The key to functionalize of engineered molecularly nanometer thick films lies in the ability to reproducibly control their structure. A number of factors influence the film morphology of self-assembled films on solid or liquid surfaces, such as the structure of the molecules/particles, wetting, solvent hydrodynamics, and evaporation. An important example is the deposition of amphiphilic molecules from a volatile solution, self-assembled onto a water surface at monolayer coverage. Upon evaporation, a myriad of microscopic two-dimensional (2D) crystallites forms a ruptured film lying in random orientation on the surface, resulting in “2D powders.” Here we present a general technique, employing linearly polarized laser pulses and varying solvent composition to influence the assembly of molecules such as poly-benzyl-L-glutamate and alamethicin on water surfaces, resulting in ultrathin molecular films with aligned regions that point in the same direction, though macroscopically separated. The experimental results are tentatively explained by a mechanism that is based on excluded volume forces and “kick model” for the effect of laser pulses to induce molecular rotation that eventually results in an aligned pattern when the system is at a collective state.

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