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| Naji, M. |
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| Motta, Antonella |
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| Mohamed, Tarek |
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| Ertürk, Emre |
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| Taccardi, Nicola |
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| Petrov, R. H. | Madrid |
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| Azam, Siraj |
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| Ali, M. A. |
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| Rančić, M. |
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| Azevedo, Nuno Monteiro |
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Ranieri, Umbertoluca
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article
High‐Pressure Synthesis of Ultra‐Incompressible, Hard and Superconducting Tungsten Nitrides
Abstract
<jats:title>Abstract</jats:title><jats:p>Transition metal nitrides, particularly those of 5<jats:italic>d</jats:italic> metals, are known for their outstanding properties, often relevant for industrial applications. Among these metal elements, tungsten is especially attractive given its low cost. In this high‐pressure investigation of the W–N system, two novel ultra‐incompressible tungsten nitride superconductors, namely W<jats:sub>2</jats:sub>N<jats:sub>3</jats:sub> and W<jats:sub>3</jats:sub>N<jats:sub>5</jats:sub>, are successfully synthesized at 35 and 56 GPa, respectively, through a direct reaction between N<jats:sub>2</jats:sub> and W in laser‐heated diamond anvil cells. Their crystal structure is determined using synchrotron single‐crystal X‐ray diffraction. While the W<jats:sub>2</jats:sub>N<jats:sub>3</jats:sub> solid's sole constituting nitrogen species are N<jats:sup>3‐</jats:sup> units, W<jats:sub>3</jats:sub>N<jats:sub>5</jats:sub> features both discrete N<jats:sup>3‐</jats:sup> as well as N<jats:sub>2</jats:sub><jats:sup>4‐</jats:sup> pernitride anions. The bulk modulus of W<jats:sub>2</jats:sub>N<jats:sub>3</jats:sub> and W<jats:sub>3</jats:sub>N<jats:sub>5</jats:sub> is experimentally determined to be 380(3) and 406(7) GPa, and their ultra‐incompressible behavior is rationalized by their constituting WN<jats:sub>7</jats:sub> polyhedra and their linkages. Importantly, both W<jats:sub>2</jats:sub>N<jats:sub>3</jats:sub> and W<jats:sub>3</jats:sub>N<jats:sub>5</jats:sub> are recoverable to ambient conditions and stable in air. Density functional theory calculations reveal W<jats:sub>2</jats:sub>N<jats:sub>3</jats:sub> and W<jats:sub>3</jats:sub>N<jats:sub>5</jats:sub> to have a Vickers hardness of 30 and 34 GPa, and superconducting transition temperatures at ambient pressure (50 GPa) of 11.6 K (9.8 K) and 9.4 K (7.2 K), respectively. Additionally, transport measurements performed at 50 GPa on W<jats:sub>2</jats:sub>N<jats:sub>3</jats:sub> corroborate with the calculations.</jats:p>