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As the oldest known magnetic material, magnetite (Fe3O4) has fascinated mankind for millennia. As the first oxide in which a relationship between electrical conductivity and fluctuating/localized electronic order was shown(1), magnetite represents a model system for understanding correlated oxides in general. Nevertheless, the exact mechanism of the insulator-metal, or Verwey, transition has long remained inaccessible(2-8). Recently, three- Fe- site lattice distortions called trimeronswere identified as the characteristic building blocks of the low-temperature insulating electronically ordered phase(9). Here we investigate the Verwey transition with pump- probe X- ray diffraction and optical reflectivity techniques, and show how trimerons become mobile across the insulator-metal transition. We find this to be a two- step process. After an initial 300 fs destruction of individual trimerons, phase separation occurs on a 1.5 +/- 0.2 ps timescale to yield residual insulating and metallic regions. This work establishes the speed limit for switching in future oxide electronics(10).
We present a statistical analysis of phase space density data from the first 26 months of the Van Allen Probes mission. In particular, we investigate the relationship between the tens and hundreds of keV seed electrons and >1 MeV core radiation belt electron population. Using a cross-correlation analysis, we find that the seed and core populations are well correlated with a coefficient of approximate to 0.73 with a time lag of 10-15 h. We present evidence of a seed population threshold that is necessary for subsequent acceleration. The depth of penetration of the seed population determines the inner boundary of the acceleration process. However, we show that an enhanced seed population alone is not enough to produce acceleration in the higher energies, implying that the seed population of hundreds of keV electrons is only one of several conditions required for MeV electron radiation belt acceleration.
Scientific Objectives of Electron Losses and Fields INvestigation Onboard Lomonosov Satellite
(2017)
The objective of the Electron Losses and Fields INvestigation on board the Lomonosov satellite ( ELFIN-L) project is to determine the energy spectrum of precipitating energetic electrons and ions and, together with other polar-orbiting and equatorial missions, to better understand the mechanisms responsible for scattering these particles into the atmosphere. This mission will provide detailed measurements of the radiation environment at low altitudes. The 400-500 km sun-synchronous orbit of Lomonosov is ideal for observing electrons and ions precipitating into the atmosphere. This mission provides a unique opportunity to test the instruments. Similar suite of instruments will be flown in the future NSF-and NASA-supported spinning CubeSat ELFIN satellites which will augment current measurements by providing detailed information on pitch-angle distributions of precipitating and trapped particles.
Femtosecond x-ray laser pulses are used to probe the carbon monoxide (CO) oxidation reaction on ruthenium (Ru) initiated by an optical laser pulse. On a time scale of a few hundred femtoseconds, the optical laser pulse excites motions of CO and oxygen (O) on the surface, allowing the reactants to collide, and, with a transient close to a picosecond (ps), new electronic states appear in the OK-edge x-ray absorption spectrum. Density functional theory calculations indicate that these result from changes in the adsorption site and bond formation between CO and O with a distribution of OC-O bond lengths close to the transition state (TS). After 1 ps, 10% of the CO populate the TS region, which is consistent with predictions based on a quantum oscillator model.
Since more than 15 years, the Cluster mission passes through Earth's radiation belts at least once every 2 days for several hours, measuring the electron intensity at energies from 30 to 400 keV. These data have previously been considered not usable due to contamination caused by penetrating energetic particles (protons at >100 keV and electrons at >400 keV). In this study, we assess the level of distortion of energetic electron spectra from the Research with Adaptive Particle Imaging Detector (RAPID)/Imaging Electron Spectrometer (IES) detector, determining the efficiency of its shielding. We base our assessment on the analysis of experimental data and a radiation transport code (Geant4). In simulations, we use the incident particle energy distribution of the AE9/AP9 radiation belt models. We identify the Roederer L values, L⋆, and energy channels that should be used with caution: at 3≤L⋆≤4, all energy channels (40–400 keV) are contaminated by protons (≃230 to 630 keV and >600 MeV); at L⋆≃1 and 4–6, the energy channels at 95–400 keV are contaminated by high-energy electrons (>400 keV). Comparison of the data with electron and proton observations from RBSP/MagEIS indicates that the subtraction of proton fluxes at energies ≃ 230–630 keV from the IES electron data adequately removes the proton contamination. We demonstrate the usefulness of the corrected data for scientific applications.
The "Lomonosov" space project is lead by Lomonosov Moscow State University in collaboration with the following key partners: Joint Institute for Nuclear Research, Russia, University of California, Los Angeles (USA), University of Pueblo (Mexico), Sungkyunkwan University (Republic of Korea) and with Russian space industry organi-zations to study some of extreme phenomena in space related to astrophysics, astroparticle physics, space physics, and space biology. The primary goals of this experiment are to study:
-Ultra-high energy cosmic rays (UHECR) in the energy range of the Greizen-ZatsepinKuzmin (GZK) cutoff;
-Ultraviolet (UV) transient luminous events in the upper atmosphere;
-Multi-wavelength study of gamma-ray bursts in visible, UV, gamma, and X-rays;
-Energetic trapped and precipitated radiation (electrons and protons) at low-Earth orbit (LEO) in connection with global geomagnetic disturbances;
-Multicomponent radiation doses along the orbit of spacecraft under different geomagnetic conditions and testing of space segments of optical observations of space-debris and other space objects;
-Instrumental vestibular-sensor conflict of zero-gravity phenomena during space flight.
This paper is directed towards the general description of both scientific goals of the project and scientific equipment on board the satellite. The following papers of this issue are devoted to detailed descriptions of scientific instruments.
We used the Linac Coherent Light Source free-electron x-ray laser to probe the electronic structure of CO molecules as their chemisorption state on Ru(0001) changes upon exciting the substrate by using a femtosecond optical laser pulse. We observed electronic structure changes that are consistent with a weakening of the CO interaction with the substrate but without notable desorption. A large fraction of the molecules (30%) was trapped in a transient precursor state that would precede desorption. We calculated the free energy of the molecule as a function of the desorption reaction coordinate using density functional theory, including van der Waals interactions. Two distinct adsorption wells-chemisorbed and precursor state separated by an entropy barrier-explain the anomalously high prefactors often observed in desorption of molecules from metals.
Ultrafast soft X-ray emission spectroscopy of surface adsorbates using an X-ray free electron laser
(2013)
We report on an experimental system designed to probe chemical reactions on solid surfaces on a sub-picosecond timescale using soft X-ray emission spectroscopy at the Linac Coherent Light Source (LCLS) free electron laser (FEL) at the SLAC National Accelerator Laboratory. We analyzed the O 1s X-ray emission spectra recorded from atomic oxygen adsorbed on a Ru(0001) surface at a synchrotron beamline (SSRL, BL13-2) and an FEL beamline (LCLS, SXR). We have demonstrated conditions that provide negligible amount of FEL induced damage of the sample. In addition we show that the setup is capable of tracking the temporal evolution of electronic structure during a surface reaction of submonolayer quantities of CO molecules desorbing from the surface.
Selective ultrafast probing of transient hot chemisorbed and precursor States of CO on Ru(0001)
(2013)
We have studied the femtosecond dynamics following optical laser excitation of CO adsorbed on a Ru surface by monitoring changes in the occupied and unoccupied electronic structure using ultrafast soft x-ray absorption and emission. We recently reported [M. Dell'Angela et al. Science 339, 1302 (2013)] a phonon-mediated transition into a weakly adsorbed precursor state occurring on a time scale of >2 ps prior to desorption. Here we focus on processes within the first picosecond after laser excitation and show that the metal-adsorbate coordination is initially increased due to hot-electron-driven vibrational excitations. This process is faster than, but occurs in parallel with, the transition into the precursor state. With resonant x-ray emission spectroscopy, we probe each of these states selectively and determine the respective transient populations depending on optical laser fluence. Ab initio molecular dynamics simulations of CO adsorbed on Ru(0001) were performed at 1500 and 3000 K providing insight into the desorption process.
We utilized femtosecond time-resolved resonant inelastic X-ray scattering and ab initio theory to study the transient electronic structure and the photoinduced molecular dynamics of a model metal carbonyl photocatalyst Fe(CO)(5) in ethanol solution. We propose mechanistic explanation for the parallel ultrafast intra-molecular spin crossover and ligation of the Fe(CO)(4) which are observed following a charge transfer photoexcitation of Fe(CO)(5) as reported in our previous study [ Wernet et al., Nature 520, 78 (2015)]. We find that branching of the reaction pathway likely happens in the (1)A(1) state of Fe(CO)(4). A sub-picosecond time constant of the spin crossover from B-1(2) to B-3(2) is rationalized by the proposed B-1(2) -> (1)A(1) -> B-3(2) mechanism. Ultrafast ligation of the B-1(2) Fe(CO)(4) state is significantly faster than the spin-forbidden and diffusion limited ligation process occurring from the B-3(2) Fe(CO)(4) ground state that has been observed in the previous studies. We propose that the ultrafast ligation occurs via B-1(2) -> (1)A(1) -> (1)A'Fe(CO)(4)EtOH pathway and the time scale of the (1)A(1) Fe(CO)(4) state ligation is governed by the solute-solvent collision frequency. Our study emphasizes the importance of understanding the interaction of molecular excited states with the surrounding environment to explain the relaxation pathways of photoexcited metal carbonyls in solution. (C) 2016 Author(s).