe experiments requires high sensitivity to small changes in the spectra which in turn necessitates the brilliance of free electron laser (FEL) pulses. However, due to the fluctuating spectral content of pulses generated by self-amplified spontaneous emission (SASE), FEL experiments often struggle to reach the full sensitivity and time-resolution that FELs can in principle enable. Here, we implement a setup which solves two common challenges in this type of spectroscopy using FELs: First, we achieve a high spectral resolution by using a spectrometer downstream of the sample instead of a monochromator upstream of the sample. Thus, the full FEL bandwidth contributes to the measurement at the same time, and the FEL pulse duration is not elongated by a monochromator. Second, the FEL beam is divided into identical copies by a transmission grating beam splitter so that two spectra from separate spots on the sample (or from the sample and known reference) can be recorded in-parallel with the same spectrometer, enabling a spectrally resolved intensity normalization of pulse fluctuations in pump-probe scenarios. We analyze the capabilities of this setup around the oxygen K- and nickel L-edges recorded with third harmonic radiation of the free electron laser in Hamburg (FLASH), demonstrating the capability for pump-probe measurements with sensitivity to reflectivity changes on the per mill level.
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| 5. |
- Gray, A. X., et al.
(författare)
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Ultrafast terahertz field control of electronic and structural interactions in vanadium dioxide
- 2018
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Ingår i: Physical Review B. - : AMER PHYSICAL SOC. - 2469-9950 .- 2469-9969. ; 98:4
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Tidskriftsartikel (refereegranskat)abstract
- Vanadium dioxide (VO2), an archetypal correlated-electron material, undergoes an insulator-metal transition near room temperature that exhibits electron-correlation-driven and structurally driven physics. Using ultrafast temperature- and fluence-dependent optical spectroscopy and x-ray scattering, we show that multiple interrelated electronic and structural processes in the nonequilibrium dynamics in VO2 can be disentangled in the time domain. Specifically, following intense subpicosecond terahertz (THz) electric-field excitation, a partial collapse of the insulating gap occurs within the first picosecond. At temperatures sufficiently close to the transition temperature and for THz peak fields above a threshold of approximately 1 MV/cm, this electronic reconfiguration initiates a change in lattice symmetry taking place on a slower timescale. We identify the kinetic energy increase of electrons tunneling in the strong electric field as the driving force, illustrating a promising method to control electronic and structural interactions in correlated materials on an ultrafast timescale.
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| 6. |
- Grånäs, Oscar, 1979-, et al.
(författare)
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Ultrafast modification of the electronic structure of a correlated insulator
- 2022
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Ingår i: Physical Review Research. - : American Physical Society. - 2643-1564. ; 4:3
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Tidskriftsartikel (refereegranskat)abstract
- A nontrivial balance between Coulomb repulsion and kinematic effects determines the electronic structure of correlated electron materials. The use of electromagnetic fields strong enough to rival these native microscopic interactions allows us to study the electronic response as well as the time scales and energies involved in using quantum effects for possible applications. We use element-specific transient x-ray absorption spectroscopy and high-harmonic generation to measure the response to ultrashort off-resonant optical fields in the prototypical correlated electron insulator NiO. Surprisingly, fields of up to 0.22 V/angstrom lead to no detectable changes in the correlated Ni 3d orbitals contrary to previous predictions. A transient directional charge transfer is uncovered, a behavior that is captured by first-principles theory. Our results highlight the importance of retardation effects in electronic screening and pinpoints a key challenge in functionalizing correlated materials for ultrafast device operation.
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| 7. |
- Gupta, Rahul, et al.
(författare)
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Strain Engineering of Epitaxial Pt/Fe Spintronic Terahertz Emitter
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Annan publikation (övrigt vetenskapligt/konstnärligt)abstract
- Spin-based terahertz (THz) emitters, utilizing the inverse spin Hall effect, are ultra-modern sources for the generation of THz electromagnetic radiation. To make a powerful emitter having large THz amplitude and bandwidth, fundamental understanding in terms of microscopic models is essential. This study reveals important factors to engineer the THzemission amplitude and bandwidth in epitaxial Pt/Fe emitters grown on MgO and MgAl2O4 (MAO) substrates, where the choice of the substrate plays an important role. The THz amplitude and bandwidth are affected by the induced strain in the Fe spin source layer. On the one hand, the THz electric field amplitude is found to be larger when Pt/Fe is grown on MgO even though the crystalline quality of the Fe film is superior when grown on MAO. This is because of the larger defect density, smaller electron relaxation time, and lower electrical conductivity in the THz regime when Fe is grown on MgO. On the other hand, the bandwidth is found to be larger for Pt/Fe grown on MAO and is explained by the uncoupled/coupled Lorentz oscillator models. This study provides an insightful pathway to further engineer metallic spintronic THz emitters in terms of the proper choice of substrate and microscopic properties of the emitter layers.
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| 8. |
- Higley, Daniel J., et al.
(författare)
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Femtosecond X-ray induced changes of the electronic and magnetic response of solids from electron redistribution
- 2019
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Ingår i: Nature Communications. - : Nature Publishing Group. - 2041-1723. ; 10
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Tidskriftsartikel (refereegranskat)abstract
- Resonant X-ray absorption, where an X-ray photon excites a core electron into an unoccupied valence state, is an essential process in many standard X-ray spectroscopies. With increasing X-ray intensity, the X-ray absorption strength is expected to become nonlinear. Here, we report the onset of such a nonlinearity in the resonant X-ray absorption of magnetic Co/Pd multilayers near the Co L-3 edge. The nonlinearity is directly observed through the change of the absorption spectrum, which is modified in less than 40 fs within 2 eV of its threshold. This is interpreted as a redistribution of valence electrons near the Fermi level. For our magnetic sample this also involves mixing of majority and minority spins, due to sample demagnetization. Our findings reveal that nonlinear X-ray responses of materials may already occur at relatively low intensities, where the macroscopic sample is not destroyed, providing insight into ultrafast charge and spin dynamics.
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| 9. |
- Higley, Daniel J., et al.
(författare)
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Stimulated resonant inelastic X-ray scattering in a solid
- 2022
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Ingår i: Communications Physics. - : Springer Science and Business Media LLC. - 2399-3650. ; 5
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Tidskriftsartikel (refereegranskat)abstract
- When materials are exposed to X-ray pulses with sufficiently high intensity, various nonlinear effects can occur. The most fundamental one consists of stimulated electronic decays after resonant absorption of X-rays. Such stimulated decays enhance the number of emitted photons and the emission direction is confined to that of the stimulating incident photons which clone themselves in the process. Here we report the observation of stimulated resonant elastic (REXS) and inelastic (RIXS) X-ray scattering near the cobalt L3 edge in solid Co/Pd multilayer samples. We observe an enhancement of order 106 of the stimulated over the conventional spontaneous RIXS signal into the small acceptance angle of the RIXS spectrometer. We also find that in solids both stimulated REXS and RIXS spectra contain contributions from inelastic electron scattering processes, even for ultrashort 5 fs pulses. Our results reveal the potential and caveats of the development of stimulated RIXS in condensed matter.
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| 10. |
- Hudl, Matthias, et al.
(författare)
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Nonlinear Magnetization Dynamics Driven by Strong Terahertz Fields
- 2019
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Ingår i: Physical Review Letters. - : AMER PHYSICAL SOC. - 0031-9007 .- 1079-7114. ; 123:19
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Tidskriftsartikel (refereegranskat)abstract
- We present a comprehensive experimental and numerical study of magnetization dynamics in a thin metallic film triggered by single-cycle terahertz pulses of ∼20 MV/m electric field amplitude and ∼1 ps duration. The experimental dynamics is probed using the femtosecond magneto-optical Kerr effect, and it is reproduced numerically using macrospin simulations. The magnetization dynamics can be decomposed in three distinct processes: a coherent precession of the magnetization around the terahertz magnetic field, an ultrafast demagnetization that suddenly changes the anisotropy of the film, and a uniform precession around the equilibrium effective field that is relaxed on the nanosecond time scale, consistent with a Gilbert damping process. Macrospin simulations quantitatively reproduce the observed dynamics, and allow us to predict that novel nonlinear magnetization dynamics regimes can be attained with existing tabletop terahertz sources.
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