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The objective of the study was to establish the direct relationship between melt pool fluid dynamics and the homogeneity of resultant microstructures produced with laser surface processing of alloys. Melt pool modeling studies indicate that surface tension driven flow is essential for obtaining homogenized microstructures at high laser scanning rates. Theoretical and experimental maps have been constructed to compare the length scales of melting and alloying obtained with a variety of processing conditions. Experimental surface-treatments of a variety of pure metals and multi-component alloys have been conducted with a 10 kW continuous wave CO2 laser. The quality of resultant alloy microstructures was influenced by both laser parameters and material properties. The most promising applications appear to be in applying refractory metal alloys to low temperature alloy substrates for corrosion, erosion, and wear applications.