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Adv Mater ; 33(41): e2102721, 2021 Oct.
Article in English | MEDLINE | ID: mdl-34427368

ABSTRACT

The sub-picosecond response of amorphous germanium telluride thin film to a femtosecond laser excitation is investigated using frequency-domain interferometry and ab initio molecular dynamics. The time-resolved measurement of the surface dynamics reveals a shrinkage of the film with a dielectric properties' response faster than 300 fs. The systematic ab initio molecular dynamics simulations in non-equilibrium conditions allow the atomic configurations to be retrieved for ionic temperature from 300 to 1100 K and width of the electron distribution from 0.001 to 1.0 eV. Local order of the structures is characterized by in-depth analysis of the angle distribution, phonon modes, and pair distribution function, which evidence a transition toward a new amorphous electronic excited state close in bonding/structure to the liquid state. The results shed a new light on the optically highly excited states in chalcogenide materials involved in both important processes: phase-change materials in memory devices and ovonic threshold switching phenomenon induced by a static field.

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