Multiferroic domain walls in functional oxides exhibit properties distinct from the bulk and are increasingly exploited as active elements in nanoelectronic and photonic devices. Deterministic control of domain populations has typically remained limited to local control, or removal with temperature. Here we demonstrate continuous, reversible manipulation of the ferroelastic domain structure in single-crystal LaAlO3 using in-situ uniaxial strain. Combining atomic force microscopy, X-ray diffraction, and Raman spectroscopy with first-principles calculations we map the complete microscopic evolution of the twin domain population through the strain-driven transition from the rhombohedral R3ˉc ground state toward the predicted orthorhombic Fmmm phase. Applied strains below 0.5% produce pronounced surface flattening and large-scale domain reorganisation, establishing uniaxial strain as a technically accessible control parameter for ferroelastic domain engineering. These results open a route to active, real-time programming of domain architectures in LaAlO3-based heterostructures, with implications for strain-tunable superconducting interfaces, nanoscale phonon-polariton optics, and ultrafast lattice control.
@article{arxiv.2604.28183,
title = {Uniaxial strain-driven ferroelastic domain control in LaAlO3},
author = {Matthias Roeper and Robin Buschbeck and Jakob Wetzel and Tobias Ritschel and Anna-Lena Hofmann and Vladyslav Kovtunovych and Mike N. Pionteck and Javier Taboada-Gutiérrez and Alexey B. Kuzmenko and Martina Basini and Vivek Unikandanunni and Iuliia Kiseleva and Jochen Geck and Susanne C. Kehr and Maximilian Lederer and Simone Sanna and Lukas M. Eng and Samuel D. Seddon},
journal= {arXiv preprint arXiv:2604.28183},
year = {2026}
}