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A photofragmentation study of gas-phase indole (C8H7N) upon single-photon ionization at a photon energy of 420 eV is presented. Indole was primarily inner-shell ionized at its nitrogen and carbon 1s orbitals. Electrons and ions were measured in coincidence by means of velocity map imaging. The angular relationship between ionic fragments is discussed along with the possibility to use the angle-resolved coincidence detection to perform experiments on molecules that are strongly oriented in their recoil-frame. The coincident measurement of electrons and ions revealed fragmentation-pathway-dependent electron spectra, linking the structural fragmentation dynamics to different electronic excitations. Evidence for photoelectron-impact self-ionization was observed.

We have developed and experimentally demonstrated an improved electrostatic deflector for the spatial separation of molecules according to their dipole-moment-to-mass ratio. The device features a very open structure that allows for significantly stronger electric fields as well as for stronger deflection without molecules crashing into the device itself. We have demonstrated its performance using the prototypical carbonyl sulfide molecule and we discuss opportunities regarding improved quantum-state-selectivity for complex molecules and the deflection of unpolar molecules.

A strong adiabatic mixed-field orientation (N up /N tot =0.882) of carbonyl sulfide (OCS) molecules in their absolute ground state is experimentally demonstrated. OCS is oriented in a combination of nonresonant laser and static electric fields inside a two-plate velocity map imaging spectrometer. The transition from nonadiabatic to adiabatic orientation for the rotational ground state is studied by varying the applied laser intensity and static electric field. Above static electric field strengths of 10 kV cm -1 and laser intensities of 10 11  W cm -2 the observed degree of orientation reaches a plateau. These results are in good agreement with computational solutions of the time-dependent Schrödinger equation., (© 2016 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.)

We demonstrate strong laser-field-free orientation of absolute-ground-state carbonyl sulfide molecules. The molecules are oriented by the combination of a 485-ps-long nonresonant laser pulse and a weak static electric field. The edges of the laser pulse create a coherent superposition of two rotational states resulting in revivals of strong transient molecular orientation after the laser pulse. The experimentally attained degree of orientation ⟨cosθ⟩≈0.6 corresponds to the theoretical maximum for mixing of the two states. Switching off the dc field would provide the same orientation completely field free.

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 (C(8)H(5)F) and dissociating, laser-aligned 1,4-dibromobenzene (C(6)H(4)Br(2)) 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.