618 research outputs found
Femtosecond photoelectron diffraction: A new approach to image molecular structure during photochemical reactions.
Continuing technical advances in the creation of (sub-) femtosecond VUV and X-ray pulses with Free-Electron Lasers and laser-based high-harmonic-generation sources have created new opportunities for studying ultrafast dynamics during chemical reactions. Here, we present an approach to image the geometric structure of gas-phase molecules with fewfemtosecond temporal and sub-Ć
ngstrƶm spatial resolution using femtosecond photoelectron diffraction. This technique allows imaging the molecules āfrom withinā by analyzing the diffraction of inner-shell photoelectrons that are created by femtosecond VUV and X-ray pulses. Using pump-probe schemes, ultrafast structural changes during photochemical reactions can thus be directly visualized with a temporal resolution that is only limited by the pulse durations of the pump and the probe pulse and the synchronization of the two light pulses. Here, we illustrate the principle of photoelectron diffraction using a simple, geometric scattering model and present results from photoelectron diffraction experiments on laser-aligned molecules using X-ray pulses from a Free-Electron Laser
Generation-free Agent-based Evolutionary Computing
AbstractMetaheuristics resulting from the hybridization of multi-agent systems with evolutionary computing are efficient in many optimization problems. Evolutionary multi-agent systems (EMAS) are more similar to biological evolution than classical evolutionary algorithms. However, technological limitations prevented the use of fully asynchronous agents in previous EMAS implementations. In this paper we present a new algorithm for agent-based evolutionary computations. The individuals are represented as fully autonomous and asynchronous agents. Evolutionary operations are performed continuously and no artificial generations need to be distinguished. Our results show that such asynchronous evolutionary operators and the resulting absence of explicit generations lead to significantly better results. An efficient implementation of this algorithm was possible through the use of Erlang technology, which natively supports lightweight processes and asynchronous communication
Diffraction effects in the Recoil-Frame Photoelectron Angular Distributions of Halomethanes
Citation: Bomme, C., Anielski, D., Savelyev, E., Boll, R., Erk, B., Bari, S., . . . Rolles, D. (2015). Diffraction effects in the Recoil-Frame Photoelectron Angular Distributions of Halomethanes. 635(11). doi:10.1088/1742-6596/635/11/112020We have measured the Recoil Frame-Photoelectron Angular Distributions (RF-PADs) for inner-shell photoionization of CH3F, CH3I and CF3I halomethane molecules for photoelectron energies up to 300 eV detected within a 4? solid angle in the gas-phase. For high kinetic energies, the RF-PADs are dominated by diffraction effects that encode information on the molecular geometry. Ā© Published under licence by IOP Publishing Ltd
Time-Resolved Measurement of Interatomic Coulombic Decay in Ne_2
The lifetime of interatomic Coulombic decay (ICD) [L. S. Cederbaum et al.,
Phys. Rev. Lett. 79, 4778 (1997)] in Ne_2 is determined via an extreme
ultraviolet pump-probe experiment at the Free-Electron Laser in Hamburg. The
pump pulse creates a 2s inner-shell vacancy in one of the two Ne atoms,
whereupon the ionized dimer undergoes ICD resulting in a repulsive
Ne^{+}(2p^{-1}) - Ne^{+}(2p^{-1}) state, which is probed with a second pulse,
removing a further electron. The yield of coincident Ne^{+} - Ne^{2+} pairs is
recorded as a function of the pump-probe delay, allowing us to deduce the ICD
lifetime of the Ne_{2}^{+}(2s^{-1}) state to be (150 +/- 50) fs in agreement
with quantum calculations.Comment: 5 pages, 3 figures, accepted by PRL on July 11th, 201
Coupled motion of Xe clusters and quantum vortices in He nanodroplets
Citation: Jones, C. F., Bernando, C., Tanyag, R. M. P., Bacellar, C., Ferguson, K. R., Gomez, L. F., . . . Vilesov, A. F. (2016). Coupled motion of Xe clusters and quantum vortices in He nanodroplets. Physical Review B - Condensed Matter and Materials Physics, 93(18). doi:10.1103/PhysRevB.93.180510Additional Authors: Erk, B.;Foucar, L.;Hartmann, R.;Neumark, D. M.;Epp, S. W.;Englert, L.;Siefermann, K. R.;Weise, F.;Rudek, B.;Sturm, F. P.;Ullrich, J.;Bostedt, C.;Gessner, O.;Vilesov, A. F.Single He nanodroplets doped with Xe atoms are studied via ultrafast coherent x-ray diffraction imaging. The diffraction images show that rotating He nanodroplets about 200 nm in diameter contain a small number of symmetrically arranged quantum vortices decorated with Xe clusters. Unexpected large distances of the vortices from the droplet center (?0.7-0.8 droplet radii) are explained by a significant contribution of the Xe dopants to the total angular momentum of the droplets and a stabilization of widely spaced vortex configurations by the trapped Xe clusters. Ā© 2016 American Physical Society
Imaging Molecular Structure through Femtosecond Photoelectron Diffraction on Aligned and Oriented Gas-Phase Molecules
This paper gives an account of our progress towards performing femtosecond
time-resolved photoelectron diffraction on gas-phase molecules in a pump-probe
setup combining optical lasers and an X-ray Free-Electron Laser. We present
results of two experiments aimed at measuring photoelectron angular
distributions of laser-aligned 1-ethynyl-4-fluorobenzene (C8H5F) and
dissociating, laseraligned 1,4-dibromobenzene (C6H4Br2) molecules and discuss
them in the larger context of photoelectron diffraction on gas-phase molecules.
We also show how the strong nanosecond laser pulse used for adiabatically
laser-aligning the molecules influences the measured electron and ion spectra
and angular distributions, and discuss how this may affect the outcome of
future time-resolved photoelectron diffraction experiments.Comment: 24 pages, 10 figures, Faraday Discussions 17
Communication: X-ray coherent diffractive imaging by immersion in nanodroplets
Citation: Tanyag, R. M. P., Bernando, C., Jones, C. F., Bacellar, C., Ferguson, K. R., Anielski, D., . . . Vilesov, A. F. (2015). Communication: X-ray coherent diffractive imaging by immersion in nanodroplets. Structural Dynamics, 2(5), 9. doi:10.1063/1.4933297Lensless x-ray microscopy requires the recovery of the phase of the radiation scattered from a specimen. Here, we demonstrate a de novo phase retrieval technique by encapsulating an object in a superfluid helium nanodroplet, which provides both a physical support and an approximate scattering phase for the iterative image reconstruction. The technique is robust, fast-converging, and yields the complex density of the immersed object. Images of xenon clusters embedded in superfluid helium droplets reveal transient configurations of quantum vortices in this fragile system. (C) 2015 Author(s). All article content, except where otherwise noted, is licensed under a Creative Commons Attribution 3.0 Unported License.Additional Authors: Neumark, D. M.;Rolles, D.;Rudek, B.;Rudenko, A.;Siefermann, K. R.;Ullrich, J.;Weise, F.;Bostedt, C.;Gessner, O.;Vilesov, A. F
towards time-resolved imaging of molecular structure
We demonstrate an experimental method to record snapshot diffraction images of
polyatomic gas-phase molecules, which can, in a next step, be used to probe
time-dependent changes in the molecular geometry during photochemical
reactions with femtosecond temporal and angstrom spatial resolution.
Adiabatically laser-aligned 1-ethynyl-4-fluorobenzene (C8H5F) molecules were
imaged by diffraction of photoelectrons with kinetic energies between 31 and
62 eV, created from core ionization of the fluorine (1s) level by ā80 fs x-ray
free-electron-laser pulses. Comparison of the experimental photoelectron
angular distributions with density functional theory calculations allows
relating the diffraction images to the molecular structure
Event-by-event mean pT fluctuations in pp and PbāPb collisions at the LHC
Event-by-event fluctuations of the mean transverse momentum of charged particles produced in pp collisions at ās = 0.9, 2.76 and 7 TeV, and PbāPb collisions at āsNN = 2.76 TeV are studied as a function of the chargedparticle multiplicity using the ALICE detector at the LHC. Dynamical fluctuations indicative of correlated particle emission are observed in all systems. The results in pp collisions show little dependence on collision energy. The Monte Carlo event generators PYTHIA and PHOJET are in qualitative agreement with the data. Peripheral PbāPb data exhibit a similar multiplicity dependence as that observed in pp. In central PbāPb, the results deviate from this trend, featuring a significant reduction of the fluctuation strength. The results in Pbā Pb are in qualitative agreement with previous measurements in AuāAu at lower collision energies and with expectations from models that incorporate collective phenomena
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