Molecular orbital breaking in photo-mediated organosilicon Schiff base ferroelectric crystals

Zhu-Xiao Gu, Nan Zhang, Yao Zhang, Bin Liu, Huan-Huan Jiang, Hua-Ming Xu, Peng Wang, Qing Jiang, Ren-Gen Xiong and Han-Yue Zhang ()
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Zhu-Xiao Gu: Nanjing University
Nan Zhang: Southeast University
Yao Zhang: Southeast University
Bin Liu: Nanjing University
Huan-Huan Jiang: Southeast University
Hua-Ming Xu: Southeast University
Peng Wang: Nanjing University
Qing Jiang: Nanjing University
Ren-Gen Xiong: Nanchang University
Han-Yue Zhang: Southeast University

Nature Communications, 2024, vol. 15, issue 1, 1-10

Abstract: Abstract Ferroelectric materials, whose electrical polarization can be switched under external stimuli, have been widely used in sensors, data storage, and energy conversion. Molecular orbital breaking can result in switchable structural and physical bistability in ferroelectric materials as traditional spatial symmetry breaking does. Differently, molecular orbital breaking interprets the phase transition mechanism from the perspective of electronics and sheds new light on manipulating the physical properties of ferroelectrics. Here, we synthesize a pair of organosilicon Schiff base ferroelectric crystals, (R)- and (S)-N-(3,5-di-tert-butylbenzylidene)-1-((triphenylsilyl)oxy)ethanamine, which show optically controlled phase transition accompanying the molecular orbital breaking. The molecular orbital breaking is manifested as the breaking and reformation of covalent bonds during the phase transition process, that is, the conversion between C = N and C–O in the enol form and C–N and C = O in the keto form. This process brings about photo-mediated bistability with multiple physical channels such as dielectric, second-harmonic generation, and ferroelectric polarization. This work further explores this newly developed mechanism of ferroelectric phase transition and highlights the significance of photo-mediated ferroelectric materials for photo-controlled smart devices and bio-sensors.

Date: 2024
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DOI: 10.1038/s41467-024-48405-y

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