Phay Ho

Nonsequential double ionization as a completely classical photoelectric effect.

We introduce a unified and simplified theory of atomic double ionization. Our results show that at high laser intensities (I>/=10(14) W/cm(2)) purely classical correlation is strong enough to account for all of the main features observed in experiments to date.

Observing the creation of electronic feshbach resonances in soft x-ray-induced O2 dissociation.

When an atom or molecule is ionized by an x-ray, highly excited states can be created that then decay, or autoionize, by ejecting a second electron from the ion. We found that autoionization after soft x-ray photoionization of molecular oxygen follows a complex multistep process. By interrupting the autoionization process with a short laser pulse, we showed that autoionization cannot occur until the internuclear separation of the fragments is greater than approximately 30 angstroms. As the ion and excited neutral atom separated, we directly observed the transformation of electronically bound states of the molecular ion into Feshbach resonances of the neutral oxygen atom that are characterized by both positive and negative binding energies. States with negative binding energies have not previously been predicted or observed in neutral atoms.

Decoherence in Attosecond Photoionization

The creation of superpositions of hole states via single-photon ionization using attosecond extreme-ultraviolet pulses is studied with the time-dependent configuration-interaction singles (TDCIS) method. Specifically, the degree of coherence between hole states in atomic xenon is investigated. We find that interchannel coupling not only affects the hole populations, but it also enhances the entanglement between the photoelectron and the remaining ion, thereby reducing the coherence within the ion. As a consequence, even if the spectral bandwidth of the ionizing pulse exceeds the energy splittings among the hole states involved, perfectly coherent hole wave packets cannot be formed. For sufficiently large spectral bandwidth, the coherence can only be increased by increasing the mean photon energy.

Molecular structure determination from x-ray scattering patterns of laser-aligned symmetric-top molecules.

We investigate the molecular structure information contained in the x-ray diffraction patterns of an ensemble of rigid CF(3)Br molecules aligned by an intense laser pulse at finite rotational temperature. The diffraction patterns are calculated at an x-ray photon energy of 20 keV to probe molecular structure at angstrom-scale resolution. We find that a structural reconstruction algorithm based on iterative phase retrieval fails to extract a reliable structure. However, the high atomic number of Br compared with C or F allows each diffraction pattern to be treated as a hologram. Using this approach, the azimuthal projection of the molecular electron density about the alignment axis may be retrieved.

Hetero-site-specific X-ray pump-probe spectroscopy for femtosecond intramolecular dynamics

New capabilities at X-ray free-electron laser facilities allow the generation of two-colour femtosecond X-ray pulses, opening the possibility of performing ultrafast studies of X-ray-induced phenomena. Particularly, the experimental realization of hetero-site-specific X-ray-pump/X-ray-probe spectroscopy is of special interest, in which an X-ray pump pulse is absorbed at one site within a molecule and an X-ray probe pulse follows the X-ray-induced dynamics at another site within the same molecule. Here we show experimental evidence of a hetero-site pump-probe signal. By using two-colour 10-fs X-ray pulses, we are able to observe the femtosecond time dependence for the formation of F ions during the fragmentation of XeF2 molecules following X-ray absorption at the Xe site.

In-Plane Theory of Nonsequential Triple Ionization

We describe first-principles in-plane calculations of nonsequential triple ionization of atoms in a linearly polarized intense laser pulse. In a fully classically correlated description, all three electrons respond dynamically to the nuclear attraction, the pairwise e-e repulsions, and the laser force throughout the duration of a 780 nm laser pulse. Nonsequential ejection is shown to occur in a multielectron, possibly multicycle and multidimensional, rescattering sequence that is coordinated by a number of sharp transverse recollimation impacts.

Computational studies of x-ray scattering from three-dimensionally-aligned asymmetric-top molecules.

We theoretically and numerically analyze x-ray scattering from asymmetric-top molecules three-dimensionally aligned using elliptically polarized laser light. A rigid-rotor model is assumed. The principal axes of the polarizability tensor are assumed to coincide with the principal axes of the moment of inertia tensor. Several symmetries in the Hamiltonian are identified and exploited to enhance the efficiency of solving the time-dependent Schroedinger equation for each rotational state initially populated in a thermal ensemble. Using a phase-retrieval algorithm, the feasibility of structure reconstruction from a quasiadiabatically aligned sample is illustrated for the organic molecule naphthalene. The spatial resolution achievable strongly depends on the laser parameters, the initial rotational temperature, and the x-ray pulse duration. We demonstrate that for a laser peak intensity of 5 TW/cm{sup 2}, a laser pulse duration of 100 ps, a rotational temperature of 10 mK, and an x-ray pulse duration of 1 ps, the molecular structure may be probed at a resolution of 1 A ring .

Classical effects of laser pulse duration on strong-field double ionization

We use classical electron ensembles and the aligned-electron approximation to examine the effect of laser pulse duration on the dynamics of strong-field double ionization. We cover the range of intensities 10(14)-10(16) W/cm2 for the laser wavelength 780 nm. The classical scenario suggests that the highest rate of recollision occurs early in the pulse and promotes double-ionization production in few-cycle pulses. In addition, the purely classical ensemble calculation predicts an exponentially decreasing recollision rate with each subsequent half cycle. We confirm the exponential behavior by trajectory back analysis.

Ultrafast x-ray-induced nuclear dynamics in diatomic molecules using femtosecond x-ray-pump-x-ray-probe spectroscopy

Citation: Lehmann, C. S., Picon, A., Bostedt, C., Rudenko, A., Marinelli, A., Moonshiram, D., . . . Southworth, S. H. (2016). Ultrafast x-ray-induced nuclear dynamics in diatomic molecules using femtosecond x-ray-pump-x-ray-probe spectroscopy. Physical Review A, 94(1), 7. doi:10.1103/PhysRevA.94.013426

Field-free molecular alignment for studies using x-ray pulses from a synchrotron radiation source

A short, intense laser pulse may be employed to create a spatially aligned molecular sample that persists after the laser pulse is over. We theoretically investigate whether this impulsive molecular alignment technique may be exploited for experiments using x-ray pulses from a third-generation synchrotron radiation facility. Using a linear rigid rotor model, the alignment dynamics of model molecular systems with systematically increasing size is calculated utilizing both a quantum density matrix formalism and a classical ensemble method. For each system, the alignment dynamics obtained for a 95 ps laser is compared with that obtained for a 10 ps laser pulse. The average degree of alignment after the laser pulse, as calculated quantum mechanically, increases with the size of the molecule. This effect is quantitatively reproduced by the classical calculations. The average degree of impulsive alignment is high enough to induce a pronounced linear dichroism in resonant x-ray absorption using the intense 100 ps x-ray pulses currently available. However, for structural studies based on elastic x-ray scattering, bright x-ray pulses with a duration of 1 ps or shorter will be required in order to make full use of impulsive molecular alignment.