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Naji, M. |
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Motta, Antonella |
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Aletan, Dirar |
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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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Casati, R. |
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Kočí, Jan | Prague |
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Azam, Siraj |
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Ali, M. A. |
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Rančić, M. |
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Ollier, Nadège |
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Azevedo, Nuno Monteiro |
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Landes, Michael |
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Rignanese, Gian-Marco |
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Anas, Mohd
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article
Robust Spin Liquidity in 2D Metal‐Organic Framework Cu<sub>3</sub> (HHTP)<sub>2</sub> with S=<sup>1</sup>/<sub>2</sub> Kagome Lattice
Abstract
<jats:title>Abstract</jats:title><jats:p>On one hand electron or hole doping of quantum spin liquid (QSL) may unlock high‐temperature superconductivity and on the other hand it can disrupt the spin liquidity, giving rise to a magnetically ordered ground state. Recently, a 2D MOF, Cu<jats:sub>3</jats:sub>(HHTP)<jats:sub>2</jats:sub> (HHTP ‐ 2,3,6,7,10,11‐hexahydroxytriphenylene), containing Cu(II) S=<jats:inline-graphic xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="graphic/chem202303718-math-0001.png" xlink:title="urn:x-wiley:09476539:media:chem202303718:chem202303718-math-0001" />frustrated spins in the Kagome lattice is emerging as a promising QSL candidate. Herein, we present an elegant in situ redox‐chemistry strategy of anchoring Cu<jats:sub>3</jats:sub>(HHTP)<jats:sub>2</jats:sub> crystallites onto diamagnetic reduced graphene oxide (rGO) sheets, resulting in the formation of electron‐doped Cu<jats:sub>3</jats:sub>(HHTP)<jats:sub>2</jats:sub>‐rGO composite which exhibited a characteristic semiconducting behavior (5 K to 300 K) with high electrical conductivity of 70 S ⋅ m<jats:sup>−1</jats:sup> and a carrier density of ~1.1×10<jats:sup>18</jats:sup> cm<jats:sup>−3</jats:sup> at 300 K. Remarkably, no magnetic transition in the Cu<jats:sub>3</jats:sub>(HHTP)<jats:sub>2</jats:sub>‐rGO composite was observed down to 1.5 K endorsing the robust spin liquidity of the 2D MOF Cu<jats:sub>3</jats:sub>(HHTP)<jats:sub>2</jats:sub>. Specific heat capacity measurements led to the estimation of the residual entropy values of 28 % and 34 % of the theoretically expected value for the pristine Cu<jats:sub>3</jats:sub>(HHTP)<jats:sub>2</jats:sub> and Cu<jats:sub>3</jats:sub>(HHTP)<jats:sub>2</jats:sub>‐rGO composite, establishing the presence of strong quantum fluctuations down to 1.5 K (two times smaller than the value of the exchange interaction <jats:italic>J</jats:italic>).</jats:p>