Electronic Excitation‐Driven β‐Ga 2 O 3 Metastability Transformation and Self‐Organization Mechanism: β→κ/γ/δ Phases

Irradiation-driven multiphase self-organization presents emergent opportunities for the customization of nanoscale engineering properties, dynamically tuning strain-field distributions and interfacial electronic structures. Responding to intense electronic excitation-induced energy deposition, the dominant phase transformations, with varying Gibbs free energy Δ G f o $\Delta \ G_f^o$ , are confirmed as β → κ → γ → δ that are located in specific microregions for Gallium (III) oxide (Ga₂O₃), as follows: (i) Surface-localized interstitial accumulation under compressive stress triggers β → δ via semi-coherent interface formation. (ii) Tensile stress within latent tracks drives vacancy-mediated oxygen layer truncation (4/12 periodicity along ⟨0001⟩), stabilizing coherent 4H (ABCB) κ and 3C (ABC) β (ABC) interfaces through strain-compensated octahedral distortion. (iii) Screw dislocation-mediated lattice relaxation induces β → γ via cation disordering (Ga³⁺ occupancy at β-interstitial sites), forming metastable spinel γ with mixed occupancy across 16d/8a Wyckoff sites. Irradiation-driven β-Ga₂O₃→κ/γ/δ transitions, as mechanistically revealed via inelastic thermal spike (i-TS) calculations and molecular dynamics simulations, induce defect-mediated nonlinear photoresponse, critical for optoelectronic engineering.