Blundell Toby J, Sneade Kathryn, Ogar Joseph O, Yamashita Satoshi, Akutsu Hiroki, Nakazawa Yasuhiro, Yamamoto Takashi, Martin Lee
School of Science and Technology, Nottingham Trent University, Clifton Lane, Clifton, Nottingham NG11 8NS, U.K.
Department of Chemistry, Graduate School of Science, Osaka University, 1-1 Machikaneyama-cho, Toyonaka, Osaka 560-0043, Japan.
J Am Chem Soc. 2025 Feb 19;147(7):5658-5668. doi: 10.1021/jacs.4c12386. Epub 2025 Feb 6.
The quantum spin-liquid state was first theorized by Anderson 50 years ago and the challenge remains to realize a quantum spin-liquid material. A handful of two-dimensional molecular candidates have attracted huge attention over the past 30 years owing to their triangular lattice possessing = 1/2 spin systems. We present a new quantum spin-liquid candidate in 2D Mott insulator κ-(BEDT-TTF)[B(salicylate)]. The structure has a double-width anion layer giving it a strong 2D character. The spiroborate anion is chiral and the salt is an inversion twin, having no inversion symmetry center and crystallizing in space group 2. This offers the possibility of novel behavior owing to the low symmetry not previously seen in molecular spin-liquid candidates. The peak height of the 6K anomaly of κ-(BEDT-TTF)[B(salicylate)] is 2 or 3 times larger than that of κ-(BEDT-TTF)Cu(CN) and EtMeSb[Pd(dmit)]. The structure presents many opportunities for crystal engineering through atom-by-atom changes to the ligands on the spiroborate anion to produce a family of materials which lie in and around the QSL region of the phase diagram for these salts. This gives the prospect of an experimental playground to deepen understanding of the QSL state. Electrical resistivity, SQUID magnetometry, band calculations, heat capacity, Infrared and Raman spectroscopy are reported for κ-(BEDT-TTF)[B(salicylate)].
量子自旋液体态是50年前由安德森首次提出理论的,而实现一种量子自旋液体材料仍然是一项挑战。在过去30年里,一些二维分子候选物因其具有1/2自旋系统的三角晶格而备受关注。我们展示了一种二维莫特绝缘体κ-(BEDT-TTF)[B(水杨酸盐)]中的新型量子自旋液体候选物。该结构具有双宽阴离子层,赋予其很强的二维特性。螺硼酸根阴离子是手性的,该盐是一个反演孪晶,没有反演对称中心,且结晶于空间群2。由于这种低对称性是分子自旋液体候选物中前所未见的,这提供了出现新行为的可能性。κ-(BEDT-TTF)[B(水杨酸盐)]在6K处异常的峰值高度比κ-(BEDT-TTF)Cu(CN)和EtMeSb[Pd(dmit)]的峰值高度大2到3倍。通过对螺硼酸根阴离子上的配体逐个原子进行改变,该结构为晶体工程提供了许多机会,从而产生一系列位于这些盐的相图的量子自旋液体(QSL)区域及其附近的材料。这为深入理解QSL态提供了一个实验平台。本文报道了κ-(BEDT-TTF)[B(水杨酸盐)]的电阻率、超导量子干涉仪磁强计测量、能带计算、热容、红外和拉曼光谱。