Emergent cooperative superstructures via order-disorder kinetics in molecular intercalation superlattices
- Taiga Ueda
- Hideki Matsuoka
- Shungo Aoyagi
- Shunsuke Kitou
- Yijin Zhang
- Fumihiko Kimura
- Kenta Hagiwara
- Masato Sakano
- Takahiro Iwagaki
- Yuiga Nakamura
- Kyoko Ishizaka
- Tomoki Machida
- Masayuki Suda
- Taka-hisa Arima
- Naoya Kanazawa
2026-08-05
Molecular intercalation superlattices, formed by inserting organic molecules into van der Waals crystals, create inorganic-organic hybrid interfaces that have enabled a variety of emergent phenomena. Traditionally, the intercalated molecules have been regarded as inactive spacers, while their collective ordering have remained largely unexplored. Here, we report the discovery of a cooperative superstructure phase in molecule-intercalated niobium diselenide (NbSe 2 ), where ordering of the guest molecules induce a superstructure in the NbSe 2 host lattice, characterized by a moiré structure due to incommensurability between molecular and inorganic lattices. Thermal-quench measurements show that the transition is governed by slow order-disorder kinetics, contrasting with fast charge or magnetic ordering in inorganic solids. Our findings establish molecular ordering as a route for engineering heterointerfaces, enabling thermally programmable superstructures.