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Autori principali: Li, Denan, Ni, Haofei, Zhang, Yi, Liu, Shi
Natura: Preprint
Pubblicazione: 2025
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Accesso online:https://arxiv.org/abs/2507.15687
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author Li, Denan
Ni, Haofei
Zhang, Yi
Liu, Shi
author_facet Li, Denan
Ni, Haofei
Zhang, Yi
Liu, Shi
contents Organic--inorganic hybrid perovskites with giant piezoelectric responses, exemplified by TMCM-CdCl$_3$, represent a promising platform for flexible and environmentally friendly electromechanical materials. However, the microscopic origin of such exceptional performance in this weakly polar system has remained elusive. Here, using deep-learning-assisted large-scale molecular dynamics simulations, we resolve this paradox by reproducing the experimentally measured piezoelectric coefficient $d_{33} \approx 220$~pC/N, and demonstrating that the giant response arises from the collective contribution of multiple intrinsic components, particularly the shear component $d_{15}$. This effect does not stem from conventional polarization rotation or phase switching, but instead originates from stochastic 120$^\circ$ in-plane rotational hopping of a small fraction of organic cations. This discrete hopping mechanism is governed by the local C$_3$-symmetric halogen-bonding network between the host framework and the guest cation. The Arrhenius-type temperature dependence of $d_{15}$ further confirms the role of thermally activated dipole hopping. This work provides a clear pathway to enhance piezoelectric performance of hybrid materials through rational engineering of host--guest interactions.
format Preprint
id arxiv_https___arxiv_org_abs_2507_15687
institution arXiv
publishDate 2025
record_format arxiv
spellingShingle Giant Reversible Piezoelectricity from Symmetry-Governed Stochastic Dipole Hopping
Li, Denan
Ni, Haofei
Zhang, Yi
Liu, Shi
Materials Science
Organic--inorganic hybrid perovskites with giant piezoelectric responses, exemplified by TMCM-CdCl$_3$, represent a promising platform for flexible and environmentally friendly electromechanical materials. However, the microscopic origin of such exceptional performance in this weakly polar system has remained elusive. Here, using deep-learning-assisted large-scale molecular dynamics simulations, we resolve this paradox by reproducing the experimentally measured piezoelectric coefficient $d_{33} \approx 220$~pC/N, and demonstrating that the giant response arises from the collective contribution of multiple intrinsic components, particularly the shear component $d_{15}$. This effect does not stem from conventional polarization rotation or phase switching, but instead originates from stochastic 120$^\circ$ in-plane rotational hopping of a small fraction of organic cations. This discrete hopping mechanism is governed by the local C$_3$-symmetric halogen-bonding network between the host framework and the guest cation. The Arrhenius-type temperature dependence of $d_{15}$ further confirms the role of thermally activated dipole hopping. This work provides a clear pathway to enhance piezoelectric performance of hybrid materials through rational engineering of host--guest interactions.
title Giant Reversible Piezoelectricity from Symmetry-Governed Stochastic Dipole Hopping
topic Materials Science
url https://arxiv.org/abs/2507.15687