Percolation-driven $\beta$ -relaxation enables resonant acceleration of crystallization in amorphous phase-change materials

TL;DR

This paper reveals that crystallization in amorphous phase-change materials is governed by percolation of mobile atomic networks linked to $eta$-relaxation, and demonstrates that ultrasonic excitation at specific frequencies can accelerate this process.

Contribution

It introduces a microscopic picture connecting $eta$-relaxation, atomic percolation, and crystallization, and shows how targeted ultrasonic excitation can modulate phase-change kinetics.

Findings

Percolation transition distinguishes nucleation mechanisms.

Ultrasonic excitation accelerates crystallization near $eta$-relaxation frequency.

Resonant excitation enhances atomic mobility and crystallization speed.

Abstract

Amorphous phase-change materials enable fast and reversible switching in optical and electronic devices, yet crystallization kinetics are still controlled primarily through empirical thermal protocols. Here we identify a microscopic picture governing crystallization in the prototypical phase-change material Ge2Sb2Te5, in which crystallization pathways are organized by the percolation of mobile atomic networks associated with $\beta$-relaxation. We show that this percolation transition distinguishes the dominance of diffusion-driven and diffusionless nucleation and growth during crystallization processes. We further demonstrate that frequency-selected ultrasonic excitation, applied in conjunction with heating, accelerates crystallization by enhancing percolation-mediated atomic dynamics. This acceleration is maximized near the $\beta$-relaxation frequency, consistent with resonant excitation of mobile atoms. Our results establish a direct link between glassy relaxation, atomic-scale percolation, and crystallization, and introduce a new route to modulating phase-change kinetics through targeted excitation of fundamental glassy dynamics.