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Investigation of electronic, optical, and magnetic properties of a quasi-one-dimensional molecular Mott insulator

Nuryadin Muhammad Khalish 東北大学

2022.09.26

概要

BEDT-TTF (bis(ethylenedithio)-tetrathiafulvalene) molecule-based organic salts have been considered as one of strongly correlated electron systems which indicate Mott insulating, charge ordering, quantum spin liquid, anisotropic superconducting states and so on [1]. In most cases of the organic molecular materials, previous studies have been carried out in BEDT-TTF salts with donor and anion molecule ratio of 2:1. These salts have one hole carrier averagely in two BEDT-TTF molecules resulting in the quarter filling conduction band in principle. In contrast, a series of κ-(BEDTTTF)2X (X = Cu[N(CN)2]Y with Y = Br and Cl, Cu2(CN)3 etc.) has the BEDT-TTF dimer structure. Strong dimerization of BEDT-TTF molecules changes the quarter filling band structure to an effective half filling band. This effective half filling band structure is the origin of the dimer Mott insulating state with strongly correlated -electrons.

Although active studies in the dimer-Mott organic salts, only few studies have been conducted in BEDTTTF salts with a 1:1 ratio, which should have a genuine Mott insulating state with a half-filling band. Previous reports in 1:1 ratio of BEDT-TTF salts such as ζ-(BEDT-TTF)PF6 and β-(BEDT-TTF)TaF6 show that both salts are considered as a genuine Mott insulator material [2]. Recently, another 1:1 BEDT-TTF organic salt, (BEDT-TTF)Ag4(CN)5, has been studied as a candidate of Dirac Semimetal (DSM) with diamond lattice structure [3]. It has a Mott-insulating ground state with antiferromagnetic order at TN = 102 K.

(BEDT-TTF)Cu[N(CN)2]2 is an organic salt with 1:1 ratio of donor BEDT-TTF+1 and anion molecules Cu[N(CN)2]2 -1 . (BEDT-TTF)Cu[N(CN)2]2 was first reported by Wang et. al. [4], where the crystal has monoclinic structure and C2/c space group. Wang et al. concluded this compound as a semiconductor. However, (BEDT-TTF)Cu[N(CN)2]2 could be considered as a genuine Mott insulator from the half-filling band structure. (BEDT-TTF)Cu[N(CN)2]2 does not have an alternating layer structure found typically in quasi-twodimensional (BEDT-TTF)2X. Instead, this compound has three-dimensional arrangement of BEDT-TTF and anion molecules. This three-dimensional arrangement of BEDT-TTF with the shortest intramolecular distance results in a distorted diamond-like lattice structure. The band structure calculation suggested that this compound has a low dimensional system resulting in the strongest transfer integral along the c-axis direction, creating one dimensional zigzag BEDT-TTF chain [5]. These characteristics make this compound a promising subject for studying quasi-one-dimensional organic material with half-filled energy band.

In this study, the fundamental physical properties like as electronic, optical, and magnetic properties of (BEDT-TTF)Cu[N(CN)2]2 are investigated. Specially a nonmagnetic state below about 26 K was found firstly in this study [7,8], and confirmed that the state was induced by spin-singlet transition, probably considered as a spin-Peierls transition. We also study molecular disorder effect by x-ray irradiation technique.

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