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We theoretically study the effects of Rabi oscillations on resonant x-ray scattering in Ne$^+$ using intense attosecond and few-femtosecond pulses. The total photon yield strongly depends on the pulse area and has an upper bound at high intensities. Resonant scattering yields with attosecond pulses can be an order of magnitude higher than those far from resonances. Interference between resonant fluorescence and elastic scattering channels depends on the pulse area and initial state. Our results suggest that resonant x-ray scattering can be exploited for high-resolution, site-specific imaging., Comment: 7 pages, 5 figures

We present a time-dependent Schr\"odinger equation (TDSE) approach within a non-relativistic quantum electrodynamics (QED) framework to investigate resonant x-ray scattering under intense x-ray pulses. This method enables us to explore how coherent x-ray electron dynamics affect scattering signals from Ne$^+$. We account for both resonant fluorescence and elastic scattering channels, while also considering competing photoionization and inner-shell decay processes. By computing the angular distribution and energy spectrum of scattered photons, we uncover the interference effects between elastic scattering and resonant fluorescence pathways. Notably, our results reveal a small asymmetry in the energy spectrum as a result of this interference. We discuss the experimental potential for detecting signatures of interference. Our findings demonstrate that the x-ray Rabi dynamics can be used to control scattering responses and offer new insights into interference mechanisms and scattering efficiency in high-intensity x-ray regimes., Comment: 17 pages, 9 Figures

The fragmentation of molecular cations following inner-shell decay processes in molecules containing heavy elements underpins the x-ray damage effects observed in x-ray scattering measurements of biological and chemical materials, as well as in medical applications involving Auger-electron emitting radionuclides. Traditionally, these processes are modeled using simulations that describe the electronic structure at an atomic level, thereby omitting molecular bonding effects. This work addresses the gap by introducing a novel approach that couples a decay spawning dynamics algorithm with ab initio molecular dynamics simulations to characterize ultrafast dynamics on the potential energy surfaces. We apply our method to a model decay cascade following K-shell ionization of IBr and subsequent K\b{eta} fluorescence decay. We examine two competing channels that undergo two decay steps, resulting in ion pairs with a total +3 charge state. This approach provides a continuous description of the electron transfer dynamics occurring during the multi-step decay cascade and molecular fragmentation, revealing the combined inner-shell decay and charge transfer timescale to be approximately 75 fs. Our computed kinetic energies of ion fragments show good agreement with experimental data.

Characterization of the inner-shell decay processes in molecules containing heavy elements is key to understanding x-ray damage of molecules and materials and for medical applications with Auger-electron-emitting radionuclides. The 1s hole states of heavy atoms can be produced by absorption of tunable x-rays and the resulting vacancy decays characterized by recording emitted photons, electrons, and ions. The 1s hole states in heavy elements have large x-ray fluorescence yields that transfer the hole to intermediate electron shells that then decay by sequential Auger-electron transitions that increase the ion's charge state until the final state is reached. In molecules the charge is spread across the atomic sites, resulting in dissociation to energetic atomic ions. We have used x-ray/ion coincidence spectroscopy to measure charge states and energies of I$^{q+}$ and Br$^{q'+}$ atomic ions following 1s ionization at the I and Br \textit{K}-edges of IBr. We present the charge states and kinetic energies of the two correlated fragment ions associated with core-excited states produced during the various steps of the cascades. To understand the dynamics leading to the ion data, we develop a computational model that combines Monte-Carlo/Molecular Dynamics simulations with a classical over-the-barrier model to track inner-shell cascades and redistribution of electrons in valence orbitals and nuclear motion of fragments.

Intense few-to-sub-femtosecond soft x-ray pulses can produce neutral, two-site excited double-core-hole states by promoting two core electrons to the same unoccupied molecular orbital. We theoretically investigate double nitrogen K-edge excitations of nitrous oxide (N2O) with multiconfigurational electronic structure calculations. We show that the second core-excitation energy is reduced with respect to its ground state value. A site-selective double core-excitation mechanism using intense few-femtosecond x-rays is investigated using time-dependent Schrodinger equation (TDSE) simulations. The subsequent two-step Auger-Meitner and two-electrons-one-electron decay spectra of the double core-excited states are analyzed using a Mulliken population analysis of the multiconfirational wavefunctions. The change in the electron emission lineshape between the absorption of 1 or 2 photons in the resonant core-excitation is predicted by combining this approach with the TDSE simulations. We examine the possibility of resolving the double core-excited states with x-ray pump-probe techniques by calculating the chemical shifts of the core-electron binding energy of the core-excited states and decay products., Comment: 12 pages, 5 figures

Diffraction-before-destruction imaging with single ultrashort X-ray pulses has the potential to visualise non-equilibrium processes, such as chemical reactions, at the nanoscale with sub-femtosecond resolution in the native environment without the need of crystallization. Here, a nanospecimen partially diffracts a single X-ray flash before sample damage occurs. The structural information of the sample can be reconstructed from the coherent X-ray interference image. State-of-art spatial resolution of such snapshots from individual heavy element nanoparticles is limited to a few nanometers. Further improvement of spatial resolution requires higher image brightness which is ultimately limited by bleaching effects of the sample. We compared snapshots from individual 100 nm Xe nanoparticles as a function of the X-ray pulse duration and incoming X-ray intensity in the vicinity of the Xe M-shell resonance. Surprisingly, images recorded with few femtosecond and sub-femtosecond pulses are up to 10 times brighter than the static linear model predicts. Our Monte-Carlo simulation and statistical analysis of the entire data set confirms these findings and attributes the effect to transient resonances. Our simulation suggests that ultrafast form factor changes during the exposure can increase the brightness of X-ray images by several orders of magnitude. Our study guides the way towards imaging with unprecedented combination of spatial and temporal resolution at the nanoscale.

We theoretically investigate the fluorescence intensity correlation (FIC) of Ar clusters and Mo-doped iron oxide nanoparticles subjected to intense, femtosecond and sub-femtosecond XFEL pulses for high-resolution and elemental contrast imaging. We present the FIC of {\Ka} and {\Kah} emission in Ar clusters and discuss the impact of sample damage on retrieving high-resolution structural information and compare the obtained structural information with those from the coherent difractive imaging (CDI) approach. We found that, while sub-femtosecond pulses will substantially benefit the CDI approach, few-femtosecond pulses may be sufficient for achieving high-resolution information with FIC. Furthermore, we show that the fluorescence intensity correlation computed from the fluorescence of Mo atoms in Mo-doped iron oxide nanoparticles can be used to image dopant distributions.

We examine x-ray scattering from an isolated organic molecule from the linear to nonlinear absorptiveregime. In the nonlinear regime, we explore the importance of both the elastic and inelastic channelsand observe the onset of nonlinear behavior as a function of pulse duration and energy. In the linearregime, we test the sensitivity of the scattering signal to molecular bonding and electronic correlationvia calculations using the independent atom model (IAM), Hartree-Fock (HF) and density functionaltheory (DFT). Finally, we describe how coherent x-ray scattering can be used to directly visualizefemtosecond charge transfer and dissociation within a single molecule undergoing x-ray multiphotonabsorption.

We present a theoretical study of temporal, spectral, and spatial reshaping of intense, ultrafast x-ray pulses propagating through a resonant medium. Our calculations are based on the solution of a 3D time-dependent Schr\"odinger-Maxwell equation, with the incident x-ray photon energy on resonance with the core-level 1s-3p transition in neon. We study the evolution of the combined incident and medium-generated field, including the effects of stimulated emission, absorption, ionization and Auger decay, as a function of the input pulse energy and duration. We find that stimulated Raman scattering between core-excited states $1s^{-1}3p$ and $2p^{-1}3p$ occurs at high x-ray intensity, and that the emission around this frequency is strongly enhanced when also including the similar $1s^{-1}-2p^{-1}$ response of the ion. We also explore the dependence of x-ray self-induced transparency (SIT) and self-focusing on the pulse intensity and duration, and we find that the stimulated Raman scattering plays an important role in both effects. Finally, we discuss how these nonlinear effects may potentially be exploited as control parameters for pulse properties of x-ray free-electron laser sources., Comment: 14 pages, 11 figures

We have unveiled coherent multiphoton interferences originating from different quantum paths taken by the Auger electron induced by a high-intensity x-ray/XUV pulse under the presence of a strong optical field. These interferences give rise to a clear signature in the angle-resolved Auger electron spectrum: an asymmetry with respect to the energy of the Auger decay channel. In order to illustrate this effect we have considered the resonant Auger decay of the transition $2p^{5} \!\leftrightarrow\! 1s^{-1}2p^{6}$ in Ne$^{+}$. The simulations show that these interferences are very sensitive to the parameters of the x-ray and optical fields.

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, 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., Comment: 4 pages, 4 figures, accepted by Physical Review Letters

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 Schr\"odinger equation for each rotational state initially populated in a thermal ensemble. Using a phase-retrieval algorithm, the feasibility of structure reconstruction from a quasi-adiabatically-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^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 \AA., Comment: 18 pages, 9 figures, accepted by Physical Review A

Exploration of a new ultrafast-ultrasmall frontier in atomic and molecular physics has begun. Not only is is possible to control outer-shell electron dynamics with intense ultrafast optical lasers, but now control of inner-shell processes has become possible by combining intense infrared/optical lasers with tunable sources of x-ray radiation. This marriage of strong-field laser and x-ray physics has led to the discovery of methods to control reversibly resonant x-ray absorption in atoms and molecules on ultrafast timescales. Using a strong optical dressing field, resonant x-ray absorption in atoms can be markedly suppressed, yielding an example of electromagnetically induced transparency for x rays. Resonant x-ray absorption can also be controlled in molecules using strong non-resonant, polarized laser fields to align the framework of a molecule, and therefore its unoccupied molecular orbitals to which resonant absorption occurs. At higher laser intensities, ultrafast field ionization produces an irreversible change in x-ray absorption. Finally, the advent of x-ray free electron lasers enables first exploration of non-linear x-ray processes., Comment: 8 pages, 11 figures, RevTeX4, submitted to Revista Mexicana de Fisica

In a fully classical simulation, we investigate the recollision mechanism of non-sequential double ionization (NSDI) and its manifestation in the end-of-pulse electron momentum distributions. We compare two different electron-electron potentials: a soft-core Coulombic potential and a Yukawa potential. We also implement the strong-field approximation (SFA), which is commonly made in quantum-mechanical $S$-matrix calculations, in our classical simulations and study its consequences. We find that, regardless of the form of the e-e potential, the SFA modifies the momentum distributions and recollision dynamics significantly, but more so for the long-range than for the short-range e-e interaction. Surprisingly, our classical results, especially those obtained with the Yukawa potential under the SFA, agree well with the results from the $S$-matrix calculations with a contact e-e interaction. This implies that the recollision dynamics initiated by a quantum tunneling process and a purely classical process do not deviate much from each other. Furthermore, our classical predictions of travel times are consistent with the results from the simple-man model, and the most probable thermalization time is found to be within 0.15 and 0.25 laser periods., Comment: 10 pages, 10 figures

We describe first-principles in-plane calculations of non-sequential triple ionization (NSTI) 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 780nm laser pulse. Nonsequential ejection is shown to occur in a multi-electron, possibly multi-cycle and multi-dimensional, rescattering sequence that is coordinated by a number of sharp transverse recollimation impacts., Comment: 4 pages, 4 figures

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 $10^{14}-10^{16} W/cm^2$ 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.

We provide a basis for the laser intensity dependence of the momentum distributions of electrons and ions arising from strong-field non-sequential double ionization (NSDI) at intensities in the range $I=1-6.5 \times 10^{14} W/cm^2$. To do this we use a completely classical method introduced previously \cite{ho-etal05}. Our calculated results reproduce the features of experimental observations at different laser intensities and depend on just two distinct categories of electon trajectories., Comment: 5 pages, 7 figures

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