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We report experimental results on the diffractive imaging of three-dimensionally aligned 2,5-diiodothiophene molecules. The molecules were aligned by chirped near-infrared laser pulses, and their structure was probed at a photon energy of 9.5 keV (λ ≈ 130 pm) provided by the Linac Coherent Light Source. Diffracted photons were recorded on the Cornell-SLAC pixel array detector, and a two-dimensional diffraction pattern of the equilibrium structure of 2,5-diiodothiophene was recorded. The retrieved distance between the two iodine atoms agrees with the quantum-chemically calculated molecular structure to be within 5%. The experimental approach allows for the imaging of intrinsic molecular dynamics in the molecular frame, albeit this requires more experimental data, which should be readily available at upcoming high-repetition-rate facilities.

Strong-field ionization of carbonyl sulphide (OCS) molecules, induced by a linearly polarized mid-infrared (mid-IR) probe laser pulse is investigated experimentally and theoretically. We focus on the dependence of the single-ionization yield on the alignment of the molecular axis with respect to the probe pulse polarization axis. In the experiment, the OCS molecules are 1-dimensionally adiabatically aligned and ionized by a 12-femtosecond pulse centered at 1850 nm. The alignment-dependent ionization yields are compared to the theory based on the two-step model for strong-field ionization. Overall the measurements are consistent with the theoretical results.

We report a quantitative study of the effect of nonaxial recoil during Coulomb explosion of laser-aligned molecules and introduce a method to remove the blurring caused by nonaxial recoil in the fragment-ion angular distributions. Simulations show that nonaxial recoil affects correlations between the emission directions of fragment ions differently from the effect caused by imperfect molecular alignment. The method, based on analysis of the correlation between the emission directions of the fragment ions from Coulomb explosion, is used to deconvolute the effect of nonaxial recoil from experimental fragment angular distributions. The deconvolution method is then applied to a number of experimental data sets to correct the degree of alignment for nonaxial recoil, to select optimal Coulomb explosion channels for probing molecular alignment, and to estimate the highest degree of alignment that can be observed from selected Coulomb explosion channels.

We apply a three-fold covariance imaging method to analyse previously acquired data [C. S. Slater et al., Phys. Rev. A 89, 011401(R) (2014)] on the femtosecond laser-induced Coulomb explosion of spatially pre-aligned 3,5-dibromo-3′,5′-difluoro-4′-cyanobiphenyl molecules. The data were acquired using the “Pixel Imaging Mass Spectrometry” camera. We show how three-fold covariance imaging of ionic photofragment recoil trajectories can be used to provide new information about the parent ion’s molecular structure prior to its Coulomb explosion. In particular, we show how the analysis may be used to obtain information about molecular conformation and provide an alternative route for enantiomer determination.

Coulomb explosion of 1,4--diiodobenzene molecules, isolated or embedded in helium nanodroplets, is induced by irradiation with an intense femtosecond laser pulse. The recoiling ion fragments are probed by time-of-flight measurements and two-dimensional velocity map imaging. Correlation analysis of the emission directions of ${\mathrm{I}}^{+}$ ions recoiling from each end of the molecules reveals significant deviation from axial recoil, i.e., where the ${\mathrm{I}}^{+}$ ions leave strictly along the I-I symmetry axis. For isolated molecules, the relative angular distribution of the ${\mathrm{I}}^{+}$ ions is centered at ${180}^{\ensuremath{\circ}}$, corresponding to perfect axial recoil, but with a full width at half maximum of ${30}^{\ensuremath{\circ}}$. For molecules inside He droplets, the width of the distribution increases to ${45}^{\ensuremath{\circ}}$. These results provide a direct measure of the accuracy of Coulomb explosion as a probe of the spatial orientation of molecules, which is particularly relevant in connection with laser-induced molecular alignment and orientation. In addition, our studies show how it is possible to identify fragmentation pathways of the Coulomb explosion for the isolated 1,4--diiodobenzene molecules. Finally, for the 1,4--diiodobenzene molecules in He droplets, it is shown that the angular correlation between fragments from the Coulomb explosion is preserved after they have interacted with the He environment.

The absolute configuration of chiral molecules in the gas phase is determined by femtosecond laser-induced Coulomb explosion and recording of the emission direction of critical ionic fragments. The spatial orientation of the 3,5-dibromo-3′,5′-diflouro-4′-cyanobiphenyl molecules studied is determined by a combination of laser-induced alignment and time-of-flight measurement of F+ ion recoils. Hereby, the enatiomeric state of the molecules could be uniquely identified through analysis of the correlation of the angular distribution of F+ and Br+ ions. The method will apply to a range of molecules and allow imaging of chiral changes on ultrafast time scales.

The torsional motion of a molecule composed of two substituted benzene rings, linked by a single bond, is coherently controlled by a pair of strong ($3\ifmmode\times\else\texttimes\fi{}1{0}^{13}\text{ }\text{ }\mathrm{W}\text{ }{\mathrm{cm}}^{\ensuremath{-}2}$), nonresonant (800 nm) 200-fs-long laser pulses---both linearly polarized perpendicular to the single-bond axis. If the second pulse is sent at the time when the two benzene rings rotate toward (away from) each other the amplitude of the torsion is strongly enhanced (reduced). The torsional motion persists for more than 150 ps corresponding to approximately 120 torsional oscillations. Our calculations show that the key to control is the strong transient modification of the natural torsional potential by the laser-induced dynamic Stark effect.

Naphthalene molecules are fixed in space by a laser field and rotated, in 2\ifmmode^\circ\else\textdegree\fi{} steps, over 180\ifmmode^\circ\else\textdegree\fi{}. For each orientation, they are ionized by an intense, circularly polarized femtosecond laser pulse, and the 2D projection of the photoelectron momentum distribution is recorded. The molecular-frame 3D momentum distribution is obtained by tomographic reconstruction from all 90 projections. It reveals an anisotropic electron distribution, angularly shifted in the polarization plane, that is not accessible by the 2D momentum images. Our theoretical analysis shows that the magnitude of the angular shift is very sensitive to the exact form of the laser-modified molecular potential.

We demonstrate a novel experimental implementation to strongly align molecules at full repetition rates of free-electron lasers. We utilized the available in-house laser system at the coherent x-ray imaging beamline at the Linac Coherent Light Source. Chirped laser pulses, i. e., the direct output from the regenerative amplifier of the Ti:Sa chirped pulse amplification laser system, were used to strongly align 2,5-diiodothiophene molecules in a molecular beam. The alignment laser pulses had pulse energies of a few mJ and a pulse duration of 94 ps. A degree of alignment of $\left$ = 0.85 was measured, limited by the intrinsic temperature of the molecular beam rather than by the available laser system. With the general availability of synchronized chirped-pulse-amplified near-infrared laser systems at short-wavelength laser facilities, our approach allows for the universal preparation of molecules tightly fixed in space for experiments with x-ray pulses., Comment: 10 pages, 5 figures