Proposed imaging of the ultrafast electronic motion in samples using x-ray phase-contrast

Tracing the motion of electrons has enormous relevance to understanding ubiquitous phenomena in ultrafast science, such as the dynamical evolution of the electron density during complex chemical and biological processes. Scattering of ultrashort x-ray pulses from an electronic wavepacket would appear to be the most obvious approach to image the electronic motion in real-time and real-space with the notion that such scattering patterns, in the far-field regime, encode the instantaneous electron density of the wavepacket. However, recent results by Dixit {\em et al.} [Proc. Natl. Acad. Sci. U.S.A., {\bf 109}, 11636 (2012)] have put this notion into question and shown that the scattering in the far-field regime probes spatio-temporal density-density correlations. Here, we propose a possible way to image the instantaneous electron density of the wavepacket via ultrafast x-ray {\em phase contrast imaging}. Moreover, we show that inelastic scattering processes, which plague ultrafast scattering in the far-field regime, do not contribute in ultrafast x-ray phase contrast imaging as a consequence of an interference effect. We illustrate our general findings by means of a wavepacket that lies in the time and energy range of the dynamics of valence electrons in complex molecular and biological systems. This present work offers a potential to image not only instantaneous snapshots of non-stationary electron dynamics, but also the Laplacian of these snapshots which provide information about the complex bonding and topology of the charge distributions in the systems.Comment: 12 pages, 2 figures, article accepted in Physical Review Letters (2013

Tailoring Photocurrent in Weyl Semimetals via Intense Laser Irradiation

Generating and tailoring photocurrent in topological materials has immense importance in fundamental studies and the technological front. Present work introduces a universal method to generate ultrafast photocurrent in {\it both} inversion-symmetric and inversion-broken Weyl semimetals with degenerate Weyl nodes at the Fermi level. Our approach harnesses the asymmetric electronic population in the conduction band induced by an intense {\it single-color} circularly polarized laser pulse. It has been found that the induced photocurrent can be tailored by manipulating helicity and ellipticity of the employed laser. Moreover, our approach generates photocurrent in realistic situations when the Weyl nodes are positioned at different energies and have finite tilt along a certain direction. Present work adds a new dimension on practical applications of Weyl semimetals for optoelectronics and photonics-based quantum technologies.Comment: 13 pages, 5 figure

Theoretical spectroscopic studies of the atomic transitions and lifetimes of low-lying states in Ti IV

The astrophysically important electric quadrupole (E2) and magnetic dipole (M1) transitions for the low-lying states of triply ionized titanium (Ti IV) are calculated very accurately using a state-of-art all-order many-body theory called Coupled Cluster (CC) theory in the relativistic frame-work. Different many-body correlations of the CC theory has been estimated by studying the core and valence electron excitations to the unoccupied states. The calculated excitation energies of different states are in very good agreement with the measurements. Also we compare our calculated electric dipole (E1) transition amplitudes of few transitions with recent many-body calculations by different groups. We have also carried out the calculations for the lifetimes of the low-lying states of Ti IV. A long lifetime is found for the first excited 3d$^{2}D_{5/2}$ state, which suggested that Ti IV may be one of the useful candidates for many important studies. Most of the results reported here are not available in the literature, to the best of our knowledge.Comment: 15 pages submitted to J. Phys.

X-ray imaging of chemically active valence electrons during a pericyclic reaction

Time-resolved imaging of chemically active valence electron densities is a long sought goal, as these electrons dictate the course of chemical reactions. However, x-ray scattering is always dominated by the core and inert valence electrons, making time-resolved x-ray imaging of chemically active valence electron densities extremely challenging. To image such electron densities, we demonstrate an effective and robust method, which emphasizes the information encoded in weakly scattered photons. The degenerate Cope rearrangement of semibullvalene, a pericyclic reaction, is used as an example to visually illustrate our approach. Our work also provides experimental access to the long-standing problem of synchronous versus asynchronous bond formation and breaking during pericyclic reactions.Comment: 19 pages, 3 figures, comments are most welcom