Christian Buth

Double Core-Hole Production in N2: Beating the Auger Clock

We investigate the creation of double K-shell holes in N2 molecules via sequential absorption of two photons on a time scale shorter than the core-hole lifetime by using intense x-ray pulses from the Linac Coherent Light Source free electron laser. The production and decay of these states is characterized by photoelectron spectroscopy and Auger electron spectroscopy. In molecules, two types of double core holes are expected, the first with two core holes on the same N atom, and the second with one core hole on each N atom. We report the first direct observations of the former type of core hole in a molecule, in good agreement with theory, and provide an experimental upper bound for the relative contribution of the latter type.

Quantum state-resolved probing of strong-field-ionized xenon atoms using femtosecond high-order harmonic transient absorption spectroscopy.

Femtosecond high-order harmonic transient absorption spectroscopy is used to resolve the complete |j,m quantum state distribution of Xe+ produced by optical strong-field ionization of Xe atoms at 800 nm. Probing at the Xe N4/5 edge yields a population distribution rhoj,|m| of rho3/2,1/2ratiorho1/2,1/2ratiorho3/2,3/2=75+/-6 :12+/-3 :13+/-6%. The result is compared to a tunnel ionization calculation with the inclusion of spin-orbit coupling, revealing nonadiabatic ionization behavior. The sub-50-fs time resolution paves the way for tabletop extreme ultraviolet absorption probing of ultrafast dynamics.

Molecular double core-hole electron spectroscopy for chemical analysis

We explore the potential of double core hole electron spectroscopy for chemical analysis in terms of x-ray two-photon photoelectron spectroscopy. The creation of deep single and double core vacancies induces significant reorganization of valence electrons. The corresponding relaxation energies and the interatomic relaxation energies are evaluated by complete active space self-consistent field (CASSCF) calculations. We propose a method on how to experimentally extract these quantities by the measurement of single ionization potentials (IPs) and double core hole ionization potentials (DIPs). The influence of the chemical environment on these DIPs is also discussed for states with two holes at the same atomic site and states with two holes at two different atomic sites. Electron density difference between the ground and double core hole states clearly shows the relaxations accompanying the double core hole ionization. The effect is also compared to the sensitivity of single core hole IPs arising in single co...

Phase Measurement of Resonant Two-Photon Ionization in Helium

We study resonant two-color two-photon ionization of helium via the 1s3p (1)P(1) state. The first color is the 15th harmonic of a tunable Ti:sapphire laser, while the second color is the fundamental laser radiation. Our method uses phase-locked high-order harmonics to determine the phase of the two-photon process by interferometry. The measurement of the two-photon ionization phase variation as a function of detuning from the resonance and intensity of the dressing field allows us to determine the intensity dependence of the transition energy.

Electromagnetically induced transparency for X rays

Electromagnetically induced transparency is predicted for x rays in laser-dressed neon gas. The x-ray photoabsorption cross section and polarizability near the Ne K edge are calculated using an ab initio theory suitable for optical strong-field problems. The laser wavelength is tuned close to the transition between 1s(-1)3s and 1s(-1)3p approximately 800 nm). The minimum laser intensity required to observe electromagnetically induced transparency is of the order of 10(12) W/cm(2). The ab initio results are discussed in terms of an exactly solvable three-level model. This work opens new opportunities for research with ultrafast x-ray sources.

X-ray quantum optics

Quantum optics with X-rays has long been a somewhat exotic activity, but it is now rapidly becoming relevant as precision x-ray optics and novel X-ray light sources, and high-intensity lasers are becoming available. This article gives an overview of the current state of the field and an outlook to future prospects.

Multiphoton Ionization as a clock to Reveal Molecular Dynamics with Intense Short X-ray Free Electron Laser Pulses

We investigate molecular dynamics of multiple ionization in N2 through multiple core-level photoabsorption and subsequent Auger decay processes induced by intense, short x-ray free electron laser pulses. The timing dynamics of the photoabsorption and dissociation processes is mapped onto the kinetic energy of the fragments. Measurements of the latter allow us to map out the average internuclear separation for every molecular photoionization sequence step and obtain the average time interval between the photoabsorption events. Using multiphoton ionization as a tool of the multiple-pulse pump-probe scheme, we demonstrate the modification of the ionization dynamics as we vary the x-ray laser pulse duration.

Impact of interatomic electronic decay processes on Xe 4d hole decay in the xenon fluorides

A hole in a 4d orbital of atomic xenon relaxes through Auger decay after a lifetime of 3 fs. Adding electronegative fluorine ligands to form xenon fluoride molecules, results in withdrawal of valence-electron density from Xe. Thus, within the one-center picture of Auger decay, a lowered Xe 4d Auger width would be expected, in contradiction, however, with experiment. Employing extensive ab initio calculations within the framework of many-body Green’s functions, we determine all available decay channels in XeFn and characterize these channels by means of a two-hole population analysis. We derive a relation between two-hole population numbers and partial Auger widths. On this basis, interatomic electronic decay processes are demonstrated to be so strong in the xenon fluorides that they overcompensate the reduction in intra-atomic Auger width and lead to the experimentally observed trend. The nature of the relevant processes is discussed. These processes presumably underlie Auger decay in a variety of systems.

An x-ray probe of laser-aligned molecules

We demonstrate a hard x-ray probe of laser-aligned small molecules. To align small molecules with optical lasers, high intensities at nonresonant wavelengths are necessary. We use 95ps pulses focused to 40μm from an 800nm Ti:sapphire laser at a peak intensity of 1012W∕cm2 to create an ensemble of aligned bromotrifluoromethane (CF3Br) molecules. Linearly polarized, 120ps x-ray pulses, focused to 10μm, tuned to the Br 1s→σ* preedge resonance at 13.476keV, probe the ensemble of laser-aligned molecules. The demonstrated methodology has a variety of applications and can enable ultrafast imaging of laser-controlled molecular motions with Angstrom-level resolution.

Broadband high-resolution X-ray frequency combs

An optical-frequency-comb laser manipulating a dipole response can imprint the comb on an excited transition with a high photon energy. The concept can be implemented using existing X-ray technology.