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    Exchange-Striction Driven Ultrafast Nonthermal Lattice Dynamics in NiO
    (College Park, Md. : APS, 2021) Windsor, Y.W.; Zahn, D.; Kamrla, R.; Feldl, J.; Seiler, H.; Chiang, C.-T.; Ramsteiner, M.; Widdra, W.; Ernstorfer, R.; Rettig, L.
    We use femtosecond electron diffraction to study ultrafast lattice dynamics in the highly correlated antiferromagnetic (AFM) semiconductor NiO. Using the scattering vector (Q) dependence of Bragg diffraction, we introduce Q-resolved effective temperatures describing the transient lattice. We identify a nonthermal lattice state with preferential displacement of O compared to Ni ions, which occurs within ∼0.3  ps and persists for 25 ps. We associate this with transient changes to the AFM exchange striction-induced lattice distortion, supported by the observation of a transient Q asymmetry of Friedel pairs. Our observation highlights the role of spin-lattice coupling in routes towards ultrafast control of spin order.
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    Unraveling the Orbital Physics in a Canonical Orbital System KCuF3
    (College Park, Md. : APS, 2021) Li, Jiemin; Xu, Lei; Garcia-Fernandez, Mirian; Nag, Abhishek; Robarts, H.C.; Walters, A.C.; Liu, X.; Zhou, Jianshi; Wohlfeld, Krzysztof; van den Brink, Jeroen; Ding, Hong; Zhou, Ke-Jin
    We explore the existence of the collective orbital excitations, orbitons, in the canonical orbital system KCuF3 using the Cu L3-edge resonant inelastic x-ray scattering. We show that the nondispersive high-energy peaks result from the Cu2+  dd orbital excitations. These high-energy modes display good agreement with the ab initio quantum chemistry calculation, indicating that the dd excitations are highly localized. At the same time, the low-energy excitations present clear dispersion. They match extremely well with the two-spinon continuum following the comparison with Müller ansatz calculations. The localized dd excitations and the observation of the strongly dispersive magnetic excitations suggest that the orbiton dispersion is below the resolution detection limit. Our results can reconcile with the strong local Jahn-Teller effect in KCuF3, which predominantly drives orbital ordering.
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    Measurement of Spin Dynamics in a Layered Nickelate Using X-Ray Photon Correlation Spectroscopy: Evidence for Intrinsic Destabilization of Incommensurate Stripes at Low Temperatures
    (College Park, Md. : APS, 2021) Ricci, Alessandro; Poccia, Nicola; Campi, Gaetano; Mishra, Shrawan; Müller, Leonard; Joseph, Boby; Shi, Bo; Zozulya, Alexey; Buchholz, Marcel; Trabant, Christoph; Lee, James C. T.; Viefhaus, Jens; Goedkoop, Jeroen B.; Nugroho, Agustinus Agung; Braden, Markus; Roy, Sujoy; Sprung, Michael; Schüßler-Langeheine, Christian
    We study the temporal stability of stripe-type spin order in a layered nickelate with x-ray photon correlation spectroscopy and observe fluctuations on timescales of tens of minutes over a wide temperature range. These fluctuations show an anomalous temperature dependence: they slow down at intermediate temperatures and speed up on both heating and cooling. This behavior appears to be directly connected with spatial correlations: stripes fluctuate slowly when stripe correlation lengths are large and become faster when spatial correlations decrease. A low-temperature decay of nickelate stripe correlations, reminiscent of what occurs in cuprates as a result of a competition between stripes and superconductivity, hence occurs via loss of both spatial and temporal correlations.
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    Evolution of a molecular shape resonance along a stretching chemical bond
    (College Park, Md. : APS, 2020) Brausse, Felix; Bach, Florian; Krečinić, Faruk; Vrakking, Marc J.J.; Rouzée, Arnaud
    We report experiments on laser-assisted electron recollisions that result from strong-field ionization of photoexcited I2 molecules in the regime of low-energy electron scattering (<25  eV impact energy). By comparing differential scattering cross sections extracted from the angle-resolved photoelectron spectra to differential scattering cross sections from quantum-scattering calculations, we demonstrate that the electron-scattering dynamics is dominated by a shape resonance. When the molecular bond stretches during the evolution of a vibrational wave packet this shape resonance shifts to lower energies, both in experiment and theory. We explain this behavior by the nature of the resonance wave function, which closely resembles an antibonding molecular orbital of I2.
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    Topology Counts: Force Distributions in Circular Spring Networks
    (College Park, Md. : APS, 2018) Heidemann, Knut M.; Sageman-Furnas, Andrew O.; Sharma, Abhinav; Rehfeldt, Florian; Schmidt, Christoph F.; Wardetzky, Max
    Filamentous polymer networks govern the mechanical properties of many biological materials. Force distributions within these networks are typically highly inhomogeneous, and, although the importance of force distributions for structural properties is well recognized, they are far from being understood quantitatively. Using a combination of probabilistic and graph-theoretical techniques, we derive force distributions in a model system consisting of ensembles of random linear spring networks on a circle. We show that characteristic quantities, such as the mean and variance of the force supported by individual springs, can be derived explicitly in terms of only two parameters: (i) average connectivity and (ii) number of nodes. Our analysis shows that a classical mean-field approach fails to capture these characteristic quantities correctly. In contrast, we demonstrate that network topology is a crucial determinant of force distributions in an elastic spring network. Our results for 1D linear spring networks readily generalize to arbitrary dimensions.
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    Ultrafast Demagnetization Dominates Fluence Dependence of Magnetic Scattering at Co M Edges
    (College Park, Md. : APS, 2020) Schneider, Michael; Pfau, Bastian; Günther, Christian M.; von Korff Schmising, Clemens; Weder, David; Geilhufe, Jan; Perron, Jonathan; Capotondi, Flavio; Pedersoli, Emanuele; Manfredda, Michele; Hennecke, Martin; Vodungbo, Boris; Lüning, Jan; Eisebitt, Stefan
    We systematically study the fluence dependence of the resonant scattering cross-section from magnetic domains in Co/Pd-based multilayers. Samples are probed with single extreme ultraviolet (XUV) pulses of femtosecond duration tuned to the Co M3,2 absorption resonances using the FERMI@Elettra free-electron laser. We report quantitative data over 3 orders of magnitude in fluence, covering 16  mJ/cm2/pulse to 10 000  mJ/cm2/pulse with pulse lengths of 70 fs and 120 fs. A progressive quenching of the diffraction cross-section with fluence is observed. Compression of the same pulse energy into a shorter pulse—implying an increased XUV peak electric field—results in a reduced quenching of the resonant diffraction at the Co M3,2 edge. We conclude that the quenching effect observed for resonant scattering involving the short-lived Co 3p core vacancies is noncoherent in nature. This finding is in contrast to previous reports investigating resonant scattering involving the longer-lived Co 2p states, where stimulated emission has been found to be important. A phenomenological model based on XUV-induced ultrafast demagnetization is able to reproduce our entire set of experimental data and is found to be consistent with independent magneto-optical measurements of the demagnetization dynamics on the same samples.
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    Robustness of Light-Transport Processes to Bending Deformations in Graded-Index Multimode Waveguides
    (College Park, Md. : APS, 2018) Boonzajer Flaes, Dirk E.; Stopka, Jan; Turtaev, Sergey; de Boer, Johannes F.; Tyc, Tomáš; Čižmár, Tomáš
    Light transport through a multimode optical waveguide undergoes changes when subjected to bending deformations. We show that optical waveguides with a perfectly parabolic refractive index profile are almost immune to bending, conserving the structure of propagation-invariant modes. Moreover, we show that changes to the transmission matrix of parabolic-index fibers due to bending can be expressed with only two free parameters, regardless of how complex a particular deformation is. We provide detailed analysis of experimentally measured transmission matrices of a commercially available graded-index fiber as well as a gradient-index rod lens featuring a very faithful parabolic refractive index profile. Although parabolic-index fibers with a sufficiently precise refractive index profile are not within our reach, we show that imaging performance with standard commercially available graded-index fibers is significantly less influenced by bending deformations than step-index types under the same conditions. Our work thus predicts that the availability of ultraprecise parabolic-index fibers will make endoscopic applications with flexible probes feasible and free from extremely elaborate computational challenges.
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    Three-Dimensional Shapes of Spinning Helium Nanodroplets
    (College Park, Md. : APS, 2018) Langbehn, Bruno; Sander, Katharina; Ovcharenko, Yevheniy; Peltz, Christian; Clark, Andrew; Coreno, Marcello; Cucini, Riccardo; Drabbels, Marcel; Finetti, Paola; Di Fraia, Michele; Giannessi, Luca; Grazioli, Cesare; Iablonskyi, Denys; LaForge, Aaron C.; Nishiyama, Toshiyuki; Oliver Álvarez de Lara, Verónica; Piseri, Paolo; Plekan, Oksana; Ueda, Kiyoshi; Zimmermann, Julian; Prince, Kevin C.; Stienkemeier, Frank; Callegari, Carlo; Fennel, Thomas; Rupp, Daniela; Möller, Thomas
    A significant fraction of superfluid helium nanodroplets produced in a free-jet expansion has been observed to gain high angular momentum resulting in large centrifugal deformation. We measured single-shot diffraction patterns of individual rotating helium nanodroplets up to large scattering angles using intense extreme ultraviolet light pulses from the FERMI free-electron laser. Distinct asymmetric features in the wide-angle diffraction patterns enable the unique and systematic identification of the three-dimensional droplet shapes. The analysis of a large data set allows us to follow the evolution from axisymmetric oblate to triaxial prolate and two-lobed droplets. We find that the shapes of spinning superfluid helium droplets exhibit the same stages as classical rotating droplets while the previously reported metastable, oblate shapes of quantum droplets are not observed. Our three-dimensional analysis represents a valuable landmark for clarifying the interrelation between morphology and superfluidity on the nanometer scale.
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    Ultrafast Optically Induced Ferromagnetic State in an Elemental Antiferromagnet
    (College Park, Md. : APS, 2021) Golias, E.; Kumberg, I.; Gelen, I.; Thakur, S.; Gördes, J.; Hosseinifar, R.; Guillet, Q.; Dewhurst, J.K.; Sharma, S.; Schüßler-Langeheine, C.; Pontius, N.; Kuch, W.
    We present evidence for an ultrafast optically induced ferromagnetic alignment of antiferromagnetic Mn in Co/Mn multilayers. We observe the transient ferromagnetic signal at the arrival of the pump pulse at the Mn L3 resonance using x-ray magnetic circular dichroism in reflectivity. The timescale of the effect is comparable to the duration of the excitation and occurs before the magnetization in Co is quenched. Theoretical calculations point to the imbalanced population of Mn unoccupied states caused by the Co interface for the emergence of this transient ferromagnetic state.
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    Low Temperature Relaxation of Donor Bound Electron Spins in 28Si:P
    (College Park, Md. : APS, 2021) Sauter, E.; Abrosimov, N.V.; Hübner, J.; Oestreich, M.
    We measure the spin-lattice relaxation of donor bound electrons in ultrapure, isotopically enriched, phosphorus-doped 28Si:P. The optical pump-probe experiments reveal at low temperatures extremely long spin relaxation times which exceed 20 h. The 28Si:P spin relaxation rate increases linearly with temperature in the regime below 1 K and shows a distinct transition to a T9 dependence which dominates the spin relaxation between 2 and 4 K at low magnetic fields. The T7 dependence reported for natural silicon is absent. At high magnetic fields, the spin relaxation is dominated by the magnetic field dependent single phonon spin relaxation process. This process is well documented for natural silicon at finite temperatures but the 28Si:P measurements validate additionally that the bosonic phonon distribution leads at very low temperatures to a deviation from the linear temperature dependence of Γ as predicted by theory.