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Electronic and magnetic structure of neutral radical FBBO

机译:中性自由基FBBO的电子和磁性结构

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The fluorinated oxobenzo-bridged bisdithiazolyl radical FBBO was recently observed to undergo a pressure-induced Mott insulator-to-metal transition, suggesting a novel organic system for studying Mott physics. This report describes the electronic structure of this material in relation to the observed magnetic response at low pressures. Through analysis of antiferromagnetic resonance measurements, we identify a layered antiferromagnetic ordered phase below T_N = 13 K at ambient pressure, which requires strong ferromagnetic coupling between nearest neighbours. The origin of such coupling is elucidated from both molecular and solid-state electronic-structure calculations, which suggest a minimal two-orbital model with strong Hund's-rule coupling. This layered phase is partially frustrated by a second-nearest-neighbor antiferromagnetic coupling, which drives a magnetic phase transition at elevated pressure. On the basis of the two-orbital model, we suggest the pressure-induced Mott transition to proceed via rehybridization of the frontier molecular orbitals, resulting in a half-filled insulator to quarter-filled metal crossover.
机译:最近观察到,氟化的氧代苯并桥连的双二噻唑基自由基FBBO经历了压力诱导的Mott绝缘体到金属的转变,这为研究Mott物理学提供了一种新颖的有机体系。该报告描述了该材料的电子结构与在低压下观察到的磁响应的关系。通过反铁磁共振测量的分析,我们确定了在环境压力下T_N = 13 K以下的分层反铁磁有序相,这需要最近邻之间的强铁磁耦合。分子和固态电子结构计算都阐明了这种耦合的起源,这表明了具有强汉德规则耦合的最小二轨道模型。第二近邻反铁磁耦合会部分阻止此分层相,该耦合会在高压下驱动磁相变。在双轨道模型的基础上,我们建议通过边界分子轨道的再杂交来进行压力诱导的Mott转变,从而导致半填充绝缘子与四分之一填充金属的交叉。

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