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Title: Quantum Dynamics of H 2 Trapped within Organic Clathrate Cages

Abstract

The rotational and translational dynamics of molecular hydrogen trapped within β-hydroquinone clathrate (H2@β-HQ)—a practical example of a quantum particle trapped within an anisotropic confining potential—were investigated using inelastic neutron scattering and Raman spectroscopy. High-resolution vibrational spectra, including those collected from the VISION spectrometer at Oak Ridge National Laboratory, indicate relatively strong attractive interaction between guest and host with a strikingly large splitting of rotational energy levels compared with similar guest-host systems. Unlike related molecular systems in which confined H2 exhibits nearly free rotation, the behavior of H2@β-HQ is explained using a two-dimensional (2D) hindered rotor model with barrier height more than 2 times the rotational constant (-16.2 meV).

Authors:
 [1];  [2];  [2];  [1];  [3];  [3];  [2]
  1. Carnegie Inst. of Washington, Washington, DC (United States)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  3. National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Energy Frontier Research Centers (EFRC) (United States). Energy Frontier Research in Extreme Environments (EFree)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1486932
Alternate Identifier(s):
OSTI ID: 1429132
Grant/Contract Number:  
AC05-00OR22725; SC0001057; AC0500OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review Letters
Additional Journal Information:
Journal Volume: 120; Journal Issue: 12; Journal ID: ISSN 0031-9007
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS

Citation Formats

Strobel, Timothy A., Ramirez-Cuesta, Anibal J., Daemen, Luke L., Bhadram, Venkata S., Jenkins, Timothy A., Brown, Craig M., and Cheng, Yongqiang. Quantum Dynamics of H2 Trapped within Organic Clathrate Cages. United States: N. p., 2018. Web. doi:10.1103/PhysRevLett.120.120402.
Strobel, Timothy A., Ramirez-Cuesta, Anibal J., Daemen, Luke L., Bhadram, Venkata S., Jenkins, Timothy A., Brown, Craig M., & Cheng, Yongqiang. Quantum Dynamics of H2 Trapped within Organic Clathrate Cages. United States. https://doi.org/10.1103/PhysRevLett.120.120402
Strobel, Timothy A., Ramirez-Cuesta, Anibal J., Daemen, Luke L., Bhadram, Venkata S., Jenkins, Timothy A., Brown, Craig M., and Cheng, Yongqiang. Fri . "Quantum Dynamics of H2 Trapped within Organic Clathrate Cages". United States. https://doi.org/10.1103/PhysRevLett.120.120402. https://www.osti.gov/servlets/purl/1486932.
@article{osti_1486932,
title = {Quantum Dynamics of H2 Trapped within Organic Clathrate Cages},
author = {Strobel, Timothy A. and Ramirez-Cuesta, Anibal J. and Daemen, Luke L. and Bhadram, Venkata S. and Jenkins, Timothy A. and Brown, Craig M. and Cheng, Yongqiang},
abstractNote = {The rotational and translational dynamics of molecular hydrogen trapped within β-hydroquinone clathrate (H2@β-HQ)—a practical example of a quantum particle trapped within an anisotropic confining potential—were investigated using inelastic neutron scattering and Raman spectroscopy. High-resolution vibrational spectra, including those collected from the VISION spectrometer at Oak Ridge National Laboratory, indicate relatively strong attractive interaction between guest and host with a strikingly large splitting of rotational energy levels compared with similar guest-host systems. Unlike related molecular systems in which confined H2 exhibits nearly free rotation, the behavior of H2@β-HQ is explained using a two-dimensional (2D) hindered rotor model with barrier height more than 2 times the rotational constant (-16.2 meV).},
doi = {10.1103/PhysRevLett.120.120402},
journal = {Physical Review Letters},
number = 12,
volume = 120,
place = {United States},
year = {Fri Mar 23 00:00:00 EDT 2018},
month = {Fri Mar 23 00:00:00 EDT 2018}
}

Journal Article:

Citation Metrics:
Cited by: 5 works
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Figures / Tables:

FIG. 1. FIG. 1. : Experimental INS spectra collected at VISION from sample formed using $n$-H2 recorded at 5 K. Pure ortho and para contributions were obtained by measuring two different samples with known concentrations. The experimental spectrum is shifted upward from the individual ortho and para contributions. The inset shows themore » low-energy region with J=1 fundamental center-of-mass rattling modes and J=0 rotational doublet. Peaks were fit using Voigt profile functions.« less

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Works referencing / citing this record:

Assignment of Terahertz Modes in Hydroquinone Clathrates
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Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.