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Laser-induced nonthermal melting in semiconductors has been studied over thelast four decades, but the underlying mechanism is still under debate. Here, byutilizing an advanced real-time time-dependent density functional theorysimulation, we reveal that the photoexcitation-induced ultrafast nonthermalmelting in silicon occurs via homogeneous nucleation with random seedsoriginating from a self-amplified local dynamic instability at the photoexcitedstates rather than by simultaneously breaking of all bonds, as suggested by theinertial model, phonon instability, or Coulombic repulsion mechanisms. Due tothis local dynamic instability, any initial small random thermal displacementsof atoms can be amplified by a charge transfer of photoexcited carriers, whichin turn creates a local self-trapping center for the excited carriers andyields the random nucleation seeds. This finding provides fresh insights intophotoinduced ultrafast nonthermal melting.

The seeds and homogeneous nucleation of photoinduced nonthermal melting in semiconductors due to self-amplified local dynamic instability