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Pressure-induced nearly perfect rectangular lattice and superconductivity in the organic molecular crystal (DMET-TTF)2AuBr2

Taiga Kato, Hanming Ma, Kazuyoshi Yoshimi, Takahiro Misawa, Shigen Kumagai, Youhei Iida, Yoshiaki Sasaki, Masashi Sawada, Jun Gouchi, Takuya Kobayashi, Hiromi Taniguchi, Yoshiya Uwatoko, Hiroyasu Sato, Noriaki Matsunaga, Atsushi Kawamoto, Kazushige Nomura

DOI 10.1103/zx3d-lwlw · Physical Review B

T1

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Abstract

External pressure and associated changes in lattice structures are key to realizing exotic quantum phases such as high-Tc superconductivity. While applying external pressure is a standard method to induce novel lattice structures, its impact on organic molecular crystals has been less explored. Here we report a unique structural phase transition in (DMET-TTF)2AuBr2 under pressure. By combining advanced high-pressure techniques and abinitio calculations, we elucidate that (DMET-TTF)2AuBr2 undergoes a transition from a quasi-one-dimensional lattice to a nearly perfect rectangular lattice around 0.9 GPa. This transition leads to the realization of an antiferromagnetic Mott insulator with TN=66 K, the highest TN in low-dimensional molecular crystal solids to date. Upon increasing the pressure, the antiferromagnetic ordering is suppressed, and a superconducting phase with Tc=4.8 K emerges around 6 GPa. Our study reveals the significant impact of external pressure on lattice structures of organic molecular crystals and offers insights into how geometrical frustration relates to superconductivity. Our findings also pave the way for realizing functional organic molecular crystals through changes in lattice structures under pressure.

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FormulaReported Tc (K)Pressure (GPa)Type
(DMET-TTF)2AuBr2

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4.89 GPaonset
β'-(BEDT-TTF)2ICl2

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14.28.2 GPaunknown

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