High-Pressure Synthesis of Magnetic Neodymium Polyhydrides
Ongoing search for room-temperature superconductivity is inspired by the unique properties of the electron–phonon interaction in metal superhydrides. Encouraged by the recently found highest-T C superconductor fcc-LaH10, here we discover several superhydrides of another lanthanoid, neodymium. We ide...
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| Published in | Journal of the American Chemical Society Vol. 142; no. 6; pp. 2803 - 2811 |
|---|---|
| Main Authors | , , , , , , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
United States
American Chemical Society
12.02.2020
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| Abstract | Ongoing search for room-temperature superconductivity is inspired by the unique properties of the electron–phonon interaction in metal superhydrides. Encouraged by the recently found highest-T C superconductor fcc-LaH10, here we discover several superhydrides of another lanthanoid, neodymium. We identify three novel metallic Nd–H phases at pressures ranging from 85 to 135 GPa: I4/mmm-NdH4, C2/c-NdH7, and P63/mmc-NdH9, synthesized by laser-heating metal samples in NH3BH3 media for in situ generation of hydrogen. A lower trihydride Fm3̅m-NdH3 is found at pressures from 2 to 52 GPa. I4/mmm-NdH4 and C2/c-NdH7 are stable from 135 to 85 GPa, and P63/mmc-NdH9 is stable from 110 to 130 GPa. Measurements of the electrical resistance of NdH9 demonstrate a possible superconducting transition at ∼4.5 K in P63/mmc-NdH9. Our theoretical calculations predict that all of the neodymium hydrides have antiferromagnetic order at pressures below 150 GPa and represent one of the first discovered examples of strongly correlated superhydrides with large exchange spin-splitting in the electronic band structure (>450 meV). The critical Néel temperatures for new neodymium hydrides are estimated using the mean-field approximation to be about 4 K (NdH4), 251 K (NdH7), and 136 K (NdH9). |
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| AbstractList | Ongoing search for room-temperature superconductivity is inspired by the unique properties of the electron-phonon interaction in metal superhydrides. Encouraged by the recently found highest-
superconductor
-LaH
, here we discover several superhydrides of another lanthanoid, neodymium. We identify three novel metallic Nd-H phases at pressures ranging from 85 to 135 GPa:
4/
-NdH
,
2/
-NdH
, and
6
/
-NdH
, synthesized by laser-heating metal samples in NH
BH
media for in situ generation of hydrogen. A lower trihydride
3̅
-NdH
is found at pressures from 2 to 52 GPa.
4/
-NdH
and
2/
-NdH
are stable from 135 to 85 GPa, and
6
/
-NdH
is stable from 110 to 130 GPa. Measurements of the electrical resistance of NdH
demonstrate a possible superconducting transition at ∼4.5 K in
6
/
-NdH
. Our theoretical calculations predict that all of the neodymium hydrides have antiferromagnetic order at pressures below 150 GPa and represent one of the first discovered examples of strongly correlated superhydrides with large exchange spin-splitting in the electronic band structure (>450 meV). The critical Néel temperatures for new neodymium hydrides are estimated using the mean-field approximation to be about 4 K (NdH
), 251 K (NdH
), and 136 K (NdH
). Ongoing search for room-temperature superconductivity is inspired by the unique properties of the electron-phonon interaction in metal superhydrides. Encouraged by the recently found highest-T-C superconductor fcc-LaH10, here we discover several superhydrides of another lanthanoid, neodymium. We identify three novel metallic Nd-H phases at pressures ranging from 85 to 135 GPa: I4/mmm-NdH4, C2/c-NdH7 , and P6(3)/mmc-NdH9, synthesized by laser-heating metal samples in NH3BH3 media for in situ generation of hydrogen. A lower trihydride Fm (3) over barm-NdH3 is found at pressures from 2 to 52 GPa. I4/mmm-NdH4 and C2/c-NdH7 are stable from 135 to 85 GPa, and P6(3) /mmc-NdH9 is stable from 110 to 130 GPa. Measurements of the electrical resistance of NdH9 demonstrate a possible superconducting transition at similar to 4.5 K in P6(3)/mmc-NdH9. Our theoretical calculations predict that all of the neodymium hydrides have antiferromagnetic order at pressures below 150 GPa and represent one of the first discovered examples of strongly correlated superhydrides with large exchange spin-splitting in the electronic band structure (>450 meV). The critical Neel temperatures for new neodymium hydrides are estimated using the mean-field approximation to be about 4 K (NdH4), 251 K (NdH7), and 136 K (NdH9). Ongoing search for room-temperature superconductivity is inspired by the unique properties of the electron–phonon interaction in metal superhydrides. Encouraged by the recently found highest-T C superconductor fcc-LaH10, here we discover several superhydrides of another lanthanoid, neodymium. We identify three novel metallic Nd–H phases at pressures ranging from 85 to 135 GPa: I4/mmm-NdH4, C2/c-NdH7, and P63/mmc-NdH9, synthesized by laser-heating metal samples in NH3BH3 media for in situ generation of hydrogen. A lower trihydride Fm3̅m-NdH3 is found at pressures from 2 to 52 GPa. I4/mmm-NdH4 and C2/c-NdH7 are stable from 135 to 85 GPa, and P63/mmc-NdH9 is stable from 110 to 130 GPa. Measurements of the electrical resistance of NdH9 demonstrate a possible superconducting transition at ∼4.5 K in P63/mmc-NdH9. Our theoretical calculations predict that all of the neodymium hydrides have antiferromagnetic order at pressures below 150 GPa and represent one of the first discovered examples of strongly correlated superhydrides with large exchange spin-splitting in the electronic band structure (>450 meV). The critical Néel temperatures for new neodymium hydrides are estimated using the mean-field approximation to be about 4 K (NdH4), 251 K (NdH7), and 136 K (NdH9). |
| Author | Galasso, Michele Kvashnin, Alexander G Kartsev, Alexey I Duan, Defang Aperis, Alex Oganov, Artem R Huang, Xiaoli Zhou, Di Semenok, Dmitrii V Cui, Tian Xie, Hui Oppeneer, Peter M |
| AuthorAffiliation | Queen’s University Belfast International Center for Materials Discovery Computing Center of Far Eastern Branch of the Russian Academy of Sciences (CC FEB RAS) State Key Laboratory of Superhard Materials, College of Physics Ningbo University School of Mathematics and Physics School of Physical Science and Technology Northwestern Polytechnical University Department of Physics and Astronomy |
| AuthorAffiliation_xml | – name: Ningbo University – name: School of Physical Science and Technology – name: Department of Physics and Astronomy – name: International Center for Materials Discovery – name: Northwestern Polytechnical University – name: Queen’s University Belfast – name: State Key Laboratory of Superhard Materials, College of Physics – name: Computing Center of Far Eastern Branch of the Russian Academy of Sciences (CC FEB RAS) – name: School of Mathematics and Physics |
| Author_xml | – sequence: 1 givenname: Di surname: Zhou fullname: Zhou, Di organization: State Key Laboratory of Superhard Materials, College of Physics – sequence: 2 givenname: Dmitrii V surname: Semenok fullname: Semenok, Dmitrii V – sequence: 3 givenname: Hui surname: Xie fullname: Xie, Hui organization: State Key Laboratory of Superhard Materials, College of Physics – sequence: 4 givenname: Xiaoli orcidid: 0000-0001-9628-5618 surname: Huang fullname: Huang, Xiaoli email: huangxiaoli@jlu.edu.cn organization: State Key Laboratory of Superhard Materials, College of Physics – sequence: 5 givenname: Defang orcidid: 0000-0002-6878-1830 surname: Duan fullname: Duan, Defang organization: State Key Laboratory of Superhard Materials, College of Physics – sequence: 6 givenname: Alex surname: Aperis fullname: Aperis, Alex organization: Department of Physics and Astronomy – sequence: 7 givenname: Peter M surname: Oppeneer fullname: Oppeneer, Peter M organization: Department of Physics and Astronomy – sequence: 8 givenname: Michele surname: Galasso fullname: Galasso, Michele – sequence: 9 givenname: Alexey I orcidid: 0000-0002-3916-3443 surname: Kartsev fullname: Kartsev, Alexey I organization: Queen’s University Belfast – sequence: 10 givenname: Alexander G orcidid: 0000-0002-0718-6691 surname: Kvashnin fullname: Kvashnin, Alexander G email: a.kvashnin@skoltech.ru – sequence: 11 givenname: Artem R orcidid: 0000-0002-9315-1419 surname: Oganov fullname: Oganov, Artem R email: a.oganov@skoltech.ru organization: Northwestern Polytechnical University – sequence: 12 givenname: Tian orcidid: 0000-0002-9664-848X surname: Cui fullname: Cui, Tian email: cuitian@jlu.edu.cn organization: Ningbo University |
| BackLink | https://www.ncbi.nlm.nih.gov/pubmed/31967807$$D View this record in MEDLINE/PubMed https://urn.kb.se/resolve?urn=urn:nbn:se:uu:diva-408203$$DView record from Swedish Publication Index |
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| Snippet | Ongoing search for room-temperature superconductivity is inspired by the unique properties of the electron–phonon interaction in metal superhydrides.... Ongoing search for room-temperature superconductivity is inspired by the unique properties of the electron-phonon interaction in metal superhydrides.... |
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| Title | High-Pressure Synthesis of Magnetic Neodymium Polyhydrides |
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