Manipulating electron redistribution to achieve electronic pyroelectricity in molecular [FeCo] crystals

Pritam Sadhukhan, Shu-Qi Wu, Jeremy Ian Long, Takumi Nakanishi, Shinji Kanegawa (), Kaige Gao, Kaoru Yamamoto, Hajime Okajima, Akira Sakamoto, Michael L. Baker, Thomas Kroll, Dimosthenis Sokaras, Atsushi Okazawa, Norimichi Kojima, Yoshihito Shiota, Kazunari Yoshizawa and Osamu Sato ()
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Pritam Sadhukhan: Kyushu University
Shu-Qi Wu: Kyushu University
Jeremy Ian Long: Kyushu University
Takumi Nakanishi: Kyushu University
Shinji Kanegawa: Kyushu University
Kaige Gao: Yangzhou University
Kaoru Yamamoto: Okayama University of Science
Hajime Okajima: Aoyama Gakuin University
Akira Sakamoto: Aoyama Gakuin University
Michael L. Baker: The University of Manchester
Thomas Kroll: Stanford University
Dimosthenis Sokaras: Stanford University
Atsushi Okazawa: Nihon University School of Medicine, 30-1 Oyaguchi Kamimachi, Itabashi-ku
Norimichi Kojima: The University of Tokyo, 3-8-1 Komaba, Meguro-ku
Yoshihito Shiota: Kyushu University
Kazunari Yoshizawa: Kyushu University
Osamu Sato: Kyushu University

Nature Communications, 2021, vol. 12, issue 1, 1-9

Abstract: Abstract Pyroelectricity plays a crucial role in modern sensors and energy conversion devices. However, obtaining materials with large and nearly constant pyroelectric coefficients over a wide temperature range for practical uses remains a formidable challenge. Attempting to discover a solution to this obstacle, we combined molecular design of labile electronic structure with the crystal engineering of the molecular orientation in lattice. This combination results in electronic pyroelectricity of purely molecular origin. Here, we report a polar crystal of an [FeCo] dinuclear complex exhibiting a peculiar pyroelectric behavior (a substantial sharp pyroelectric current peak and an unusual continuous pyroelectric current at higher temperatures) which is caused by a combination of Fe spin crossover (SCO) and electron transfer between the high-spin Fe ion and redox-active ligand, namely valence tautomerism (VT). As a result, temperature dependence of the pyroelectric behavior reported here is opposite from conventional ferroelectrics and originates from a transition between three distinct electronic structures. The obtained pyroelectric coefficient is comparable to that of polyvinylidene difluoride at room temperature.

Date: 2021
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DOI: 10.1038/s41467-021-25041-4

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