Emergent Cooperative Superstructures via Order-Disorder Kinetics in Molecule-Intercalated NbSe2

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Main Authors: Ueda, Taiga, Matsuoka, Hideki, Aoyagi, Shungo, Kitou, Shunsuke, Zhang, Yijin, Kimura, Fumihiko, Hagiwara, Kenta, Sakano, Masato, Iwagaki, Takahiro, Nakamura, Yuiga, Ishizaka, Kyoko, Machida, Tomoki, Suda, Masayuki, Arima, Taka-hisa, Kanazawa, Naoya
Format: Preprint
Published: 2026
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author Ueda, Taiga
Matsuoka, Hideki
Aoyagi, Shungo
Kitou, Shunsuke
Zhang, Yijin
Kimura, Fumihiko
Hagiwara, Kenta
Sakano, Masato
Iwagaki, Takahiro
Nakamura, Yuiga
Ishizaka, Kyoko
Machida, Tomoki
Suda, Masayuki
Arima, Taka-hisa
Kanazawa, Naoya
author_facet Ueda, Taiga
Matsuoka, Hideki
Aoyagi, Shungo
Kitou, Shunsuke
Zhang, Yijin
Kimura, Fumihiko
Hagiwara, Kenta
Sakano, Masato
Iwagaki, Takahiro
Nakamura, Yuiga
Ishizaka, Kyoko
Machida, Tomoki
Suda, Masayuki
Arima, Taka-hisa
Kanazawa, Naoya
contents The design of quantum states at heterointerfaces has enabled a variety of emergent phenomena. Among them, molecular intercalation superlattices have attracted attention as tunable hybrid materials, formed by inserting organic molecules into van der Waals crystals, where molecular structure and chemistry provide new degrees of freedom. Traditionally, the intercalated molecules have been regarded as inactive spacers, while possible molecular ordering and its impact on the host lattice have remained largely unexplored. Here, we report the discovery of a cooperative superstructure (CSS) phase in molecule intercalated NbSe2, where ordering of the guest molecules induce a concomitant superstructure in the NbSe2 host lattice, characterized by a moiré structure due to incommensurability between the molecular layer and the inorganic lattice. Synchrotron X-ray diffraction reveals the emergence of CSS phase, accompanied by crystal symmetry lowering. Complementary resistivity and thermal-quench measurements show that the transition is governed by unusually slow order-disorder kinetics, so that the CSS phase can be selectively accessed under standard laboratory cooling rates. This kinetic behavior arises from slow molecular dynamics coupled to the host lattice, 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.
format Preprint
id arxiv_https___arxiv_org_abs_2601_07216
institution arXiv
publishDate 2026
record_format arxiv
spellingShingle Emergent Cooperative Superstructures via Order-Disorder Kinetics in Molecule-Intercalated NbSe2
Ueda, Taiga
Matsuoka, Hideki
Aoyagi, Shungo
Kitou, Shunsuke
Zhang, Yijin
Kimura, Fumihiko
Hagiwara, Kenta
Sakano, Masato
Iwagaki, Takahiro
Nakamura, Yuiga
Ishizaka, Kyoko
Machida, Tomoki
Suda, Masayuki
Arima, Taka-hisa
Kanazawa, Naoya
Materials Science
The design of quantum states at heterointerfaces has enabled a variety of emergent phenomena. Among them, molecular intercalation superlattices have attracted attention as tunable hybrid materials, formed by inserting organic molecules into van der Waals crystals, where molecular structure and chemistry provide new degrees of freedom. Traditionally, the intercalated molecules have been regarded as inactive spacers, while possible molecular ordering and its impact on the host lattice have remained largely unexplored. Here, we report the discovery of a cooperative superstructure (CSS) phase in molecule intercalated NbSe2, where ordering of the guest molecules induce a concomitant superstructure in the NbSe2 host lattice, characterized by a moiré structure due to incommensurability between the molecular layer and the inorganic lattice. Synchrotron X-ray diffraction reveals the emergence of CSS phase, accompanied by crystal symmetry lowering. Complementary resistivity and thermal-quench measurements show that the transition is governed by unusually slow order-disorder kinetics, so that the CSS phase can be selectively accessed under standard laboratory cooling rates. This kinetic behavior arises from slow molecular dynamics coupled to the host lattice, 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.
title Emergent Cooperative Superstructures via Order-Disorder Kinetics in Molecule-Intercalated NbSe2
topic Materials Science
url https://arxiv.org/abs/2601.07216