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We report experimental results on x-ray diffraction of quantum-state-selected and strongly aligned ensembles of the prototypical asymmetric rotor molecule 2,5-diiodobenzonitrile using the Linac Coherent Light Source. The experiments demonstrate first steps toward a new approach to diffractive imaging of distinct structures of individual, isolated gas-phase molecules. We confirm several key ingredients of single molecule diffraction experiments: the abilities to detect and count individual scattered x-ray photons in single shot diffraction data, to deliver state-selected, e.g., structural-isomer-selected, ensembles of molecules to the x-ray interaction volume, and to strongly align the scattering molecules. Our approach, using ultrashort x-ray pulses, is suitable to study ultrafast dynamics of isolated molecules.

We report the breakdown of the electric dipole approximation in the long-wavelength limit in strong-field ionization with linearly polarized few-cycle mid-infrared laser pulses at intensities on the order of 10¹³ W/cm². Photoelectron momentum distributions were recorded by velocity map imaging and projected onto the beam propagation axis. We observe an increasing shift of the peak of this projection opposite to the beam propagation direction with increasing laser intensities. From a comparison with semiclassical simulations, we identify the combined action of the magnetic field of the laser pulse and the Coulomb potential as the origin of our observations.

We investigate experimentally the validity of proposed theories extending the tunneling approximation towards the multiphoton regime in strong-field ionization of helium. We employ elliptically polarized laser pulses and demonstrate how the influence of the ion potential on the released electron encoded in the measured observable provides the desired sensitivity to detect nonadiabatic effects in tunnel ionization. Our results show that for a large intensity range the proposed nonadiabatic theories contradict the experimental trends of the data, while adiabatic assumptions are confirmed.

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We explore ionization and rescattering in strong mid-infrared laser fields in the nondipole regime over the full range of polarization ellipticity. In three-dimensional photoelectron momentum distributions (3D PMDs) measured with velocity map imaging spectroscopy, we observe the appearance of a sharp ridge structure along the major polarization axis. Within a certain range of ellipticity, the electrons in this ridge are clearly separated from the two lobes that commonly appear in the PMD with elliptically polarized laser fields. In contrast to the well-known lobes of direct electrons, the sharp ridge is created by Coulomb focusing of the softly recolliding electrons. These ridge electrons are directly related to a counterintuitive shift of the PMD peak opposite to the laser beam propagation direction when the dipole approximation breaks down. The ellipticity-dependent 3D PMDs give access to different ionization and recollision dynamics with appropriate filters in the momentum space. For example, we can extract information about the spread of the initial wave packet and the Coulomb momentum transfer of the rescattering electrons.

The 3D photoelectron momentum distributions created by the strong-field ionization of argon atoms and naphthalene molecules with intense, large ellipticity (∼0.7) femtosecond laser pulses are studied. The experiment reveals the presence of low-energy electrons for randomly oriented naphthalene, but not for argon. Our theory shows that the induced dipole part of the cationic potential facilitates the creation of the low-energy electrons. We establish the conditions in terms of laser pulse parameters and molecular properties for which this type of low-energy electrons can be observed and point to applications thereof.