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Register a new userIntrinsic ionic screening of the ferroelectric polarization of KTP
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Mobile charges and lattice polarization interact in ferroelectric materials because of the Coulomb interaction between the mobile free charges and the fixed lattice dipoles. We have investigated this mutual screening in KTiOPO4, a ferroelectric/superionic single crystal in which the mobile charges are K+ ions. The ionic accumulation close to the crystal surfaces leads to orders of magnitude increase of the Second Harmonic Generation. This ionic space charge model is supported by the absence of such an effect in non-ionic conductor but ferroelectric BaTiO3, by its temperature dependence in KTiOPO4 and by its broad depletion at domain walls.
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Ferroelectrics that are also ionic conductors offer possibilities for novel applications with high tunability, especially if the same atomic species causes both phenomena. In particular, at temperatures just below the Curie temperature, polarized states may be sustainable as the mobile species is driven in a controlled way over the energy barrier that governs ionic conduction, resulting in unique control of the polarization. This possibility was recently demonstrated in CuInP2S6, a layered ferroelectric ionic conductor in which Cu ions cause both ferroelectricity and ionic conduction. Here, we show that the commonly used approach to calculate the polarization of evolving atomic configurations in ferroelectrics using the modern theory of polarization, namely concerted (synchronous) migration of the displacing ions, is not well suited to describe the polarization evolution as the Cu ions cross the van der Waals gaps. We introduce an asynchronous Cu-migration scheme, which reflects the physical process by which Cu ions migrate, resolves the difficulties, and describes the polarization evolution both for normal ferroelectric switching and for transitions across the van der Waals gaps, providing a single framework to discuss ferroelectric ionic conductors.
The effect of a variety of intrinsic defects and defect clusters in bulk and thin films of SrTiO$_3$ on ferroelectric polarization and switching mechanism is investigated by means of density-functional-theory (DFT) based calculations and the Berry phase approach. Our results show that both the titanium Ti$_mathrm{Sr}^{bullet bullet}$ and strontium Sr$_mathrm{Ti}^{}$ antisite defects induce ferroelectric polarization in SrTiO$_3$, with the Ti$_mathrm{Sr}^{bullet bullet}$ defect causing a more pronounced spontaneous polarization and higher activation barriers of polarization reversal than Sr$_mathrm{Ti}^{}$. The presence of oxygen vacancies bound to the antisite defects can either enhance or diminish polarization depending on the configuration of the defect pair, but it always leads to larger activation barriers of polarization switching as compared to the antisite defects with no oxygen vacancies. We also show that the magnitude of spontaneous polarization in SrTiO$_3$ can be tuned by controlling the degree of Sr/Ti nonstroichiometry. Other intrinsic point defects such as Frenkel defect pairs and electron small polarons also contribute to the emergence of ferroelectric polarization in SrTiO$_{3}$.
Tunnel devices based on ferroelectric Hf0.5Zr0.5O2 (HZO) barriers hold great promises for emerging data storage and computing technologies. The resistance state of the device can be changed by a suitable writing voltage. However, the microscopic mechanisms leading to the resistance change are an intricate interplay between ferroelectric polarization controlled barrier properties and defect-related transport mechanisms. Here is shown the fundamental role of the microstructure of HZO films setting the balance between those contributions. The oxide film presents coherent or incoherent grain boundaries, associated to the existence of monoclinic and orthorhombic phases in HZO films, which are dictated by the mismatch with the substrates for epitaxial growth. These grain boundaries are the toggle that allows to obtain either large (up to 450 %) and fully reversible genuine polarization controlled electroresistance when only the orthorhombic phase is present or an irreversible and extremely large (1000-100000 %) electroresistance when both phases coexist.
We measured the intrinsic hysteretic polarization in lossy improper and nanoferroelectric systems where the nonhysteretic polarization and leakage are large and the relaxation takes place over a broader time scale. We used different measurement protocols such as standard single triangular voltage pulse, a pulse train of PUND (Positive Up Negative Down), and an even more complicated pulse train of fourteen voltage pulses and compared the results obtained. We show that a protocol which sends a train of fourteen pulses is more appropriate for extracting relaxed (i.e., time scale independent) and intrinsic remanent polarization for these samples. We also point out that it is possible to select and design an appropriate measurement protocol depending on the magnitude of polarization and leakage of the system.
The ability to manipulate ferroelectrics at ultrafast speeds has long been an elusive target for materials research. Coherently exciting the ferroelectric mode with ultrashort optical pulses holds the promise to switch the ferroelectric polarization on femtosecond timescale, two orders of magnitude faster compared to what is possible today with pulsed electric fields. Here, we report on the demonstration of ultrafast optical reversal of the ferroelectric polarization in LiNbO3. Rather than driving the ferroelectric mode directly, we couple to it indirectly by resonant excitation of an auxiliary high-frequency phonon mode with femtosecond mid-infrared pulses. Due to strong anharmonic coupling between these modes, the atoms are directionally displaced along the ferroelectric mode and the polarization is transiently reversed, as revealed by time-resolved, phase-sensitive second-harmonic generation. This reversal can be induced in both directions, a key pre-requisite for practical applications.
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