<p>  </p> <p>The investigation of laser-matter interactions has gained interest over the years due to the importance of these interactions in materials synthesis, diagnostics, electronics, and photonics. In-situ transmission electron microscopy (TEM) techniques are invaluable for real-time monitoring of dynamic processes in these systems at the nanoscale. In this work, the effect of pulsed laser heating on the reactions of energetic materials, plasmonic structures, and multilayer thin films has been studied by utilizing ultrafast transmission electron microscopy (UTEM) techniques. Heat transfer and electric field calculations have been carried out to compare and support the experimental findings. </p> <p>The photothermal reaction of an aluminum-fluoropolymer composite is studied to show the effect of pulsed laser heating on reactions of reactive materials. An aluminum nanoparticle - THV (terpolymer of tetrafluoroethylene, hexafluoropropylene, and vinylidene fluoride) sample is subjected to rapid heating and cooling cycles by employing the integrated laser system of an UTEM. TEM images and real-time movies (30 frame/s) are acquired to reveal the changes during the reaction. Heat transfer simulations proved that the temperature of the sample was high enough to trigger the decomposition of THV and start its reaction with Al nanoparticles. Electron diffraction patterns revealed that the reaction product was the rare and metastable η-phase aluminum fluoride (AlF3). The experimental and theoretical results showed that rapid pulsed laser heating and subsequent cooling of a nanoscale sample influences the phases that can form and be utilized to investigate other systems.</p> <p>Pulsed laser-assisted merging and alloying of noble metals are also studied to explore the fabrication of beaded gold-silver nanowires with a variety of morphology and composition. In-situ laser heating of plasmonic silver nanowire (Ag NW) - gold nanoparticle (Au NP) couples are performed inside an UTEM, and direct visualization of the evolution process gives insights into the formation mechanism. Experimental results show that silver melts at the surface to bridge the nanometer-sized gap between the NP and the NW, forming a cup-like morphology underneath the Au NP via capillary action. Progressive laser irradiation leads to wetting of the Au NP and the formation of a valley in the Ag NW around the NP, which flattens gradually by partial embedding of the NP. Inter-diffusion of Au into Ag and vice versa sets in at this stage, leading to depletion of Au from the Au-rich NP region. Prolonged irradiation and heating lead to gradual inter-mixing of Au-Ag, forming a beaded Au-doped Ag nanowire with homogeneous composition. Such a step-by-step understanding of the merging and alloying process has implications in nanowelding, which holds a future in designing efficient, transparent conductors and printed electronics. Numerical simulations are performed to calculate the electromagnetic enhancement at the interface of adjacent NPs and NWs and provide information on heat generation rates in NP-NW couples at the early stages of the nanowelding process. </p> <p>In the third chapter, laser-induced irreversible dynamics in electron beam sensitive organic energetic crystals and ultrathin multilayer films are studied by single-shot UTEM imaging. After various sample preparation methods are developed and compared for the well-controlled synthesis of nanoscale ammonium perchlorate samples on TEM grids, decomposition dynamics of ammonium perchlorate crystals are captured via single-shot imaging. The experimental data showed that the sublimation and decomposition are visible ~30 ns after the sample excitation laser in crystals smaller than 5 µm. Dependency of decomposition to crystal porosity and thickness is also observed with crack formation in some cases. In the following section, pulsed-laser irradiation is utilized to realize deformation in thin multilayer films under high temperatures, and triggered dynamic processes are investigated through single-shot imaging. Laser-assisted periodic wrinkle formation is demonstrated on SiN membranes coated with Ti/Ni bilayers. The resulting structures showed periodic wrinkling of the SiN membrane and corrugated surface formation on both sides of the film. Overall, the dissertation highlights the potential of ultrafast transmission electron microscopy in discovering fundamental processes related to, but not limited to, reactive materials, plasmonic nanomaterials, and ultrathin multilayer films. </p>