Using the dynamic transmission electron microscope (DTEM), the dewetting of thin nickel films was monitored at nanometer spatial and nanosecond timescales to provide insight into the liquidphase assembly dynamics. Correlated time and length scales indicate that a spinodal instability drives the assembly process. Measured lifetimes of the liquid metal agree with finite-element simulations of the laser-irradiated film. These results can be used to design improved synthesis and assembly routes toward achieving advanced functional nanomaterials and devices. Keywords assembly dynamics, dynamic transmission electron microscopy, pulsed-laser heating, thin-film dewetting
LetterThe synthesis and organization of functional nanomaterials via bottom-up self-and directed assembly represents a critical challenge for the future of nanoscience. Generating arrays of nanoparticles with controlled size and spatial distributions is key to this challenge, and processes that exploit morphological instabilities offer the potential to attain these fine-scale spatially correlated structures. There has been long-standing interest in the capillarity and surface tension effects on morphological evolution in various materials systems, dating back to the work of Plateau 1 and Rayleigh 2 . Recently, pulsed-laser-induced dewetting of two-dimensional films 3-9 , one-dimensional lines and rings [10][11][12][13] , and lithographically patterned nanostructures 14,15 has demonstrated that understanding and controlling thin-film and Rayleigh-Plateau instabilities improves the ability to create organized metallic nanoparticle ensembles. Assembled particles have also been shown to "jump" or eject from one substrate and transfer to another depending on the energetics and dynamics of various laser-melted nanostructures [16][17][18] . Heretofore, the as described in the Methods section, the laser spot has a Gaussian profile and thus the radial profile of each image also contains thermal and temporal information. Figure 2d) shows an image taken long after a laser pulse to show the resultant nanoparticle structure in the same field of view. The images in Figure 2 were filtered to remove noise and irrelevant intensity variations using a 3x3 median filter followed by a local brightness and contrast equalization filter using a Gaussian kernel with an rms width of 33 pixels in the x-and y-directions. The raw images are provided in the Supporting Information.Dynamic selected-area diffraction (SAD) patterns were recorded as a function of time to complement the dynamic imaging and estimate the nickel liquid lifetime. Figure 3a) shows a series of SAD patterns taken at various times relative to the specimen pump laser's interaction with the specimen (including as-deposited and post-laser-pulse diffraction patterns using a long exposure time). The simulated diffraction pattern for polycrystalline nickel is included in the long-exposure as-deposited diffraction pattern. The conventional diffraction pattern from the asdeposited film shows broad diffraction ri...