The performance of electro-optic devices based on organic second order NLO materials has been improved by orders of magnitude through theory-guided improvement in the electrooptic activity and other relevant properties of organic materials and by field compression of radio frequency (RF) and optical fields associated with the transition from microscale/mesoscale devices to silicon−organic hybrid (SOH) and plasmonic−organic hybrid (POH) devices with nanoscopic dimensions. This paradigm shift in organic electro-optic R&D has led to many performance improvements, including record performance for voltage-length performance of less than 50 V-μm, energy consumption of less than 70 attojoules/bit, bandwidths of greater than 500 gigahertz (GHz), and device footprints of less than 20 μm 2 . Another consequence of improving electro-optic performance is the corresponding improvement of the converse second order nonlinear optical property of optical rectification (transparent photodetection). Theory has permitted identification of optimum optical nonlinearity/transparency values and dipole moments for newly developed chromophores, which have led, in turn, to state-of-the-art materials and device performance.