Inelastic neutron scattering evidence for anomalous H–H distances in metal hydrides

Andreas Borgschulte; Jasmin Terreni; Emanuel Billeter; Luke Daemen; Yongqiang Cheng; Anup Pandey; Zbigniew Łodziana; Russell J. Hemley; Anibal J. Ramirez-Cuesta

doi:10.1073/pnas.1912900117

Inelastic neutron scattering evidence for anomalous H–H distances in metal hydrides

Andreas Borgschulte, Jasmin Terreni, Emanuel Billeter, Luke Daemen, Yongqiang Cheng, Anup Pandey, Zbigniew Łodziana, Russell J. Hemley, Anibal J. Ramirez-Cuesta

Research output: Contribution to journal › Article › peer-review

29 Scopus citations

Abstract

Hydrogen-containing materials are of fundamental as well as technological interest. An outstanding question for both is the amount of hydrogen that can be incorporated in such materials, because that determines dramatically their physical properties such as electronic and crystalline structure. The number of hydrogen atoms in a metal is controlled by the interaction of hydrogens with the metal and by the hydrogen–hydrogen interactions. It is well established that the minimal possible hydrogen–hydrogen distances in conventional metal hydrides are around 2.1 Å under ambient conditions, although closer H–H distances are possible for materials under high pressure. We present inelastic neutron scattering measurements on hydrogen in ZrV₂Hx showing nonexpected scattering at low-energy transfer. The analysis of the spectra reveals that these spectral features in part originate from hydrogen vibrations confined by neighboring hydrogen at distances as short as 1.6 Å. These distances are much smaller than those found in related hydrides, thereby violating the so-called Switendick criterion. The results have implications for the design and creation of hydrides with additional properties and applications.

Original language	English
Pages (from-to)	4021-4026
Number of pages	6
Journal	Proceedings of the National Academy of Sciences of the United States of America
Volume	117
Issue number	8
DOIs	https://doi.org/10.1073/pnas.1912900117
State	Published - Feb 25 2020
Externally published	Yes

Funding

ACKNOWLEDGMENTS. This research benefited from the use of the VISION beamline (IPTS-16527) at the Spallation Neutron Source, Oak Ridge National Laboratory (ORNL), which is supported by the Scientific User Facilities Division, Office of Basic Energy Sciences, US Department of Energy (DOE). This research used resources of the Oak Ridge Leadership Computing Facility at the ORNL, which is supported by the Office of Science of the DOE under Contract DE-AC05-00OR22725. oClimax is a part of the Integrated Computational Environment Modeling and Analysis of Neutron Data (ICEMAN) (LDRD 8237) project, funded by the Laboratory Directed Research and Development program at ORNL. This work was partly supported by the UZH-UFSP program LightChEC. We also acknowledge the financial support from the Swiss National Science Foundation (Grant 172662), the US NSF (DMR-1809783), and the US DOE/National Nuclear Security Administration (DE-NA0003858, CDAC). Financial support from NCBiR Project BIOSTRATEG2/297310/13/NCBR/2016 and CPU allocation at PL-Grid is also kindly acknowledged. Beam time at ISIS, Rutherford Appleton Laboratory is also greatly acknowledged. We thank Jon Taylor, Stewart Ross, Elsa Callini, and Andreas Züttel for help and support for measurements at the TOSCA and MARI beam lines, ISIS, Rutherford Appleton Laboratory, United Kingdom. This research benefited from the use of the VISION beamline (IPTS-16527) at the Spallation Neutron Source, Oak Ridge National Laboratory (ORNL), which is supported by the Scientific User Facilities Division, Office of Basic Energy Sciences, US Department of Energy (DOE). This research used resources of the Oak Ridge Leadership Computing Facility at the ORNL, which is supported by the Office of Science of the DOE under Contract DE-AC05-00OR22725. oClimax is a part of the Integrated Computational Environment Modeling and Analysis of Neutron Data (ICEMAN) (LDRD 8237) project, funded by the Laboratory Directed Research and Development program at ORNL. This work was partly supported by the UZH-UFSP program LightChEC. We also acknowledge the financial support from the Swiss National Science Foundation (Grant 172662), the US NSF (DMR-1809783), and the US DOE/National Nuclear Security Administration (DE-NA0003858, CDAC). Financial support from NCBiR Project BIOSTRATEG2/297310/13/NCBR/2016 and CPU allocation at PL-Grid is also kindly acknowledged. Beam time at ISIS, Rutherford Appleton Laboratory is also greatly acknowledged. We thank Jon Taylor, Stewart Ross, Elsa Callini, and Andreas Z?ttel for help and support for measurements at the TOSCA and MARI beam lines, ISIS, Rutherford Appleton Laboratory, United Kingdom.

Funders	Funder number
CDAC
ISIS
NCBiR
Office of Basic Energy Sciences
Scientific User Facilities Division
US DOE/National Nuclear Security Administration
US Department of Energy
UZH-UFSP
National Science Foundation	1933622, DMR-1809783
U.S. Department of Energy
Office of Science	DE-AC05-00OR22725, LDRD 8237
Basic Energy Sciences
National Nuclear Security Administration	DE-NA0003858
Oak Ridge National Laboratory
Laboratory Directed Research and Development
Rutherford Appleton Laboratory
Schweizerischer Nationalfonds zur Förderung der Wissenschaftlichen Forschung	172662
Narodowe Centrum Badań i Rozwoju	BIOSTRATEG2/297310/13/NCBR/2016

Keywords

Diffusion
Hydrogen correlation
Inelastic neutron scattering
Intermetallic hydrides
Switendick criterion

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10.1073/pnas.1912900117

Cite this

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title = "Inelastic neutron scattering evidence for anomalous H–H distances in metal hydrides",

abstract = "Hydrogen-containing materials are of fundamental as well as technological interest. An outstanding question for both is the amount of hydrogen that can be incorporated in such materials, because that determines dramatically their physical properties such as electronic and crystalline structure. The number of hydrogen atoms in a metal is controlled by the interaction of hydrogens with the metal and by the hydrogen–hydrogen interactions. It is well established that the minimal possible hydrogen–hydrogen distances in conventional metal hydrides are around 2.1 {\AA} under ambient conditions, although closer H–H distances are possible for materials under high pressure. We present inelastic neutron scattering measurements on hydrogen in ZrV2Hx showing nonexpected scattering at low-energy transfer. The analysis of the spectra reveals that these spectral features in part originate from hydrogen vibrations confined by neighboring hydrogen at distances as short as 1.6 {\AA}. These distances are much smaller than those found in related hydrides, thereby violating the so-called Switendick criterion. The results have implications for the design and creation of hydrides with additional properties and applications.",

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author = "Andreas Borgschulte and Jasmin Terreni and Emanuel Billeter and Luke Daemen and Yongqiang Cheng and Anup Pandey and Zbigniew {\L}odziana and Hemley, {Russell J.} and Ramirez-Cuesta, {Anibal J.}",

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doi = "10.1073/pnas.1912900117",

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AU - Borgschulte, Andreas

AU - Terreni, Jasmin

AU - Billeter, Emanuel

AU - Daemen, Luke

AU - Cheng, Yongqiang

AU - Pandey, Anup

AU - Łodziana, Zbigniew

AU - Hemley, Russell J.

AU - Ramirez-Cuesta, Anibal J.

PY - 2020/2/25

Y1 - 2020/2/25

N2 - Hydrogen-containing materials are of fundamental as well as technological interest. An outstanding question for both is the amount of hydrogen that can be incorporated in such materials, because that determines dramatically their physical properties such as electronic and crystalline structure. The number of hydrogen atoms in a metal is controlled by the interaction of hydrogens with the metal and by the hydrogen–hydrogen interactions. It is well established that the minimal possible hydrogen–hydrogen distances in conventional metal hydrides are around 2.1 Å under ambient conditions, although closer H–H distances are possible for materials under high pressure. We present inelastic neutron scattering measurements on hydrogen in ZrV2Hx showing nonexpected scattering at low-energy transfer. The analysis of the spectra reveals that these spectral features in part originate from hydrogen vibrations confined by neighboring hydrogen at distances as short as 1.6 Å. These distances are much smaller than those found in related hydrides, thereby violating the so-called Switendick criterion. The results have implications for the design and creation of hydrides with additional properties and applications.

AB - Hydrogen-containing materials are of fundamental as well as technological interest. An outstanding question for both is the amount of hydrogen that can be incorporated in such materials, because that determines dramatically their physical properties such as electronic and crystalline structure. The number of hydrogen atoms in a metal is controlled by the interaction of hydrogens with the metal and by the hydrogen–hydrogen interactions. It is well established that the minimal possible hydrogen–hydrogen distances in conventional metal hydrides are around 2.1 Å under ambient conditions, although closer H–H distances are possible for materials under high pressure. We present inelastic neutron scattering measurements on hydrogen in ZrV2Hx showing nonexpected scattering at low-energy transfer. The analysis of the spectra reveals that these spectral features in part originate from hydrogen vibrations confined by neighboring hydrogen at distances as short as 1.6 Å. These distances are much smaller than those found in related hydrides, thereby violating the so-called Switendick criterion. The results have implications for the design and creation of hydrides with additional properties and applications.

KW - Diffusion

KW - Hydrogen correlation

KW - Inelastic neutron scattering

KW - Intermetallic hydrides

KW - Switendick criterion

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Inelastic neutron scattering evidence for anomalous H–H distances in metal hydrides

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