Hybrid organic electro-optic (OEO) devices consist of a layer of ordered organic chromophores confined between layers of metals or semiconductors, enabling optical fields to be tightly confined within the OEO material. The combination of tight confinement with the high electro-optic (EO) performance of state-of-the art OEO materials enables exceptional electro-optic switching performance in silicon-organic hybrid (SOH) and plasmonic-organic hybrid (POH) device architectures. Recent records in POH devices include bandwidths < 500 GHz and energy efficiency < 100 aJ/bit. However, optimization of device performance requires both understanding and improving the degree to which chromophores can be acentrically ordered near a metal or semiconductor interface. Applying bulk and/or isotropic models of OEO materials to nanophotonic device architectures often lead to overly optimistic translation of materials performance to device performance. Prior work has identified influences of high centrosymmetric order (birefringence), altered relations between acentric and centrosymmetric order (dimensionality), and surface electrostatics on chromophore ordering. We combine these models into a representation that can be used to understand the influences of these phenomena on device performance, how some prior OEO materials exhibited unusually high performance under confinement, how ordering close to surfaces may be improved, and implications for future electro-optic device design.
Standard models for evaluating the electro-optic (EO) response of organic materials typically assume that the refractive index of the material in the absence of a RF modulation field is isotropic and homogeneous. Such assumptions work very well for low-concentration guest-host materials in bulk devices. However, current generation organic EO materials at high densities and under nanoscale confinement can show sufficient birefringence to affect device performance. We use computer simulations and spectroscopic experiments to characterize and predict changes in the index of refraction under poling. We also demonstrate that poling-induced birefringence can lead to a non-linear relationship between the apparent EO coefficient and poling field strength.
Multi-scale (correlated quantum and statistical mechanics) modeling methods have been advanced and employed to guide the improvement of organic electro-optic (OEO) materials, including by analyzing electric field poling induced electro-optic activity in nanoscopic plasmonic-organic hybrid (POH) waveguide devices. The analysis of in-device electro-optic activity emphasizes the importance of considering both the details of intermolecular interactions within organic electro-optic materials and interactions at interfaces between OEO materials and device architectures. Dramatic improvement in electro-optic device performance--including voltage-length performance, bandwidth, energy efficiency, and lower optical losses have been realized. These improvements are critical to applications in telecommunications, computing, sensor technology, and metrology. Multi-scale modeling methods illustrate the complexity of improving the electro-optic activity of organic materials, including the necessity of considering the trade-off between improving poling-induced acentric order through chromophore modification and the reduction of chromophore number density associated with such modification. Computational simulations also emphasize the importance of developing chromophore modifications that serve multiple purposes including matrix hardening for enhanced thermal and photochemical stability, control of matrix dimensionality, influence on material viscoelasticity, improvement of chromophore molecular hyperpolarizability, control of material dielectric permittivity and index of refraction properties, and control of material conductance. Consideration of new device architectures is critical to the implementation of chipscale integration of electronics and photonics and achieving the high bandwidths for applications such as next generation (e.g., 5G) telecommunications.
Taken together, theory-guided nano-engineering of organic electro-optic materials and hybrid device architectures have permitted dramatic improvement of the performance of electro-optic devices. For example, the voltage-length product has been improved by nearly a factor of 104 , bandwidths have been extended to nearly 200 GHz, device footprints reduced to less than 200 μm2 , and femtojoule energy efficiency achieved. This presentation discusses the utilization of new coarse-grained theoretical methods and advanced quantum mechanical methods to quantitatively simulate the physical properties of new classes of organic electro-optic materials and to evaluate their performance in nanoscopic device architectures, accounting for the effect on chromophore ordering at interfaces in nanoscopic waveguides.
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