Large-scale atomistic calculations of clusters in intense x-ray pulses
Abstract
Here, we present the methodology of our recently developed Monte-Carlo/ Molecular-Dynamics method for studying the fundamental ultrafast dynamics induced by high-fluence, high-intensity x-ray free electron laser (XFEL) pulses in clusters. The quantum nature of the initiating ionization process is accounted for by a Monte Carlo method to calculate probabilities of electronic transitions, including photo absorption, inner-shell relaxation, photon scattering, electron collision and recombination dynamics, and thus track the transient electronic configurations explicitly. The freed electrons and ions are followed by classical particle trajectories using a molecular dynamics algorithm. These calculations reveal the surprising role of electron-ion recombination processes that lead to the development of nonuniform spatial charge density profiles in x-ray excited clusters over femtosecond timescales. In the high-intensity limit, it is important to include the recombination dynamics in the calculated scattering response even for a 2- fs pulse. We also demonstrate that our numerical codes and algorithms can make e!cient use of the computational power of massively parallel supercomputers to investigate the intense-field dynamics in systems with increasing complexity and size at the ultrafast timescale and in non-linear x-ray interaction regimes. In particular, picosecond trajectories of XFEL clusters with attosecond time resolution containing millions of particles can be e!cientlymore »
- Authors:
-
- Argonne National Lab. (ANL), Argonne, IL (United States)
- Publication Date:
- Research Org.:
- Argonne National Laboratory (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1374543
- Grant/Contract Number:
- AC02-06CH11357
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Physics. B, Atomic, Molecular and Optical Physics
- Additional Journal Information:
- Journal Volume: 50; Journal Issue: 10; Journal ID: ISSN 0953-4075
- Publisher:
- IOP Publishing
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 74 ATOMIC AND MOLECULAR PHYSICS; light matter interaction; x-ray free-electron laser; multi-photon ionization and excitation; laser cluster interaction; high-performance computing
Citation Formats
Ho, Phay J., and Knight, Chris. Large-scale atomistic calculations of clusters in intense x-ray pulses. United States: N. p., 2017.
Web. doi:10.1088/1361-6455/aa69e6.
Ho, Phay J., & Knight, Chris. Large-scale atomistic calculations of clusters in intense x-ray pulses. United States. https://doi.org/10.1088/1361-6455/aa69e6
Ho, Phay J., and Knight, Chris. Fri .
"Large-scale atomistic calculations of clusters in intense x-ray pulses". United States. https://doi.org/10.1088/1361-6455/aa69e6. https://www.osti.gov/servlets/purl/1374543.
@article{osti_1374543,
title = {Large-scale atomistic calculations of clusters in intense x-ray pulses},
author = {Ho, Phay J. and Knight, Chris},
abstractNote = {Here, we present the methodology of our recently developed Monte-Carlo/ Molecular-Dynamics method for studying the fundamental ultrafast dynamics induced by high-fluence, high-intensity x-ray free electron laser (XFEL) pulses in clusters. The quantum nature of the initiating ionization process is accounted for by a Monte Carlo method to calculate probabilities of electronic transitions, including photo absorption, inner-shell relaxation, photon scattering, electron collision and recombination dynamics, and thus track the transient electronic configurations explicitly. The freed electrons and ions are followed by classical particle trajectories using a molecular dynamics algorithm. These calculations reveal the surprising role of electron-ion recombination processes that lead to the development of nonuniform spatial charge density profiles in x-ray excited clusters over femtosecond timescales. In the high-intensity limit, it is important to include the recombination dynamics in the calculated scattering response even for a 2- fs pulse. We also demonstrate that our numerical codes and algorithms can make e!cient use of the computational power of massively parallel supercomputers to investigate the intense-field dynamics in systems with increasing complexity and size at the ultrafast timescale and in non-linear x-ray interaction regimes. In particular, picosecond trajectories of XFEL clusters with attosecond time resolution containing millions of particles can be e!ciently computed on upwards of 262,144 processes.},
doi = {10.1088/1361-6455/aa69e6},
journal = {Journal of Physics. B, Atomic, Molecular and Optical Physics},
number = 10,
volume = 50,
place = {United States},
year = {Fri Apr 28 00:00:00 EDT 2017},
month = {Fri Apr 28 00:00:00 EDT 2017}
}
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Figure 1: Processes in x-ray-nanoparticle interaction included in MC/MD model. S: x-ray scattering, P: photoionization, RE: resonant excitation, RC: electron-ion recombination, EI: electron-impact ionization, A: Auger (CosterKronig) decay, F: fluorescence, and L: Lattice dynamics. The smaller colored are ionized electrons.
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