Rate equations for nitrogen molecules in ultrashort and intense x-ray pulses
Abstract
Here, we study theoretically the quantum dynamics of nitrogen molecules (N2) exposed to intense and ultrafast x-rays at a wavelength of $$1.1\;{\rm{nm}}$$ ($$1100\;{\rm{eV}}$$ photon energy) from the Linac Coherent Light Source (LCLS) free electron laser. Molecular rate equations are derived to describe the intertwined photoionization, decay, and dissociation processes occurring for N2. This model complements our earlier phenomenological approaches, the single-atom, symmetric-sharing, and fragmentation-matrix models of 2012 (J. Chem. Phys. 136 214310). Our rate-equations are used to obtain the effective pulse energy at the sample and the time scale for the dissociation of the metastable dication $${{\rm{N}}}_{2}^{2+}$$. This leads to a very good agreement between the theoretically and experimentally determined ion yields and, consequently, the average charge states. The effective pulse energy is found to decrease with shortening pulse duration. This variation together with a change in the molecular fragmentation pattern and frustrated absorption—an effect that reduces absorption of x-rays due to (double) core hole formation—are the causes for the drop of the average charge state with shortening LCLS pulse duration discovered previously.
- Authors:
-
- North China Electric Power Univ., Beijing (China); Max-Planck-Institut fur Kernphysik, Heidelberg (Germany)
- Univ. of Connecticut, Storrs, CT (United States)
- Ruprecht-Karls-Univ. Heidelberg, Heidelberg (Germany)
- SLAC National Accelerator Lab., Menlo Park, CA (United States); Stanford Univ., Stanford, CA (United States)
- SLAC National Accelerator Lab., Menlo Park, CA (United States); Louisiana State Univ., Baton Rouge, LA (United States)
- Max-Planck-Institut fur Kernphysik, Heidelberg (Germany); Ruprecht-Karls-Univ. Heidelberg, Heidelberg (Germany); SLAC National Accelerator Lab., Menlo Park, CA (United States); Louisiana State Univ., Baton Rouge, LA (United States)
- Publication Date:
- Research Org.:
- SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC)
- OSTI Identifier:
- 1254737
- Report Number(s):
- SLAC-PUB-16535
Journal ID: ISSN 0953-4075; arXiv:1508.05223
- Grant/Contract Number:
- AC02-76SF00515
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Physics. B, Atomic, Molecular and Optical Physics
- Additional Journal Information:
- Journal Volume: 49; Journal Issue: 7; Journal ID: ISSN 0953-4075
- Publisher:
- IOP Publishing
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; nitrogen molecule; molecular rate equations; frustrated absorption; ultrafast; intense; x rays; fragmentation
Citation Formats
Liu, Ji -Cai, Berrah, Nora, Cederbaum, Lorenz S., Cryan, James P., Glownia, James M., Schafer, Kenneth J., and Buth, Christian. Rate equations for nitrogen molecules in ultrashort and intense x-ray pulses. United States: N. p., 2016.
Web. doi:10.1088/0953-4075/49/7/075602.
Liu, Ji -Cai, Berrah, Nora, Cederbaum, Lorenz S., Cryan, James P., Glownia, James M., Schafer, Kenneth J., & Buth, Christian. Rate equations for nitrogen molecules in ultrashort and intense x-ray pulses. United States. https://doi.org/10.1088/0953-4075/49/7/075602
Liu, Ji -Cai, Berrah, Nora, Cederbaum, Lorenz S., Cryan, James P., Glownia, James M., Schafer, Kenneth J., and Buth, Christian. Wed .
"Rate equations for nitrogen molecules in ultrashort and intense x-ray pulses". United States. https://doi.org/10.1088/0953-4075/49/7/075602. https://www.osti.gov/servlets/purl/1254737.
@article{osti_1254737,
title = {Rate equations for nitrogen molecules in ultrashort and intense x-ray pulses},
author = {Liu, Ji -Cai and Berrah, Nora and Cederbaum, Lorenz S. and Cryan, James P. and Glownia, James M. and Schafer, Kenneth J. and Buth, Christian},
abstractNote = {Here, we study theoretically the quantum dynamics of nitrogen molecules (N2) exposed to intense and ultrafast x-rays at a wavelength of $1.1\;{\rm{nm}}$ ($1100\;{\rm{eV}}$ photon energy) from the Linac Coherent Light Source (LCLS) free electron laser. Molecular rate equations are derived to describe the intertwined photoionization, decay, and dissociation processes occurring for N2. This model complements our earlier phenomenological approaches, the single-atom, symmetric-sharing, and fragmentation-matrix models of 2012 (J. Chem. Phys. 136 214310). Our rate-equations are used to obtain the effective pulse energy at the sample and the time scale for the dissociation of the metastable dication ${{\rm{N}}}_{2}^{2+}$. This leads to a very good agreement between the theoretically and experimentally determined ion yields and, consequently, the average charge states. The effective pulse energy is found to decrease with shortening pulse duration. This variation together with a change in the molecular fragmentation pattern and frustrated absorption—an effect that reduces absorption of x-rays due to (double) core hole formation—are the causes for the drop of the average charge state with shortening LCLS pulse duration discovered previously.},
doi = {10.1088/0953-4075/49/7/075602},
journal = {Journal of Physics. B, Atomic, Molecular and Optical Physics},
number = 7,
volume = 49,
place = {United States},
year = {Wed Mar 16 00:00:00 EDT 2016},
month = {Wed Mar 16 00:00:00 EDT 2016}
}
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