Subscribe to the gold package and get unlimited access to Shamra Academy
Register a new userNonlinear resonant X-ray Raman scattering
161
0
0.0
(
0
)
Ask ChatGPT about the research
No Arabic abstract
We report the observation of a novel nonlinear effect in the hard x-ray range. Upon illuminating Fe and Cu metal foils with intense x-ray pulses tuned near their respective K edges, photons at nearly twice the incoming photon energy are emitted. The signal rises quadratically with the incoming intensity, consistent with two-photon excitation. The spectrum of emitted high-energy photons comprises multiple Raman lines that disperse with the incident photon energy. Upon reaching the double K-shell ionization threshold, the signal strength undergoes a marked rise. Above this threshold, the lines cease dispersing, turning into orescence lines with energies much greater than obtainable by single electron transitions, and additional Raman lines appear. We attribute these processes to electron-correlation mediated multielectron transitions involving double-core hole excitation and various two-electron de-excitation processes to a final state involving one or more L and M core-holes.
rate research
Read More
Impulsive X-ray Raman excitations of Lithium, Neon, and Sodium are calculated using the Multiconfiguration Time-Dependent Hartree-Fock method. Using linearly polarized laser pulses without chirp, we determine the optimum central frequency, intensity, and duration for maximum population transfer to valence excited states. We demonstrate the existence of two local optima or sweet spots for population transfer, either of which, depending on the system, may be superior. For some systems we find that population transfer can be maximized by nonresonant Raman transitions, red-detuned below K-edge, because such detuning minimizes core-excited populations and ionization loss. For instance, in Neon near the K-edge the global optimum for population transfer occurs at high intensity (8 $times$ 10$^{19}$ W cm$^{-2}$), short duration (82as full-width-at-half-maximum), and 24eV red-detuned from the K-edge.
In this work we report the modification of the normal Auger line shape under the action of an intense x-ray radiation. Under strong Rabi-type coupling of the core, the Auger line profile develops into a doublet structure with an energy separation mainly determined by the relative strength of the Rabi coupling. In addition, we find that the charge resolved ion yields can be controlled by judicious choice of the x-ray frequency.
X-ray scattering is a weak linear probe of matter. It is primarily sensitive to the position of electrons and their momentum distribution. Elastic X-ray scattering forms the basis of atomic structural determination while inelastic Compton scattering is often used as a spectroscopic probe of both single-particle excitations and collective modes. X-ray free-electron lasers (XFELs) are unique tools for studying matter on its natural time and length scales due to their bright and coherent ultrashort pulses. However, in the focus of an XFEL the assumption of a weak linear probe breaks down, and nonlinear light-matter interactions can become ubiquitous. The field can be sufficiently high that even non-resonant multiphoton interactions at hard X-rays wavelengths become relevant. Here we report the observation of one of the most fundamental nonlinear X-ray-matter interactions, the simultaneous Compton scattering of two identical photons producing a single photon at nearly twice the photon energy. We measure scattered photons with an energy near 18 keV generated from solid beryllium irradiated by 8.8-9.75 keV XFEL pulses. The intensity in the X-ray focus reaches up to 4x20 W/cm2, which corresponds to a peak electric field two orders of magnitude higher than the atomic unit of field-strength and within four orders of magnitude of the quantum electrodynamic critical field. The observed signal scales quadratically in intensity and is emitted into a non-dipolar pattern, consistent with the simultaneous two-photon scattering from free electrons. However, the energy of the generated photons shows an anomalously large redshift only present at high intensities. This indicates that the instantaneous high-intensity scattering effectively interacts with a different electron momentum distribution than linear Compton scattering, with implications for the study of atomic-scale structure and dynamics of matter
The capability of generating two intense, femtosecond x-ray pulses with controlled time delay opens the possibility of performing time-resolved experiments for x-ray induced phenomena. We have applied this capability to study the photoinduced dynamics in diatomic molecules. In molecules composed of low-Z elements, textit{K}-shell ionization creates a core-hole state in which the main decay mode is an Auger process involving two electrons in the valence shell. After Auger decay, the nuclear wavepackets of the transient two-valence-hole states continue evolving on the femtosecond timescale, leading either to separated atomic ions or long-lived quasi-bound states. By using an x-ray pump and an x-ray probe pulse tuned above the textit{K}-shell ionization threshold of the nitrogen molecule, we are able to observe ion dissociation in progress by measuring the time-dependent kinetic energy releases of different breakup channels. We simulated the measurements on N$_2$ with a molecular dynamics model that accounts for textit{K}-shell ionization, Auger decay, and the time evolution of the nuclear wavepackets. In addition to explaining the time-dependent feature in the measured kinetic energy release distributions from the dissociative states, the simulation also reveals the contributions of quasi-bound states.
We report non-resonant x-ray Raman scattering (XRS) measurements from hexagonal boron nitride for transferred momentum from 2 to 9 $mathrm{AA}^{-1}$ along directions both in and out of the basal plane. A symmetry-based argument, together with real-space full multiple scattering calculations of the projected density of states in the spherical harmonics basis, reveals that a strong pre-edge feature is a dominantly $Y_{10}$-type Frenkel exciton with no other textit{s}-, textit{p}-, or textit{d}- components. This conclusion is supported by a second, independent calculation of the textbf{q}-dependent XRS cross-section based on the Bethe-Salpeter equation.
Log in to be able to interact and post comments
comments
Fetching comments
Sign in to be able to follow your search criteria
