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This work presents the first atomic scale evidence for ferroelectric polarization inversion on the unit cell level in a wurtzite-type material based on epitaxial Al0.75Sc0.25N thin films. The electric field induced formation of Al-polar inversion domains in the originally N-polar film is unambiguously determined by atomic resolution imaging using aberration-corrected scanning transmission electron microscopy (STEM). Anisotropic etching supports STEM results confirming a complete and homogenous polarization inversion at the film surface for the switched regions and the virtual absence of previous inversion domains in as-deposited regions. Local evidence of residual N-polar domains at the bottom electrode interface is observed and can be explained by both stress gradients and electric field deflection. The epitaxial relationship of the sapphire/AlN/Mo/AlScN multilayer stack is discussed in detail. Selected-area electron diffraction experiments and XRD pole figures reveal a Pitsch–Schrader type orientation relation between the Mo electrode and the AlScN film.

Ferroelectric switching is unambiguously demonstrated for the first time in a III-V semiconductor based material: Al1-xScxN-A discovery which could help to satisfy the urgent demand for thin film ferroelectrics with high performance and good technological compatibility with generic semiconductor technology which arises from a multitude of memory, micro/nano-actuator, and emerging applications based on controlling electrical polarization. The appearance of ferroelectricity in Al1-xScxN can be related to the continuous distortion of the original wurtzite-type crystal structure towards a layered-hexagonal structure with increasing Sc content and tensile strain, which is expected to be extendable to other III-nitride based solid solutions. Coercive fields which are systematically adjustable by more than 3 MV/cm, high remnant polarizations in excess of 100 mC/cm2-which constitute the first experimental estimate of the previously inaccessible spontaneous polarization in a III-nitride based material, an almost ideally square-like hysteresis resulting in excellent piezoelectric linearity over a wide strain interval from −0.3% to + 0.4% and a paraelectric transition temperature in excess of 600 °C are confirmed. This intriguing combination of properties is to our knowledge as of now unprecedented in the field of polycrystalline ferroelectric thin films and promises to significantly advance the commencing integration of ferroelectric functionality to micro- and nanotechnology, while at the same time providing substantial insight to one of the central open questions of the III-nitride semiconductors-that of their spontaneous polarization.

Enhancing the piezoelectric activity of AlN by partially substituting Al with Sc to form Al1-xScxN is a promising approach to improve the performance of piezoelectric micro-electromechanical systems. Here, we present evidence of an instability in the morphology of Al1-xScxN, which originates at, or close to, the substrate/Al1-xScxN interface and becomes more pronounced as the Sc content is increased. Based on Transmission electron microscopy, piezoresponse force microscopy, X-ray diffraction, and SEM analysis, it is identified to be the incipient formation of (100) oriented grains. Approaches to successfully reestablish exclusive c-axis orientation up to x = 0.43 are revealed, with electrode pre-treatment and cathode-substrate distance found to exert significant influence. This allows us to present first measurements of the transversal thin film piezoelectric coefficient e(31,f) and dielectric loss tangent tan delta beyond x = 0.3.

The real structure and morphology of piezoelectric aluminum nitride (AlN) thin films as essential components of magnetoelectric sensors are investigated via advanced transmission electron microscopy methods. State of the art electron diffraction techniques, including precession electron diffraction and automated crystal orientation mapping (ACOM), indicate a columnar growth of the AlN grains optimized for piezoelectric application with a {0 0 0 1} texture. Comparing ACOM with piezoresponse force microscopy measurements, a visual correlation of the structure and the piezoelectric properties is enabled. With a quantitative analysis of the ACOM measurements, a statistical evaluation of grain rotations is performed, indicating the presence of coincidence site lattices with Sigma 7, Sigma 13a, Sigma 13b, Sigma 25. Using a geometric phase analysis on high resolution micrographs, the occurrence of strain is detected almost exclusively at the grain boundaries. Moreover, high resolution imaging was applied for solving the atomic structure at stacking mismatch boundaries with a displacement vector of 1/2 < 1 0 - 1 1 >. All real structural features can be interpreted via simulations based on crystallographic computing in terms of a supercell approach.