Time-resolved holography with photoelectrons.
ABSTRACT Ionization is the dominant response of atoms and molecules to intense laser fields and is at the basis of several important techniques, such as the generation of attosecond pulses that allow the measurement of electron motion in real time. We present experiments in which metastable xenon atoms were ionized with intense 7-micrometer laser pulses from a free-electron laser. Holographic structures were observed that record underlying electron dynamics on a sublaser-cycle time scale, enabling photoelectron spectroscopy with a time resolution of almost two orders of magnitude higher than the duration of the ionizing pulse.
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ABSTRACT: We present ab initio numerical study of ultrafast ionization dynamics of H 2 + as well as CO2 and N2 exposed to linearly polarized attosecond extreme ultraviolet pulses. When the molecules are aligned perpendicular to laser polarization direction, photonionization of these molecules show clear and distinguishing diffraction patterns in molecular attosecond photoelectron momentum distributions. The internuclear distances of the molecules are related to the position of the associated diffraction patterns, which can be determined with high accuracy. Moreover, the relative heights of the diffraction fringes contain fruitful information of the molecular orbital structures. We show that the diffraction spectra can be well produced using the two-center interference model. By adopting a simple inversion algorithm which takes into account the symmetry of the initial molecular orbital, we can retrieve the molecular orbital from which the electron is ionized. Our results offer possibility for imaging of molecular structure and orbitals by performing molecular attosecond photoelectron diffraction.Optics Express 04/2015; 23(8). DOI:10.1364/OE.23.010687 · 3.53 Impact Factor
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ABSTRACT: Strong-field ionization provides fundamental insight into light-matter interactions, encoding the structure of atoms and molecules on the subångström and subfemtosecond scales. In this Rapid Communication, we explore an important regime: strong-field ionization by two-color circularly polarized laser fields. In contrast to past work using linearly polarized drivers, we probe electron trajectories that are driven in a two-dimensional plane, thus separating the tunneling angle from the rescattering angle. This allows us to make several findings. First, we observe a single-lobed electron distribution for co-rotating fields, and a three-lobed distribution for counter-rotating fields, providing experimental validation of the theoretical model explaining the generation of circularly polarized high harmonic light. Second, we discover that there is significant electron-ion rescattering using counter-rotating fields, but not with co-rotating fields. Finally, we show that the rescattered electrons are well separated from the directly ionized electrons, in striking contrast to similar low-energy structures seen with linearly polarized fields. These findings help overcome the long-standing problem of how to decouple the tunneling and rescattering steps in strong-field ionization, which will enable new dynamic probes of atomic and molecular structure.Physical Review A 03/2015; 91:031402(R). DOI:10.1103/PhysRevA.91.031402 · 2.99 Impact Factor
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ABSTRACT: Photoelectron interferograms, manifested in photoelectron angular distributions (PADs), are a high-information, coherent observable. In order to obtain the maximum information from angle-resolved photoionization experiments it is desirable to record the full, 3D, photoelectron momentum distribution. Here we apply tomographic reconstruction techniques to obtain such 3D distributions from multiphoton ionization of potassium atoms, and fully analyse the energy and angular content of the 3D data. The PADs obtained as a function of energy indicate good agreement with previous 2D data and detailed analysis [Hockett et. al., Phys. Rev. Lett. 112, 223001 (2014)] over the main spectral features, but also indicate unexpected symmetry-breaking in certain regions of momentum space, thus revealing additional continuum interferences which cannot otherwise be observed. These observations reflect the presence of additional ionization pathways and, most generally, illustrate the power of maximum information measurements of this coherent observable.