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. © Published under licence by IOP Publishing Ltd

Nearest-Neighbor-Atom Core-Hole Transfer in Isolated Molecules

A new phenomenon sensitive only to next-door-neighbor atoms in isolated molecules is demonstrated using angle-resolved photoemission of site-selective core electrons. Evidence for this interatomic core-to-core electron interaction is observable only by measuring nondipolar angular distributions of photoelectrons. In essence, the phenomenon acts as a very fine atomic-scale sensor of nearest-neighbor elemental identity

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. © 2016 American Physical Society

Charge transfer in dissociating iodomethane and fluoromethane molecules ionized by intense femtosecond X-ray pulses

Citation: Boll, R., Erk, B., Coffee, R., Trippel, S., Kierspel, T., Bomme, C., . . . Rudenko, A. (2016). Charge transfer in dissociating iodomethane and fluoromethane molecules ionized by intense femtosecond X-ray pulses. Structural Dynamics, 3(4). doi:10.1063/1.4944344Additional Authors: Marchenko, T.;Miron, C.;Patanen, M.;Osipov, T.;Schorb, S.;Simon, M.;Swiggers, M.;Techert, S.;Ueda, K.;Bostedt, C.;Rolles, D.;Rudenko, A.Ultrafast electron transfer in dissociating iodomethane and fluoromethane molecules was studied at the Linac Coherent Light Source free-electron laser using an ultraviolet-pump, X-ray-probe scheme. The results for both molecules are discussed with respect to the nature of their UV excitation and different chemical properties. Signatures of long-distance intramolecular charge transfer are observed for both species, and a quantitative analysis of its distance dependence in iodomethane is carried out for charge states up to I21+. The reconstructed critical distances for electron transfer are in good agreement with a classical over-the-barrier model and with an earlier experiment employing a near-infrared pump pulse. © 2016 Author(s)

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

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

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

Coulomb explosion imaging of small organic molecules at LCLS.

Fragmentation of small organic molecules by intense few-femtosecond X-ray free-electron laser pulses has been studied using Coulomb explosion imaging. By measuring kinetic energies and emission angles of the ionic fragments in coincidence, we disentangle different fragmentation pathways, for certain cases can reconstruct molecular geometry at the moment of explosion, and show how it depends on LCLS pulse duration