Attosecond imaging of molecules using high harmonic spectroscopy

The availability of attosecond-duration extreme ultraviolet or soft X-ray light sources has opened up new fields of research in atomic and molecular physics. These pulses can be as short as 50 as, fast enough to freeze the motion of electrons within molecules, to resolve how electrons rearrange themselves after the removal of an electron and to study electron–electron correlations. Gas-phase molecules can be aligned in space using short laser pulses, permitting the measurement of molecular parameters in the molecular frame. Aligned molecules can be photoionized using a train of attosecond pulses, enabling the complete characterization of the partial waves making up the photoelectron angular distributions. Using a recolliding electron in the high harmonic process allows complex transition dipole matrix elements to be recorded (including their amplitude and phase) in the molecular frame. High harmonic spectroscopy makes it possible to image molecular orbitals and for unimolecular chemical reactions to be followed with femtosecond resolution. For example, the behaviour around conical intersections can be probed. Charge migration within molecules can be observed with sub-femtosecond resolution.