Mroweh Nabil, Mézière Cécile, Pop Flavia, Auban-Senzier Pascale, Alemany Pere, Canadell Enric, Avarvari Narcis
MOLTECH-Anjou, UMR 6200, CNRS, UNIV Angers, 2 bd Lavoisier, Angers Cedex, 49045, France.
Laboratoire de Physique des Solides, Université Paris-Saclay, CNRS UMR 8502, Orsay, 91405, France.
Adv Mater. 2020 Sep;32(36):e2002811. doi: 10.1002/adma.202002811. Epub 2020 Jul 26.
The relationship between chirality and superconductivity is an intriguing question. The two enantiomeric crystalline radical cation salts κ-[(S,S)-DM-BEDT-TTF] ClO and κ-[(R,R)-DM-BEDT-TTF] ClO , showing κ-type arrangement of the organic layers, are investigated in search for superconducting chiral molecular materials following a 1992 report indicating the occurrence of a superconducting transition in the former compound. While the initial interpretation is presently challenged through in-depth temperature and pressure dependent single crystal resistivity measurements combined with band structure calculations, the two chiral conductors show metal like behavior with room temperature conductivities of 10-30 S cm at ambient pressure and stabilization of the metallic state down to the lowest temperatures under moderate pressures. Moreover, their structural and theoretical investigations reveal an original feature, namely the existence of two different κ layers with 1D and 2D electronic dimensionality, respectively, as a consequence of an interlayer charge transfer. The resistivity drop observed for one sample below 1 K and insensitive to magnetic field, possibly results from mixing in-plane and out-of-plane contributions to the measured resistance and suggests current induced charge order melting. This feature contradicts the occurrence of superconductivity in these chiral molecular conductors and leaves open the discovery of the first chiral molecular superconductors.
手性与超导性之间的关系是一个引人入胜的问题。我们对两种对映体结晶自由基阳离子盐κ-[(S,S)-DM-BEDT-TTF]ClO和κ-[(R,R)-DM-BEDT-TTF]ClO进行了研究,这两种盐呈现出有机层的κ型排列。1992年有报告指出前一种化合物中发生了超导转变,之后我们便开始寻找超导手性分子材料。虽然目前通过结合能带结构计算的深入的温度和压力依赖性单晶电阻率测量对最初的解释提出了挑战,但这两种手性导体在室温下具有10-30 S/cm的电导率,在环境压力下表现出类似金属的行为,并且在中等压力下金属态能稳定到最低温度。此外,它们的结构和理论研究揭示了一个原始特征,即由于层间电荷转移,分别存在具有一维和二维电子维度的两种不同的κ层。在一个样品中观察到低于1 K时电阻率下降且对磁场不敏感,这可能是由于测量电阻中面内和面外贡献的混合导致的,表明电流诱导电荷序熔化。这一特征与这些手性分子导体中存在超导性相矛盾,使得首个手性分子超导体的发现仍未确定。