Abstract
α-Glycine is studied up to 50 GPa using synchrotron angle-dispersive X-ray powder diffraction (XRD), Raman spectroscopy, and quantum chemistry calculations performed at multiples levels of theory. Results from both XRD and Raman experiments reveal an extended pressure stability of the α phase up to 50 GPa and the room temperature (RT) equation of state (EOS) was determined up to this pressure. This extended stability is corroborated by density functional theory (DFT) based calculations using the USPEX evolutionary structural search algorithm. Two calculated EOSs, as determined by DFT at T = 0 K and semiempirical density functional tight-binding (DFTB) at RT, and the calculated Raman modes frequencies show a good agreement with the corresponding experimental results. Our work provides a definitive phase diagram and EOS for α-glycine up to 50 GPa, which informs prebiotic synthesis scenarios that can involve pressures well in excess of 10 GPa.
| Original language | English |
|---|---|
| Pages (from-to) | 4457-4464 |
| Number of pages | 8 |
| Journal | CrystEngComm |
| Volume | 21 |
| Issue number | 30 |
| DOIs | |
| State | Published - 2019 |
Funding
This work was performed under the auspices of the U. S. Department of Energy by Lawrence Livermore National Security, LLC under Contract DE-AC52-07NA27344. We gratefully acknowledge the LLNL LDRD program for funding support of this project under 18-LW-036. Part of this work was performed at GeoSoilEnviroCARS (The University of Chicago, Sector 13), Advanced Photon Source (APS), Argonne National Laboratory. GeoSoilEnviroCARS is supported by the National Science Foundation - Earth Sciences (EAR-1634415) and Department of Energy-GeoSciences (DE-FG02-94ER14466). This research used resources of the Advanced Photon Source, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE-AC02-06CH11357. Use of the COMPRES-GSECARS gas loading system was supported by COMPRES under NSF Cooperative Agreement EAR -1606856 and by GSECARS through NSF grant EAR-1634415 and DOE grant DE-FG02-94ER14466. The ALS is supported by the Direc- tor, Office of Science, BES of DOE under Contract No. DE-AC02-05CH11231, DE-AC02-06CH11357. The authors thank Sergey N. Tkachev and Andrew Doran for helping with the gas loading at sector 13 GSECARS (APS) and Beamline 12.2.2. (ALS) respectively. We thank J. M. Zaug and A. Salamat for fruitful discussions and for a critical reading of the manuscript. This work was performed under the auspices of the U. S. Department of Energy by Lawrence Livermore National Security, LLC under Contract DE-AC52-07NA27344. We gratefully acknowledge the LLNL LDRD program for funding support of this project under 18-LW-036. Part of this work was performed at GeoSoilEnviroCARS (The University of Chicago, Sector 13), Advanced Photon Source (APS), Argonne National Laboratory. GeoSoilEnviroCARS is supported by the National Science Foundation - Earth Sciences (EAR-1634415) and Department of Energy-GeoSciences (DE-FG02-94ER14466). This research used resources of the Advanced Photon Source, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE-AC02-06CH11357. Use of the COMPRES-GSECARS gas loading system was supported by COMPRES under NSF Cooperative Agreement EAR-1606856 and by GSECARS through NSF grant EAR-1634415 and DOE grant DE-FG02-94ER14466. The ALS is supported by the Director, Office of Science, BES of DOE under Contract No. DEAC02-05CH11231, DE-AC02-06CH11357. The authors thank Sergey N. Tkachev and Andrew Doran for helping with the gas loading at sector 13 GSECARS (APS) and Beamline 12.2.2. (ALS) respectively. We thank J. M. Zaug and A. Salamat for fruitful discussions and for a critical reading of the manuscript.