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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

Recent theoretical studies of 2,6-diamino-3,5-dinitropyrazine-1-oxide (C 4H 4N 6O 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. As a result, we find very good agreement between the experimental and theoretically derived EOS.
Authors:
 [1] ;  [1] ;  [1] ;  [1] ;  [1] ;  [1] ;  [1] ;  [2]
  1. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Hacettepe Univ., Ankara (Turkey)
Publication Date:
Report Number(s):
LLNL-JRNL-670642
Journal ID: ISSN 0021-9606; JCPSA6
Grant/Contract Number:
AC52-07NA27344; 114C120; AC02-05CH11231
Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 143; Journal Issue: 14; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)
Research Org:
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPER FLUIDITY; 37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; 97 MATHEMATICS, COMPUTING, AND INFORMATION SCIENCE; high pressure; equations of state; X-ray diffraction; phase transitions; molecular dynamics
OSTI Identifier:
1251076
Alternate Identifier(s):
OSTI ID: 1421222; OSTI ID: 1440912

Stavou, Elissaios, Manaa, M. Riad, Zaug, Joseph M., Kuo, I-Feng W., Pagoria, Philip F., Crowhurst, Jonathan C., Armstrong, Michael R., and Kalkan, Bora. 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., Web. doi:10.1063/1.4932683.
Stavou, Elissaios, Manaa, M. Riad, Zaug, Joseph M., Kuo, I-Feng W., Pagoria, Philip F., Crowhurst, Jonathan C., Armstrong, Michael R., & Kalkan, Bora. 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. doi:10.1063/1.4932683.
Stavou, Elissaios, Manaa, M. Riad, Zaug, Joseph M., Kuo, I-Feng W., Pagoria, Philip F., Crowhurst, Jonathan C., Armstrong, Michael R., and Kalkan, Bora. 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. doi:10.1063/1.4932683. https://www.osti.gov/servlets/purl/1251076.
@article{osti_1251076,
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 = {Stavou, Elissaios and Manaa, M. Riad and Zaug, Joseph M. and Kuo, I-Feng W. and Pagoria, Philip F. and Crowhurst, Jonathan C. and Armstrong, Michael R. and Kalkan, Bora},
abstractNote = {Recent theoretical studies of 2,6-diamino-3,5-dinitropyrazine-1-oxide (C4H4N6O5 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. As a result, we find very good agreement between the experimental and theoretically derived EOS.},
doi = {10.1063/1.4932683},
journal = {Journal of Chemical Physics},
number = 14,
volume = 143,
place = {United States},
year = {2015},
month = {10}
}

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