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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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