Optically Induced Multistage Phase Transition in Coherent Phonon-Dominated a-GeTe

Abstract

Ultrafast photoexcitation can decouple the multilevel nonequilibrium dynamics of electron–lattice interactions, providing an ideal probe for dissecting photoinduced phase transition in solids. Here, real-time time-dependent density functional theory simulations combined with occupation-constrained DFT methods are employed to explore the nonadiabatic paths of optically excited a-GeTe. Results show that the short-wavelength ultrafast laser is capable of generating full-domain carrier excitation and repopulation, whereas the long-wavelength ultrafast laser favors the excitation of lone pair electrons in the antibonded state. Photodoping makes the double-valley potential energy surface shallower and allows the insertion of A1g coherent forces in the atomic pairs, by which the phase reversal of Ge and Te atoms in the ⟨001⟩ direction is activated with ultrafast suppression of the Peierls distortion. These findings have far-reaching implications regarding nonequilibrium phase engineering strategies based on phase-change materials.

Phase transition in WSe2−xTex monolayers driven by charge injection and pressure: a first-principles study

“…Controlling the stability of multi-phase structures with unique properties can be applied to monolayer phase engineering, phase-change memory and other technical fields. 5–9 One of the most explored systems is group VI TMDs, whose molecular formula can be expressed as MX 2 (M = Mo or W, X = S, Se or Te). Polymorphic TMDs include the trigonal prismatic phase (H), the orthorhombic phase (Td) and the octahedral phase (T), while the unstable T phase tends more readily to the distorted octahedral phase (T′).…”