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Title: The high pressure structure and equation of state of 2,6-diamino-3,5-dinitropyrazine-1-oxide (LLM-105) up to 20 GPa: X-ray diffraction measurements and first principles molecular dynamics simulations

Abstract

Recent theoretical studies of 2,6-diamino-3,5-dinitropyrazine-1-oxide (C{sub 4}H{sub 4}N{sub 6}O{sub 5} Lawrence Livermore Molecule No. 105, LLM-105) report unreacted high pressure equations of state that include several structural phase transitions, between 8 and 50 GPa, while one published experimental study reports equation of state (EOS) data up to a pressure of 6 GPa with no observed transition. Here we report the results of a synchrotron-based X-ray diffraction study and also ambient temperature isobaric-isothermal atomistic molecular dynamics simulations of LLM-105 up to 20 GPa. We find that the ambient pressure phase remains stable up to 20 GPa; there is no indication of a pressure induced phase transition. We do find a prominent decrease in b-axis compressibility starting at approximately 13 GPa and attribute the stiffening to a critical length where inter-sheet distance becomes similar to the intermolecular distance within individual sheets. The ambient temperature isothermal equation of state was determined through refinements of measured X-ray diffraction patterns. The pressure-volume data were fit using various EOS models to yield bulk moduli with corresponding pressure derivatives. We find very good agreement between the experimental and theoretically derived EOS.

Authors:
; ; ; ; ;  [1];  [2]
  1. Lawrence Livermore National Laboratory, Physical and Life Sciences Directorate, P.O. Box 808 L-350, Livermore, California 94550 (United States)
  2. Advanced Light Source, Lawrence Berkeley Laboratory, Berkeley, California 94720 (United States)
Publication Date:
OSTI Identifier:
22489715
Resource Type:
Journal Article
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 143; Journal Issue: 14; Other Information: (c) 2015 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA); Journal ID: ISSN 0021-9606
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; AMBIENT TEMPERATURE; APPROXIMATIONS; COMPRESSIBILITY; EQUATIONS OF STATE; MOLECULAR DYNAMICS METHOD; MOLECULES; OXIDES; PHASE TRANSFORMATIONS; SIMULATION; SYNCHROTRONS; X-RAY DIFFRACTION

Citation Formats

Stavrou, Elissaios, Riad Manaa, M., E-mail: manaa1@llnl.gov, Zaug, Joseph M., Kuo, I-Feng W., Pagoria, Philip F., Crowhurst, Jonathan C., Armstrong, Michael R., Kalkan, Bora, and Advanced Materials Research Laboratory, Department of Physics Engineering, Hacettepe University 06800, Beytepe, Ankara. The high pressure structure and equation of state of 2,6-diamino-3,5-dinitropyrazine-1-oxide (LLM-105) up to 20 GPa: X-ray diffraction measurements and first principles molecular dynamics simulations. United States: N. p., 2015. Web. doi:10.1063/1.4932683.
Stavrou, Elissaios, Riad Manaa, M., E-mail: manaa1@llnl.gov, Zaug, Joseph M., Kuo, I-Feng W., Pagoria, Philip F., Crowhurst, Jonathan C., Armstrong, Michael R., Kalkan, Bora, & Advanced Materials Research Laboratory, Department of Physics Engineering, Hacettepe University 06800, Beytepe, Ankara. The high pressure structure and equation of state of 2,6-diamino-3,5-dinitropyrazine-1-oxide (LLM-105) up to 20 GPa: X-ray diffraction measurements and first principles molecular dynamics simulations. United States. https://doi.org/10.1063/1.4932683
Stavrou, Elissaios, Riad Manaa, M., E-mail: manaa1@llnl.gov, Zaug, Joseph M., Kuo, I-Feng W., Pagoria, Philip F., Crowhurst, Jonathan C., Armstrong, Michael R., Kalkan, Bora, and Advanced Materials Research Laboratory, Department of Physics Engineering, Hacettepe University 06800, Beytepe, Ankara. 2015. "The high pressure structure and equation of state of 2,6-diamino-3,5-dinitropyrazine-1-oxide (LLM-105) up to 20 GPa: X-ray diffraction measurements and first principles molecular dynamics simulations". United States. https://doi.org/10.1063/1.4932683.
@article{osti_22489715,
title = {The high pressure structure and equation of state of 2,6-diamino-3,5-dinitropyrazine-1-oxide (LLM-105) up to 20 GPa: X-ray diffraction measurements and first principles molecular dynamics simulations},
author = {Stavrou, Elissaios and Riad Manaa, M., E-mail: manaa1@llnl.gov and Zaug, Joseph M. and Kuo, I-Feng W. and Pagoria, Philip F. and Crowhurst, Jonathan C. and Armstrong, Michael R. and Kalkan, Bora and Advanced Materials Research Laboratory, Department of Physics Engineering, Hacettepe University 06800, Beytepe, Ankara},
abstractNote = {Recent theoretical studies of 2,6-diamino-3,5-dinitropyrazine-1-oxide (C{sub 4}H{sub 4}N{sub 6}O{sub 5} Lawrence Livermore Molecule No. 105, LLM-105) report unreacted high pressure equations of state that include several structural phase transitions, between 8 and 50 GPa, while one published experimental study reports equation of state (EOS) data up to a pressure of 6 GPa with no observed transition. Here we report the results of a synchrotron-based X-ray diffraction study and also ambient temperature isobaric-isothermal atomistic molecular dynamics simulations of LLM-105 up to 20 GPa. We find that the ambient pressure phase remains stable up to 20 GPa; there is no indication of a pressure induced phase transition. We do find a prominent decrease in b-axis compressibility starting at approximately 13 GPa and attribute the stiffening to a critical length where inter-sheet distance becomes similar to the intermolecular distance within individual sheets. The ambient temperature isothermal equation of state was determined through refinements of measured X-ray diffraction patterns. The pressure-volume data were fit using various EOS models to yield bulk moduli with corresponding pressure derivatives. We find very good agreement between the experimental and theoretically derived EOS.},
doi = {10.1063/1.4932683},
url = {https://www.osti.gov/biblio/22489715}, journal = {Journal of Chemical Physics},
issn = {0021-9606},
number = 14,
volume = 143,
place = {United States},
year = {2015},
month = {10}
}

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Works referencing / citing this record:

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Effects of pressure on the structure and lattice dynamics of ammonium perchlorate: A combined experimental and theoretical study
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Pressure-induced phase transition in 1,3,5-triamino-2,4,6-trinitrobenzene (TATB)
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