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Robin Santra

Publications and source records attributed to Robin Santra.

At least 55 records · Page 3Linked to original sources
arXiv2015

Efficient electronic structure calculation for molecular ionization dynamics at high x-ray intensity

We present the implementation of an electronic-structure approach dedicated to ionization dynamics of molecules interacting with x-ray free-electron laser (XFEL) pulses. In our scheme, molecular orbitals for molecular core-hole states are represented by linear combination of numerical atomic orbitals that are solutions of corresponding atomic core-hole states. We demonstrate that our scheme efficiently calculates all possible multiple-hole configurations of molecules formed during XFEL pulses. The present method is suitable to investigate x-ray multiphoton multiple ionization dynamics and accompanying nuclear dynamics, providing essential information on the chemical dynamics relevant for high-intensity x-ray imaging.

physics.chem-ph↗
arXiv2015

Hydrodynamic model for picosecond propagation of laser-created nanoplasmas

The interaction of a free-electron-laser pulse with a moderate or large size cluster is known to create a quasi-neutral nanoplasma, which then expands on hydrodynamic timescale, i.e., $>1$ ps. To have a better understanding of ion and electron data from experiments derived from laser-irradiated clusters, one needs to simulate cluster dynamics on such long timescales for which the molecular dynamics approach becomes inefficient. We therefore propose a two-step Molecular Dynamics-Hydrodynamic scheme. In the first step we use molecular dynamics code to follow the dynamics of an irradiated cluster until all the photo-excitation and corresponding relaxation processes are finished and a nanoplasma, consisting of ground-state ions and thermalized electrons, is formed. In the second step we perform long-timescale propagation of this nanoplasma with a computationally efficient hydrodynamic approach. In the present paper we examine the feasibility of a hydrodynamic two-fluid approach to follow the expansion of spherically symmetric nanoplasma, without accounting for the impact ionization and three-body recombination processes at this stage. We compare our results with the corresponding molecular dynamics simulations. We show that all relevant information about the nanoplasma propagation can be extracted from hydrodynamic simulations at a significantly lower computational cost when compared to a molecular dynamics approach. Finally, we comment on the accuracy and limitations of our present model and discuss possible future developments of the two-step strategy.

physics.plasm-ph↗
arXiv2015

Theoretical characterization of the collective resonance states underlying the xenon giant dipole resonance

We present a detailed theoretical characterization of the two fundamental collective resonances underlying the xenon giant dipole resonance (GDR). This is achieved consistently by two complementary methods implemented within the framework of the configuration-interaction singles (CIS) theory. The first method accesses the resonance states by diagonalizing the many-electron Hamiltonian using the smooth exterior complex scaling technique. The second method involves a new application of the Gabor analysis to wave-packet dynamics. We identify one resonance at an excitation energy of 74 eV with a lifetime of 27 as, and the second at 107 eV with a lifetime of 11 as. Our work provides a deeper understanding of the nature of the resonances associated with the GDR: a group of close-lying intrachannel resonances splits into two far-separated resonances through interchannel couplings involving the 4d electrons. The CIS approach allows a transparent interpretation of the two resonances as new collective modes. Due to the strong entanglement between the excited electron and the ionic core, the resonance wave functions are not dominated by any single particle-hole state. This gives rise to plasma-like collective oscillations of the 4d shell as a whole.

physics.atom-ph↗
arXiv2015

Wave-packet propagation based calculation of above-threshold ionization in the x-ray regime

We investigate the multi-photon process of above-threshold ionization for the light elements hydrogen, carbon, nitrogen and oxygen in the hard x-ray regime. Numerical challenges are discussed and by comparing Hartree-Fock-Slater calculations to configuration-interaction-singles results we justify the mean-field potential approach in this regime. We present a theoretical prediction of two-photon above-threshold-ionization cross sections for the mentioned elements. Moreover, we study how the importance of above-threshold ionization varies with intensity. We find that for carbon, at x-ray intensities around $10^{23}{\rm Wcm}^{-2}$, two-photon above-threshold ionization of the K-shell electrons is as probable as one-photon ionization of the L-shell electrons.

physics.atom-ph↗
arXiv2014

Incoherent x-ray scattering in single molecule imaging

Imaging of the structure of single proteins or other biomolecules with atomic resolution would be enormously beneficial to structural biology. X-ray free-electron lasers generate highly intense and ultrashort x-ray pulses, providing a route towards imaging of single molecules with atomic resolution. The information on molecular structure is encoded in the coherent x-ray scattering signal. In contrast to crystallography there are no Bragg reflections in single molecule imaging, which means the coherent scattering is not enhanced. Consequently, a background signal from incoherent scattering deteriorates the quality of the coherent scattering signal. This background signal cannot be easily eliminated because the spectrum of incoherently scattered photons cannot be resolved by usual scattering detectors. We present an ab initio study of incoherent x-ray scattering from individual carbon atoms, including the electronic radiation damage caused by a highly intense x-ray pulse. We find that the coherent scattering pattern suffers from a significant incoherent background signal at high resolution. For high x-ray fluence the background signal becomes even dominating. Finally, based on the atomic scattering patterns, we present an estimation for the average photon count in single molecule imaging at high resolution. By varying the photon energy from 3.5 keV to 15 keV, we find that imaging at higher photon energies may improve the coherent scattering signal quality.

physics.atom-ph↗
arXiv2014

Quantum-mechanical calculation of ionization potential lowering in dense plasmas

The charged environment within a dense plasma leads to the phenomenon of ionization potential depression (IPD) for ions embedded in the plasma. Accurate predictions of the IPD effect are of crucial importance for modeling atomic processes occurring within dense plasmas. Several theoretical models have been developed to describe the IPD effect, with frequently discrepant predictions. Only recently, first experiments on IPD in Al plasma have been performed with an x-ray free-electron laser (XFEL), where their results were found to be in disagreement with the widely-used IPD model by Stewart and Pyatt. Another experiment on Al, at the Orion laser, showed disagreement with the model by Ecker and Kröll. This controversy shows a strong need for a rigorous and consistent theoretical approach to calculate the IPD effect. Here we propose such an approach: a two-step Hartree-Fock-Slater model. With this parameter-free model we can accurately and efficiently describe the experimental Al data and validate the accuracy of standard IPD models. Our model can be a useful tool for calculating atomic properties within dense plasmas with wide-ranging applications to studies on warm dense matter, shock experiments, planetary science, inertial confinement fusion and studies of non-equilibrium plasmas created with XFELs.

physics.plasm-ph↗
arXiv2014

Dynamics of fluctuations in a quantum system

"\textit{The noise is the signal}"[R. Landauer, Nature \textbf{392}, 658 (1998)] emphasizes the rich information content encoded in fluctuations. This paper assesses the dynamical role of fluctuations of a quantum system driven far from equilibrium, with laser-aligned molecules as a physical realization. Time evolutions of the expectation value and the uncertainty of a standard observable are computed quantum mechanically and classically. We demonstrate the intricate dynamics of the uncertainty that are strikingly independent of those of the expectation value, and their exceptional sensitivity to quantum properties of the system. In general, detecting the time evolution of the fluctuations of a given observable provides information on the dynamics of correlations in a quantum system.

quant-ph↗
arXiv2014

Theory of time-resolved non-resonant x-ray scattering for imaging ultrafast coherent electron motion

Future ultrafast x-ray light sources might image ultrafast coherent electron motion in real-space and in real-time. For a rigorous understanding of such an imaging experiment, we extend the theory of non-resonant x-ray scattering to the time-domain. The role of energy resolution of the scattering detector is investigated in detail. We show that time-resolved non-resonant x-ray scattering with no energy resolution offers an opportunity to study time-dependent electronic correlations in non- equilibrium quantum systems. Furthermore, our theory presents a unified description of ultrafast x-ray scattering from electronic wave packets and the dynamical imaging of ultrafast dynamics using inelastic x-ray scattering by Abbamonte and co-workers. We examine closely the relation of the scattering signal and the linear density response of electronic wave packets. Finally, we demonstrate that time-resolved x-ray scattering from a crystal consisting of identical electronic wave packets recovers the instantaneous electron density.

physics.atom-ph↗
arXiv2014

Controlling the $2p$ Hole Alignment in Neon via the $2s$-$3p$ Fano Resonance

We study the state-resolved production of neon ion after resonant photoionization of Ne via the $2s$-$3p$ Fano resonance. We find that by tuning the photon energy across the Fano resonance a surprisingly high control over the alignment of the final $2p$ hole along the polarization direction can be achieved. In this way hole alignments can be created that are otherwise very hard to achieve. The mechanism responsible for this hole alignment is the destructive interference of the direct and indirect (via the autoionizing $2s^{-1}3p$ state) ionization pathways of $2p$. By changing the photon energy the strength of the interference varies and $2p$-hole alignments with ratios up to 19:1 between $2p_0$ and $2p_{\pm 1}$ holes can be created: an effect normally only encountered in tunnel ionization using strong-field IR pulses. Including spin-orbit interaction does not change the qualitative feature and leads only to a reduction in the alignment by $2/3$. Our study is based on a time-dependent configuration-interaction singles (TDCIS) approach which solves the multichannel time-dependent Schrödinger equation.

physics.atom-ph↗
arXiv2014

Calculation of photoelectron spectra within the time-dependent configuration interaction singles scheme

We present the extension of the time-dependent configuration interaction singles (TDCIS) method to the computation of the electron kinetic-energy spectrum in photoionization processes. Especially for strong and long ionizing light pulses the detection of the photoelectron poses a computational challenge because propagating the outgoing photoelectron wavepacket requires large grid sizes. Two different methods which allow for the extraction of the asymptotic photoelectron momentum are compared regarding their methodological and computational performance. The first method follows the scheme of Tong et al. \cite{tong} where the photoelectron wavefunction is absorbed by a real splitting function. The second method after Tao and Scrinzi \cite{scrinzi} measures the flux of the electron wavepacket through a surface at a fixed radius. With both methods the full angle- and energy-resolved photoelectron spectrum is obtained. Combined with the TDCIS scheme it is possible to analyze the dynamics of the outgoing electron in a channel-resolved way and, additionally, to study the dynamics of the bound electrons in the parent ion. As an application, one-photon and above-threshold ionization (ATI) of argon following strong XUV irradiation are studied via energy- and angle-resolved photoelectron spectra.

physics.atom-ph↗
arXiv2014

Imaging ultrafast electronic motion by x-ray scattering

Time-resolved ultrafast x-ray scattering is an emerging approach to probe the temporally evolving electronic charge distribution in real-space and in real-time. In this contribution, time-resolved ultrafast x-ray scattering from an electronic wave packet is presented. It is shown that the spatial and temporal correlations are imprinted in the scattering patterns, obtained by ultrafast x-ray scattering from an electronic wave packet, which deviate drastically from the notion that the instantaneous electronic density is the key quantity being probed. Furthermore, a detailed analysis of ultrafast x-ray scattering from a sample containing a mixture of non-stationary and stationary electrons along with the role of scattering interference between a non-stationary and several stationary electrons to the total scattering signal is discussed.

physics.atom-ph↗
arXiv2014

Strong-Field Many-Body Physics and the Giant Enhancement in the High-Harmonic Spectrum of Xenon

We resolve an open question about the origin of the giant enhancement in the high-harmonic generation (HHG) spectrum of atomic xenon around 100 eV. By solving the many-body time-dependent Schrödinger equation with all orbitals in the 4d, 5s, and 5p shells active, we demonstrate the enhancement results truly from collective many-body excitation induced by the returning photoelectron via two-body interchannel interactions. Without the many-body interactions, which promote a 4d electron into the 5p vacancy created by strong-field ionization, no collective excitation and no enhancement in the HHG spectrum exist.

physics.atom-ph↗
arXiv2014

X-ray diffraction from isolated and strongly aligned gas-phase molecules with a free-electron laser

We report experimental results on x-ray diffraction of quantum-state-selected and strongly aligned ensembles of the prototypical asymmetric rotor molecule 2,5-diiodobenzonitrile using the Linac Coherent Light Source. The experiments demonstrate first steps toward a new approach to diffractive imaging of distinct structures of individual, isolated gas-phase molecules. We confirm several key ingredients of single molecule diffraction experiments: the abilities to detect and count individual scattered x-ray photons in single shot diffraction data, to deliver state-selected, e. g., structural-isomer-selected, ensembles of molecules to the x-ray interaction volume, and to strongly align the scattering molecules. Our approach, using ultrashort x-ray pulses, is suitable to study ultrafast dynamics of isolated molecules.

physics.atom-ph↗
arXiv2013

Spin-Orbit Effects in Atomic High-Harmonic Generation

Spin-orbit interactions lead to small energy gaps between the outer-most $p_{1/2}$ and $p_{3/2}$ shells of noble gas atoms. Strong-field pulses tunnel-ionize an electron out of either shell resulting in spin-orbit-driven hole motion. These hole dynamics affect the HHG yield. However, the spectral shape as well as the angular distribution of the HHG emission is not influenced by spin-orbit coupling. We demonstrate the spin-orbit effect on atomic krypton by solving the multi-electron Schrödinger equation with the time-dependent configuration-interaction singles (TDCIS) approach. We also provide pulse parameters where this effect can be identified in experiments through an enhancement in the HHG yield as the wavelength of the strong-field pulse increases.

physics.atom-ph↗
arXiv2013

Introducing many-body physics using atomic spectroscopy

Atoms constitute relatively simple many-body systems, making them suitable objects for developing an understanding of basic aspects of many-body physics. Photoabsorption spectroscopy is a prominent method to study the electronic structure of atoms and the inherent many-body interactions. In this article the impact of many-body effects on well-known spectroscopic features such as Rydberg series, Fano resonances, Cooper minima, and giant resonances is studied, and related many-body phenomena in other fields are outlined. To calculate photoabsorption cross sections the time-dependent configuration interaction singles (TDCIS) model is employed. The conceptual clearness of TDCIS in combination with the compactness of atomic systems allows for a pedagogical introduction to many-body phenomena.

physics.atom-ph↗
arXiv2013

Recombination Amplitude Calculations of Noble Gases, in Length and Acceleration Forms, beyond Strong Field Approximation

Transition of an electron from a free to a bound state is critical in determining the qualitative shape of the spectrum in high-order harmonic generation (HHG), and in tomographic imaging of orbitals. We calculate and compare the recombination amplitude, from a continuum state described by a plane wave and an outgoing scattering eigenstate, to the bound state for the noble gases that are commonly used in HHG. These calculations are based on the single active electron model and the Hartree-Fock-Slater method, using both the length form and the acceleration form of the dipole matrix element. We confirm that the recombination amplitude versus emitted photon energy strongly depends upon the wavefunction used to describe the free electron. Depending on the choice of the wavefunction and the dipole form, the square of the absolute value of the recombination amplitude can differ by almost two orders of magnitude near the experimentally measured Cooper minima. Moreover, only the outgoing scattering eigenstates with the length form roughly predict the experimentally observed Cooper minimum for Ar (~50 eV) and Kr (~85 eV). We provide a detailed derivation of the photorecombination cross sections (PRCSs) from photo ionization cross sections (PICSs) calculated by the relativistic random phase approximation (RRPA)., For Ar, Kr and Xe, compare the total PICSs calculated using our recombination amplitudes with that obtained from RRPA. We find that PICS calculated using the outgoing scattering eigenstates with the length form is in better agreement with the RRPA calculations than the acceleration form.

physics.atom-ph↗
arXiv2013

Determination of multiwavelength anomalous diffraction coefficients at high x-ray intensity

The high-intensity version of multiwavelength anomalous diffraction (MAD) has a potential for solving the phase problem in femtosecond crystallography with x-ray free-electron lasers (XFELs). For MAD phasing, it is required to calculate or measure the MAD coefficients involved in the key equation, which depend on XFEL pulse parameters. In the present work, we revisit the generalized Karle-Hendrickson equation to clarify the importance of configurational fluctuations of heavy atoms induced by intense x-ray pulses, and investigate the high-intensity cases of transmission and fluorescence measurements of samples containing heavy atoms. Based on transmission/fluorescence and diffraction experiments with crystalline samples of known structures, we propose an experimental procedure to determine all MAD coefficients at high x-ray intensity, which can be used in \emph{ab initio} phasing for unknown structures.

physics.atom-ph↗