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Subject: Epitaxial ferroelectric ×

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    Origin of Terahertz Soft-Mode Nonlinearities in Ferroelectric Perovskites
    (College Park, Md. : APS, 2021) Pal, Shovon; Strkalj, Nives; Yang, Chia-Jung; Weber, Mads C.; Trassin, Morgan; Woerner, Michael; Fiebig, Manfred
    Soft modes are intimately linked to structural instabilities and are key for the understanding of phase transitions. The soft modes in ferroelectrics, for example, map directly the polar order parameter of a crystal lattice. Driving these modes into the nonlinear, frequency-changing regime with intense terahertz (THz) light fields is an efficient way to alter the lattice and, with it, the physical properties. However, recent studies show that the THz electric-field amplitudes triggering a nonlinear soft-mode response are surprisingly low, which raises the question on the microscopic picture behind the origin of this nonlinear response. Here, we use linear and two-dimensional terahertz (2D THz) spectroscopy to unravel the origin of the soft-mode nonlinearities in a strain-engineered epitaxial ferroelectric SrTiO3 thin film. We find that the linear dielectric function of this mode is quantitatively incompatible with pure ionic or pure electronic motions. Instead, 2D THz spectroscopy reveals a pronounced coupling of electronic and ionic-displacement dipoles. Hence, the soft mode is a hybrid mode of lattice (ionic) motions and electronic interband transitions. We confirm this conclusion with model calculations based on a simplified pseudopotential concept of the electronic band structure. It reveals that the entire THz nonlinearity is caused by the off-resonant nonlinear response of the electronic interband transitions of the lattice-electronic hybrid mode. With this work, we provide fundamental insights into the microscopic processes that govern the softness that any material assumes near a ferroic phase transition. This knowledge will allow us to gain an efficient all-optical control over the associated large nonlinear effects.
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    Huge impact of compressive strain on phase transition temperatures in epitaxial ferroelectric KxNa1-xNbO3 thin films
    (Melville, NY : American Inst. of Physics, 2019) Von Helden, L.; Bogula, L.; Janolin, P.-E.; Hanke, M.; Breuer, T.; Schmidbauer, M.; Ganschow, S.; Schwarzkopf, J.
    We present a study in which ferroelectric phase transition temperatures in epitaxial KxNa1-xNbO3 films are altered systematically by choosing different (110)-oriented rare-earth scandate substrates and by variation of the potassium to sodium ratio. Our results prove the capability to continuously shift the ferroelectric-to-ferroelectric transition from the monoclinic MC to orthorhombic c-phase by about 400 °C via the application of anisotropic compressive strain. The phase transition was investigated in detail by monitoring the temperature dependence of ferroelectric domain patterns using piezoresponse force microscopy and upon analyzing structural changes by means of high resolution X-ray diffraction including X-ray reciprocal space mapping. Moreover, the temperature evolution of the effective piezoelectric coefficient d33,f was determined using double beam laser interferometry, which exhibits a significant dependence on the particular ferroelectric phase. © 2019 Author(s).