Laser-induced adiabatic alignment and mixed-field orientation of 2,6-difluoroiodobenzene (C6H3F2I) molecules are probed by Coulomb explosion imaging following either near-infrared strong-field ionization or extreme-ultraviolet multi-photon inner-shell ionization using free-electron laser pulses. The resulting photoelectrons and fragment ions are captured by a double-sided velocity map imaging spectrometer and projected onto two position-sensitive detectors. The ion side of the spectrometer is equipped with the Pixel Imaging Mass Spectrometry (PImMS) camera, a timestamping pixelated detector that can record the hit positions and arrival times of up to four ions per pixel per acquisition cycle. Thus, the time-of-flight trace and ion momentum distributions for all fragments can be recorded simultaneously. We show that we can obtain a high degree of one-and three-dimensional alignment and mixedfield orientation, and compare the Coulomb explosion process induced at both wavelengths.
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IntroductionUltrafast lasers provide opportunities to image molecular dynamics taking place on the femtosecond timescale [Baumert 1991, Zewail 2000, Chergui 2009. Table-top Ti:Sapphire laser systems are the most commonly used ultrafast laser systems, producing radiation in the near-infrared (NIR) range. High-intensity femtosecond NIR pulses can rapidly remove several valence electrons from a molecule, producing a multiply charged molecular ion that explodes due to the Coulomb repulsion between its components. The resulting recoil velocities and directions of the product ions depend on the position of the atoms in the molecule before ionization, and consequently can provide structural information about the molecule [Vager 1989, Stapelfeldt 1995, Posthumus 1996, Hishikawa 1998, Sanderson 1999. They can also be used to determine the orientation of molecules in the laboratory frame, for example, to probe the degree of molecular alignment induced by intense laser fields [Stapelfeldt 2003], or to probe structural changes of the molecule in time-resolved experiments [Legare 2005, Hishikawa 2007, Matsuda 2011, Bocharova 2011, Ibrahim 2014, Christensen 2014.Absorption of extreme ultraviolet (XUV) and soft X-ray photons can also induce Coulomb explosion when the resulting inner-shell ionization is followed by an Auger process that leads to a multiply charged molecular ion [Muramatsu 2002, Ueda 2005, Ullrich 2012, Erk 2014, Murphy 2014, Ablikim 2016, Ablikim 2017. Free-electron lasers (FELs) produce extremely intense (>10 12 photons/pulse) and ultrashort (few to few hundred fs) pulses of XUV and X-ray radiation [Ackermann 2007, Shintake 2008, Emma 2010, Allaria 2012, Ishikawa 2012, unlocking opportunities to probe ultrafast processes in gas-phase molecules through time-resolved Coulomb explosion imaging experiments [Johnsson 2009, Jiang 2010, Ullrich 2012, Schnorr 2013, Rouzee 2013, Erk 2014, Schnorr 2014, Fang 2014, Rudenko 2015, Liekhus 2015, Picon 2015, Lehmann 2016, Boll 2016. A good understanding of the Coulomb explosion of polyatomic...