| 1. |
- Assefa, T. A., et al.
(författare)
-
The fluctuation–dissipation measurement instrument at the Linac Coherent Light Source
- 2022
-
Ingår i: Review of Scientific Instruments. - : AIP Publishing. - 1089-7623 .- 0034-6748. ; 93
-
Tidskriftsartikel (refereegranskat)abstract
- The development of new modes at x-ray free electron lasers has inspired novel methods for studying fluctuations at different energies and timescales. For closely spaced x-ray pulses that can be varied on ultrafast time scales, we have constructed a pair of advanced instruments to conduct studies targeting quantum materials. We first describe a prototype instrument built to test the proof-of-principle of resonant magnetic scattering using ultrafast pulse pairs. This is followed by a description of a new endstation, the so-called fluctuation–dissipation measurement instrument, which was used to carry out studies with a fast area detector. In addition, we describe various types of diagnostics for single-shot contrast measurements, which can be used to normalize data on a pulse-by-pulse basis and calibrate pulse amplitude ratios, both of which are important for the study of fluctuations in materials. Furthermore, we present some new results using the instrument that demonstrates access to higher momentum resolution.
|
|
| 2. |
|
|
| 3. |
- Mitzner, Rolf, et al.
(författare)
-
L-Edge X-ray Absorption Spectroscopy of Dilute Systems Relevant to Metalloproteins Using an X-ray Free-Electron Laser
- 2013
-
Ingår i: The Journal of Physical Chemistry Letters. - : American Chemical Society (ACS). - 1948-7185. ; 4:21, s. 3641-3647
-
Tidskriftsartikel (refereegranskat)abstract
- L-edge spectroscopy of 3d transition metals provides important electronic structure information and has been used in many fields. However, the use of this method for studying dilute aqueous systems, such as metalloenzymes, has not been prevalent because of severe radiation damage and the lack of suitable detection systems. Here we present spectra from a dilute Mn aqueous solution using a high-transmission zone-plate spectrometer at the Linac Coherent Light Source (LCLS). The spectrometer has been optimized for discriminating the Mn L-edge signal from the overwhelming 0 K-edge background that arises from water and protein itself, and the ultrashort LCLS X-ray pulses can outrun X-ray induced damage. We show that the deviations of the partial-fluorescence yield-detected spectra from the true absorption can be well modeled using the state-dependence of the fluorescence yield, and discuss implications for the application of our concept to biological samples.
|
|
| 4. |
- Parchenko, Sergii, et al.
(författare)
-
Orbital dynamics during an ultrafast insulator to metal transition
- 2020
-
Ingår i: Physical Review Research. - : AMER PHYSICAL SOC. - 2643-1564. ; 2:2
-
Tidskriftsartikel (refereegranskat)abstract
- We present ultrafast resonant inelastic x-ray scattering (RIXS) experiments performed at the vanadium L edge to track changes in the electronic structure of V2O3, a classical Mott-Hubbard material. The probed orbital excitations within the d shell of the V ion show a sub-ps time response, which evolves at later times to a state that appears electronically indistinguishable from the high-temperature metallic state. For low excitation fluences, a transient recovery or delay is observed, which could be related to a transient dimerization of the V-V bonds. Our results demonstrate the great potential for RIXS spectroscopy to study the ultrafast orbital dynamics in strongly correlated materials.
|
|
| 5. |
- Wernet, Philippe, 1971-, et al.
(författare)
-
Orbital-specific mapping of the ligand exchange dynamics of Fe(CO)5 in solution
- 2015
-
Ingår i: Nature. - : Springer Science and Business Media LLC. - 0028-0836 .- 1476-4687. ; 520:7545, s. 78-81
-
Tidskriftsartikel (refereegranskat)abstract
- Transition-metal complexes have long attracted interest for fundamental chemical reactivity studies and possible use in solar energy conversion. Electronic excitation, ligand loss from the metal centre, or a combination of both, creates changes in charge and spin density at the metal site that need to be controlled to optimize complexes for photocatalytic hydrogen production and selective carbon-hydrogen bond activation. An understanding at the molecular level of how transition-metal complexes catalyse reactions, and in particular of the role of the short-lived and reactive intermediate states involved, will be critical for such optimization. However, suitable methods for detailed characterization of electronic excited states have been lacking. Here we show, with the use of X-ray laser-based femtosecond resolution spectroscopy and advanced quantum chemical theory to probe the reaction dynamics of the benchmark transition-metal complex Fe(CO)5 insolution, that the photoinduced removal of CO generates the 16-electron Fe(CO)4 species, a homogeneous catalyst with an electron deficiency at the Fe centre, in a hitherto unreported excited singlet state that either converts to the triplet ground state or combines with a CO or solvent molecule to regenerate a penta-coordinated Fe species on a sub-picosecond timescale. This finding, which resolves the debate about the relative importance of different spin channels in the photochemistry of Fe(CO)5 (refs 4, 16,17,18,19 and 20), was made possible by the ability of femtosecond X-ray spectroscopy to probe frontier-orbital interactions with atom specificity. We expect the method to be broadly applicable in the chemical sciences, and to complement approaches that probe structural dynamics in ultrafast processes.
|
|
| 6. |
- Zusin, Dmitriy, et al.
(författare)
-
Ultrafast perturbation of magnetic domains by optical pumping in a ferromagnetic multilayer
- 2022
-
Ingår i: Physical Review B. - : American Physical Society. - 2469-9950 .- 2469-9969. ; 106:14
-
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.
|
|
| 7. |
- Beye, Martin, et al.
(författare)
-
Chemical Bond Activation Observed with an X-ray Laser
- 2016
-
Ingår i: The Journal of Physical Chemistry Letters. - : American Chemical Society (ACS). - 1948-7185. ; 7:18, s. 3647-3651
-
Tidskriftsartikel (refereegranskat)abstract
- The concept of bonding and antibonding orbitals is fundamental in chemistry. The population of those orbitals and the energetic difference between the two reflect the strength of the bonding interaction. Weakening the bond is expected to reduce this energetic splitting, but the transient character of bond-activation has so far prohibited direct experimental access. Here we apply time-resolved soft X-ray spectroscopy at a free electron laser to directly observe the decreased bonding antibonding splitting following bond-activation using an ultrashort optical laser pulse.
|
|
| 8. |
- Eckert, Sebastian, et al.
(författare)
-
Ultrafast Independent N-H and N-C Bond Deformation Investigated with Resonant Inelastic X-Ray Scattering
- 2017
-
Ingår i: Angewandte Chemie International Edition. - : Wiley. - 1433-7851 .- 1521-3773. ; 56:22, s. 6088-6092
-
Tidskriftsartikel (refereegranskat)abstract
- The femtosecond excited-state dynamics following resonant photoexcitation enable the selective deformation of N-H and N-C chemical bonds in 2-thiopyridone in aqueous solution with optical or X-ray pulses. In combination with multiconfigurational quantum-chemical calculations, the orbital-specific electronic structure and its ultrafast dynamics accessed with resonant inelastic X-ray scattering at the N 1s level using synchrotron radiation and the soft X-ray free-electron laser LCLS provide direct evidence for this controlled photoinduced molecular deformation and its ultrashort time-scale.
|
|
| 9. |
- Higley, Daniel J., et al.
(författare)
-
Femtosecond X-ray induced changes of the electronic and magnetic response of solids from electron redistribution
- 2019
-
Ingår i: Nature Communications. - : Nature Publishing Group. - 2041-1723. ; 10
-
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.
|
|
| 10. |
- Higley, Daniel J., et al.
(författare)
-
Stimulated resonant inelastic X-ray scattering in a solid
- 2022
-
Ingår i: Communications Physics. - : Springer Science and Business Media LLC. - 2399-3650. ; 5
-
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.
|
|
