“…Two-photon absorption (2PA), an instantaneous χ (3) optical nonlinear process, has potential applications in microfabrication, , optical data storage, optical limiting, microscopic imaging, and upconverted emission for laser applications. − The search for large 2PA materials spans from bulk solid-state materials (e.g., semiconductors), to engineered nanostructured materials (e.g., semiconductor quantum dots), and to organic molecules. , Organic molecules possess the advantage of greater degrees of freedom in custom material design and fabrication. With the capability to enhance nonlinear optical properties by directional modification of their molecular structures, cyanine-like dyes exhibit a linear extended π-conjugated system with π-electrons delocalized along the molecular backbone.…”