Damage and the Mechanism in PIN–PMN–PT Relaxor Ferroelectric Single Crystals by H ⁺ Ion Implantation Technology for Nanoscale Thin Films

H + ion implantation technology, the cornerstone of the Smart-Cut, plays a vital role in fabricating advanced microelectromechanical systems. This work systematically investigates the damage mechanisms induced by H + ion implantation in Pb(I n 1/2 N b 1/2 )O 3 –Pb(Mg 1/3 Nb 2/3 )O 3 –PbTiO 3 (PIN–PMN–PT) relaxor ferroelectric single crystals for the preparation of nanoscale thin films for high-frequency optoelectronic devices. The adjustment of key ion implantation parameters, such as energy (70 and 100 keV) and fluence (0.5 × 10 17 to 3 × 10 17 ions/cm 2 ), was used to explore the changes in the microstructure and defects within the crystal lattice. The simulation ion implantation range was experimentally verified by time-of-flight secondary ion mass spectrometry (TOF-SIMS), scanning electron microscopy (SEM), and high-resolution transmission electron microscopy (HRTEM), confirming that implantation at 70 and 100 keV resulted in the formation of approximately 200 nm damage layers at 529 and 758 nm, respectively, characterized by lattice defects and dislocations. This work analyzed and established a quantitative correlation between implantation fluence and damage evolution and explored the separation mechanism of thin film blistering caused by hydrogen ion defect aggregation and increased internal pressure and determined the optimal injection conditions, annealing temperature (≥300 °C), and blistering activation energy (2.71 eV). It not only provides a viable pathway for producing high-quality single-crystal films but also significantly expands the applicability of the ion-slicing technique to complex functional oxides.