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Temporal modulation of second harmonic generation in ferroelectrics by a pulsed electric field
Phys. Rev. B 112, 115146 – Published 25 September, 2025
DOI: https://doi.org/10.1103/xsrf-t1hj
Abstract
We revisit the relationship between electric polarization modulation in ferroelectrics induced by a low-frequency pulsed electric field and the corresponding second harmonic intensity modulation . Using nonlinear response theory, we derive their time-domain expressions linear in the pulse amplitude, revealing that not only the electric field but also its time derivative contributes to . Furthermore, even when the time-derivative component is negligible, can be in antiphase with the pulsed field and thus with . These theoretical predictions are further supported by real-time simulations of a model for electronic ferroelectrics. Our results demonstrate that the commonly assumed relation can break down under certain conditions, reflecting the complex-valued and frequency-dependent nature of nonlinear dynamical susceptibilities.
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