Novel Cooperative Interactions and Structural Ordering in H[subscript 2]S-H[subscript 2]
Abstract
Hydrogen sulfide (H{sub 2}S) and hydrogen (H{sub 2}) crystallize into a 'guest-host' structure at 3.5 GPa and, at the initial formation pressure, the rotationally disordered component molecules exhibit weak van der Waals-type interactions. With increasing pressure, hydrogen bonding develops and strengthens between neighboring H{sub 2}S molecules, reflected in a pronounced drop in S-H vibrational stretching frequency and also observed in first-principles calculations. At 17 GPa, an ordering process occurs where H{sub 2}S molecules orient themselves to maximize hydrogen bonding and H{sub 2} molecules simultaneously occupy a chemically distinct lattice site. Intermolecular forces in the H{sub 2}S+H{sub 2} system may be tuned with pressure from the weak hydrogen-bonding limit to the ordered hydrogen-bonding regime, resulting in a novel clathrate structure stabilized by cooperative interactions.
- Authors:
-
- ORNL
- Publication Date:
- Research Org.:
- Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
- Sponsoring Org.:
- NSFDOE - BASIC ENERGY SCIENCESNNSA
- OSTI Identifier:
- 1032650
- Resource Type:
- Journal Article
- Journal Name:
- Physical Review Letters
- Additional Journal Information:
- Journal Volume: 107; Journal Issue: 25; Journal ID: ISSN 0031-9007
- Country of Publication:
- United States
- Language:
- ENGLISH
- Subject:
- 08 HYDROGEN; CHEMICAL BONDS; CLATHRATES; HYDROGEN; HYDROGEN SULFIDES; INTERACTIONS; INTERMOLECULAR FORCES; MOLECULES; PRESSURE RANGE GIGA PA; RESERVOIR PRESSURE; VAN DER WAALS FORCES
Citation Formats
Strobel, Timothy A, Ganesh, P, Somayazulu, Maddury, Kent, P R.C., Hemley, Russell J, and CIW). Novel Cooperative Interactions and Structural Ordering in H[subscript 2]S-H[subscript 2]. United States: N. p., 2012.
Web. doi:10.1103/PhysRevLett.107.255503.
Strobel, Timothy A, Ganesh, P, Somayazulu, Maddury, Kent, P R.C., Hemley, Russell J, & CIW). Novel Cooperative Interactions and Structural Ordering in H[subscript 2]S-H[subscript 2]. United States. https://doi.org/10.1103/PhysRevLett.107.255503
Strobel, Timothy A, Ganesh, P, Somayazulu, Maddury, Kent, P R.C., Hemley, Russell J, and CIW). 2012.
"Novel Cooperative Interactions and Structural Ordering in H[subscript 2]S-H[subscript 2]". United States. https://doi.org/10.1103/PhysRevLett.107.255503.
@article{osti_1032650,
title = {Novel Cooperative Interactions and Structural Ordering in H[subscript 2]S-H[subscript 2]},
author = {Strobel, Timothy A and Ganesh, P and Somayazulu, Maddury and Kent, P R.C. and Hemley, Russell J and CIW)},
abstractNote = {Hydrogen sulfide (H{sub 2}S) and hydrogen (H{sub 2}) crystallize into a 'guest-host' structure at 3.5 GPa and, at the initial formation pressure, the rotationally disordered component molecules exhibit weak van der Waals-type interactions. With increasing pressure, hydrogen bonding develops and strengthens between neighboring H{sub 2}S molecules, reflected in a pronounced drop in S-H vibrational stretching frequency and also observed in first-principles calculations. At 17 GPa, an ordering process occurs where H{sub 2}S molecules orient themselves to maximize hydrogen bonding and H{sub 2} molecules simultaneously occupy a chemically distinct lattice site. Intermolecular forces in the H{sub 2}S+H{sub 2} system may be tuned with pressure from the weak hydrogen-bonding limit to the ordered hydrogen-bonding regime, resulting in a novel clathrate structure stabilized by cooperative interactions.},
doi = {10.1103/PhysRevLett.107.255503},
url = {https://www.osti.gov/biblio/1032650},
journal = {Physical Review Letters},
issn = {0031-9007},
number = 25,
volume = 107,
place = {United States},
year = {Tue Feb 07 00:00:00 EST 2012},
month = {Tue Feb 07 00:00:00 EST 2012}
}