Engineering topics

Santra, R

Publications and source records attributed to Santra, R.

10 records

DOE OSTI2011

Unveiling and Driving Hidden Resonances with High-Fluence, High-Intensity X-Ray Pulses

We show that high fluence, high-intensity x-ray pulses from the world's first hard x-ray free-electron laser produce nonlinear phenomena that differ dramatically from the linear x-ray-matter interaction processes that are encountered at synchrotron x-ray sources. We use intense x-ray pulses of sub-10-fs duration to first reveal and subsequently drive the 1s{r_reversible}2p resonance in singly ionized neon. This photon-driven cycling of an inner-shell electron modifies the Auger decay process, as evidenced by line shape modification. Our work demonstrates the propensity of high-fluence, femtosecond x-ray pulses to alter the target within a single pulse, i.e., to unveil hidden resonances, by cracking open inner shells energetically inaccessible via single-photon absorption, and to consequently trigger damaging electron cascades at unexpectedly low photon energies.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2011

Heterogeneous clusters as a model system for the study of ionization dynamics within tampered samples

Tampering of a sample with a layer of another material is a promising technique to slow down the expansion dynamics within laser irradiated samples, with sound implications for single-particle diffraction imaging. Ideally, if an imaged object is covered by a layer of another material, during the irradiation this layer will be primarily ionized and will expand fast due to Coulomb repulsion, whereas the object located within the net neutral core will expand more slowly (hydrodynamically). We investigate the details of the electronic damage within the tampered samples during their irradiation with an intense extreme ultraviolet (EUV) pulse. We study heterogeneous clusters composed of noble gas atoms, Xe and Ar, for which chemical-bond effects can be neglected. Using a fully nonequilibrium kinetic equation code, we demonstrate the influence of cluster composition on ionization dynamics; in particular, on the electronic damage. The results are obtained for the wavelength of 32 nm, which is available at the free-electron laser in Hamburg (FLASH) facility, but our conclusions can also have implications for samples with a more complex structure and irradiated at a much shorter wavelength.

74 ATOMIC AND MOLECULAR PHYSICS↗

DOE OSTI2011

Nonlinear Atomic Response to Intense Ultrashort X Rays

The nonlinear absorption mechanisms of neon atoms to intense, femtosecond kilovolt x rays are investigated. The production of Ne{sup 9+} is observed at x-ray frequencies below the Ne{sup 8+}, 1s{sup 2} absorption edge and demonstrates a clear quadratic dependence on fluence. Theoretical analysis shows that the production is a combination of the two-photon ionization of Ne{sup 8+} ground state and a high-order sequential process involving single-photon production and ionization of transient excited states on a time scale faster than the Auger decay. We find that the nonlinear direct two-photon ionization cross section is orders of magnitude higher than expected from previous calculations.

74 ATOMIC AND MOLECULAR PHYSICS↗

DOE OSTI2011

Inner-shell and double ionization potentials of aminophenol isomers.

A comprehensive study of single and double core ionization potentials of the aminophenol molecule is reported. The role of relaxation, correlation, relativistic, and basis set effects in these potentials is clarified. Special attention is paid to the isomer dependence of the single and double core ionization potentials. Some of them are also compared with the respective values of the phenol and aniline molecules. It is shown that the core level single ionization potentials of the para-, meta-, and ortho-aminophenol molecules differ only slightly from each other, rendering these structural isomers challenging to distinguish for conventional x-ray photoelectron spectroscopy. In contrast, the energy needed to remove two core electrons from different atoms depends noticeably on the mutual arrangement and even on the relative orientations of the hydroxyl and amine groups. Together with the electrostatic repulsion between the two core holes, relaxation effects accompanying double core ionization play a crucial role here. The pronounced sensitivity of the double ionization potentials, therefore, enables a spectroscopic characterization of the electronic structure of aminophenol isomers by means of x-ray two-photon photoelectron spectroscopy.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2010

Real-time observation of valence electron motion.

The superposition of quantum states drives motion on the atomic and subatomic scales, with the energy spacing of the states dictating the speed of the motion. In the case of electrons residing in the outer (valence) shells of atoms and molecules which are separated by electronvolt energies, this means that valence electron motion occurs on a subfemtosecond to few-femtosecond timescale (1 fs = 10{sup -15} s). In the absence of complete measurements, the motion can be characterized in terms of a complex quantity, the density matrix. Here we report an attosecond pump-probe measurement of the density matrix of valence electrons in atomic krypton ions. We generate the ions with a controlled few-cycle laser field and then probe them through the spectrally resolved absorption of an attosecond extreme-ultraviolet pulse, which allows us to observe in real time the subfemtosecond motion of valence electrons over a multifemtosecond time span. We are able to completely characterize the quantum mechanical electron motion and determine its degree of coherence in the specimen of the ensemble. Although the present study uses a simple, prototypical open system, attosecond transient absorption spectroscopy should be applicable to molecules and solid-state materials to reveal the elementary electron motions that control physical, chemical and biological properties and processes.

74 ATOMIC AND MOLECULAR PHYSICS↗

DOE OSTI2010

Femtosecond electronic response of atoms to ultra-intense x-rays.

An era of exploring the interactions of high-intensity, hard X-rays with matter has begun with the start-up of a hard-X-ray free-electron laser, the Linac Coherent Light Source (LCLS). Understanding how electrons in matter respond to ultra-intense X-ray radiation is essential for all applications. Here we reveal the nature of the electronic response in a free atom to unprecedented high-intensity, short-wavelength, high-fluence radiation (respectively 10{sup 18} W cm{sup -2}, 1.5-0.6 nm, {approx}10{sup 5} X-ray photons per {angstrom}{sup 2}). At this fluence, the neon target inevitably changes during the course of a single femtosecond-duration X-ray pulse - by sequentially ejecting electrons - to produce fully-stripped neon through absorption of six photons. Rapid photoejection of inner-shell electrons produces 'hollow' atoms and an intensity-induced X-ray transparency. Such transparency, due to the presence of inner-shell vacancies, can be induced in all atomic, molecular and condensed matter systems at high intensity. Quantitative comparison with theory allows us to extract LCLS fluence and pulse duration. Our successful modelling of X-ray/atom interactions using a straightforward rate equation approach augurs favourably for extension to complex systems.

43 PARTICLE ACCELERATORS↗

DOE OSTI2010

Alignment of asymmetric-top molecules using multiple-pulse trains

We theoretically analyze the effectiveness of multiple-pulse laser alignment methods for asymmetric-top molecules. As an example, we choose SO{sub 2} and investigate the alignment dynamics induced by two different sequences, each consisting of four identical laser pulses. Each sequence differs only in the time delay between the pulses. Equally spaced pulses matching the alignment revival of the symmetrized SO{sub 2} rotor model are exploited in the first sequence. The pulse separations in the second sequence are short compared to the rotation dynamics of the molecule and monotonically increase the degree of alignment until the maximum alignment is reached. We point out the significant differences between the alignment dynamics of SO{sub 2} treated as an asymmetric-top and a symmetric-top rotor, respectively. We also explain why the fast sequence of laser pulses creates considerably stronger one-dimensional molecular alignment for asymmetric-top molecules. In addition, we show that multiple-pulse trains with elliptically polarized pulses do not enhance one-dimensional alignment or create three-dimensional alignment.

74 ATOMIC AND MOLECULAR PHYSICS↗

DOE OSTI2010

Using strong electromagnetic fields to control x-ray processes.

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.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2010

Refraction and absorption of x rays by laser-dressed atoms.

X-ray refraction and absorption by neon atoms under the influence of an 800 nm laser with an intensity of 10{sup 13} W/cm{sup 2} is investigated. For this purpose, we use an ab initio theory suitable for optical strong-field problems. Its results are interpreted in terms of a three-level model. On the Ne 1s {yields} 3p resonance, we find electromagnetically induced transparency (EIT) for x rays. Our work opens novel perspectives for ultrafast x-ray pulse shaping.

99 GENERAL AND MISCELLANEOUS↗

DOE OSTI2010

Theory of x-ray diffraction from laser-aligned molecules.

We present the theory of x-ray diffraction from an ensemble of symmetric-top molecules aligned by an intense optical laser pulse at finite rotational temperature. Using QED, the x-ray/molecule interaction is treated as an electronically elastic one-photon scattering process. In the practically important case that the x-ray pulse is quasi-monochromatic and its coherence time is much shorter than the time scale of molecular rotational dynamics in the laser field, there is a simple connection between the rotational wave-packet dynamics and the diffraction pattern obtained. Our theory thus opens up a new perspective for quantum molecular imaging using x-ray radiation.

99 GENERAL AND MISCELLANEOUS↗