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Phase evolution induced by single or repeated excitation with energetic femtosecond laser pulses is examined. Of primary interest is the solidification behavior of pure metals at deep undercoolings and self-organization in simple eutectic alloys. Time resolved measurements using third harmonic generation (THG) of light and ultrafast electron diffraction (UED) are employed to elucidate several issues related to fast laser excitation, including heat transport by ballistic and diffusional electrons through multilayer films, the dependence of crystallization velocities on materials properties, mechanisms controlling the transport of heat away from the crystal-liquid interface, and the possibility for quenching pure metals, such as Cu, Ni, and Fe, into the amorphous state. Special samples designed to maximize the quenching speed are developed. The properties of such pure metallic glasses, such as glass and crystallization temperatures, will be measured, if such samples are successfully produced. The measurements are complemented by molecular dynamics computer simulations of the solidification process. The second interest of this research is mesoscopic, self-organization of materials under repeated laser melting, with diffusional relaxation between pulses. We select binary alloys that are immiscible in the solid state but miscible in the liquid state, such as Ag-Cu. Femtosecond laser irradiation is employed to induce meltingmore » and to vary the melting time over a wide range, from a few ps to hundreds of ps. This enables us to perform critical experimental tests of key theoretical predictions self-organization in alloys under external forcing, in particular the existence of a threshold value of the forced mixing length for patterning to take place.« less